Featured
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| Open AccessSynergetic regulation of SEI mechanics and crystallographic orientation for stable lithium metal pouch cells
The application of Li-metal batteries (LMBs) is impeded by unstable solid electrolyte interphase (SEI) and uncontrollable Li dendrites growth. Here, the authors present an YF3/PMMA composite layer to achieve high-performance LMBs via the synergetic regulation of SEI mechanics and Li crystallography.
- Yanhua Zhang
- , Rui Qiao
- & Jiangxuan Song
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Article
| Open AccessLaCl3-based sodium halide solid electrolytes with high ionic conductivity for all-solid-state batteries
The advancement of sodium halide solid-state electrolytes can propel high-energy-density all-solid-state sodium-ion batteries. Here, the authors present a LaCl3-based electrolyte facilitating rapid Na+ ion conduction along the c-axis diffusion channel, ensuring high capacity even at elevated current densities.
- Chengyu Fu
- , Yifan Li
- & Hongfa Xiang
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Article
| Open AccessPhysics-informed neural network for lithium-ion battery degradation stable modeling and prognosis
Reliable lithium-ion battery health assessment is vital for safety. Here, authors present a physics-informed neural network for accurate and stable state-of-health estimation, overcoming challenges of varied battery types and usage conditions.
- Fujin Wang
- , Zhi Zhai
- & Xuefeng Chen
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Article
| Open AccessA scalable Li-Al-Cl stratified structure for stable all-solid-state lithium metal batteries
Sulfide electrolytes’ incompatibility with Li metal hinders their use in all-solid-state Li metal batteries. Here, the authors propose a scalable Li-Al-Cl stratified structure, formed via strain-activated phase separation, to effectively stabilize the negative electrode/electrolyte interface.
- Han Su
- , Jingru Li
- & Jiangping Tu
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Comment
| Open AccessA critical discussion of the current availability of lithium and zinc for use in batteries
Aqueous zinc batteries are currently being explored as potential alternatives to non-aqueous lithium-ion batteries. In this comment, the authors highlight zinc’s global supply chain resilience and lower material costs yet caution about its higher mass requirement for comparable charge storage.
- Alessandro Innocenti
- , Dominic Bresser
- & Stefano Passerini
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Article
| Open AccessSustainable upcycling of mixed spent cathodes to a high-voltage polyanionic cathode material
Direct recycling of critical battery materials bring promise but a challenge for the mixed cathode chemistries. Here, the authors report a sustainable upcycling approach, transforming degraded LiFePO4 and Mn-rich cathodes into a high-voltage polyanionic material with an increased energy density and economic value.
- Guanjun Ji
- , Di Tang
- & Hui-Ming Cheng
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Article
| Open AccessA locally solvent-tethered polymer electrolyte for long-life lithium metal batteries
Solid polymer electrolytes containing N,N-dimethylformamide (DMF) exhibit improved Li+ conductivity but poor cycle life due to incompatibility between the Li metal anode and DMF. Here, the authors report a polymer electrolyte composited with Hofmann-DMF complex that achieves both high Li+ conductivity and long cycle life.
- Yanfei Zhu
- , Zhoujie Lao
- & Guangmin Zhou
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Article
| Open AccessStarch-mediated colloidal chemistry for highly reversible zinc-based polyiodide redox flow batteries
The development of porous membranes that could work under high power density brings promise but a challenge with polyiodide cross-over for aqueous Zn-I flow batteries. Here, the authors develop a colloidal starch-based catholyte to inhibit cross-over that endows reversible flow cell performance.
- Zhiquan Wei
- , Zhaodong Huang
- & Chunyi Zhi
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Article
| Open AccessPolymer hetero-electrolyte enabled solid-state 2.4-V Zn/Li hybrid batteries
Zn batteries suffer from low voltage due to the high redox potential of the Zn anode and the low potential of traditional cathodes. Here, the authors develop a polymer hetero-electrolyte, which allows separated Zn and Li reversibility and achieves a 2.4 V-Zn battery based on the LiNi0.5Mn1.5O4 cathode.
- Ze Chen
- , Tairan Wang
- & Chunyi Zhi
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Article
| Open AccessCreep-type all-solid-state cathode achieving long life
Electrochemical-mechanical issues bring challenges but create new opportunities to design innovative all-solid-state batteries. Here, the authors propose to use the (de)lithiation-stress-creep synergistic time-dependent evolution to boost the electrochemical performance of all-solid-state batteries.
- Xiaolin Xiong
- , Ting Lin
- & Liumin Suo
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Article
| Open AccessNear-strain-free anode architecture enabled by interfacial diffusion creep for initial-anode-free quasi-solid-state batteries
Initially anode-free batteries with garnet-type solid-state electrolytes suffer from internal strain by repeated Li plating/stripping. Here, the authors propose a near-strain-free anode architecture for interfacial diffusion of Li metal that suppresses volume expansion during cycling.
- Kwang Hee Kim
- , Myung-Jin Lee
- & Jong Hyeok Park
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Article
| Open AccessSub-millisecond lithiothermal synthesis of graphitic meso–microporous carbon
Porous carbons with high specific surface area and electronic conductivity are of interest for their electron and ion transport ability. Here authors use ultra-high temperature reactions of Li metal and polytetrafluoroethylene to make graphitized porous carbon for electrochemical energy storage.
- Huimin Zhang
- , Jingyi Qiu
- & Hao Zhang
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Article
| Open AccessCatalytic role of in-situ formed C-N species for enhanced Li2CO3 decomposition
Sluggish kinetics of the CO2 reactions lead to the accumulation of Li2CO3 residuals, which hinders the cycling stability of Li-CO2 batteries. Here, the authors reveal the catalytic role of in-situ formed C-N species in enhancing the reversibility of Li2CO3 and cycle life of Li-CO2 batteries.
- Fangli Zhang
- , Wenchao Zhang
- & Zaiping Guo
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Article
| Open AccessUnderstanding the charge transfer effects of single atoms for boosting the performance of Na-S batteries
Efficient charge transfer in sulfur electrodes is a crucial challenge for sodium-sulfur batteries. Here, the authors developed a machine-learning-assisted approach to quickly identify effective single-atom catalysts that enhance selectivity for short-chain sodium polysulfides, leading to improved battery performance.
- Yao-Jie Lei
- , Xinxin Lu
- & Guoxiu Wang
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Article
| Open AccessHybridizing carbonate and ether at molecular scales for high-energy and high-safety lithium metal batteries
Here, authors report a linear functionalized solvent through molecular hybridization. Complementary ethers and carbonates are integrated into a single molecule, exhibiting properties suited for high-energy and high safety lithium metal batteries.
- Jiawei Chen
- , Daoming Zhang
- & Yongyao Xia
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Article
| Open AccessChlorine bridge bond-enabled binuclear copper complex for electrocatalyzing lithium–sulfur reactions
Here, the authors report a homonuclear cooper dual-atom electrocatalyst with high activity designed for synchronously boosting the sulfur and lithium evolutions.
- Qin Yang
- , Jinyan Cai
- & Yingze Song
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Article
| Open AccessManipulating the diffusion energy barrier at the lithium metal electrolyte interface for dendrite-free long-life batteries
Constructing an artificial solid electrolyte interphase to protect the lithium metal electrode is promising but challenging. Here, authors report a facile approach to form a layer to simultaneously overcome diffusion and advection-limited ion transport to achieve dendrite-free Li plating/stripping.
- Jyotshna Pokharel
- , Arthur Cresce
- & Yue Zhou
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Article
| Open AccessEnhancements of electric field and afterglow of non-equilibrium plasma by Pb(ZrxTi1−x)O3 ferroelectric electrode
The physics of how ferroelectric materials enhance plasma properties and discharge is unclear. Here, the authors enhance surface charge, electric field and afterglow of nonequilibrium plasma by ferroelectric barrier discharge with evidence from laser diagnostics.
- Yijie Xu
- , Ning Liu
- & Yiguang Ju
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Article
| Open AccessOvercoming low initial coulombic efficiencies of Si anodes through prelithiation in all-solid-state batteries
All-solid-state batteries with silicon anodes have high capacities but low initial coulombic efficiencies (ICEs) because of first cycle irreversible capacity loss. Here, the authors report a prelithiation strategy to improve ICEs and reversibility.
- So-Yeon Ham
- , Elias Sebti
- & Ying Shirley Meng
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Article
| Open AccessActivating reversible carbonate reactions in Nasicon solid electrolyte-based Na-air battery via in-situ formed catholyte
Metal-air batteries, operated in ambient air, suffer from irreversible redox reactions, limiting their energy density. Herein, the authors present a solid electrolyte-based sodium-air battery with a reversible carbonate reaction, facilitated by the in-situ formed catholyte enabled by moisture.
- Heetaek Park
- , Minseok Kang
- & Byoungwoo Kang
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Article
| Open AccessIsotope engineering achieved by local coordination design in Ti-Pd co-doped ZrCo-based alloys
Hydrogen isotope effect in metal-hydrogen systems disturbs precise Deuterium/Tritium (D/T) ratio control. Here, the authors demonstrate a local coordination strategy that comprises thermodynamic destabilization with vibration enhancement of interstitial isotopes for isotope engineering.
- Jiacheng Qi
- , Xu Huang
- & Lixin Chen
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Article
| Open AccessMonolithically integrated micro-supercapacitors with high areal number density produced by surface adhesive-directed electrolyte assembly
A challenge for densely packed micro-supercapacitors (MSCs) is accurate electrolyte placement. Here authors report a surface adhesive-directed electrolyte assembly strategy for precise isolation of densely packed MSCs at micron scale.
- Sen Wang
- , Shuanghao Zheng
- & Zhong-Shuai Wu
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Article
| Open AccessAtomic reconstruction for realizing stable solar-driven reversible hydrogen storage of magnesium hydride
Researchers demonstrate a single phase Mg2Ni(Cu) alloy via atomic reconstruction to achieve the ideal integration of photothermal and catalytic effects, leading to a 6.1 wt. % H2 reversible capacity with 95 % retention under 3.5 W cm−2.
- Xiaoyue Zhang
- , Shunlong Ju
- & Xuebin Yu
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Article
| Open AccessDynamical evolution of CO2 and H2O on garnet electrolyte elucidated by ambient pressure X-ray spectroscopies
Li6.5La3Zr1.5Ta0.5O12 (LLZO) is a promising solid electrolyte but suffers from severe surface degradation in air. Here, authors use mapping of resonant Auger spectroscopy and various ambient pressure X-ray spectroscopies to elucidate the dynamical evolution of CO2 and H2O on clean LLZO surfaces.
- Nian Zhang
- , Guoxi Ren
- & Xiaosong Liu
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Article
| Open AccessAn integrated high-throughput robotic platform and active learning approach for accelerated discovery of optimal electrolyte formulations
Solubility determines energy density in redox flow batteries. Here, authors combine automated experiments with machine learning to efficiently identify solvents that significantly enhance solubility, testing less than 10% of over 2000 candidates.
- Juran Noh
- , Hieu A. Doan
- & Yangang Liang
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Article
| Open AccessGrave-to-cradle photothermal upcycling of waste polyesters over spent LiCoO2
The increasing production of lithium-ion batteries and plastics presents significant challenges to resource sustainability and ecosystem integrity. This study highlights the utilization of spent lithium cobalt oxide cathodes as photothermal catalysts to transform various waste polyesters into valuable monomers.
- Xiangxi Lou
- , Penglei Yan
- & Jinxing Chen
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Article
| Open AccessPhosphonate-based iron complex for a cost-effective and long cycling aqueous iron redox flow battery
Here, authors report an iron flow battery, using earth-abundant materials like iron, ammonia, and phosphorous acid. This work offers a solution to reduce materials cost and extend cycle life in energy storage applications for grid decarbonization.
- Gabriel S. Nambafu
- , Aaron M. Hollas
- & Guosheng Li
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Article
| Open AccessDeciphering the critical role of interstitial volume in glassy sulfide superionic conductors
Glass sulfide electrolytes are promising materials for solid-state Li metal batteries, yet limited understanding hinders their progress. Here, the authors decipher the dissolution process of halogen dopants in glass and introduce a synthetic strategy to increase halogen dopant’s dissolution capacity.
- Han Su
- , Yu Zhong
- & Jiangping Tu
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Article
| Open AccessA solid-state lithium-ion battery with micron-sized silicon anode operating free from external pressure
Applying high stack pressure is primarily done to address the mechanical failure issue of solid-state batteries. Here, the authors propose a mechanical optimization strategy involving elastic electrolyte to realize solid-state batteries operating without external pressurizing.
- Hui Pan
- , Lei Wang
- & Haoshen Zhou
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Article
| Open AccessDeciphering the contributing motifs of reconstructed cobalt (II) sulfides catalysts in Li-CO2 batteries
Improving catalyst efficiency is vital for Li-CO2 batteries, but understanding catalyst structures during battery operation is hard. Here, the authors uncover catalyst reconstruction and its link to activity, highlighting a self-constructed oxysulfide structure with high activity and stability in Li-CO2 batteries.
- Yingqi Liu
- , Zhiyuan Zhang
- & Hui-Ming Cheng
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Article
| Open AccessElectric vehicle battery chemistry affects supply chain disruption vulnerabilities
Electric vehicle battery supply chains are currently vulnerable to supply disruptions in China, but research shows that the cumulative effect of multiple supply chain steps creates additional vulnerabilities across multiple critical battery minerals.
- Anthony L. Cheng
- , Erica R. H. Fuchs
- & Jeremy J. Michalek
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Article
| Open AccessProton-selective coating enables fast-kinetics high-mass-loading cathodes for sustainable zinc batteries
Sluggish Zn2+-dominated Faradic reactions lead to suboptimal charge-storage capacity and durability of aqueous zinc battery cathodes. Here, the authors present a proton-selective interfacial coating strategy that enables high-performance cathodes with fast-kinetics proton-dominated Faradic reactions.
- Quanquan Guo
- , Wei Li
- & Xinliang Feng
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Article
| Open AccessMolecular anchoring of free solvents for high-voltage and high-safety lithium metal batteries
Advanced electrolyte is essential for high-energy-density lithium metal batteries. Here, the authors design a molecular anchoring dilute electrolyte via intermolecular hydrogen bonding with free solvents to improve the battery electrochemical and thermal stabilities.
- Zhuangzhuang Cui
- , Zhuangzhuang Jia
- & Xiaodi Ren
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Article
| Open AccessCation desolvation-induced capacitance enhancement in reduced graphene oxide (rGO)
Understanding local electrochemical processes can help improve electrochemical energy storage. Here, the authors report a charge storage mechanism in aqueous electrolyte for reduced graphene oxide using an electrochemical quartz crystal microbalance.
- Kangkang Ge
- , Hui Shao
- & Patrice Simon
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Article
| Open AccessEfficient direct repairing of lithium- and manganese-rich cathodes by concentrated solar radiation
Rapid capacity decay and voltage drop hinder lithium- and manganese-rich cathode material (LMRO) development. Here, the authors apply concentrated solar radiation arrays on cycled LMRO electrodes, inducing inverse spinel phase to boost redox activity and reversibility, yielding enhanced electrochemical performance.
- Hailong Wang
- , Xin Geng
- & Xin He
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Article
| Open AccessLiquid Madelung energy accounts for the huge potential shift in electrochemical systems
Electrode potential in any electrochemical systems has long been discussed by classical Debye-Hückel theory which holds only under extremely dilute concentrations. Here, the authors establish the concept ‘liquid Madelung potential’ to comprehensively describe the potential shift at practical concentrations.
- Norio Takenaka
- , Seongjae Ko
- & Atsuo Yamada
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Article
| Open AccessKirkendall effect-induced uniform stress distribution stabilizes nickel-rich layered oxide cathodes
Nickel-rich layered oxide cathodes offer high energy density yet suffer from mechanical degradation during (de)lithiation. Here, the authors present a strategy that leverages the Kirkendall effect to equalize stress within the cathode particles, thereby stabilizing their structure and enhancing the cycling stability.
- Ziyao Gao
- , Chenglong Zhao
- & Baohua Li
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Article
| Open AccessPromoting high-voltage stability through local lattice distortion of halide solid electrolytes
Solid electrolytes play a crucial role as ion conductors and separator between electrodes in all-solid-state batteries. Here, the authors report a high-entropy halide solid electrolyte, which reveals the structure evolution with the increasing configurational entropy and improves the high-voltage stability.
- Zhenyou Song
- , Tengrui Wang
- & Wei Luo
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Article
| Open AccessCa-dimers, solvent layering, and dominant electrochemically active species in Ca(BH4)2 in THF
Alternatives to lithium-ion electrochemistry present challenges due to undesirable phenomena at the electrode-electrolyte interface. Through simulations, the authors find that the performance of a calcium-based electrolyte is driven entirely by molecular-scale processes within approximately 1 nm of the electrode.
- Ana Sanz Matias
- , Fabrice Roncoroni
- & David Prendergast
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Article
| Open AccessHierarchical Li electrochemistry using alloy-type anode for high-energy-density Li metal batteries
Utilizing an ultra-thin Li anode with a thickness below 50 μm is crucial for enhancing the energy density of batteries. Here, the authors develop a finely tunable, thin alloy-based Li anode that features a hierarchical Li electrochemistry, enabling stable cycling and superior energy density in Li metal batteries.
- Jiaqi Cao
- , Yuansheng Shi
- & Xia Lu
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Article
| Open AccessStructurally robust lithium-rich layered oxides for high-energy and long-lasting cathodes
O2-type Li-rich layered cathodes suppress voltage decay and aid in oxygen redox research. Here, the authors report trilateral relationship among anionic redox utilization, bulk chemo-mechanical degradation, and electrochemical fading, which can be mitigated by balancing the redox center capabilities.
- Ho-Young Jang
- , Donggun Eum
- & Kisuk Kang
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Article
| Open AccessSolvation-property relationship of lithium-sulphur battery electrolytes
In the Li-S battery, a promising next-generation battery chemistry, electrolytes are vital because of solvated polysulfide species. Here, the authors investigate solvation-property relationships via the measurement of solvation free energy of the electrolytes, guiding advanced electrolyte design for Li-S batteries.
- Sang Cheol Kim
- , Xin Gao
- & Yi Cui
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Article
| Open AccessHigh voltage electrolytes for lithium-ion batteries with micro-sized silicon anodes
Micro-sized silicon are promising anode materials due to low-cost and high-energy, yet their application is hindered by inaccessible electrolytes. Here, the authors report sulfolane-based electrolytes that form silicon-phobic interphases and enable high-voltage pouch cells to achieve superior cycle life.
- Ai-Min Li
- , Zeyi Wang
- & Chunsheng Wang
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Article
| Open AccessCapacitive tendency concept alongside supervised machine-learning toward classifying electrochemical behavior of battery and pseudocapacitor materials
Analysis of capacitive behavior of electrode materials used in batteries and pseudocapacitors is challenging. Here, authors report an electrochemical signal analysis method available as an online tool to classify the charge storage behavior of a material as battery-like or a pseudocapacitor-like.
- Siraprapha Deebansok
- , Jie Deng
- & Olivier Fontaine
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Article
| Open AccessDesigning lithium halide solid electrolytes
The pursuit of all-solid-state batteries has motivated advancements in materials design. Here, the authors present a methodology demonstrating that ionic potential effectively captures crucial interactions within halide materials, guiding the design of the new materials with enhanced performance.
- Qidi Wang
- , Yunan Zhou
- & Marnix Wagemaker
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Article
| Open AccessSubtractive transformation of cathode materials in spent Li-ion batteries to a low-cobalt 5 V-class cathode material
Direct recycling or upcycling is promising for sustainable battery resource management. Here, the authors report a subtractive transformation strategy for upcycling spent cathode materials to high-performance 5 V-class cathodes, reducing reliance on rare elements for the sustainable Li-ion battery industry.
- Jun Ma
- , Junxiong Wang
- & Guangmin Zhou
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Article
| Open AccessSelf-assembled hydrated copper coordination compounds as ionic conductors for room temperature solid-state batteries
The design of inorganic-organic hybrid solid-state electrolytes is expected to merge the merits of both inorganic and organic material. Here, the authors craft Li-ion-implanted copper maleate hydrate nanoflakes via a bottom-up self-assembly approach to reveal superior room-temperature Li-ion conductivity.
- Xiao Zhan
- , Miao Li
- & Li Zhang
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Article
| Open AccessOptimizing potassium polysulfides for high performance potassium-sulfur batteries
Potassium-sulfur battery are promising materials for next-generation high energy, low cost batteries. Here the authors explore a tungsten based catalytic composite for optimizing potassium polysulfides and improve K-S electrochemistry in batteries
- Wanqing Song
- , Xinyi Yang
- & Wenbin Hu
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Comment
| Open AccessThe rise of high-entropy battery materials
The emergence of high-entropy materials has inspired the exploration of novel materials in diverse technologies. In electrochemical energy storage, high-entropy design has shown advantageous impacts on battery materials such as suppressing undesired short-range order, frustrating energy landscape, decreasing volumetric change and reducing the reliance on critical metals. This comment addresses the definition and potential improper use of the term “high entropy” in the context of battery materials design, highlights the unique properties of high-entropy materials in battery applications, and outlines the remaining challenges in the synthesis, characterization, and computational modeling of high-entropy battery materials.
- Bin Ouyang
- & Yan Zeng