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Catalytic 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
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Understanding 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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Hybridizing 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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Chlorine 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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Manipulating 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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Enhancements 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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Overcoming 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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Activating 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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Isotope 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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Monolithically 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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Atomic 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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Dynamical 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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An 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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Grave-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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Phosphonate-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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Deciphering 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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A 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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Deciphering 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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Electric 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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Proton-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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Molecular 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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Cation 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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Efficient 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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Liquid 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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Kirkendall 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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Promoting 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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Ca-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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Hierarchical 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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Structurally 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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Solvation-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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High 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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Capacitive 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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Designing 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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Subtractive 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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Self-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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Optimizing 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
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The 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
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Integrated energy storage and CO2 conversion using an aqueous battery with tamed asymmetric reactions
A system integrating CO2 conversion and energy storage holds great promise, but faces a major challenge due to degraded catalysts on charge. Here, the authors present a highly efficient energy storage and CO2 reduction method in an aqueous battery, achieved through oxidation of reducing molecules.
- Yumei Liu
- , Yun An
- & Quanquan Pang
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Article
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Experimentally validated design principles of heteroatom-doped-graphene-supported calcium single-atom materials for non-dissociative chemisorption solid-state hydrogen storage
Via the first-principles calculations and experimental verifications, a guiding principle is established to design heteroatom-doped-graphene-supported Ca single-atom carbon nanomaterials for efficient non-dissociative solid-state hydrogen storage.
- Yong Gao
- , Zhenglong Li
- & Hongge Pan
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Article
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A rechargeable Ca/Cl2 battery
The development of practical Ca metal batteries has been hindered by the cathode chemistry. Here, the authors report a rechargeable Ca/Cl2 battery, which involves the reversible cathode redox reaction between CaCl2 and Cl2.
- Shitao Geng
- , Xiaoju Zhao
- & Hao Sun
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Highly loaded bimetallic iron-cobalt catalysts for hydrogen release from ammonia
Inexpensive iron catalysts often exhibit low activity in ammonia decomposition due to a strong iron-nitrogen binding energy. Here the authors demonstrate that combining iron with cobalt to form a Fe-Co bimetallic catalyst overcomes this limitation, presenting a promising solution for enhancing ammonia decomposition efficiency.
- Shilong Chen
- , Jelena Jelic
- & Malte Behrens
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Article
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Effect of solid-electrolyte pellet density on failure of solid-state batteries
A critical challenge of solid-state batteries is Li-filament penetration. Here, by quantifying microstructural properties and employing modeling techniques, the authors provide insight into solid-state battery failure modes and offer design guidelines to enhance safety and performance.
- Mouhamad S. Diallo
- , Tan Shi
- & Gerbrand Ceder
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Boosting a practical Li-CO2 battery through dimerization reaction based on solid redox mediator
Li–CO2 batteries following Li2CO3-product route suffers from low output voltage and severe parasitic reactions. Here, the authors introduce a copper-based solid redox mediator in Li–CO2 batteries with an efficient Li2C2O4 product route to circumvent the shuttle effect and sluggish kinetics caused by soluble mediators.
- Wei Li
- , Menghang Zhang
- & Haoshen Zhou
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Article
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An extended substrate screening strategy enabling a low lattice mismatch for highly reversible zinc anodes
The growth of dendrites and the occurrence of side reactions at zinc anodes currently impede the practical use of aqueous zinc batteries. Here, the authors present an advanced substrate screening approach aimed at stabilizing zinc anodes, thereby enabling the development of high-rate zinc-metal batteries.
- Zhiyang Zheng
- , Xiongwei Zhong
- & Guangmin Zhou
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Article
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Rapid-charging aluminium-sulfur batteries operated at 85 °C with a quaternary molten salt electrolyte
Molten salt aluminium-sulfur batteries exhibit high-rate capability and moderate energy density, but suffer from high operating temperature. Here the authors demonstrate a rapidly charging aluminum-sulfur battery operating at 85 °C enabled by a quaternary alkali chloroaluminate electrolyte.
- Jiashen Meng
- , Xufeng Hong
- & Quanquan Pang
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Article
| Open Access
Alkaline-based aqueous sodium-ion batteries for large-scale energy storage
Aqueous sodium-ion batteries show promise for large-scale energy storage, yet face challenges due to water decomposition, limiting their energy density and lifespan. Here, the authors report a cathode surface coating strategy in an alkaline electrolyte to enhance the stability of both electrolyte and battery.
- Han Wu
- , Junnan Hao
- & Shi-Zhang Qiao
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Article
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A dicarbonate solvent electrolyte for high performance 5 V-Class Lithium-based batteries
Rechargeable lithium batteries featuring 5 V cathodes offer high energy density yet struggle with stability. Here, the authors formulate an electrolyte incorporating dimethyl 2,5-dioxahexanedioate solvent, which facilitates stable lithium plating and stripping while offering an extended cycle life.
- Xiaozhe Zhang
- , Pan Xu
- & Alexandru Vlad
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Cobalt-free composite-structured cathodes with lithium-stoichiometry control for sustainable lithium-ion batteries
As electric vehicle batteries adopt cobalt-free layered cathodes to tackle supply chain issues, it greatly impacts battery lifespan. Here, the authors develop a lithium stoichiometry control method to synthesize cobalt-free composite-structured cathodes with high cycling stability, enabling long-life sustainable batteries.
- Ke Chen
- , Pallab Barai
- & Feng Wang
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A cross-scale framework for evaluating flexibility values of battery and fuel cell electric vehicles
Electrified transportation exhibits great potential to provide flexibility. This article analyzed and compared the flexibility values of battery electric vehicles and fuel cell electric vehicles for planning and operating interdependent electricity and hydrogen supply chains.
- Ruixue Liu
- , Guannan He
- & Benben Jiang
Sub-millisecond lithiothermal synthesis of graphitic meso–microporous carbon