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Engineering â€ș Electrical and Electronic Engineering

Advanced Battery Materials and Technologies

Works Count: 72152

Description

This cluster of papers focuses on advances in lithium battery technologies, including topics such as lithium-sulfur batteries, solid-state electrolytes, nanostructured cathodes, high-energy storage, dendrite-free deposition of lithium metal, polymer electrolytes, sulfur hosts for cathodes, ionic conductivity, cathode materials, and electrochemical stability.

Keywords

Lithium-Sulfur Batteries; Solid-State Electrolytes; Nanostructured Cathodes; High-Energy Storage; Dendrite-Free Deposition; Polymer Electrolytes; Sulfur Hosts; Ionic Conductivity; Cathode Materials; Electrochemical Stability

Nanocomposite polymer electrolytes for lithium batteries

1998-07-01
F. Croce , G. B. Appetecchi , L. Persi +1 more

Issues and challenges facing rechargeable lithium batteries

2001-11-01
J. M. Tarascon , Michel Armand

Lithium metal anodes for rechargeable batteries

2013-10-29
Wu Xu , Jiulin Wang , Fei Ding +4 more
Lithium (Li) metal is an ideal anode material for rechargeable batteries due to its extremely high theoretical specific capacity (3860 mA h g−1), low density (0.59 g cm−3) and the 
 Lithium (Li) metal is an ideal anode material for rechargeable batteries due to its extremely high theoretical specific capacity (3860 mA h g−1), low density (0.59 g cm−3) and the lowest negative electrochemical potential (−3.040 V vs. the standard hydrogen electrode). Unfortunately, uncontrollable dendritic Li growth and limited Coulombic efficiency during Li deposition/stripping inherent in these batteries have prevented their practical applications over the past 40 years. With the emergence of post-Li-ion batteries, safe and efficient operation of Li metal anodes has become an enabling technology which may determine the fate of several promising candidates for the next generation energy storage systems, including rechargeable Li–air batteries, Li–S batteries, and Li metal batteries which utilize intercalation compounds as cathodes. In this paper, various factors that affect the morphology and Coulombic efficiency of Li metal anodes have been analyzed. Technologies utilized to characterize the morphology of Li deposition and the results obtained by modelling of Li dendrite growth have also been reviewed. Finally, recent development and urgent need in this field are discussed.

Challenges and Prospects of Lithium–Sulfur Batteries

2012-10-25
Arumugam Manthiram , Yongzhu Fu , Yu‐Sheng Su
Electrical energy storage is one of the most critical needs of 21st century society. Applications that depend on electrical energy storage include portable electronics, electric vehicles, and devices for renewable 
 Electrical energy storage is one of the most critical needs of 21st century society. Applications that depend on electrical energy storage include portable electronics, electric vehicles, and devices for renewable energy storage from solar and wind. Lithium-ion (Li-ion) batteries have the highest energy density among the rechargeable battery chemistries. As a result, Li-ion batteries have proven successful in the portable electronics market and will play a significant role in large-scale energy storage. Over the past two decades, Li-ion batteries based on insertion cathodes have reached a cathode capacity of ∌250 mA h g(-1) and an energy density of ∌800 W h kg(-1), which do not meet the requirement of ∌500 km between charges for all-electric vehicles. With a goal of increasing energy density, researchers are pursuing alternative cathode materials such as sulfur and O2 that can offer capacities that exceed those of conventional insertion cathodes, such as LiCoO2 and LiMn2O4, by an order of magnitude (>1500 mA h g(-1)). Sulfur, one of the most abundant elements on earth, is an electrochemically active material that can accept up to two electrons per atom at ∌2.1 V vs Li/Li(+). As a result, sulfur cathode materials have a high theoretical capacity of 1675 mA h g(-1), and lithium-sulfur (Li-S) batteries have a theoretical energy density of ∌2600 W h kg(-1). Unlike conventional insertion cathode materials, sulfur undergoes a series of compositional and structural changes during cycling, which involve soluble polysulfides and insoluble sulfides. As a result, researchers have struggled with the maintenance of a stable electrode structure, full utilization of the active material, and sufficient cycle life with good system efficiency. Although researchers have made significant progress on rechargeable Li-S batteries in the last decade, these cycle life and efficiency problems prevent their use in commercial cells. To overcome these persistent problems, researchers will need new sulfur composite cathodes with favorable properties and performance and new Li-S cell configurations. In this Account, we first focus on the development of novel composite cathode materials including sulfur-carbon and sulfur-polymer composites, describing the design principles, structure and properties, and electrochemical performances of these new materials. We then cover new cell configurations with carbon interlayers and Li/dissolved polysulfide cells, emphasizing the potential of these approaches to advance capacity retention and system efficiency. Finally, we provide a brief survey of efficient electrolytes. The Account summarizes improvements that could bring Li-S technology closer to mass commercialization.

Nanostructured sulfur cathodes

2013-01-01
Yuan Yang , Guangyuan Zheng , Yi Cui
Rechargeable Li/S batteries have attracted significant attention lately due to their high specific energy and low cost. They are promising candidates for applications, including portable electronics, electric vehicles and grid-level 
 Rechargeable Li/S batteries have attracted significant attention lately due to their high specific energy and low cost. They are promising candidates for applications, including portable electronics, electric vehicles and grid-level energy storage. However, poor cycle life and low power capability are major technical obstacles. Various nanostructured sulfur cathodes have been developed to address these issues, as they provide greater resistance to pulverization, faster reaction kinetics and better trapping of soluble polysulfides. In this review, recent developments on nanostructured sulfur cathodes and mechanisms behind their operation are presented and discussed. Moreover, progress on novel characterization of sulfur cathodes is also summarized, as it has deepened the understanding of sulfur cathodes and will guide further rational design of sulfur electrodes.

A highly ordered nanostructured carbon–sulphur cathode for lithium–sulphur batteries

2009-05-17
Xiulei Ji , Kyu Tae Lee , Linda F. Nazar

A highly efficient polysulfide mediator for lithium–sulfur batteries

2015-01-06
Xiao Liang , Connor J. Hart , Quanquan Pang +3 more
The lithium–sulfur battery is receiving intense interest because its theoretical energy density exceeds that of lithium-ion batteries at much lower cost, but practical applications are still hindered by capacity decay 
 The lithium–sulfur battery is receiving intense interest because its theoretical energy density exceeds that of lithium-ion batteries at much lower cost, but practical applications are still hindered by capacity decay caused by the polysulfide shuttle. Here we report a strategy to entrap polysulfides in the cathode that relies on a chemical process, whereby a host—manganese dioxide nanosheets serve as the prototype—reacts with initially formed lithium polysulfides to form surface-bound intermediates. These function as a redox shuttle to catenate and bind 'higher' polysulfides, and convert them on reduction to insoluble lithium sulfide via disproportionation. The sulfur/manganese dioxide nanosheet composite with 75 wt% sulfur exhibits a reversible capacity of 1,300 mA h g−1 at moderate rates and a fade rate over 2,000 cycles of 0.036%/cycle, among the best reported to date. We furthermore show that this mechanism extends to graphene oxide and suggest it can be employed more widely. The polysulfide shuttle is a major problem leading to capacity decay in lithium–sulfur batteries. Here, the authors show that in-situ-generated thiosulfate species on a manganese oxide nanosheet act as a polysulfide mediator, which effectively prevents polysulfide dissolution, leading to enhanced cyclability.
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Sulphur–TiO2 yolk–shell nanoarchitecture with internal void space for long-cycle lithium–sulphur batteries

2013-01-08
Zhi Wei Seh , Weiyang Li , J. Judy +5 more
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Smaller Sulfur Molecules Promise Better Lithium–Sulfur Batteries

2012-10-26
Sen Xin , Lin Gu , Nahong Zhao +4 more
The lithium-sulfur battery holds a high theoretical energy density, 4-5 times that of today's lithium-ion batteries, yet its applications have been hindered by poor electronic conductivity of the sulfur cathode 
 The lithium-sulfur battery holds a high theoretical energy density, 4-5 times that of today's lithium-ion batteries, yet its applications have been hindered by poor electronic conductivity of the sulfur cathode and, most importantly, the rapid fading of its capacity due to the formation of soluble polysulfide intermediates (Li(2)S(n), n = 4-8). Despite numerous efforts concerning this issue, combatting sulfur loss remains one of the greatest challenges. Here we show that this problem can be effectively diminished by controlling the sulfur as smaller allotropes. Metastable small sulfur molecules of S(2-4) were synthesized in the confined space of a conductive microporous carbon matrix. The confined S(2-4) as a new cathode material can totally avoid the unfavorable transition between the commonly used large S(8) and S(4)(2-). Li-S batteries based on this concept exhibit unprecedented electrochemical behavior with high specific capacity, good cycling stability, and superior rate capability, which promise a practicable battery with high energy density for applications in portable electronics, electric vehicles, and large-scale energy storage systems.

Insertion Electrode Materials for Rechargeable Lithium Batteries

1998-07-01
Martin Winter , JĂŒrgen Besenhard , Michael E. Spahr +1 more
The performance and safety of rechargeable batteries depend strongly on the materials used. Lithium insertion materials suitable for negative and positive insertion electrodes are reviewed. Future trends, such as alternative 
 The performance and safety of rechargeable batteries depend strongly on the materials used. Lithium insertion materials suitable for negative and positive insertion electrodes are reviewed. Future trends, such as alternative materials for achieving higher specific charges—the Figure shows a scheme for reversible lithium storage in a high specific charge carbonaceous material—are discussed.

Polysulfide Shuttle Study in the Li/S Battery System

2004-01-01
Yuriy Mikhaylik , James R. Akridge
This work reports a quantitative analysis of the shuttle phenomenon in Li/S rechargeable batteries. The work encompasses theoretical models of the charge process, charge and discharge capacity, overcharge protection, thermal 
 This work reports a quantitative analysis of the shuttle phenomenon in Li/S rechargeable batteries. The work encompasses theoretical models of the charge process, charge and discharge capacity, overcharge protection, thermal effects, self-discharge, and a comparison of simulated and experimental data. The work focused on the features of polysulfide chemistry and polysulfide interaction with the Li anode, a quantitative description of these phenomena, and their application to the development of a high-energy rechargeable battery. The objective is to present experimental evidence that self-discharge, charge-discharge efficiency, charge profile, and overcharge protection are all facets of the same phenomenon. © 2004 The Electrochemical Society. All rights reserved.
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Determination of the Kinetic Parameters of Mixed‐Conducting Electrodes and Application to the System Li3Sb

1977-10-01
W. Weppner , Robert A. Huggins
An electrochemical galvanostatic intermittent titration technique (GITT) is described which combines both transient and steady‐state measurements to obtain kinetic properties of solid mixed‐conducting electrodes, as well as thermodynamic data. The 
 An electrochemical galvanostatic intermittent titration technique (GITT) is described which combines both transient and steady‐state measurements to obtain kinetic properties of solid mixed‐conducting electrodes, as well as thermodynamic data. The derivation of quantities such as the chemical and component diffusion coefficients, the partial conductivity, the mobility, the thermodynamic enhancement factor, and the parabolic rate constant as a function of stoichiometry is presented. A description of the factors governing the equilibration of composition gradients in such phases is included. The technique is applied to the determination of the kinetic parameters of the compound which has a narrow composition range. For the chemical diffusion coefficient is at 360°C. This value is quite high, due to a large thermodynamic enhancement factor of . The lithium component diffusion coefficient is comparatively small at this composition, . The partial conductivity and electrical mobility of lithium are and , respectively, at the same stoichiometry and temperature. Because of the very large values of the chemical diffusion coefficient and the fact that 3 moles of lithium can react per mole of antimony, this system may be of interest for use in new types of secondary batteries.

Na-ion batteries, recent advances and present challenges to become low cost energy storage systems

2012-01-01
VerĂłnica Palomares , Paula Serras , Irune Villaluenga +3 more
Energy production and storage have become key issues concerning our welfare in daily life. Present challenges for batteries are twofold. In the first place, the increasing demand for powering systems 
 Energy production and storage have become key issues concerning our welfare in daily life. Present challenges for batteries are twofold. In the first place, the increasing demand for powering systems of portable electronic devices and zero-emission vehicles stimulates research towards high energy and high voltage systems. In the second place, low cost batteries are required in order to advance towards smart electric grids that integrate discontinuous energy flow from renewable sources, optimizing the performance of clean energy sources. Na-ion batteries can be the key for the second point, because of the huge availability of sodium, its low price and the similarity of both Li and Na insertion chemistries. In spite of the lower energy density and voltage of Na-ion based technologies, they can be focused on applications where the weight and footprint requirement is less drastic, such as electrical grid storage. Much work has to be done in the field of Na-ion in order to catch up with Li-ion technology. Cathodic and anodic materials must be optimized, and new electrolytes will be the key point for Na-ion success. This review will gather the up-to-date knowledge about Na-ion battery materials, with the aim of providing a wide view of the systems that have already been explored and a starting point for the new research on this battery technology.

A Reversible and Higher-Rate Li-O <sub>2</sub> Battery

2012-07-24
Zhangquan Peng , Stefan A. Freunberger , Yuhui Chen +1 more
The rechargeable nonaqueous lithium-air (Li-O(2)) battery is receiving a great deal of interest because, theoretically, its specific energy far exceeds the best that can be achieved with lithium-ion cells. Operation 
 The rechargeable nonaqueous lithium-air (Li-O(2)) battery is receiving a great deal of interest because, theoretically, its specific energy far exceeds the best that can be achieved with lithium-ion cells. Operation of the rechargeable Li-O(2) battery depends critically on repeated and highly reversible formation/decomposition of lithium peroxide (Li(2)O(2)) at the cathode upon cycling. Here, we show that this process is possible with the use of a dimethyl sulfoxide electrolyte and a porous gold electrode (95% capacity retention from cycles 1 to 100), whereas previously only partial Li(2)O(2) formation/decomposition and limited cycling could occur. Furthermore, we present data indicating that the kinetics of Li(2)O(2) oxidation on charge is approximately 10 times faster than on carbon electrodes.

High rate and stable cycling of lithium metal anode

2015-02-20
Jiangfeng Qian , Wesley A. Henderson , Wu Xu +4 more
Abstract Lithium metal is an ideal battery anode. However, dendrite growth and limited Coulombic efficiency during cycling have prevented its practical application in rechargeable batteries. Herein, we report that the 
 Abstract Lithium metal is an ideal battery anode. However, dendrite growth and limited Coulombic efficiency during cycling have prevented its practical application in rechargeable batteries. Herein, we report that the use of highly concentrated electrolytes composed of ether solvents and the lithium bis(fluorosulfonyl)imide salt enables the high-rate cycling of a lithium metal anode at high Coulombic efficiency (up to 99.1%) without dendrite growth. With 4 M lithium bis(fluorosulfonyl)imide in 1,2-dimethoxyethane as the electrolyte, a lithium|lithium cell can be cycled at 10 mA cm −2 for more than 6,000 cycles, and a copper|lithium cell can be cycled at 4 mA cm −2 for more than 1,000 cycles with an average Coulombic efficiency of 98.4%. These excellent performances can be attributed to the increased solvent coordination and increased availability of lithium ion concentration in the electrolyte. Further development of this electrolyte may enable practical applications for lithium metal anode in rechargeable batteries.
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Mechanisms for Lithium Insertion in Carbonaceous Materials

1995-10-27
J. R. Dahn , Tao Zheng , Yinghu Liu +1 more
Lithium can be inserted reversibly within most carbonaceous materials. The physical mechanism for this insertion depends on the carbon type. Lithium intercalates in layered carbons such as graphite, and it 
 Lithium can be inserted reversibly within most carbonaceous materials. The physical mechanism for this insertion depends on the carbon type. Lithium intercalates in layered carbons such as graphite, and it adsorbs on the surfaces of single carbon layers in nongraphitizable hard carbons. Lithium also appears to reversibly bind near hydrogen atoms in carbonaceous materials containing substantial hydrogen, which are made by heating organic precursors to temperatures near 700°C. Each of these three classes of materials appears suitable for use in advanced lithium batteries.

Graphene-Wrapped Sulfur Particles as a Rechargeable Lithium–Sulfur Battery Cathode Material with High Capacity and Cycling Stability

2011-06-24
Hailiang Wang , Yuan Yang , Yongye Liang +5 more
We report the synthesis of a graphene-sulfur composite material by wrapping polyethyleneglycol (PEG) coated submicron sulfur particles with mildly oxidized graphene oxide sheets decorated by carbon black nanoparticles. The PEG 
 We report the synthesis of a graphene-sulfur composite material by wrapping polyethyleneglycol (PEG) coated submicron sulfur particles with mildly oxidized graphene oxide sheets decorated by carbon black nanoparticles. The PEG and graphene coating layers are important to accommodating volume expansion of the coated sulfur particles during discharge, trapping soluble polysulfide intermediates and rendering the sulfur particles electrically conducting. The resulting graphene-sulfur composite showed high and stable specific capacities up to ~600mAh/g over more than 100 cycles, representing a promising cathode material for rechargeable lithium batteries with high energy density.
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Towards greener and more sustainable batteries for electrical energy storage

2014-11-17
Dominique Larcher , J. M. Tarascon

Advances in Li–S batteries

2010-01-01
Xiulei Ji , Linda F. Nazar
Rechargeable Li–S batteries have received ever-increasing attention recently due to their high theoretical specific energy density, which is 3 to 5 times higher than that of Li ion batteries based 
 Rechargeable Li–S batteries have received ever-increasing attention recently due to their high theoretical specific energy density, which is 3 to 5 times higher than that of Li ion batteries based on intercalation reactions. Li–S batteries may represent a next-generation energy storage system, particularly for large scale applications. The obstacles to realize this high energy density mainly include high internal resistance, self-discharge and rapid capacity fading on cycling. These challenges can be met to a large degree by designing novel sulfur electrodes with "smart" nanostructures. This highlight provides an overview of major developments of positive electrodes based on this concept.

A Polymer Electrolyte‐Based Rechargeable Lithium/Oxygen Battery

1996-01-01
K. M. Abraham , Zong‐Pei Jiang
A novel rechargeable battery is reported. It comprises a conductive organic polymer electrolyte membrane sandwiched by a thin Li metal foil anode, and a thin carbon composite electrode on which 
 A novel rechargeable battery is reported. It comprises a conductive organic polymer electrolyte membrane sandwiched by a thin Li metal foil anode, and a thin carbon composite electrode on which oxygen, the electroactive cathode material, accessed from the environment, is reduced during discharge to generate electric power. It features an all solid state design in which electrode and electrolyte layers are laminated to form a 200 to 300 ÎŒm thick battery cell. The overall cell reaction during discharge appears to be . It has an open‐circuit voltage of about 3 V, and a load voltage that spans between 2 and 2.8 V depending upon the load resistance. The cell can be recharged with good coulombic efficiency using a cobalt phthalocyanine catalyzed carbon electrode.

Metal–Air Batteries with High Energy Density: Li–Air versus Zn–Air

2010-12-08
Jang‐Soo Lee , Sun Tai Kim , Ruiguo Cao +4 more
Abstract In the past decade, there have been exciting developments in the field of lithium ion batteries as energy storage devices, resulting in the application of lithium ion batteries in 
 Abstract In the past decade, there have been exciting developments in the field of lithium ion batteries as energy storage devices, resulting in the application of lithium ion batteries in areas ranging from small portable electric devices to large power systems such as hybrid electric vehicles. However, the maximum energy density of current lithium ion batteries having topatactic chemistry is not sufficient to meet the demands of new markets in such areas as electric vehicles. Therefore, new electrochemical systems with higher energy densities are being sought, and metal‐air batteries with conversion chemistry are considered a promising candidate. More recently, promising electrochemical performance has driven much research interest in Li‐air and Zn‐air batteries. This review provides an overview of the fundamentals and recent progress in the area of Li‐air and Zn‐air batteries, with the aim of providing a better understanding of the new electrochemical systems.

The Emerging Chemistry of Sodium Ion Batteries for Electrochemical Energy Storage

2015-02-04
Dipan Kundu , Elahe Talaie , Victor Duffort +1 more
Energy storage technology has received significant attention for portable electronic devices, electric vehicle propulsion, bulk electricity storage at power stations, and load leveling of renewable sources, such as solar energy 
 Energy storage technology has received significant attention for portable electronic devices, electric vehicle propulsion, bulk electricity storage at power stations, and load leveling of renewable sources, such as solar energy and wind power. Lithium ion batteries have dominated most of the first two applications. For the last two cases, however, moving beyond lithium batteries to the element that lies below-sodium-is a sensible step that offers sustainability and cost-effectiveness. This requires an evaluation of the science underpinning these devices, including the discovery of new materials, their electrochemistry, and an increased understanding of ion mobility based on computational methods. The Review considers some of the current scientific issues underpinning sodium ion batteries.

Electrode Materials for Rechargeable Sodium‐Ion Batteries: Potential Alternatives to Current Lithium‐Ion Batteries

2012-05-14
Sung‐Wook Kim , Dong‐Hwa Seo , Xiaohua Ma +2 more
Abstract Lithium (Li)‐ion batteries (LIB) have governed the current worldwide rechargeable battery market due to their outstanding energy and power capability. In particular, the LIB's role in enabling electric vehicles 
 Abstract Lithium (Li)‐ion batteries (LIB) have governed the current worldwide rechargeable battery market due to their outstanding energy and power capability. In particular, the LIB's role in enabling electric vehicles (EVs) has been highlighted to replace the current oil‐driven vehicles in order to reduce the usage of oil resources and generation of CO 2 gases. Unlike Li, sodium is one of the more abundant elements on Earth and exhibits similar chemical properties to Li, indicating that Na chemistry could be applied to a similar battery system. In the 1970s‐80s, both Na‐ion and Li‐ion electrodes were investigated, but the higher energy density of Li‐ion cells made them more applicable to small, portable electronic devices, and research efforts for rechargeable batteries have been mainly concentrated on LIB since then. Recently, research interest in Na‐ion batteries (NIB) has been resurrected, driven by new applications with requirements different from those in portable electronics, and to address the concern on Li abundance. In this article, both negative and positive electrode materials in NIB are briefly reviewed. While the voltage is generally lower and the volume change upon Na removal or insertion is larger for Na‐intercalation electrodes, compared to their Li equivalents, the power capability can vary depending on the crystal structures. It is concluded that cost‐effective NIB can partially replace LIB, but requires further investigation and improvement.
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Lithium–Sulfur Batteries: Electrochemistry, Materials, and Prospects

2013-11-14
Ya‐Xia Yin , Sen Xin , Yu‐Guo Guo +1 more
Abstract With the increasing demand for efficient and economic energy storage, Li‐S batteries have become attractive candidates for the next‐generation high‐energy rechargeable Li batteries because of their high theoretical energy 
 Abstract With the increasing demand for efficient and economic energy storage, Li‐S batteries have become attractive candidates for the next‐generation high‐energy rechargeable Li batteries because of their high theoretical energy density and cost effectiveness. Starting from a brief history of Li‐S batteries, this Review introduces the electrochemistry of Li‐S batteries, and discusses issues resulting from the electrochemistry, such as the electroactivity and the polysulfide dissolution. To address these critical issues, recent advances in Li‐S batteries are summarized, including the S cathode, Li anode, electrolyte, and new designs of Li‐S batteries with a metallic Li‐free anode. Constructing S molecules confined in the conductive microporous carbon materials to improve the cyclability of Li‐S batteries serves as a prospective strategy for the industry in the future.

Porous Hollow Carbon@Sulfur Composites for High‐Power Lithium–Sulfur Batteries

2011-05-17
N. Jayaprakash , Jie Shen , Surya S. Moganty +2 more
Slowing down the shuttle: [email protected] nanocomposites (see TEM images) based on mesoporous, hollow carbon capsules were generated by a template-based approach. As the cathode material in a Li–S secondary 
 Slowing down the shuttle: [email protected] nanocomposites (see TEM images) based on mesoporous, hollow carbon capsules were generated by a template-based approach. As the cathode material in a Li–S secondary battery, they display outstanding electrochemical features attributed to sequestration of elemental sulfur in the carbon capsules and to its favorable effect in limiting polysulfide shuttling as well as to enhanced electron transport from the sulfur. Detailed facts of importance to specialist readers are published as "Supporting Information". Such documents are peer-reviewed, but not copy-edited or typeset. They are made available as submitted by the authors. Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article.

Nanostructured materials for advanced energy conversion and storage devices

2005-05-01
A.S. AricĂČ , Peter G. Bruce , Bruno Scrosati +2 more

Fast Lithium Ion Conduction in Garnet‐Type Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub>

2007-09-05
Ramaswamy Murugan , Venkataraman Thangadurai , W. Weppner
Low activation energy and fast lithium ion conduction have been observed for the new compound Li7La3Zr2O12. Relative to previously reported lithium garnets, the solid electrolyte shows a larger cubic lattice 
 Low activation energy and fast lithium ion conduction have been observed for the new compound Li7La3Zr2O12. Relative to previously reported lithium garnets, the solid electrolyte shows a larger cubic lattice constant, higher lithium ion concentration, lower degree of chemical interaction between the Li+ ions and the other lattice constituents, and higher densification.

A lithium superionic conductor

2011-07-29
Noriaki Kamaya , Kenji Homma , Yuichiro Yamakawa +7 more

Electrical Energy Storage and Intercalation Chemistry

1976-06-11
M. Stanley Whittingham
The electrochemical reaction of layered titanium disulfide with lithium giving the intercalation compound lithium titanium disulfide is the basis of a new battery system. This reaction occurs very rapidly and 
 The electrochemical reaction of layered titanium disulfide with lithium giving the intercalation compound lithium titanium disulfide is the basis of a new battery system. This reaction occurs very rapidly and in a highly reversible manner at ambient temperatures as a result of structural retention. Titanium disulfide is one of a new generation of solid cathode materials.

A new class of Solvent-in-Salt electrolyte for high-energy rechargeable metallic lithium batteries

2013-02-12
Liumin Suo , Yong‐Sheng Hu , Hong Li +2 more

Lithium-ion batteries. A look into the future

2011-01-01
Bruno Scrosati , Jusef Hassoun , Yang‐Kook Sun
A critical overview of the latest developments in the lithium ion batteries technology is reported. We first describe the evolution in the electrolyte area with particular attention to ionic liquids, 
 A critical overview of the latest developments in the lithium ion batteries technology is reported. We first describe the evolution in the electrolyte area with particular attention to ionic liquids, discussing the expected application of these room temperature molten salts and listing the issues that still prevent their practical implementation. The attention is then focused on the electrode materials presently considered the most promising for enhancing the energy density of the batteries. At the anode side a discussion is provided on the status of development of high capacity tin and silicon lithium alloys. We show that the morphology that is the most likely to ensure commercial exploitation of these alloy electrodes is that involving carbon-based nanocomposites. We finally touch on super-high-capacity batteries, discussing the key cases of lithium-sulfur and lithium-air and attempting to forecast their chances to eventually reach the status of practically appealing energy storage systems. We conclude with a brief reflection on the amount of lithium reserves in view of its large use in the case of global conversion from gasoline-powered cars to hybrid and electric cars.

Electrical energy storage for transportation—approaching the limits of, and going beyond, lithium-ion batteries

2012-01-01
Michael M. Thackeray , Christopher Wolverton , E. D. Isaacs
The escalating and unpredictable cost of oil, the concentration of major oil resources in the hands of a few politically sensitive nations, and the long-term impact of CO2 emissions on 
 The escalating and unpredictable cost of oil, the concentration of major oil resources in the hands of a few politically sensitive nations, and the long-term impact of CO2 emissions on global climate constitute a major challenge for the 21st century. They also constitute a major incentive to harness alternative sources of energy and means of vehicle propulsion. Today's lithium-ion batteries, although suitable for small-scale devices, do not yet have sufficient energy or life for use in vehicles that would match the performance of internal combustion vehicles. Energy densities 2 and 5 times greater are required to meet the performance goals of a future generation of plug-in hybrid-electric vehicles (PHEVs) with a 40–80 mile all-electric range, and all-electric vehicles (EVs) with a 300–400 mile range, respectively. Major advances have been made in lithium-battery technology over the past two decades by the discovery of new materials and designs through intuitive approaches, experimental and predictive reasoning, and meticulous control of surface structures and chemical reactions. Further improvements in energy density of factors of two to three may yet be achievable for current day lithium-ion systems; factors of five or more may be possible for lithium–oxygen systems, ultimately leading to our ability to confine extremely high potential energy in a small volume without compromising safety, but only if daunting technological barriers can be overcome.

Nonaqueous Liquid Electrolytes for Lithium-Based Rechargeable Batteries

2004-09-16
Kang Xu
ADVERTISEMENT RETURN TO ISSUEPREVarticleNEXTNonaqueous Liquid Electrolytes for Lithium-Based Rechargeable BatteriesKang XuKang XuElectrochemistry Branch, Sensor and Electron Devices Directorate, U.S. Army Research Laboratory, Adelphi, Maryland 20783-1197 More by Kang XuCite this: 
 ADVERTISEMENT RETURN TO ISSUEPREVarticleNEXTNonaqueous Liquid Electrolytes for Lithium-Based Rechargeable BatteriesKang XuKang XuElectrochemistry Branch, Sensor and Electron Devices Directorate, U.S. Army Research Laboratory, Adelphi, Maryland 20783-1197 More by Kang XuCite this: Chem. Rev. 2004, 104, 10, 4303–4418Publication Date (Web):September 16, 2004Publication History Received3 November 2003Published online16 September 2004Published inissue 1 October 2004https://pubs.acs.org/doi/10.1021/cr030203ghttps://doi.org/10.1021/cr030203gresearch-articleACS PublicationsCopyright © 2004 American Chemical SocietyRequest reuse permissionsArticle Views89913Altmetric-Citations5770LEARN ABOUT THESE METRICSArticle Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated. Share Add toView InAdd Full Text with ReferenceAdd Description ExportRISCitationCitation and abstractCitation and referencesMore Options Share onFacebookTwitterWechatLinked InRedditEmail Other access optionsGet e-Alertsclose SUBJECTS:Electrodes,Electrolytes,Ions,Lithium,Solvents Get e-Alerts

A Review of Solid Electrolyte Interphases on Lithium Metal Anode

2015-11-17
Xin‐Bing Cheng , Rui Zhang , Chen‐Zi Zhao +3 more
Lithium metal batteries (LMBs) are among the most promising candidates of high‐energy‐density devices for advanced energy storage. However, the growth of dendrites greatly hinders the practical applications of LMBs in 
 Lithium metal batteries (LMBs) are among the most promising candidates of high‐energy‐density devices for advanced energy storage. However, the growth of dendrites greatly hinders the practical applications of LMBs in portable electronics and electric vehicles. Constructing stable and efficient solid electrolyte interphase (SEI) is among the most effective strategies to inhibit the dendrite growth and thus to achieve a superior cycling performance. In this review, the mechanisms of SEI formation and models of SEI structure are briefly summarized. The analysis methods to probe the surface chemistry, surface morphology, electrochemical property, dynamic characteristics of SEI layer are emphasized. The critical factors affecting the SEI formation, such as electrolyte component, temperature, current density, are comprehensively debated. The efficient methods to modify SEI layer with the introduction of new electrolyte system and additives, ex‐situ‐formed protective layer, as well as electrode design, are summarized. Although these works afford new insights into SEI research, robust and precise routes for SEI modification with well‐designed structure, as well as understanding of the connection between structure and electrochemical performance, is still inadequate. A multidisciplinary approach is highly required to enable the formation of robust SEI for highly efficient energy storage systems.
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Inorganic Solid-State Electrolytes for Lithium Batteries: Mechanisms and Properties Governing Ion Conduction

2015-12-29
John C. Bachman , Sokseiha Muy , Alexis Grimaud +7 more
This Review is focused on ion-transport mechanisms and fundamental properties of solid-state electrolytes to be used in electrochemical energy-storage systems. Properties of the migrating species significantly affecting diffusion, including the 
 This Review is focused on ion-transport mechanisms and fundamental properties of solid-state electrolytes to be used in electrochemical energy-storage systems. Properties of the migrating species significantly affecting diffusion, including the valency and ionic radius, are discussed. The natures of the ligand and metal composing the skeleton of the host framework are analyzed and shown to have large impacts on the performance of solid-state electrolytes. A comprehensive identification of the candidate migrating species and structures is carried out. Not only the bulk properties of the conductors are explored, but the concept of tuning the conductivity through interfacial effects-specifically controlling grain boundaries and strain at the interfaces-is introduced. High-frequency dielectric constants and frequencies of low-energy optical phonons are shown as examples of properties that correlate with activation energy across many classes of ionic conductors. Experimental studies and theoretical results are discussed in parallel to give a pathway for further improvement of solid-state electrolytes. Through this discussion, the present Review aims to provide insight into the physical parameters affecting the diffusion process, to allow for more efficient and target-oriented research on improving solid-state ion conductors.
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“Water-in-salt” electrolyte enables high-voltage aqueous lithium-ion chemistries

2015-11-19
Liumin Suo , Oleg Borodin , Tao Gao +6 more
A concentrated effort for battery safety Aqueous electrolytes are limited to run below 1.23 V to avoid degradation. Suo et al. smash through this limit with an aqueous salt solution 
 A concentrated effort for battery safety Aqueous electrolytes are limited to run below 1.23 V to avoid degradation. Suo et al. smash through this limit with an aqueous salt solution containing lithium (Li) bis(trifluoromethane sulfonyl)imide to create an electrolyte that has an electrochemical window of 3 V (see the Perspective by Smith and Dunn). They used extremely high-concentration solutions, which suppressed hydrogen evolution and electrode oxidation. At these concentrations, the Li solvation shell changes because there simply is not enough water to neutralize the Li + charge. Thus, flammable organic electrolytes could potentially be replaced with a safer aqueous alternative. Science , this issue p. 938 ; see also p. 918

Layered reduced graphene oxide with nanoscale interlayer gaps as a stable host for lithium metal anodes

2016-03-18
Dingchang Lin , Yayuan Liu , Zheng Liang +6 more

Origin of Outstanding Stability in the Lithium Solid Electrolyte Materials: Insights from Thermodynamic Analyses Based on First-Principles Calculations

2015-10-06
Yizhou Zhu , Xingfeng He , Yifei Mo
First-principles calculations were performed to investigate the electrochemical stability of lithium solid electrolyte materials in all-solid-state Li-ion batteries. The common solid electrolytes were found to have a limited electrochemical window. 
 First-principles calculations were performed to investigate the electrochemical stability of lithium solid electrolyte materials in all-solid-state Li-ion batteries. The common solid electrolytes were found to have a limited electrochemical window. Our results suggest that the outstanding stability of the solid electrolyte materials is not thermodynamically intrinsic but is originated from kinetic stabilizations. The sluggish kinetics of the decomposition reactions cause a high overpotential leading to a nominally wide electrochemical window observed in many experiments. The decomposition products, similar to the solid-electrolyte-interphases, mitigate the extreme chemical potential from the electrodes and protect the solid electrolyte from further decompositions. With the aid of the first-principles calculations, we revealed the passivation mechanism of these decomposition interphases and quantified the extensions of the electrochemical window from the interphases. We also found that the artificial coating layers applied at the solid electrolyte and electrode interfaces have a similar effect of passivating the solid electrolyte. Our newly gained understanding provided general principles for developing solid electrolyte materials with enhanced stability and for engineering interfaces in all-solid-state Li-ion batteries.

Designing high-energy lithium–sulfur batteries

2016-01-01
Zhi Wei Seh , Yongming Sun , Qianfan Zhang +1 more
Due to their high energy density and low material cost, lithium-sulfur batteries represent a promising energy storage system for a multitude of emerging applications, ranging from stationary grid storage to 
 Due to their high energy density and low material cost, lithium-sulfur batteries represent a promising energy storage system for a multitude of emerging applications, ranging from stationary grid storage to mobile electric vehicles. This review aims to summarize major developments in the field of lithium-sulfur batteries, starting from an overview of their electrochemistry, technical challenges and potential solutions, along with some theoretical calculation results to advance our understanding of the material interactions involved. Next, we examine the most extensively-used design strategy: encapsulation of sulfur cathodes in carbon host materials. Other emerging host materials, such as polymeric and inorganic materials, are discussed as well. This is followed by a survey of novel battery configurations, including the use of lithium sulfide cathodes and lithium polysulfide catholytes, as well as recent burgeoning efforts in the modification of separators and protection of lithium metal anodes. Finally, we conclude with an outlook section to offer some insight on the future directions and prospects of lithium-sulfur batteries.

Rechargeable Lithium–Sulfur Batteries

2014-07-15
Arumugam Manthiram , Yongzhu Fu , Sheng‐Heng Chung +2 more
ADVERTISEMENT RETURN TO ISSUEPREVReviewNEXTRechargeable Lithium–Sulfur BatteriesArumugam Manthiram*, Yongzhu Fu, Sheng-Heng Chung, Chenxi Zu, and Yu-Sheng SuView Author Information Materials Science and Engineering Program and Texas Materials Institute, The University of 
 ADVERTISEMENT RETURN TO ISSUEPREVReviewNEXTRechargeable Lithium–Sulfur BatteriesArumugam Manthiram*, Yongzhu Fu, Sheng-Heng Chung, Chenxi Zu, and Yu-Sheng SuView Author Information Materials Science and Engineering Program and Texas Materials Institute, The University of Texas at Austin, Austin, Texas 78712, United States*E-mail: [email protected]. Phone: 512-471-1791. Fax: 512-471-7681.Cite this: Chem. Rev. 2014, 114, 23, 11751–11787Publication Date (Web):July 15, 2014Publication History Received3 February 2014Published online15 July 2014Published inissue 10 December 2014https://pubs.acs.org/doi/10.1021/cr500062vhttps://doi.org/10.1021/cr500062vreview-articleACS PublicationsCopyright © 2014 American Chemical SocietyRequest reuse permissionsArticle Views65410Altmetric-Citations3845LEARN ABOUT THESE METRICSArticle Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated. Share Add toView InAdd Full Text with ReferenceAdd Description ExportRISCitationCitation and abstractCitation and referencesMore Options Share onFacebookTwitterWechatLinked InRedditEmail Other access optionsGet e-AlertscloseSupporting Info (1)»Supporting Information Supporting Information SUBJECTS:Batteries,Composites,Electrodes,Electrolytes,Sulfur Get e-Alerts

Advances in lithium–sulfur batteries based on multifunctional cathodes and electrolytes

2016-09-08
Quanquan Pang , Xiao Liang , Chun Yuen Kwok +1 more

Lithium battery chemistries enabled by solid-state electrolytes

2017-02-14
Arumugam Manthiram , Xingwen Yu , Shaofei Wang

More Reliable Lithium‐Sulfur Batteries: Status, Solutions and Prospects

2017-04-05
Ruopian Fang , Shiyong Zhao , Zhenhua Sun +3 more
Abstract Lithium‐sulfur (Li‐S) batteries have attracted tremendous interest because of their high theoretical energy density and cost effectiveness. The target of Li‐S battery research is to produce batteries with a 
 Abstract Lithium‐sulfur (Li‐S) batteries have attracted tremendous interest because of their high theoretical energy density and cost effectiveness. The target of Li‐S battery research is to produce batteries with a high useful energy density that at least outperforms state‐of‐the‐art lithium‐ion batteries. However, due to an intrinsic gap between fundamental research and practical applications, the outstanding electrochemical results obtained in most Li‐S battery studies indeed correspond to low useful energy densities and are not really suitable for practical requirements. The Li‐S battery is a complex device and its useful energy density is determined by a number of design parameters, most of which are often ignored, leading to the failure to meet commercial requirements. The purpose of this review is to discuss how to pave the way for reliable Li‐S batteries. First, the current research status of Li‐S batteries is briefly reviewed based on statistical information obtained from literature. This includes an analysis of how the various parameters influence the useful energy density and a summary of existing problems in the current Li‐S battery research. Possible solutions and some concerns regarding the construction of reliable Li‐S batteries are comprehensively discussed. Finally, insights are offered on the future directions and prospects in Li‐S battery field.

Review on High‐Loading and High‐Energy Lithium–Sulfur Batteries

2017-05-08
Hong‐Jie Peng , Jia‐Qi Huang , Xin‐Bing Cheng +1 more
Abstract Owing to high specific energy, low cost, and environmental friendliness, lithium–sulfur (Li–S) batteries hold great promise to meet the increasing demand for advanced energy storage beyond portable electronics, and 
 Abstract Owing to high specific energy, low cost, and environmental friendliness, lithium–sulfur (Li–S) batteries hold great promise to meet the increasing demand for advanced energy storage beyond portable electronics, and to mitigate environmental problems. However, the application of Li–S batteries is challenged by several obstacles, including their short life and low sulfur utilization, which become more serious when sulfur loading is increased to the practically accepted level above 3–5 mg cm −2 . More and more efforts have been made recently to overcome the barriers toward commercially viable Li–S batteries with a high sulfur loading. This review highlights the recent progress in high‐sulfur‐loading Li–S batteries enabled by hierarchical design principles at multiscale. Particularly, basic insights into the interfacial reactions, strategies for mesoscale assembly, unique architectures, and configurational innovation in the cathode, anode, and separator are under specific concerns. Hierarchy in the multiscale design is proposed to guide the future development of high‐sulfur‐loading Li–S batteries.

Review—SEI: Past, Present and Future

2017-01-01
E. Peled , Svetlana Menkin
The Solid-Electrolyte-Interphase (SEI) model for non-aqueous alkali-metal batteries constitutes a paradigm change in the understanding of lithium batteries and has thus enabled the development of safer, durable, higher-power and lower-cost 
 The Solid-Electrolyte-Interphase (SEI) model for non-aqueous alkali-metal batteries constitutes a paradigm change in the understanding of lithium batteries and has thus enabled the development of safer, durable, higher-power and lower-cost lithium batteries for portable and EV applications. Prior to the publication of the SEI model (1979), researchers used the Butler-Volmer equation, in which a direct electron transfer from the electrode to lithium cations in the solution is assumed. The SEI model proved that this is a mistaken concept and that, in practice, the transfer of electrons from the electrode to the solution in a lithium battery, must be prevented, since it will result in fast self-discharge of the active materials and poor battery performance. This model provides [E. Peled, in "Lithium Batteries," J.P. Gabano (ed), Academic Press, (1983), E. Peled, J. Electrochem. Soc., 126, 2047 (1979).] new equations for: electrode kinetics (io and b), anode corrosion, SEI resistivity and growth rate and irreversible capacity loss of lithium-ion batteries. This model became a cornerstone in the science and technology of lithium batteries. This paper reviews the past, present and the future of SEI batteries.
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Toward Safe Lithium Metal Anode in Rechargeable Batteries: A Review

2017-07-28
Xin‐Bing Cheng , Rui Zhang , Chen‐Zi Zhao +1 more
The lithium metal battery is strongly considered to be one of the most promising candidates for high-energy-density energy storage devices in our modern and technology-based society. However, uncontrollable lithium dendrite 
 The lithium metal battery is strongly considered to be one of the most promising candidates for high-energy-density energy storage devices in our modern and technology-based society. However, uncontrollable lithium dendrite growth induces poor cycling efficiency and severe safety concerns, dragging lithium metal batteries out of practical applications. This review presents a comprehensive overview of the lithium metal anode and its dendritic lithium growth. First, the working principles and technical challenges of a lithium metal anode are underscored. Specific attention is paid to the mechanistic understandings and quantitative models for solid electrolyte interphase (SEI) formation, lithium dendrite nucleation, and growth. On the basis of previous theoretical understanding and analysis, recently proposed strategies to suppress dendrite growth of lithium metal anode and some other metal anodes are reviewed. A section dedicated to the potential of full-cell lithium metal batteries for practical applications is included. A general conclusion and a perspective on the current limitations and recommended future research directions of lithium metal batteries are presented. The review concludes with an attempt at summarizing the theoretical and experimental achievements in lithium metal anodes and endeavors to realize the practical applications of lithium metal batteries.

Fundamentals of inorganic solid-state electrolytes for batteries

2019-08-19
Theodosios Famprikis , Pieremanuele Canepa , James A. Dawson +2 more

Designing solid-state electrolytes for safe, energy-dense batteries

2020-02-05
Qing Zhao , Sanjuna Stalin , Chen‐Zi Zhao +1 more

Review of electrical energy storage technologies, materials and systems: challenges and prospects for large-scale grid storage

2018-01-01
Turgut M. GĂŒr
Large scale storage technologies are vital to increase the share of renewable electricity in the global energy mix. Large scale storage technologies are vital to increase the share of renewable electricity in the global energy mix.

Unlocking the Potential of Epoxidized Natural Rubber (ENR)-Based Polymer Electrolytes: Key Strategies, Bibliometric Insights, and Future Directions

2025-06-25
Rawdah Whba , Sevda Sahinbay , Fathyah Whba +2 more | Langmuir
Natural rubber (NR) and its modified forms, such as epoxidized NR (ENR), are widely used in industries due to their versatility, biodegradability, and unique elastomeric properties. ENR has recently gained 
 Natural rubber (NR) and its modified forms, such as epoxidized NR (ENR), are widely used in industries due to their versatility, biodegradability, and unique elastomeric properties. ENR has recently gained attention as a sustainable alternative to synthetic polymer electrolytes (PEs) in low- to moderate-temperature electrochemical devices, including lithium-ion batteries (LIBs), supercapacitors, and proton exchange membrane fuel cells (PEMFCs). It offers advantages such as low cost, eco-friendliness, and excellent film-forming ability. However, its practical application is hindered by poor mechanical strength, low ionic conductivity, and limited thermal and chemical stability, making it unsuitable for high-temperature systems like solid oxide fuel cells (SOFCs). Advanced modification techniques─such as blending with reinforcing polymers, chemical cross-linking, graft copolymerization, and nanofiller incorporation─have been explored to overcome these limitations. These strategies significantly enhance ENR's mechanical robustness, ionic transport, and resistance to heat and solvents, improving its viability for targeted electrochemical applications. This perspective discusses recent progress in ENR-based PEs, emphasizing conductivity, moisture resistance, and long-term durability improvements. Sustainable fabrication methods are also critical to developing high-performance membranes that minimize fuel crossover while maintaining efficient ion transport. Therefore, future research should optimize ENR's electrochemical properties and thermal stability to support performance under challenging operating conditions.

A cost-effective all-in-one halide material for all-solid-state batteries

2025-06-25
Jiamin Fu , Changhong Wang , Shuo Wang +7 more | Nature

Magnetic Field‐Driven Catalysis: Revealing Enhanced Oxygen Reactions in Li‐O<sub>2</sub> Batteries Using Tailored Magnetic Nanocatalysts

2025-06-25
Yimin Chen , Xin Hu , Min Hong +7 more | Advanced Science
Abstract Lithium‐oxygen (Li‐O 2 ) batteries offer immense promise for next‐generation energy storage technology due to their ultra‐high theoretical energy density. However, their adoption faces challenges like large overpotential and 
 Abstract Lithium‐oxygen (Li‐O 2 ) batteries offer immense promise for next‐generation energy storage technology due to their ultra‐high theoretical energy density. However, their adoption faces challenges like large overpotential and slow oxygen reaction kinetics. This study introduces a novel strategy that leverages custom‐designed magnetic nanocatalysts and external magnetic fields to boost electrochemical performance. Mn‐Co‐Fe oxide catalysts with adjustable magnetic properties is developed and demonstrated the correlation between the magnetism of the catalysts and the enhancement of battery performance. In the presence of an external magnetic field, the paramagnetic oxygen molecules experience a Kelvin force, while the Li + ions are influenced by a Lorentz force. This accelerates their diffusion, significantly enhancing the kinetics of both the oxygen reduction and oxygen evolution reactions. The catalyst with the highest magnetization boosted specific capacity by 52.9% (from 8143 to 12 455 mAh g⁻Âč) and significantly lowered the overpotential. This breakthrough underscores magnetic field‐driven catalysis as a crucial advancement in unlocking the full potential of Li‐O 2 batteries, setting new benchmarks for energy storage technology.

Electrolyte Transport Parameters and Interfacial Effects in Calcium Metal Batteries: Analogies and Differences to Magnesium and Lithium Counterparts

2025-06-25
Joachim HĂ€cker , Tobias Rommel , Laurin Rademacher +5 more | Advanced Science
Abstract Magnesium and calcium metal batteries are promising emerging technologies. Their high capacity and low redox potential translate to a high theoretical energy density, making them attractive candidates for future 
 Abstract Magnesium and calcium metal batteries are promising emerging technologies. Their high capacity and low redox potential translate to a high theoretical energy density, making them attractive candidates for future energy storage solutions. Owing to their neighboring position and the diagonal relationship in the periodic table to lithium, Mg 2+ , Ca 2+ , and Li + ions feature commonalities in terms of ionic radius, carried charge, and charge density. The present study aims to shed light on the similarities but also differences of Ca electrolytes and metal anodes in comparison to their Mg and Li counterparts in terms of transport properties and processes at the anode/electrolyte interface, respectively. To ensure comparability, an electrolyte comprising B(hfip) 4 − anions in monoglyme is applied in either case. By executing galvanostatic polarization and pulsing with different separator materials, the separator tortuosity, diffusion coefficient, and transference number are determined. Further, the charge transfer characteristics as well as the adsorption layer and solid electrolyte interphase formation are investigated by electrochemical impedance spectroscopy. The cation charge density was found to be crucial for diffusion and desolvation processes, yet surprisingly, also a cation‐dependent separator tortuosity was observed. The study concludes with a recommendation on suitable separators for each metal battery system.

Corrigendum to “Inorganic Solid‐State Electrolytes in Potassium Batteries: Advances, Challenges, and Future Prospects”

2025-06-25
| ChemElectroChem

Early Terminating Solid Electrolyte Interphase Formation via Nucleophilic Fluorination to Achieve High Initial Coulombic Efficiency

2025-06-25
Shengkai Cao , Yuan Song , Wei Zhang +7 more | Advanced Materials
Abstract The initial Coulombic efficiency (ICE) of lithium‐ion batteries, quantifying the irreversible Li + loss during the first cycle, is critical for determining practical energy density. Many electrode materials exhibit 
 Abstract The initial Coulombic efficiency (ICE) of lithium‐ion batteries, quantifying the irreversible Li + loss during the first cycle, is critical for determining practical energy density. Many electrode materials exhibit substandard ICEs (&lt;90%) due to excessive formation of solid electrolyte interphase (SEI). Traditional strategies modifying SEI formation mainly focus on the generating process but often consume extra Li + and yield limited improvements. Here, a strategy is introduced that targets the terminating process of SEI formation, usually impeded by interfacial parasitic reactions, to achieve ICEs exceeding 90%. Using TiO 2 as a model electrode, it is demonstrated that equivalent chemical fluorination suppresses the parasitic reaction between phosphorus pentafluoride (PF₅) and surface hydroxyl groups (─OH), early terminating SEI formation. Interfacial analysis and theoretical simulations reveal that this approach reduces organic SEI formation while preserving the beneficial LiF‐rich inner SEI layer. As a result, the fluorinated TiO 2 anode exhibits an ICE of 92.1%, significantly higher than the 74.1% of pristine TiO 2 , without compromising other electrochemical performance metrics. Pouch cell tests confirm the practical applicability of the method. This work provides deep insights into mechanisms of terminating SEI formation and opens a new pathway for optimizing the battery performances through inherent SEI manipulation.

Evolution of Pore Volume During Stripping of Lithium Metal in Solid‐State Batteries Observed with Operando Dilatometry

2025-06-25
Thomas J. Schall , Till Fuchs , Janis K. Eckhardt +5 more | Small
Abstract Lithium metal solid‐state batteries are prone to pore formation at the interface between the metal anode and the solid electrolyte during discharge, when the applied current density exceeds the 
 Abstract Lithium metal solid‐state batteries are prone to pore formation at the interface between the metal anode and the solid electrolyte during discharge, when the applied current density exceeds the lithium vacancy diffusion rate in the metal. This leads to contact loss and eventually battery failure. To better understand the mechanisms of pore formation at the anode interface, operando information on the total pore volume is essential. In this study, a dedicated dilatometric measurement setup for operando tracking of pore volume is presented and validated. The working principle of this method is demonstrated in a case study on symmetric lithium‐garnet cells. The combination of the dilatometric data with galvanostatic electrochemical impedance spectroscopy (GEIS) allows for a systematic study of pore formation in any metal solid‐state battery. To quantify this process, the vacancy injection ratio is introduced, as a measure of the fraction of lithium atom sites that remain empty during stripping. These experimental results reveal that, under the conditions applied, pore formation begins immediately upon stripping, even before becoming detectable by GEIS. Furthermore, it is shown that pores initially grow laterally near the surface before deepening at later stages. Based on these findings, a pore formation and growth mechanism is proposed.

Unveiling conductivity, dielectric, morphological and thermal properties of PEMA-KSCN electrolytes doped with Nano-TiO₂

2025-06-25
Mani Ulaganathan , S. Jayanthi | Applied Physics A

Comprehensively Upgraded Lithium-Metal Batteries Achieved by the ÎČ/ÎČ″-Al<sub>2</sub>O<sub>3</sub> Ceramic Solid Electrolyte

2025-06-24
Pengyu Zhang , Junting Li , Yunlong Cui +2 more | ACS Sustainable Chemistry & Engineering

Flaky aluminum hydroxide/titania nanocomposite modified separator for high-performance lithium metal batteries

2025-06-24
Chang Hong , Yanyan Zhang , Huiying Li +7 more | Journal of Energy Storage

Impact of the Si Electrode Morphology and of the Added Li‐Salt on the SEI Formed Using EMIFSI‐Based Ionic‐Liquid Electrolytes

2025-06-24
Nicholas Carboni , Sergio Brutti , Oriele Palumbo +7 more | Advanced Sustainable Systems
Abstract This work presents an in‐depth chemical and morphological investigation of the solid electrolyte interphase (SEI) formed on binder‐free silicon electrodes, which include both nanowire (Si‐NW) and amorphous (a‐Si) configurations, 
 Abstract This work presents an in‐depth chemical and morphological investigation of the solid electrolyte interphase (SEI) formed on binder‐free silicon electrodes, which include both nanowire (Si‐NW) and amorphous (a‐Si) configurations, for next‐generation lithium‐ion battery systems. The study focuses on the first five galvanostatic cycles to capture the critical early‐stage SEI consolidation process, essential for understanding the interfacial phenomena that dictate long‐term performance. By employing innovative electrode fabrication techniques such as plasma‐enhanced chemical vapor deposition and utilizing ionic liquid (IL)‐based electrolytes—specifically 1‐ethyl‐3‐methylimidazolium bis(fluorosulfonyl)imide (EMIFSI) formulations known for their low viscosity and high conductivity—this work addresses the challenges posed by the significant volume changes inherent to Si‐based materials. Advanced characterization methodologies, notably Optical‐Photothermal Infrared Spectroscopy (O‐PTIR) and Raman spectroscopy are utilized to probe the chemical and structural evolution of the SEI with high spatial resolution. This multifaceted approach reveals the interplay between electrode morphology and electrolyte composition on SEI formation and provides valuable insights into the fundamental processes governing irreversible capacity losses and electrode degradation. The findings demonstrate clear material‐ and electrolyte‐dependent differences in SEI characteristics, thereby establishing new avenues for optimizing interfacial stability and battery performance. Overall, the study contributes innovative perspectives on early SEI formation mechanisms critical for the design of safer and more durable high‐capacity battery electrodes.

Electronic Structure Engineering in Electrocatalysts: Enabling Regulated Redox Mediation for Advanced Lithium‐Sulfur Chemistry

2025-06-24
Pan Zeng , Xiaoqin Li , Bo Zhao +4 more | Advanced Energy Materials
Abstract The practical deployment of lithium‐sulfur (Li–S) battery is fundamentally constrained by the intrinsic shuttle effect and the kinetically sluggish conversion of lithium polysulfides (LiPSs). To mitigate these challenges, rational 
 Abstract The practical deployment of lithium‐sulfur (Li–S) battery is fundamentally constrained by the intrinsic shuttle effect and the kinetically sluggish conversion of lithium polysulfides (LiPSs). To mitigate these challenges, rational design of advanced electrocatalysts capable of dual‐functional LiPSs immobilization and catalytic conversion has been recognized as a pivotal solution. Critically, the catalytic efficacy of electrocatalysts is intrinsically governed by their electronic structure characteristics, which dictate adsorption energies, charge transfer dynamics, and reaction pathway selectivity during the redox process. However, a systematic review correlating electronic modulation strategies with mechanistic enhancements in Li–S chemistry still remains absent. This review emphasizes recent advances in the fascinating strategies to tailor the electronic structure of electrocatalysts, including but not limited to d ‐band position, d ‐band valence electron/vacancy, spin state, e g /t 2g orbitals, electron filling of anti‐bonding, p ‐band, d‐p orbital hybridization, f ‐orbital, and geometric structure engineering. The fundamental relationships between electronic structure and catalytic activity are discussed in detail, highlighting mechanistic insights into the origins of enhanced activity. Finally, the major challenges in modulating electronic structure are summarized, and an outlook for further development of electronic structure strategies is briefly proposed. This review can afford cutting‐edge insights into the electronic structure regulation in Li–S chemistry.

A High‐Performance Garnet‐Based All‐Solid‐State Battery Fabricated Through Room‐Temperature Ultrasonic Welding

2025-06-24
Tianlu Pang , Shu–Fen Wu , Han Wu +7 more | Advanced Science
Garnet-type Li6.5La3Zr1.5Ta0.5O12 (LLZO) has emerged as a highly promising solid electrolyte for next-generation Li metal batteries due to its high Li+ conductivity and stability against metallic lithium. However, its practical 
 Garnet-type Li6.5La3Zr1.5Ta0.5O12 (LLZO) has emerged as a highly promising solid electrolyte for next-generation Li metal batteries due to its high Li+ conductivity and stability against metallic lithium. However, its practical application is hindered by poor interfacial contact between Li and LLZO, as well as the persistent issue of lithium dendrite formation during cycling. In this study, a novel and efficient strategy is proposed to address these challenges by employing a room-temperature ultrasonic treatment combined with a LiMg alloy anode. The fabricated symmetrical UW-LiMg/LLZO/UW-LiMg cell exhibits a low interfacial resistance and achieves an unprecedented critical current density of 4.45 mA cm-2. Furthermore, these cells demonstrate excellent cycling stability, maintaining stable lithium plating/stripping for over 1000 h at a high current density of 1 mA cm- 2 with a low overpotential of ≈30 mV. The superior performance is attributed to the enhanced anode ductility achieved through Mg alloying and the formation of an ultra-stable interface layer. The all-solid-state UW-LiMg/LLZO/LiFePO4 battery, incorporating an ultrasonically treated alloy anode and a fluorinated cathode interface, delivers a specific capacity of 153 mAh g-1 at 0.5 C and retains an impressive capacity retention of 90% after 200 cycles at room temperature.

Crosslinked Poly(Ionic Liquid) Pentablock Terpolymer Electrolytes for Lithium Metal Batteries

2025-06-24
Do-Hyun Kim , Rui Sun , Roger Tocchetto +3 more | Journal of Applied Polymer Science
ABSTRACT In this study, solid polymer electrolytes (SPEs) containing crosslinked poly(ionic liquid) pentablock terpolymer (X‐PILPTP) (at varying crosslinking degrees from 1% to 20% [mol%]), ionic liquid, and lithium salt are 
 ABSTRACT In this study, solid polymer electrolytes (SPEs) containing crosslinked poly(ionic liquid) pentablock terpolymer (X‐PILPTP) (at varying crosslinking degrees from 1% to 20% [mol%]), ionic liquid, and lithium salt are investigated with respect to morphology, ionic conductivity, mechanical properties, electrochemical stability, and lithium metal battery performance. Selective crosslinking is used to covalently connect the middle block of ABCBA pentablock terpolymers with an ionic crosslinker to minimize the loss of microphase separation and self‐assembled morphology. Interestingly, all X‐PILPTP SPEs with absorption of lithium salt and ionic liquid exhibit lamellar morphologies in the presence of crosslinked networks. Additionally, mechanical strength is well preserved despite the high absorption of lithium salt and ionic liquid, providing outstanding ionic conductivity and mechanical properties. High ionic conductivity is achieved at a 5% crosslinking degree without significant mechanical loss, improving its electrochemical stability. X‐PILPTP SPE as the separator within lithium metal batteries delivers an initial discharge capacity of 128 mAh g −1 at room temperature with outstanding capacity retention of 96.8% after the 100th cycle, highlighting the prospect of crosslinked PIL multiblock polymers as a potential candidate for SPEs in solid‐state lithium metal batteries.

Dual‐Site Ni Nanoparticles‐Ru Clusters Anchored on Hierarchical Carbon with Decoupled Gas and Ion Diffusion Channels Enabling Low‐Overpotential, Highly Stable Li‐CO<sub>2</sub> Batteries

2025-06-24
Zhan Jiang , Xinxin Zhang , Jinxi Ruan +7 more | Advanced Functional Materials
Abstract Li‐CO₂ batteries present an innovative electrochemical approach, integrating CO₂ capture and energy storage. Nevertheless, slow CO₂ reduction and evolution reaction kinetics lead to substantial overpotentials and limited cycling lifespans. 
 Abstract Li‐CO₂ batteries present an innovative electrochemical approach, integrating CO₂ capture and energy storage. Nevertheless, slow CO₂ reduction and evolution reaction kinetics lead to substantial overpotentials and limited cycling lifespans. This study introduces a hierarchical gas electrode derived from wood, functionalized with nickel nanoparticles and ruthenium clusters. The three dimensional (3D) hierarchical porous structure serves dual purposes: 1) It provides separate channels for gas and ion diffusion, enhancing transport kinetics during Li‐CO₂ redox reactions. 2) It offers ample space for discharge product deposition, mitigating surface passivation. Furthermore, the dual‐site Ni–Ru active centers enhance the co‐oxidation reversibility of Li₂CO₃‐C aggregates through electronic structure optimization. This suppresses electrolyte decomposition and side reactions, especially at high current rates. These advantageous structural features enable Li‐CO₂ batteries with optimized cathodes to achieve: 1) A discharge platform below 3.16 V, 2) An ultralow discharge–charge overpotential gap of 0.619 V, 3) A full discharge capacity of 34.681 mAh cm⁻ 2 , and 4) A long cycle life exceeding 1100 cycles (2200 h). This study presents an effective design strategy that combines electrode architecture and metal catalytic centers for gas cathodes. The findings advance the development of aprotic Li‐CO₂ batteries as a viable electrochemical energy storage solution.

Rational Design of High-Performance Li<sub>1.5</sub>La<sub>1.5</sub>TeO<sub>6</sub>-Based Composite Solid Electrolyte for Lithium Metal Batteries with Fast-Charging and Long-Life Stability

2025-06-24
Zhuoyuan Zheng , Zhengfeng Zhu , Xianlong Zhou +3 more | ACS Applied Materials & Interfaces
Solid-state electrolytes (SSEs) are increasingly recognized for their potential to enhance the performance of lithium-metal batteries (LMBs). In this study, to tackle the inherent trade-offs in SSEs between mechanical stability 
 Solid-state electrolytes (SSEs) are increasingly recognized for their potential to enhance the performance of lithium-metal batteries (LMBs). In this study, to tackle the inherent trade-offs in SSEs between mechanical stability and ionic conductivity, we propose a composite solid electrolyte (CSE) by integrating perovskite Li1.5La1.5TeO6 (LLTeO) with lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) and a polymer blend of poly(methyl methacrylate) (PMMA) and poly(vinylidene fluoride) (PVDF). This rational design features an ion-conducting double-network, enhanced mechanical flexibility, and robustness, which facilitate improved ion migration, excellent compatibility with lithium electrodes, and effective dendrite suppression. The CSE demonstrates a mechanical strength of 27 MPa, an impressive ionic conductivity of 0.826 mS cm-1, and a broad electrochemical window of 4.88 V. The Li//Li symmetric cells display stable cycling for over 600 h at 1 mA cm-2. Additionally, the corresponding Li//LiFePO4 (LFP) and Li//LiNi0.8Co0.1Mn0.1O2 (NCM811) cells exhibit remarkable rate performance and cyclic stability. Specifically, the Li/CSE/LFP cell sustains a high capacity of 131.7 mAh g-1 after 300 cycles at 3C, achieving a capacity retention rate of 98.1% and an average Coulombic efficiency of 100%. This research presents a viable strategy for the development of solid-state LMBs, offering high energy density, extended cycle life, and enhanced safety.

Vertically Directed Ion Transport at the Molecular Scale in Composite Solid Electrolytes Enabled by Nanofiber-Confined Alignment of Single-Crystal MOF Tubes

2025-06-24
Kai Chen , Mingjia Lu , Xiaoxiao Li +6 more | ACS Applied Materials & Interfaces
The incorporation of a metal-organic framework, impregnated with ionic liquid (MOF@IL), into solid polymer electrolytes (SPE) is indeed a promising approach for advancing solid-state lithium batteries. However, the randomly distributed 
 The incorporation of a metal-organic framework, impregnated with ionic liquid (MOF@IL), into solid polymer electrolytes (SPE) is indeed a promising approach for advancing solid-state lithium batteries. However, the randomly distributed polycrystalline MOF particles inevitably lead to discontinuous and tortuous ion transport at the nano and molecular scales, drastically compromising the overall performance of these electrolytes. Herein, a composite solid electrolyte (CSE) incorporating vertically aligned single-crystal MOF@IL tubes (VMTSE) is developed by aligning the single-crystal MOF tubes along the same direction as that of the vertically aligned polyacrylonitrile (PAN) nanofibers. The PAN nanofiber substrate can confine and guide the continuous vertical alignment of MOF tubes to ensure the directed ion transport at the nanoscale. Meanwhile, compared to the long-range disordered pore structures in polycrystalline MOFs, the orientation of the one-dimensional (1D) channel pores within the single-crystal MOF tubes aligns with the tubular axis, thereby further enabling continuously directed ion transport at the molecular scale. As a result, the VMTSE exhibits a high ionic conductivity of 3.33 × 10-3 S cm-1 at 60 °C, and the corresponding LiFePO4 || Li full battery achieves a stable discharge capacity of 101.04 mAh g-1 with 78% capacity retention after 200 cycles at 1 C (60 °C). This work demonstrates the feasibility of precisely regulating Li+ transport pathways at multiscales by confining and guiding the directed arrangement of single-crystal MOF tubes within nanofibers to boost the performance of CSEs.

Atomic layer deposition for protecting lithium metal anodes to high-voltage battery applications

2025-06-24
Sara Pakseresht , Ville Miikkulainen , Filipp A. Obrezkov +3 more | Journal of Power Sources

Stable Operation of High‐Voltage Sodium‐Ion Batteries via Cathode Interphase Reconstruction with Competitive Anion Coordination Chemistry

2025-06-24
Shi Wu , Haojie Liang , Zhen‐Yi Gu +7 more | Advanced Functional Materials
Abstract High‐voltage sodium‐ion batteries (SIBs) have significant application prospects in low‐cost energy‐storage systems. However, their performance is limited by sluggish Na + desolvation kinetics and the formation of an unstable 
 Abstract High‐voltage sodium‐ion batteries (SIBs) have significant application prospects in low‐cost energy‐storage systems. However, their performance is limited by sluggish Na + desolvation kinetics and the formation of an unstable cathode‐electrolyte interphase (CEI) in traditional electrolyte systems. This study introduces an anionic competitive coordination strategy in which SO 2 CF 3 − from sodium trifluoromethanesulfonate (NaSO 2 CF 3 ), with delocalized electron structures, preferentially occupy the inner layer of the Na + solvation sheath, replacing traditional sodium salt anions and solvent molecules to construct a highly dynamic solvation microstructure. This novel solvation structure facilitates Na + ion desolvation and induces the formation of a thin and robust CEI rich in sulfur/fluorine‐containing organic and inorganic species by regulating the interfacial decomposition pathway, thereby ensuring interfacial stability at a high voltage of 4.4 V. As a proof of concept, the optimized electrolyte effectively mitigates the structural degradation of high‐voltage cathodes such as NaFe 1/3 Ni 1/3 Mn 1/3 O 2 and Na 3 V 2 (PO 4 ) 2 O 2 F and simultaneously enhances their rate performance and cycling stability. Furthermore, NFN||hard carbon full cells incorporating the optimized electrode exhibit excellent cycling stability under a high mass loading. This study establishes an innovative electrolyte design paradigm that overcomes interface failure issues in high‐voltage SIBs by precisely regulating the CEI composition and structure via anionic coordination chemistry.

High ionic conductivity polymer modified commercial separator for lithium metal battery

2025-06-24
Jiangchao Chen , Guisheng Zhu , Huarui Xu +7 more | Journal of Power Sources

Inhibiting Interfacial Failure in Garnet‐Based Solid‐State Batteries with High‐Capacity Anodes: Mechanism and Strategies

2025-06-23
Zhexi Xiao , Zewei Zou , Kehao Zhao +7 more | Advanced Materials
Abstract Garnet‐based solid‐state electrolytes (SSEs) with exceptional reductive stability and superior ionic conductivity have emerged as promising candidates for next‐generation solid‐state batteries (SSBs). However, critical interface challenges still persist in 
 Abstract Garnet‐based solid‐state electrolytes (SSEs) with exceptional reductive stability and superior ionic conductivity have emerged as promising candidates for next‐generation solid‐state batteries (SSBs). However, critical interface challenges still persist in practical implementations. This review systematically examines interfacial failure mechanisms in garnet SSE systems with high‐capacity anodes (Si, metallic Li) through combined mechanical‐electrochemical perspectives. For Si‐based anodes, a microstructure‐property‐performance relationship is established by analyzing strain mismatch‐induced degradation, correlating ionic transport barriers with lithiation kinetics under varying internal microstructures, particle sizes, and external pressures. Multiscale stress‐relief strategies spanning atomic‐level interface engineering to macroscopic pressure optimization are proposed. Regarding Li metal interfaces, breakthrough understandings of grain boundary (GB) charge distribution effects on Li filament propagation are highlighted, along with innovative solutions for kinetic inhibition. Particular emphasis is placed on dry battery electrode (DBE) fabrication techniques as scalable approaches for achieving intimate interfacial contact in industrial‐scale SSB production. By integrating fundamental mechanical‐electrochemical insights with practical engineering considerations, this work quantitatively decouple the strain‐lithiation interplay at Si/garnet interfaces, the regulation law of GB charge distribution on lithium dendrites and the industrial potential of combining DBE with fluidized bed technology for the first time, charting a viable path toward industrial SSBs with &gt;400 Wh kg −1 energy density.

A polymer-modified separator with lithiophilic nanocapsules for high-performance lithium metal batteries

2025-06-23
Jiangchao Chen , Guisheng Zhu , Huarui Xu +2 more | Journal of Energy Storage

Molecular Engineering Enabled In Situ 3D Cross‐Linked and Thermo‐Electrochemically Stable Poly(1,3‐dioxolane) Solid Polymer Electrolyte

2025-06-23
Keding Chen , Xiaolong Shi , Yanghuan Shen +7 more | Small
Abstract The narrow electrochemical stability window (ESW) and poor thermal stability of poly(1,3‐dioxolane) (PDOL) solid polymer electrolyte severely restrict its application. In this study, poly(1,3‐dioxolane) dimethacrylate (PDOL‐DMA) is designed and 
 Abstract The narrow electrochemical stability window (ESW) and poor thermal stability of poly(1,3‐dioxolane) (PDOL) solid polymer electrolyte severely restrict its application. In this study, poly(1,3‐dioxolane) dimethacrylate (PDOL‐DMA) is designed and synthesized to replace the unstable terminal hydroxyl groups with unsaturated C═C double bond. The cross‐linked quasi‐solid electrolyte (CPDOL‐DMA QSE) demonstrates a wide ESW of 4.5 V versus Li + /Li and a high Li + transference number of 0.64. This crosslinked network facilitates lithium salt dissociation, weakens Li + ‐polymer interactions, and achieves the reversibility of lithium metal anode disolution/deposition. For CPDOL‐DMA QSE, capacity retention is 83% after the 400th cycle at 25 °C. Moreover, it can perform stable cycling with 82% retention after 200 cycles at an elevated temperature of 80 °C. Due to the high oxygen content of the repeating units in CPDOL‐DMA, microcalorimetry and accelerated calorimetry results further confirm the high safety of the CPDOL‐DMA QSE. This work provides insights into the design of polyether polymer electrolytes with high oxygen contents, realizing thermo‐electrochemical stability in lithium metal batteries.

Surface Fluorination Shielding of Sulfide Solid Electrolytes for Enhanced Electrochemical Stability in All‐Solid‐State Batteries

2025-06-23
Kyu Tae Kim , Jae‐Seung Kim , Ki Heon Baeck +7 more | Advanced Materials
Abstract Despite their high Li + conductivity and deformability, sulfide solid electrolytes suffer from limited electrochemical stability, which prevents all‐solid‐state batteries (ASSBs) from reaching their full performance potential. Herein, a 
 Abstract Despite their high Li + conductivity and deformability, sulfide solid electrolytes suffer from limited electrochemical stability, which prevents all‐solid‐state batteries (ASSBs) from reaching their full performance potential. Herein, a facile surface fluorination strategy is presented for Li 6 PS 5 Cl using XeF 2 as a solid‐state fluorinating agent, enabling a scalable dry process at moderate temperatures. An ≈37.3 nm‐thick uniform fluorinated layer is coated on an Li 6 PS 5 Cl surface, preserving 82.8% of the initial Li + conductivity (from 2.9 × 10⁻ 3 only to 2.4 × 10⁻ 3 S cm⁻Âč at 30 °C). The underlying fluorination mechanism, deduced through systematic investigations using X‐ray photoelectron spectroscopy, X‐ray Rietveld refinement, nuclear magnetic resonance, and density functional theory calculations, involves the formation of surface oxidative byproducts and F substitution within the lattice. When applied to LiNi 0.90 Co 0.05 Mn 0.05 O 2 electrodes in LiNi 0.90 Co 0.05 Mn 0.05 O 2 ||(Li‐In) half cells at 30 °C, the fluorinated Li 6 PS 5 Cl substantially improves the electrochemical performance, delivering superior discharge capacities (e.g., 186.9 vs 173.6 mA h g −1 at 0.33C), capacity retention, and safety characteristics compared to unmodified Li 6 PS 5 Cl. This enhancement is attributed to the formation of a robust fluorinated cathode electrolyte interphase that mitigates Li 6 PS 5 Cl oxidation. Finally, the stable operation of a pouch‐type LiNi 0.90 Co 0.05 Mn 0.05 O 2 ||Li ASSB is demonstrated, highlighting the scalability of the proposed approach.

A Perspective on Computer Simulation of Liquid Electrolytes for Energy Storage

2025-06-23
Adriano Pierini , Enrico Bodo | ACS electrochemistry.

Experimental and Theoretical Determination of Limiting Current of SEO/LiTFSI Block Copolymer Electrolytes from the Dilute Limit to the Solubility Limit

2025-06-23
Lily A. Gido , Eric Schaible , Chenhui Zhu +1 more | Macromolecules

Data-Driven Insight into the Universal Structure–Property Relationship of Catalysts in Lithium–Sulfur Batteries

2025-06-23
Zhiyuan Han , Shengyu Tao , Yeyang Jia +7 more | Journal of the American Chemical Society
Despite tremendous efforts in catalyzing the sulfur reduction reaction (SRR) in high-capacity lithium-sulfur (Li-S) batteries, understanding the universal and quantitative structure-property relationships (UQSPRs) of SRR remains elusive. Such an unclarity 
 Despite tremendous efforts in catalyzing the sulfur reduction reaction (SRR) in high-capacity lithium-sulfur (Li-S) batteries, understanding the universal and quantitative structure-property relationships (UQSPRs) of SRR remains elusive. Such an unclarity results from the limitations of first-principle calculations in analyzing vast, high-dimensional, and heterogeneous data. Here, we present a collaborative data-driven model for heterogeneous catalytic knowledge fusion, detecting over 2,900 articles on SRR published between 2004 and 2024. By using sure independence screening and sparsifying operator, we surprisingly identified a composite descriptor, D, dominated by the dispersion factor. In contrast to the classical electronic state analysis framework, the dispersion factor directly established UQSPRs between atom topological arrangement and catalyst-polysulfide interaction intensity, accurately predicting the catalytic activity of over 800 types of catalysts. Combined with a volcano plot linking the overpotential to the interaction intensity, we determined the D value range of high catalytic activity, facilitating the discovery of tens of novel SRR catalysts from 374,833 candidates, many of which escaped previous human chemical intuition. As a representative, CrB2 demonstrated superior catalytic activity under high sulfur loadings of 12.0 mg cm-2 and low temperatures of -25 °C. Pouch cells with CrB2 achieved a gravimetric specific energy of 436 Wh kg-1 under a high sulfur content of 76.1% and lean-electrolyte conditions of 2.8 ÎŒL mg-1. Our data-driven method enables new opportunities to fundamentally identify UQSPRs using vast and heterogeneous data, suggesting the promise of revisiting under-exploited knowledge from the historical literature for novel catalyst discovery.

Enhancing homogeneity and ionic conductivity in phosphorus-based ultra-high capacity anodes with a natural polysaccharide Binder: Guar gum

2025-06-23
Shaowen Dong , Li Wang , Xiaolong Huang +2 more | Journal of Power Sources

Enhancement of PPC-PVdF blend electrolyte properties via incorporation of WO3 nanoparticles for advanced energy storage applications

2025-06-23
K. Sashmitha , Usha Rani M | Emergent Materials

Fluorinated gel polymer electrolytes for high performance lithium metal batteries: a mechanism analysis and systematic review

2025-06-23
Ronggen Zhang , Chenyu Li , Bingbing Yang +5 more | Science China Chemistry

Revealing the Hidden Polysulfides in Solid-State Na–S Batteries: How Pressure and Electrical Transport Control Kinetic Pathways

2025-06-23
Hung Quoc Nguyen , Mikael Dahl Kanedal , Juraj Todt +7 more | Journal of the American Chemical Society
Room temperature operation of Na-S batteries with liquid electrolytes is plagued by fundamental challenges stemming from polysulfide solubility and their shuttle effects. Inorganic solid electrolytes offer a promising solution by 
 Room temperature operation of Na-S batteries with liquid electrolytes is plagued by fundamental challenges stemming from polysulfide solubility and their shuttle effects. Inorganic solid electrolytes offer a promising solution by acting as barriers to polysulfide migration, mitigating capacity loss. While the sequential formation of cycling products in molten-electrode and liquid electrolytes-based Na-S batteries generally aligns with the expectations from the Na-S phase diagram, their presence, stability, and transitory behavior in systems with inorganic solid electrolytes at room temperature, remain poorly understood. To address this, we employed operando scanning microbeam X-ray diffraction, operando X-ray photoelectron spectroscopy and ex-situ X-ray absorption spectroscopy to investigate the sulfur conversion mechanisms in Na-S cells with Na3PS4 and Na4(B10H10)(B12H12) electrolytes. Our findings reveal the formation of crystalline and amorphous polysulfides, including those predicted by the Na-S phase diagram (e.g., Na2S5, Na2S4, Na2S2, Na2S), high-order polysulfides observed in liquid-electrolyte systems (e.g., Na2Sx, where x = 6-8), and phases like Na2S3 typically stable only under high-temperature or high-pressure conditions. We demonstrate that these transitions are governed by diffusion-limited kinetics and localized stress concentrations, emphasizing the critical role of pressure, which serves as both a thermodynamic variable, as well as a design parameter, for optimizing solid-state Na-S battery performance necessary for pushing these cells closer to the commercial frontier.

The Development of Lithium Solid-state Batteries and the Comparisons Between Lithium and OtherMetal Elements

2025-06-23
yingxin li | Applied and Computational Engineering
Due to the global trend of electric transportation and green energy storage, there has been an increase in research on battery materials. In particular, lithium-ion batteries are currently the most 
 Due to the global trend of electric transportation and green energy storage, there has been an increase in research on battery materials. In particular, lithium-ion batteries are currently the most popular mobile electric energy source. Through the method of literature review, this paper discusses the advantages and operation principle of solid-state lithium-ion (Li-ion) batteries, and the comparisons between the Li-ion and other replaceable elements for batteries under different conditions. This paper gives conclusions that although large human forces researched lithium-ion batteries in the past and they became the most commonly applied metal ion battery, some other replaceable metal-ions also attracted much recent innovation attention due to some of their technical advances compared to Li-ion, but cannot replace lithium in the short run as a result of some other problems related to application in real situations.

Enhanced Li Transference in Polymer Electrolytes: Why Anion Size Affects Cation Mobility

2025-06-23
Simon Buyting , Monika Schönhoff | ACS Applied Polymer Materials

Improve the Internal and Interface Stability of Sulfide‐Based Composite Electrolytes Through High Concentration Electrolyte and Continuous Li<sup>+</sup> Conductive Frameworks

2025-06-23
Jie Zhang , Chengshuai Bao , Jun Jin +2 more | Small Methods
Abstract Composite electrolytes have received widespread attention due to their potential to simultaneously integrate the advantages of different types of electrolytes. However, composite electrolytes based on sulfides and polymers electrolyte 
 Abstract Composite electrolytes have received widespread attention due to their potential to simultaneously integrate the advantages of different types of electrolytes. However, composite electrolytes based on sulfides and polymers electrolyte still face issues such as instability toward lithium metal, low ion transference number, and instability between polymers and sulfides. Based on this, a composite electrolyte based on a continuous conductive Li 5.4 PS 4.4 Cl 1.6 (LPSC) framework with polytetrafluoroethylene (PTFE) is prepared as a binder (LPSC@PTFE) and gel electrolyte containing high concentration lithium salt. The gel electrolyte fills the pores in the LPSC@PTFE membrane and protects the interface between the sulfide electrolyte and lithium metal. In addition, high‐concentration electrolytes exhibit better stability compared to low‐concentration electrolytes, whether for lithium metal or sulfides. The improvement has been demonstrated in stability through analysis of in‐situ electrochemical impedance spectroscopy (EIS) combined with relaxation time distribution (DRT), as well as characterization by X‐ray photoelectron spectroscopy (XPS) and Raman spectroscopy. The mechanism behind the performance enhancement through theoretical calculations and simulations has also been speculated on. The optimized composite electrolyte membrane has an electrochemical window of 4.98 V, an increased ion transference number of 0.74, a critical current density of 1.8 mA cm −2 @0.1 mAh cm −2 , and can cycle for more than 4000 h at a current density of 0.1 mA cm −2 @0.1 mAh cm −2 . After matching with LiFePO 4 (LFP) cathode, the capacity retention rate is 94.1% after 150 cycles at a rate of 1C and 89.7% after 150 cycles at a rate of 2C.

Impact of Cathode Microstructure on Sulfur Redox Kinetics in Lithium–Sulfur Batteries

2025-06-23
K. H. Liao , Arumugam Manthiram | Advanced Energy Materials
Abstract Lithium–sulfur (Li–S) batteries offer high theoretical energy density and employ earth‐abundant sulfur, making them a promising next‐generation energy storage technology. Although essential for practical energy densities, high sulfur loadings, 
 Abstract Lithium–sulfur (Li–S) batteries offer high theoretical energy density and employ earth‐abundant sulfur, making them a promising next‐generation energy storage technology. Although essential for practical energy densities, high sulfur loadings, and lean‐electrolyte contents lead to poor sulfur kinetics/utilization and cycle life. This study highlights the critical role of electrode microstructure in resolving these challenges. The particle morphology and size of a ketjenblack/sulfur composite are controlled through a scalable spray‐drying procedure (SD‐KB/S), producing an optimized cathode structure with uniform sulfur distribution and enhanced mechanical integrity with minimal electrode cracking. At a sulfur loading of 4 mg cm −2 and an electrolyte‐to‐sulfur (E/S) ratio of 6, SD‐KB/S cathodes exhibit stable cycling performance, retaining a capacity of 768 mA h g −1 after 100 cycles, contrasting severe capacity fade with conventional electrodes. A cell overpotential deconvolution unveils that the activation overpotential (typically the largest barrier in conventional cells) is notably reduced in SD‐KB/S cells. Although the concentration overpotential is also reduced with SD‐KB/S, it becomes a prominent contributor to cell polarization, revealing the need to consider diffusional limitations in practical Li–S batteries. This work emphasizes the importance of advancing electrode and catalyst design concurrently—rather than sole catalyst development—to achieve high‐performance and commercially viable Li–S batteries.

Iridium Cluster Decoration on Amorphous Cobalt Oxide‐Coated Carbon Nanotubes for High‐Performance Lithium‐Oxygen Battery Cathodes

2025-06-23
Yuqing Yao , Shang Wang , Xinyang Ma +7 more | Small
Abstract Lithium‐oxygen batteries hold great promise for next‐generation energy storage due to their exceptionally high theoretical energy density. However, their practical application is hindered by the sluggish kinetics associated with 
 Abstract Lithium‐oxygen batteries hold great promise for next‐generation energy storage due to their exceptionally high theoretical energy density. However, their practical application is hindered by the sluggish kinetics associated with the oxygen reduction reaction and oxygen evolution reaction, resulting in severe voltage polarization and limited cycling stability. Herein, a simple solvent thermal reaction and a one‐step reduction reaction is developed, where amorphous cobalt oxide (CoO) is uniformly coated on multi‐walled carbon nanotubes (CNT) and further decorated with highly dispersed iridium (Ir) clusters. The amorphous CoO coatings preferentially nucleate at CNT defect sites, which not only passivates surface defects but also facilitates the homogeneous distribution of Ir clusters. This unique Ir/CoO@CNT architecture provides abundant active sites and promotes efficient electronic and ionic transport, thereby enhancing the electrocatalytic activity and overall battery performance. The synergistic effect between the highly active Ir clusters and the amorphous CoO, which accelerates reaction kinetics and stabilizes the electrode interface. As a result, the Ir/CoO@CNT cathode achieves a high discharge capacity of ≈6700 mAh g −1 , with a low overpotential of 0.96 V and exhibits excellent cycling stability, sustaining over 150 cycles under a limited capacity of 500 mAh g −1 at 500 mA g −1 .

Manganese‐Incorporated Single‐Phase High‐Entropy Oxide Modified Separator Enabled High Performance of Lithium‐Sulfur Batteries at High Sulfur Loading

2025-06-22
Hassan Raza , Junye Cheng , Subash Kandasamy +7 more | Energy & environment materials
High‐entropy oxides (HEOs) have sparked scientific interest recently as a potential material technology for lithium‐sulfur (Li–S) batteries. This interest stems from their simultaneous roles as sulfur hosts and electrocatalysts, which 
 High‐entropy oxides (HEOs) have sparked scientific interest recently as a potential material technology for lithium‐sulfur (Li–S) batteries. This interest stems from their simultaneous roles as sulfur hosts and electrocatalysts, which provide enhancements to the performance of sulfur cathode composites. Nonetheless, their incorporation into the active material blend results in compromised energy density, particularly when their gravimetric proportion is substantial (≄10 wt.%, in the sulfur‐based cathode). In this study, a manganese (Mn)‐containing HEO (S config ≄ 1.5R) was synthesized and subsequently coated onto a commercial Celgard separator at a low areal loading (~0.23 mg cm −2 ) with the aim of decreasing HEO content in the cathode composite material while still boosting lithium polysulfide (LPS) conversion kinetics. Li–S batteries incorporating this modified separator‐high entropy oxide (MS‐HEO) demonstrate exceptional electrochemical performance, achieving a high initial discharge capacity of ~1642 mAh g −1 at 0.1 C and a remarkably low‐capacity fade rate of 0.055% per cycle over 450 cycles at 1 C. Remarkably, the MS‐HEO batteries exhibited commendable electrochemical performance at high sulfur loading (~7 mg cm −2 ), delivering an initial discharge capacity of ~819 mAh g −1 during the first discharge and maintaining stable cycling up to 30 cycles at 0.1 C thereafter. Collectively, this work underscores the significance of precise adjustment of HEO compositions through low‐temperature MOF calcination strategies and demonstrates their potential to enhance the electrochemical performance of Li–S batteries under the high‐sulfur loading conditions necessary for future commercial applications.

Advancements in Molecular Sieves for Emerging Energy Applications

2025-06-22
Fernando G. Torres , JesĂșs Tapia Sagarna , Omar P. Troncoso | Energy Technology
The limitations of traditional energy technologies have become increasingly evident as the demand for sustainable energy solutions rises, particularly concerning efficiency and environmental impact. In this context, molecular sieves (MS) 
 The limitations of traditional energy technologies have become increasingly evident as the demand for sustainable energy solutions rises, particularly concerning efficiency and environmental impact. In this context, molecular sieves (MS) emerge as key materials to improve the properties of these energy systems due to their porous structure and high surface area. These features make them ideal for their use as electrodes or separators in batteries and capacitors, while their ability to separate molecules based on size is helpful in fuel refining for fuel cells. Common types of MS include zeolites, metal‐organic framework‐based materials, carbon MS, and polymers of intrinsic microporosity. In this review, the applications of MS in energy storage and conversion systems are explored examining their roles in batteries, capacitors, fuel cells, and solar cells. The mechanisms behind the performance improvement of electrodes, electrolytes, and separators are reviewed, including the mitigation of dendrite formation, the increment in catalytic activity, and the increment of cycle durability, among others. By summarizing these advancements, this work aims to show an overview of the potential of MS in the development of novel components for the fabrication of long‐lasting, efficient, and ecologically friendly energy storage and generation devices.

Ultra‐Thin Lithium–Phosphorus–Sulfur (LPS) Interfacial Electrolyte Layer for All‐Solid‐State Lithium Metal Battery with High‐Rate and High‐Areal‐Capacity Performance

2025-06-22
Yu Su , Yuxi Deng , Yu Luo +7 more | Advanced Functional Materials
Abstract To solve the challenging interfacial issues of all‐solid‐state lithium batteries (ASSLBs), a novel strategy to construct a nano‐scale lithium‐phosphorus‐sulfur (LPS) electrolyte film by atomic layer deposition (ALD) technique and 
 Abstract To solve the challenging interfacial issues of all‐solid‐state lithium batteries (ASSLBs), a novel strategy to construct a nano‐scale lithium‐phosphorus‐sulfur (LPS) electrolyte film by atomic layer deposition (ALD) technique and to coat it on Li 6 PS 5 Cl (LPSCl) electrolyte is proposed and demonstrated for the first time. The modified LPS@LPSCl electrolytes exhibit excellent compatibility with both high‐voltage cathodes and pure lithium metal anode with enhanced ionic conductivity, much reduced electronic conductivity, and modified mechanical strength, which can fill the gaps in the base electrolytes after electrolyte pellet pressing and reduce interfacial defects in the composite electrolytes. The sulfide‐based ASSLBs, assembled with LPS@LPSCl, Al‐GL@NCM811 materials, and a lithium indium anode, achieves a high areal capacity of 10.6 mAh cm −2 at high‐temperature and high mass loading (60 °C, 51.9 mg cm −2 ). Additionally, LPS@LPSCl has high stability toward lithium metal, suppressing interfacial side reactions and improving physical contact, enabling charge and discharge testing at a high current density of 1.5 mA cm −2 . This study demonstrates that the nano‐scaled film formation of sulfide solid‐state electrolytes can significantly reduce the polarization voltage of traditional double‐layer electrolytes toward lithium metal, and provide a new approach for interfacial modification in sulfide solid‐state batteries.

Minimizing Solvent‐Coordination in Ether Electrolytes for Lithium Metal Batteries under Extreme Operating Conditions

2025-06-22
Haipeng Zhu , Qiangfeng Cliff Zhang , Kefei Wang +6 more | Advanced Materials
Abstract Ether‐based electrolytes are considered to be one of the most promising systems for high‐performing lithium metal batteries (LMBs). However, the poor oxidation stability (&lt;4.5 V) of ether solvents seriously 
 Abstract Ether‐based electrolytes are considered to be one of the most promising systems for high‐performing lithium metal batteries (LMBs). However, the poor oxidation stability (&lt;4.5 V) of ether solvents seriously limit their practical applications. Herein, high‐voltage LMBs with LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) cathode operated under extreme conditions by minimizing solvent‐coordination in ether electrolytes with fluoroethers, nitrile ethers, and highly fluorinated additives, are demonstrated. It is revealed that ethylene glycol bis(propionitrile) ether (DENE) inhibits the lone‐pair electrons loss on ether oxygen through strongly electron‐withdrawing cyano groups to increase the electrochemical window to ≄5 V. Heptafluorobutyric anhydride (HFAA) triggers the formation of solid electrolyte interphase rich‐in LiF‐species, ensuring uniform deposition/stripping and high reversibility of Li + . Especially, DENE and HFAA synergistically minimizes the coordination number of ethylene glycol dimethyl ether (DME) and hexafluorophosphate (PF 6 ‐ ), thereby promoting the desolvation process of Li + and inhibiting the interfacial side reactions. Therefore, the NCM811 cathodes using modified electrolytes exhibit excellent electrochemical performance at ultrahigh voltage (4.7 V), ultrahigh rate (20 C), and ultrawide temperature range (−30 to 120 °C), and achieve stable operation in a high‐capacity Li metal pouch cell of 30 Ah and a high‐energy density Li metal pouch cell of 502.7 Wh kg −1 , respectively.

Progress in graphene–sulfur–lithium-ion batteries for electric vehicles: a forward-looking evaluation

2025-06-21
Abu Shadate Faisal Mahamude , Kaniz Farhana , Wan Sharuzi Wan Harun | Deleted Journal

Recent progress and application frontiers of 2D layered double hydroxides in lithium-sulfur batteries

2025-06-21
Jia‐Wei Feng , Yanshuang Meng , Dongming Qi +3 more | Journal of Energy Storage

Ionic Conductivity and Lithium Transference Number in LiClO<sub>4</sub>-Doped Carboxymethyl Cellulose

2025-06-20
Marco Luis Lobato de Faria , Anh Ngoc Tram , Arqum Shami +1 more | The Journal of Physical Chemistry C

Separator Engineering Regulating Reversible Li Electrodeposition Enabled by Lithiophilic Polyimide@Ag Coating Layer for Dendrite‐Free Lithium Metal Batteries

2025-06-20
Zhaoyi Wang , Hanrui Xu , Kefan Liu +7 more | Small
Abstract Heterogeneity Li deposition predominantly induce the growth of Li dendrite, which hinders the practical application of lithium metal batteries (LMBs). Previous researches have mainly focused on the modification of 
 Abstract Heterogeneity Li deposition predominantly induce the growth of Li dendrite, which hinders the practical application of lithium metal batteries (LMBs). Previous researches have mainly focused on the modification of lithium anode, but lithium is sensitive to water and oxygen, which consequently limits its industrialization process. Herein, a novel polyimide@Ag coated polyethylene separator ((PI@Ag)/PE) strategy is reported to inhibit Li dendrites growth. It has been clarified that the lithiophilic PI@Ag microspheres can greatly reduce the nucleation barrier of Li electrodeposition. Consequently, the Li//Li cells with this separator exhibit stable and dendrite‐free Li + plating/stripping over 2000 h at 1 mAh cm −2 and 500 h at 5 mAh cm −2 . Moreover, the LiFePO 4 //Li cells and Ni 0.8 Co 0.1 Mn 0.1 //Li cells exhibit excellent cycling performance and capacity retention after 400 cycles at 1C. Multiple characterization analyses have proved that the lithiophilic PI@Ag layer can significantly inhibit the growth of Li dendrites and help to construct a stable solid electrolyte interfacial (SEI) layer. The above results manifest that the present strategy provides a simple and generalized achievable method to solve the lithium dendrite problem, demonstrating bright engineering application value and broad prospect.

Synergistic Lithium Alloying and Plating in 3D Cu/CNT/Sn Electrodes for Stable Lithium Metal Batteries

2025-06-20
Sul Ki Park , Soochan Kim , Ruhan He +6 more | Small
Abstract Anode‐less Li‐ion batteries, in which Li is reversibly plated onto and stripped from a metal current collector during charge and discharge, theoretically offer the highest possible anode energy density. 
 Abstract Anode‐less Li‐ion batteries, in which Li is reversibly plated onto and stripped from a metal current collector during charge and discharge, theoretically offer the highest possible anode energy density. However, such systems suffer from rapid self‐discharge, excessive solid electrolyte interphase (SEI) formation, and dendritic lithium growth, resulting in severe performance degradation and safety concerns. Here, these challenges are addressed by introducing a novel 3D current collector that enables energy storage via a hybrid mechanism of alloying and plating. The 3D current collectors are fabricated through two scalable electroplating processes involving a porous Cu plating process followed by a Sn surface coating, and are structurally reinforced with carbon nanotubes (CNTs) to form a mechanically robust and conductive scaffold. The relative contributions of the alloying and plating reactions to the cell capacity are modulated by adjusting the thickness of the Sn layer, which governs the extent of lithiation through alloy formation. By optimizing the capacity distribution between Sn alloying and Li plating, the resulting half‐cell exhibits stable cycling over 200 cycles with an average Coulombic efficiency of 93.9%, significantly outperforming a control cell with planar Cu foils, which retain only 71.3% efficiency after 110 cycles.

Simultaneous Effects of C‐N‐V Bonds and Multiple Sulfides Anchoring Active V and Na Enables Honeycomb‐Like Porous Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> with Non‐Attenuation Characteristics for Na‐Ion Batteries

2025-06-20
Rui Du , Changcheng Liu , Que Huang +4 more | Small
Abstract For Na 3 V 2 (PO 4 ) 3 (NVP) cathode, the activity and utilization rate of Na and V is the key to affecting its electrochemical properties. However, 
 Abstract For Na 3 V 2 (PO 4 ) 3 (NVP) cathode, the activity and utilization rate of Na and V is the key to affecting its electrochemical properties. However, few studies can simultaneously optimize both. Currently, a facile hydrothermal route is proposed to successfully synthesize the honeycomb‐like porous NVP@CHSLS cathodes possessing anchoring effects to enhance the immobilization of active Na/V through in situ carbonation with chitosan and sodium lignosulfonate. DFT calculations demonstrate the N/S co‐doped carbon skeleton gains more electrons and behaves with superior charge transfer capability. Accordingly, XAFS verifies the existence of hypervalent V 4+ for the charge balance, as well as a newly generated C‐N‐V bond inside the bulk, which significantly inhibits the dissolution of V in the electrolyte. Moreover, ex‐situ and after‐cycled XRD verifies beneficial electrochemical intermediums such as Na 2 S manifest extra sodium fixation characteristics, which not only enter into the CEI membrane to reduce the loss of Na + , but also participate in the de‐intercalation of Na + . Furthermore, honeycomb‐like porous morphology enriches the active sites for Na + migration and improves the wettability of electrolytes, demonstrated by contact Angle and AFM tests. Consequently, the optimized NVP@CHSLS‐2 reveals a high postactivated capacity of 104.5 mAh g −1 at 60 C, and it remains at 98.8% after 10 000 cycles at 60 C.

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