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| 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
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Article
| Open AccessIntegrated 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
| Open AccessA 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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Article
| Open AccessEffect 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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Article
| Open AccessBoosting 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
| Open AccessAn 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
| Open AccessRapid-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 AccessAlkaline-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
| Open AccessA 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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Article
| Open AccessImproving rechargeable magnesium batteries through dual cation co-intercalation strategy
Rechargeable magnesium batteries suffer from poor mobility of Mg-ions, severely affecting the electrochemical performance. Here, authors demonstrate a strategy of co-intercalation of monovalent ions into the host lattice, which substantially improves Mg-ion mobility and battery performance.
- Ananyo Roy
- , Mohsen Sotoudeh
- & Zhenyou Li
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Article
| Open AccessCobalt-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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Article
| Open AccessInterfacial self-healing polymer electrolytes for long-cycle solid-state lithium-sulfur batteries
Low ion conductivity, large interfacial resistance, and dendrite growth hinder the practical use of solid-state batteries. Here, the authors introduce a self-healing poly(ether-urethane)-based solid-state polymer electrolyte to address these issues, resulting in high performance solid-state lithium-sulfur batteries.
- Fei Pei
- , Lin Wu
- & Yunhui Huang
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Article
| 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