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| Open AccessA weakly solvating electrolyte towards practical rechargeable aqueous zinc-ion batteries
The practical deployment of aqueous zinc-ion batteries is hindered by the structure deterioration and side reactions at electrodes. Here, the authors introduce a weakly solvating electrolyte with butanone as an electrolyte additive to stabilize both the cathode and anode of aqueous zinc-ion batteries simultaneously.
- Xin Shi
- , Jinhao Xie
- & Xihong Lu
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Article
| Open AccessA 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
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Article
| Open AccessElectronic paddle-wheels in a solid-state electrolyte
Conduction in solid-state electrolytes composed of monatomic ions is found to be analogous to the paddle-wheel mechanism in molecular solid electrolytes, facilitated by rotational motion of lone pair electrons, helping unify understanding of mechanisms.
- Harender S. Dhattarwal
- , Rahul Somni
- & Richard C. Remsing
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Article
| Open AccessStructural regulation of halide superionic conductors for all-solid-state lithium batteries
Predicting the structure of lithium halide solid-state electrolytes from their composition alone is a challenge. Here, the authors introduce the “cationic polarization factor” that captures the key interactions of halide-based solid-state electrolytes and predicts the stacking structures.
- Xiaona Li
- , Jung Tae Kim
- & Xueliang Sun
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Article
| Open AccessAsynchronous domain dynamics and equilibration in layered oxide battery cathode
The battery performance at the cell level is an integration of contributions from many active particles. Here, the authors present a direct visualization of the active cathode particles that react heterogeneously and asynchronously by using coherent multi-crystal diffraction and optical microscopy.
- Zhichen Xue
- , Nikhil Sharma
- & Yijin Liu
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Article
| Open AccessAn inorganic-rich but LiF-free interphase for fast charging and long cycle life lithium metal batteries
Fluorinated interphases are often pursued as a design strategy for Li metal batteries. In contrast, here the authors show that an electrolyte with a non-fluorinated solvent and CsNO3 additive results in an LiF-free but inorganic-rich interphase that enables fast-charging of Li metal batteries.
- Muhammad Mominur Rahman
- , Sha Tan
- & Enyuan Hu
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Article
| Open AccessDiscovery of fast and stable proton storage in bulk hexagonal molybdenum oxide
Nanostructured electrode materials pose several challenges, including poor volumetric performance, severe side reactions, high costs, and complexity. Here, the authors develop a micrometer-sized bulk hexagonal molybdenum oxide with unconventional charge storage mechanism for fast and stable proton storage.
- Tiezhu Xu
- , Zhenming Xu
- & Laifa Shen
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Article
| Open AccessBreaking solvation dominance of ethylene carbonate via molecular charge engineering enables lower temperature battery
Low-temperature operation remains challenging for batteries. Here, the authors report an electrolyte solvation structure design strategy to break solvation dominance of ethylene carbonate to facilitate the desolvation process that improves the low-temperature performance of lithium-ion batteries even below −100 °C.
- Yuqing Chen
- , Qiu He
- & Jilei Liu
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Article
| Open AccessA corrosion inhibiting layer to tackle the irreversible lithium loss in lithium metal batteries
Lithium metal electrodes suffer from both chemical and electrochemical corrosion during battery storage and operation. Here, the authors show that lithium corrosion is due to dissolution of the solid-electrolyte interphase and suppress this by utilizing a multifunctional passivation layer.
- Chengbin Jin
- , Yiyu Huang
- & Xinyong Tao
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Article
| Open AccessNonintrusive thermal-wave sensor for operando quantification of degradation in commercial batteries
Monitoring real-world battery degradation is crucial for the widespread application of batteries in different scenarios. Here, the authors report a simple non-embedded thermal-wave sensing technique that can quantitatively distinguish different battery degradation sources during operation.
- Yuqiang Zeng
- , Fengyu Shen
- & Ravi S. Prasher
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Article
| Open AccessDefective oxygen inert phase stabilized high-voltage nickel-rich cathode for high-energy lithium-ion batteries
The oxygen evolutions from layered cathode surfaces cause battery degradation during high-voltage operation and pose thermal safety concerns. Here, the authors propose a strategy to anchor and reserve surface oxygen with defective oxygen inert phase for high-voltage nickel-rich cathodes in lithium-ion batteries.
- Zhongsheng Dai
- , Zhujie Li
- & Li Li
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Article
| Open AccessElectrochemical nitrate reduction in acid enables high-efficiency ammonia synthesis and high-voltage pollutes-based fuel cells
Research on electrochemical nitrate reduction to ammonia in acidic conditions has been less extensive than that conducted in alkaline conditions. Here, the authors report a hybrid of iron phthalocyanine and TiO2 catalyst with improved efficiency toward acidic nitrate reduction and its application in Zn-nitrate batteries and high-voltage pollutes-based fuel cell.
- Rong Zhang
- , Chuan Li
- & Chunyi Zhi
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Article
| Open AccessCollaborative and privacy-preserving retired battery sorting for profitable direct recycling via federated machine learning
Unsorted retired batteries pose recycling challenges due to diverse cathodes. Here, the authors propose a privacy-preserving machine learning system that enables accurate sorting with minimal data, important for a sustainable battery recycling industry.
- Shengyu Tao
- , Haizhou Liu
- & Hongbin Sun
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Article
| Open AccessOperando analysis of a solid oxide fuel cell by environmental transmission electron microscopy
By contacting a solid oxide fuel cell to a microelectromechanical system inside an environmental electron microscope, the authors establish links between environmental conditions (gas atmosphere, temperature), cell voltage and atomic-scale structure.
- Q. Jeangros
- , M. Bugnet
- & M. Duchamp
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Article
| Open AccessStabilizing lattice oxygen redox in layered sodium transition metal oxide through spin singlet state
Oxygen redox in transition metal oxides enhances the energy content of Na-ion batteries but is typically plagued by poor reversibility. Here, the authors achieve non-hysteresis through the formation of a spin singlet state to stabilize the active oxygen redox reaction in P3-type Na2/3Cu1/3Mn2/3O2.
- Xuelong Wang
- , Liang Yin
- & Jue Liu
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Article
| Open AccessAtomic-scale probing of short-range order and its impact on electrochemical properties in cation-disordered oxide cathodes
Derivation of atomic arrangements of short-range-order from diffused intensity pattern in reciprocal space for Li-excess cation-disordered rocksalt cathode remains as a challenge. Here, the authors reveal the short-range-order is a convolution of three basic types: tetrahedron, octahedron, and cube.
- Linze Li
- , Bin Ouyang
- & Chongmin Wang
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Article
| Open AccessDetangling electrolyte chemical dynamics in lithium sulfur batteries by operando monitoring with optical resonance combs
The shuttle effect of polysulfides in lithium sulfur batteries leads to performance degradation. Here, authors use fiber-based sensors to track and quantify the dissolved polysulfide concentration in the electrolyte during cell charge and discharge, revealing insights on stability and performance.
- Fu Liu
- , Wenqing Lu
- & Jean-Marie Tarascon
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Article
| Open AccessOperando Li metal plating diagnostics via MHz band electromagnetics
Internal growth of Li-metal deposition is critical for evaluating the state of safety in lithium-ion batteries. Here the authors show a Li-metal detection method utilizing high-frequency electromagnetics, which can be assembled as a sensor for monitoring cycle-by-cycle growth of Li-metal plating.
- Masanori Ishigaki
- , Keisuke Ishikawa
- & Tsuyoshi Sasaki
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Article
| Open AccessTailoring chemical composition of solid electrolyte interphase by selective dissolution for long-life micron-sized silicon anode
The severe volume expansion during the lithiation of micron-sized Si in Li-ion batteries requires a solid electrolyte interphase with reinforced mechanical stability. Here, the authors propose a solvent-induced selective dissolution strategy to regulate the mechanical properties of the interphase.
- Yi-Fan Tian
- , Shuang-Jie Tan
- & Yu-Guo Guo
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Article
| Open AccessTailoring grain boundary stability of zinc-titanium alloy for long-lasting aqueous zinc batteries
The electrochemical performance of metal electrodes is significantly influenced by their grain boundary stability. Here, the authors propose a zinc-titanium two-phase alloy via grain boundary engineering to inhibit intergranular corrosion and tailor deposition behavior for stable aqueous zinc batteries.
- Yunxiang Zhao
- , Shan Guo
- & Jiang Zhou
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Article
| Open AccessDefects and nanostrain gradients control phase transition mechanisms in single crystal high-voltage lithium spinel
Lithiation dynamics and phase transition mechanisms in battery materials remain poorly understood. Here authors use operando X-ray nanodiffraction microscopy to reveal how domains relate to defects and how cycling affects the lattice domain reorientation in LiMn1.5Ni0.5O4 single crystals.
- Isaac Martens
- , Nikita Vostrov
- & Tobias U. Schulli
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Article
| Open AccessSEI growth on Lithium metal anodes in solid-state batteries quantified with coulometric titration time analysis
In lithium-metal batteries, it is vital to quantify electrolyte side reactions occurring at the metal anode surface. Here, the authors introduce an electrochemical technique, using a series of small-step lithium deposition followed by open circuit voltage analysis, to accurately measure these reactions.
- Burak Aktekin
- , Luise M. Riegger
- & Jürgen Janek
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Article
| Open AccessWhat dictates soft clay-like lithium superionic conductor formation from rigid salts mixture
Soft clay-like superionic conductors are integral for realising all-solid-state batteries. Here the authors provide fundamental insights into how a soft clay-like Li-superionic conductor, and soft clays in general can be created from a rigid-salts mixture.
- Sunny Gupta
- , Xiaochen Yang
- & Gerbrand Ceder
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Article
| Open AccessBoosting lithium ion conductivity of antiperovskite solid electrolyte by potassium ions substitution for cation clusters
All-solid-state electrolytes for lithium batteries generally suffer from low ionic conductivity. Here, authors manipulate the lattice of antiperovskite-type Li2OHCl by potassium ion substitution, which alters the lattice structure and improves the lithium ion transport properties.
- Lei Gao
- , Xinyu Zhang
- & Ruqiang Zou
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Article
| Open AccessKnowledge-driven design of solid-electrolyte interphases on lithium metal via multiscale modelling
The application of Li metal electrodes in rechargeable batteries is limited by inherent high reactivity. Here, the authors provide model-based insights into the composition and formation mechanisms of the solid-electrolyte interphase on the µs-scale and suggest design strategies for the interphase.
- Janika Wagner-Henke
- , Dacheng Kuai
- & Ulrike Krewer
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Article
| Open AccessManipulating coordination environment for a high-voltage aqueous copper-chlorine battery
Aqueous copper-based batteries suffer from low voltage due to the high copper negative electrode potential. Here, utilizing the coordination of chloride with copper ions, authors lower copper’s redox potential by 0.3 V, resulting in a high-voltage aqueous copper-chlorine battery.
- Xiangyong Zhang
- , Hua Wei
- & Zhuoxin Liu
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Perspective
| Open AccessBenchmarking organic active materials for aqueous redox flow batteries in terms of lifetime and cost
To guide research and implementation of aqueous organic redox flow batteries it is essential to estimate their potential costs. In this perspective, the authors present an overview of the potential cost of organic active materials for aqueous flow batteries and identify cost reduction routes.
- Dominik Emmel
- , Simon Kunz
- & Daniel Schröder
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Article
| Open AccessLattice pinning in MoO3 via coherent interface with stabilized Li+ intercalation
Large lattice variation of electrode materials upon lithiation and delithiation limits the cycle life of lithium batteries. Here, authors introduce a lattice pinning strategy via heterostructure design to suppress lattice expansion in MoO3 and improve cycle life in all-solid-state lithium batteries.
- Shuo Sun
- , Zhen Han
- & Hui Xia
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Article
| Open AccessIntercalation-type catalyst for non-aqueous room temperature sodium-sulfur batteries
Sodium-sulfur batteries show potential as attractive alternatives to Li-ion batteries due to their high energy density but practicality is hampered by sodium polysulfide issues. Here, the authors introduce an intercalation-type catalyst MoTe2 to improve the redox kinetics in Na-S batteries.
- Jiarui He
- , Amruth Bhargav
- & Arumugam Manthiram
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Article
| Open AccessA biocompatible electrolyte enables highly reversible Zn anode for zinc ion battery
Aqueous zinc metal batteries utilized in wearable and implanted devices require good biosecurity, long lifespan, and high flexibility. Here, the authors proposed a biocompatible hyaluronic acid-based gel electrolyte to improve the reversibility of zinc anodes and prolong the cycle life of batteries.
- Guanjie Li
- , Zihan Zhao
- & Zaiping Guo
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Article
| Open AccessElectrochemically induced crystalline-to-amorphization transformation in sodium samarium silicate solid electrolyte for long-lasting sodium metal batteries
Solid-state sodium metal batteries require solid electrolytes with high ionic conductivity and optimal electrode compatibility. Here, the authors introduce the Na5SmSi4O12 solid electrolyte with a crystalline-to-amorphous transformation, achieving 4000 cycles lifetime without capacity decline.
- Ge Sun
- , Chenjie Lou
- & Fei Du
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Article
| Open AccessManipulating Li2S2/Li2S mixed discharge products of all-solid-state lithium sulfur batteries for improved cycle life
All-solid-state lithium sulfur batteries may avoid some of the drawbacks of their liquid electrolyte counterparts. Here, the authors elucidate the composition of discharge products in all-solid-state cells using spectroscopic techniques and propose a strategy to control the discharge product.
- Jung Tae Kim
- , Adwitiya Rao
- & Xueliang Sun
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Article
| Open AccessPhase regulation enabling dense polymer-based composite electrolytes for solid-state lithium metal batteries
Polymer electrolytes based on poly(vinylidene fluoride) with residual solvents are appealing for room-temperature battery operations. Here, the authors present a phase regulation approach to achieve a dense electrolyte and enhance ionic conductivity through the incorporation of MoSe2 sheets.
- Qian Wu
- , Mandi Fang
- & Yingying Lu
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Article
| Open AccessRevealing the aging process of solid electrolyte interphase on SiOx anode
Observing the evolution of the solid electrolyte interphase on SiOx-based electrodes in Li-ion batteries is challenging. Here, authors use three-dimensional tomography to visualize the growth of the interphase on single SiOx particles and propose a mechanical confinement strategy to prevent aging.
- Guoyu Qian
- , Yiwei Li
- & Feng Pan
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Article
| Open AccessRevealing the closed pore formation of waste wood-derived hard carbon for advanced sodium-ion battery
It is essential to investigate the formation mechanism of closed pore, which contributes to low-voltage plateau capacity of hard carbon anode in sodium ion batteries. Herein, the authors explore the impact of wood precursor components and carbonization temperature on closed pore formation in hard carbon for enhanced battery performance.
- Zheng Tang
- , Rui Zhang
- & Minhua Shao
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Article
| Open AccessLow-temperature anode-free potassium metal batteries
Low temperature operation of anode-free batteries is limited by poor reversibility of metal plating/stripping. Here, via electrolyte engineering, authors enable −40 °C operation of an anode-free K metal battery by tailoring a weakly solvating electrolyte with a silicone polymer additive.
- Mengyao Tang
- , Shuai Dong
- & Hua Wang
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Article
| Open AccessRealistic fault detection of li-ion battery via dynamical deep learning
Accurate evaluation of Li-ion battery safety conditions can reduce unexpected cell failures. Here, authors present a large-scale electric vehicle charging dataset for benchmarking existing algorithms, and develop a deep learning algorithm for detecting Li-ion battery faults.
- Jingzhao Zhang
- , Yanan Wang
- & Minggao Ouyang
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Article
| Open AccessRegulating electrostatic phenomena by cationic polymer binder for scalable high-areal-capacity Li battery electrodes
Binders employed in battery electrodes are conventionally neutral linear polymers. Here, authors present a cationic semi-interpenetrating polymer network binder to regulate electrostatic phenomena, improving the properties and performance of high-capacity positive electrodes for Li metal batteries.
- Jung-Hui Kim
- , Kyung Min Lee
- & Sang-Young Lee
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Article
| Open AccessInterfacial friction enabling ≤ 20 μm thin free-standing lithium strips for lithium metal batteries
Thin, freestanding Li metal foils are key to improving the energy density of Li batteries but are difficult to manufacture. Here, authors achieve thin Li foils by mechanical rolling, exploiting tribochemistry to form a protective surface film that improves mechanical and electrochemical properties.
- Shaozhen Huang
- , Zhibin Wu
- & Libao Chen
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Article
| Open AccessA twelve-electron conversion iodine cathode enabled by interhalogen chemistry in aqueous solution
Enhancing energy density of batteries is a crucial focus within the field of energy storage. Here, the authors introduce a twelve-electron conversion iodine cathode (iodide/iodate) for high energy density zinc-iodine batteries, achieved through interhalogen chemistry in an acidic aqueous electrolyte.
- Wenjiao Ma
- , Tingting Liu
- & Xiao Liang
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Article
| Open AccessDiscovery of a three-proton insertion mechanism in α-molybdenum trioxide leading to enhanced charge storage capacity
The proton insertion mechanism in α-molybdenum trioxide remains incompletely elucidated. Herein, the authors uncover a three-proton intercalation mechanism within α-molybdenum trioxide using a specially designed electrolyte, which endows α-molybdenum trioxide with an improved specific discharge capacity.
- Yongjiu Lei
- , Wenli Zhao
- & Husam N. Alshareef
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Article
| Open AccessRegulating interfacial reaction through electrolyte chemistry enables gradient interphase for low-temperature zinc metal batteries
Zinc batteries have received intense attentions but suffer from inferior low-temperature performance. Here, the authors constructed a gradient phosphatized interphase in situ on zinc surface to accelerate zinc-ion desolvation and transport, greatly enhancing the cycling performance at subzero temperatures.
- Wei Wang
- , Shan Chen
- & Huan Wang
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Article
| Open AccessIntegration of microbattery with thin-film electronics for constructing an integrated transparent microsystem based on InGaZnO
In this work, authors demonstrate the full integration of miniaturized InGaZnO-based transparent energy device (lithium-ion battery), electronic device (thin-film transistor) and sensing device (photodetector) to form a monolithic integrated transparent microsystem with synergistic functions.
- Bin Jia
- , Chao Zhang
- & Xiaodong Huang
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Article
| Open AccessOperando monitoring of thermal runaway in commercial lithium-ion cells via advanced lab-on-fiber technologies
Operando monitoring of thermal runaway in Li-ion batteries is critical. Here, authors develop an optical fiber sensor capable of insertion into 18650 batteries to monitor internal temperature and pressure during thermal runaway, facilitating battery safety assessment and early warning capability.
- Wenxin Mei
- , Zhi Liu
- & Tuan Guo
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Article
| Open AccessTuning electron delocalization of hydrogen-bonded organic framework cathode for high-performance zinc-organic batteries
The practical use of zinc-organic batteries has been hindered by their low energy density and rapid capacity decay. Here, the authors introduce a super electron-delocalized hydrogen-bonded organic framework by tuning electron delocalization as a cathode material for high-performance zinc-organic batteries.
- Wenda Li
- , Hengyue Xu
- & Shaohua Liu
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Article
| Open AccessDesign principles for NASICON super-ionic conductors
Na Super Ionic Conductor (NASICON) materials are an important class of solid-state electrolytes. Here, authors combine calculations, experimental synthesis and testing, and text-mined historical data on NASICON ionic conductivity to understand how composition influences the Na-ion conductivity.
- Jingyang Wang
- , Tanjin He
- & Gerbrand Ceder
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Article
| Open AccessIdentifying and preventing degradation in flavin mononucleotide-based redox flow batteries via NMR and EPR spectroscopy
Aqueous organic redox-flow batteries are known to suffer capacity loss via degradation of the redox-active species. Here, the authors use in situ methods to study the electrolyte flavin mononucleotide, identifying a redox mediator mechanism that mitigates capacity loss and a route to prevent its degradation.
- Dominic Hey
- , Rajesh B. Jethwa
- & Clare P. Grey
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Article
| Open AccessMultiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling
Improved understanding of the spatial dynamics in graphite electrodes is needed to improve fast-charging protocols for Li-ion batteries. Here, authors highlight that lithiation heterogeneity leads to early lithium plating onset and find distinct relaxation behaviors at various states of charge.
- Xuekun Lu
- , Marco Lagnoni
- & Paul R. Shearing
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Article
| Open AccessAn aqueous electrolyte densified by perovskite SrTiO3 enabling high-voltage zinc-ion batteries
Conventional electrolytes of aqueous zinc-ion batteries suffer from serious side reactions. Here, the authors develop a densified electrolyte with perovskite additives to achieve reversible zinc plating/stripping with robust interface and improved performance of full cells at an extended voltage range.
- Rongyu Deng
- , Zhenjiang He
- & Feixiang Wu