Featured
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| Open AccessOn the nanoscale structural evolution of solid discharge products in lithium-sulfur batteries using operando scattering
Understanding lithium sulfide’s electrodeposition and stripping is key to developing practical Li-S batteries. Here, the authors demonstrate that the discharge product in Li-S batteries consists of nano-size solid polysulfide particles and nano-crystalline lithium sulfide.
- Christian Prehal
- , Jean-Marc von Mentlen
- & Vanessa Wood
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Article
| Open AccessRevealing solid electrolyte interphase formation through interface-sensitive Operando X-ray absorption spectroscopy
Solid electrolyte interphase (SEI) formation on Li-ion battery anodes is critical for long-term performance. Here, the authors use operando soft X-ray absorption spectroscopy in total electron yield mode to resolve the chemical evolution of the SEI during electrochemical formation on silicon anodes.
- Jack E. N. Swallow
- , Michael W. Fraser
- & Robert S. Weatherup
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Article
| Open AccessSolvent-free protic liquid enabling batteries operation at an ultra-wide temperature range
It is challenging to prepare electrolyte that could achieve wide electrochemical window, broad working temperature, non-inflammability, and fast ion transport simultaneously. Here the authors report a rocking-chair proton battery utilizing a solvent-free protic liquid electrolyte, which could operate in a broad temperature range from 0 to 250 celsius degree.
- Mochou Liao
- , Xiao Ji
- & Yongyao Xia
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Article
| Open AccessThree-dimensional hierarchically porous MoS2 foam as high-rate and stable lithium-ion battery anode
The stacked and brittle 2D layered structure of molybdenum disulphide limits its practical application in lithium ion batteries. Here, authors report a dewetting-induced manufacture strategy to create the interpenetrating network and induce the pseudocapacity to improve the electrochemical performance.
- Xuan Wei
- , Chia-Ching Lin
- & Vincent Tung
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Matters Arising
| Open AccessReply to: Critical evaluation of (110) texture in lithium electrodeposits on isotropic Cu polycrystals
- Qing Zhao
- , Jingxu Zheng
- & Lynden A. Archer
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Article
| Open AccessAutonomous optimization of non-aqueous Li-ion battery electrolytes via robotic experimentation and machine learning coupling
Human-operated optimization of non-aqueous Li-ion battery liquid electrolytes is a time-consuming process. Here, the authors propose an automated workflow that couples robotic experiments with machine learning to optimize liquid electrolyte formulations without human intervention.
- Adarsh Dave
- , Jared Mitchell
- & Venkatasubramanian Viswanathan
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Article
| Open AccessStrain-regulated Gibbs free energy enables reversible redox chemistry of chalcogenides for sodium ion batteries
Manipulating the redox chemistry of transition metal dichalcogenides still faces challenges. Here the authors report that tensile-strained MoSe2 can pass on the strain to its sodiated product Mo, and thus regulate the Gibbs free energy in the charging process to enable the reversible sodium storage.
- Minxia Jiang
- , Yingjie Hu
- & Minhua Cao
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Article
| Open AccessTackling realistic Li+ flux for high-energy lithium metal batteries
The low conductivity of LiF disturbs Li+ diffusion across solid electrolyte interphase (SEI) and induces Li+ transfer-driven dendritic growth. Herein, the authors establish a mechanistic model to decipher how the SEI affects realistic Li plating in high-fluorine electrolytes.
- Shuoqing Zhang
- , Ruhong Li
- & Xiulin Fan
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Article
| Open AccessSelf-repairing interphase reconstructed in each cycle for highly reversible aqueous zinc batteries
Metallic zinc is an ideal anode material for aqueous rechargeable batteries but reversibility is a challenge. Here, the authors realise a dynamic real-time reconstructed interphase on zinc anode formed by graphitic carbon nitride quantum dot as an electrolyte additive to improve the performance of Zn metal anodes.
- Wenyao Zhang
- , Muyao Dong
- & Zhi Li
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Comment
| Open AccessThe role of concentration in electrolyte solutions for non-aqueous lithium-based batteries
The quest for high-energy electrochemical energy storage systems has driven researchers to look toward highly concentrated electrolytes. Here, the author discusses the recent progress and future perspectives of such electrolytes and their ability to improve the performances of lithium-based batteries.
- Guinevere A. Giffin
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Article
| Open AccessExtending the low-temperature operation of sodium metal batteries combining linear and cyclic ether-based electrolyte solutions
The low-temperature operation of non-aqueous sodium-based batteries is affected by the properties of the electrolyte. Here the authors propose specific electrolyte formulations that are thermally stable down to −150 °C and enable a stable electrode|electrolyte interface at low temperatures.
- Chuanlong Wang
- , Akila C. Thenuwara
- & Weiyang Li
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Article
| Open AccessCodoped porous carbon nanofibres as a potassium metal host for nonaqueous K-ion batteries
The use of electrochemical energy storage systems based on alkali metal electrodes is hindered by the dendrites’ growth and volume changes upon cycling. Here, the authors propose nitrogen and zinc co-doped porous carbon nanofibers as potassium metal hosting material for reversible metal deposition.
- Siwu Li
- , Haolin Zhu
- & Jia Xie
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Article
| Open AccessOxidative decomposition mechanisms of lithium carbonate on carbon substrates in lithium battery chemistries
Lithium carbonate is ubiquitous in lithium battery chemistries and leads to overpotentials, however its oxidative decomposition is unclear. Here, the authors study its decomposition in ether electrolyte, clarify the role of the carbon substrate, and propose a route to limit released singlet oxygen.
- Deqing Cao
- , Chuan Tan
- & Yuhui Chen
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Article
| Open AccessImpedance-based forecasting of lithium-ion battery performance amid uneven usage
Accurate forecasts of lithium-ion battery performance will ease concerns about the reliability of electric vehicles. Here, the authors leverage electrochemical impedance spectroscopy and machine learning to show that future capacity can be predicted amid uneven use, with no historical data requirement.
- Penelope K. Jones
- , Ulrich Stimming
- & Alpha A. Lee
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Article
| Open AccessMolecular engineering of dihydroxyanthraquinone-based electrolytes for high-capacity aqueous organic redox flow batteries
Aqueous organic redox flow batteries are affected by short cycle life and low capacity. Here, the authors develop composite dihydroxyanthraquinone/polymer anolytes capable of improving the cycling stability and discharge capacity of aqueous organic redox flow batteries.
- Shiqiang Huang
- , Hang Zhang
- & Qing Wang
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Article
| Open AccessDevelopment of high-energy non-aqueous lithium-sulfur batteries via redox-active interlayer strategy
Lithium-sulfur batteries promise high energy density, but polysulfide shuttling acts as a major stumbling block toward practical development. Here, a redox-active interlayer is proposed to confine polysulfides, increase the cell capacity and improve cell cycle life.
- Byong-June Lee
- , Chen Zhao
- & Jong-Sung Yu
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Article
| Open AccessFundamental investigations on the sodium-ion transport properties of mixed polyanion solid-state battery electrolytes
Battery solid-state electrolytes rely on mixed polyanion networks to attain high ionic conductivities. Here, the authors investigate the effect of polyanion mixing on the solid-state electrolyte ion conductivity via theoretical calculations and electrochemical measurements.
- Zeyu Deng
- , Tara P. Mishra
- & Pieremanuele Canepa
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Article
| Open AccessDevelopment of quasi-solid-state anode-free high-energy lithium sulfide-based batteries
The development of anode-free batteries requires investigations at the electrode and electrolyte levels. Here, the authors report a high-energy quasi-solid-state anode-free pouch cell with a Li2S-based cathode that demonstrates enhanced safety features.
- Yuzhao Liu
- , Xiangyu Meng
- & Jieshan Qiu
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Article
| Open AccessCO-tolerant RuNi/TiO2 catalyst for the storage and purification of crude hydrogen
Efficient storage of crude hydrogen, through toluene hydrogenation to methylcyclohexane, is often inhibited by CO impurities. Here, the authors develop a RuNi/TiO2 catalyst which avoids deactivation through promoting simultaneous CO methanation.
- Zhaohua Wang
- , Chunyang Dong
- & Ding Ma
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Article
| Open AccessTracing the origin of lithium in Li-ion batteries using lithium isotopes
Rechargeable Li-ion batteries play a key role in the energy transition towards clean energy. It is challenging for end users to ensure that Li comes from environmentally and responsible sources. Here the authors show that Li isotope ‘fingerprints’ are a useful tool for determining the origin of Li in battery.
- Anne-Marie Desaulty
- , Daniel Monfort Climent
- & Catherine Guerrot
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Article
| Open AccessRational design of a topological polymeric solid electrolyte for high-performance all-solid-state alkali metal batteries
Solid-state polymer electrolytes are crucial for developing future rechargeable batteries, but they are still limited in performance. Here, the authors designed a topological polymeric solid electrolyte, enabling an all-solid-state high-voltage lithium metal pouch cell to cycle 200 times efficiently.
- Yun Su
- , Xiaohui Rong
- & Yong-Sheng Hu
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Article
| Open AccessDevelopment of vanadium-based polyanion positive electrode active materials for high-voltage sodium-based batteries
The development of high-capacity and high-voltage electrode materials can boost the performance of sodium-based batteries. Here, the authors report the synthesis of a polyanion positive electrode active material that enables high-capacity and high-voltage sodium battery performance.
- Semyon D. Shraer
- , Nikita D. Luchinin
- & Stanislav S. Fedotov
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Article
| Open AccessElectrical resistance of the current collector controls lithium morphology
The deployment of lithium metal batteries is forestalled by poor control over the deposition morphology of lithium. Here, the authors discover that high electrical resistance can be leveraged for controlling lithium morphology and enabling high-performing lithium metal batteries.
- Solomon T. Oyakhire
- , Wenbo Zhang
- & Stacey F. Bent
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Article
| Open AccessCalcium-tin alloys as anodes for rechargeable non-aqueous calcium-ion batteries at room temperature
The key challenge for rechargeable Ca batteries originates from the severe passivation of the calcium metal anode in electrolyte solutions. Here, the authors demonstrate the feasibility and elucidate the electrochemical properties of calcium-tin (Ca–Sn) alloy anodes for rechargeable Ca batteries.
- Zhirong Zhao-Karger
- , Yanlei Xiu
- & Maximilian Fichtner
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Article
| Open AccessTailoring the metal electrode morphology via electrochemical protocol optimization for long-lasting aqueous zinc batteries
Long-lasting zinc metal electrodes are crucial in developing commercial zinc-based batteries. Here, the authors investigate the different morphology evolution between the stripping and plating process and propose electrochemical protocols to prolong the lifespan of zinc anodes.
- Qing Li
- , Ao Chen
- & Chunyi Zhi
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Article
| Open AccessQuasi-solid-state Zn-air batteries with an atomically dispersed cobalt electrocatalyst and organohydrogel electrolyte
Quasi-solid-state Zn-air batteries are limited by sluggish kinetics and low temperature incompatibility. Here, the authors use a single-atom catalyst and an organohydrogel electrolyte to enable a 100 mA cm−2 cycling current density at 25 °C and a −60 to 60 °C operational window.
- Qichen Wang
- , Qingguo Feng
- & Xiang Xiong
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Article
| Open AccessEffect of the grain arrangements on the thermal stability of polycrystalline nickel-rich lithium-based battery cathodes
Enhancing the stability of positive electrodes at thermally-abused conditions is vital for next-generation lithium-based batteries. Here, the authors report in situ physicochemical characterizations to improve the fundamental understanding of the degradation mechanism in polycrystalline Ni-rich cathodes.
- Dong Hou
- , Zhengrui Xu
- & Feng Lin
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Article
| Open AccessNiobium-doped layered cathode material for high-power and low-temperature sodium-ion batteries
The practical application of sodium-ion batteries at subzero temperatures is hindered by the slow Na-ion transfer kinetics. Here, the authors reported the niobium doping of P2-type cathode active material capable of efficient battery cycling at low temperatures such as −40 °C.
- Qinhao Shi
- , Ruijuan Qi
- & Yufeng Zhao
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Article
| Open AccessExpanding the active charge carriers of polymer electrolytes in lithium-based batteries using an anion-hosting cathode
The energy content of secondary batteries is often limited by the charge carriers available in the system. Here, the authors employed an anion acceptor cathode for simultaneous use of electrolyte anions and cations as effective charge carriers in solid polymer electrolytes for lithium-based batteries.
- Zongjie Sun
- , Kai Xi
- & Shujiang Ding
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Article
| Open AccessDevelopment of efficient aqueous organic redox flow batteries using ion-sieving sulfonated polymer membranes
Aqueous organic redox flow batteries are promising for grid-scale energy storage, although their practical application is still limited. Here, the authors report highly ion-conductive and selective polymer membranes, which boost the battery’s efficiency and stability, offering cost-effective electricity storage.
- Chunchun Ye
- , Anqi Wang
- & Qilei Song
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Article
| Open AccessLanthanum nitrate as aqueous electrolyte additive for favourable zinc metal electrodeposition
Zinc metal is a promising anode material for aqueous secondary batteries. However, the unfavourable morphologies formed on the electrode surface during cycling limit its application. Here, the authors report the tailoring of the surface morphology using a lanthanum nitrate aqueous electrolyte additive.
- Ruirui Zhao
- , Haifeng Wang
- & Yunhui Huang
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Article
| Open AccessGiant energy-storage density with ultrahigh efficiency in lead-free relaxors via high-entropy design
Dielectric ceramics are widely used in advanced high/pulsed power capacitors. Here, the authors propose a high-entropy strategy to design “local polymorphic distortion” in lead-free ceramics, achieving high energy storage performance.
- Liang Chen
- , Shiqing Deng
- & Jun Chen
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Article
| Open AccessPhase-transition tailored nanoporous zinc metal electrodes for rechargeable alkaline zinc-nickel oxide hydroxide and zinc-air batteries
Secondary alkaline Zn-based batteries are limited in terms of cycle life. Here, the authors report a nanoporous Zn electrode that stabilizes the electrochemical transition between Zn and ZnO and improves the cycling performance of rechargeable alkaline zinc-based batteries.
- Liangyu Li
- , Yung Chak Anson Tsang
- & Qing Chen
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Article
| Open AccessAn electrochemically stable homogeneous glassy electrolyte formed at room temperature for all-solid-state sodium batteries
Single sodium-ion solid electrolyte that meets the requirements of practical applications is difficult to design. Here, the authors show how kinetic stability via the creation of a self-passivating solid electrolyte interphase allows a homogenous glass solid electrolyte to exhibit remarkable electrochemical stability with sodium metal.
- Xiaowei Chi
- , Ye Zhang
- & Yan Yao
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Article
| Open AccessProduction of a hybrid capacitive storage device via hydrogen gas and carbon electrodes coupling
Conventional electric double-layer capacitors show limited energy content for energy storage applications. Here, the authors report an electrocatalytic hydrogen gas capacitor with improved specific energy, which can operate in pH-universal aqueous electrolyte solutions and a wide temperature range.
- Zhengxin Zhu
- , Zaichun Liu
- & Wei Chen
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Article
| Open AccessRedox-homogeneous, gel electrolyte-embedded high-mass-loading cathodes for high-energy lithium metal batteries
The development of high energy lithium metal batteries is affected by the mass loading of the cathode. Here, the authors report a lithium metal pouch cell with a cathode capacity of 12 mAh cm-2. The positive electrode is prepared by applying UV-curable gel electrolyte as a processing solvent.
- Jung-Hui Kim
- , Ju-Myung Kim
- & Sang-Young Lee
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Article
| Open AccessFluorinated ether electrolyte with controlled solvation structure for high voltage lithium metal batteries
The development of lithium-metal batteries is limited by the low thermodynamic and/or low voltage stability of conventional electrolytes. Here, the authors combined the high voltage stability of fluorinated ethers with high Li+ solvation ability of ethers in a single molecule and realized highly stable lithium-metal batteries.
- Yan Zhao
- , Tianhong Zhou
- & Ali Coskun
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Article
| Open AccessA cost-effective alkaline polysulfide-air redox flow battery enabled by a dual-membrane cell architecture
Polysulfide-air redox flow batteries are an appealing energy storage technology but suffer from polysulfide crossover and the use of costly catalysts. Here, the authors report a cell structure that enables battery operation using a cost-effective catalyst while mitigating polysulfide crossover.
- Yuhua Xia
- , Mengzheng Ouyang
- & Nigel P. Brandon
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Article
| Open AccessCorrosion as the origin of limited lifetime of vanadium oxide-based aqueous zinc ion batteries
Aqueous zinc ion batteries are good systems for large-scale energy storage. Here, the authors report that the corrosion of zinc metal anode is the origin of limited lifetime of vanadium oxide-based aqueous zinc ion batteries, and supressing corrosion improves the calendar and cycle lifetime markedly.
- Yangmoon Kim
- , Youngbin Park
- & Jang Wook Choi
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Article
| Open AccessEnabling high energy lithium metal batteries via single-crystal Ni-rich cathode material co-doping strategy
Li-ion cathode active materials are transitioning from poly- to single-crystal structures. However, the performance of high Ni-content single-crystal cathodes remains below expectations. Here, via Al/Zr co-doping, the authors propose a strategy to mitigate structural degradation in this class of materials.
- Xing Ou
- , Tongchao Liu
- & Jun Lu
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Article
| Open AccessData-driven capacity estimation of commercial lithium-ion batteries from voltage relaxation
Accurate capacity estimation is crucial for lithium-ion batteries' reliable and safe operation. Here, the authors propose an approach exploiting features from the relaxation voltage curve for battery capacity estimation without requiring other previous cycling information.
- Jiangong Zhu
- , Yixiu Wang
- & Helmut Ehrenberg
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Article
| Open AccessProduction of fast-charge Zn-based aqueous batteries via interfacial adsorption of ion-oligomer complexes
Aqueous zinc batteries attract interest because of their potential for cost-effective and safe electricity storage. Here, the authors develop an in situ formed ion-oligomer nanometric interphase strategy to enable fast-charge aqueous Zn cells.
- Shuo Jin
- , Jiefu Yin
- & Lynden A. Archer
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Article
| Open AccessEngineering a passivating electric double layer for high performance lithium metal batteries
Developing an electrolyte that is compatible with both high-voltage cathodes and Li metal anodes has always been challenging. Here, the authors created a new strategy by engineering a passivating electric double layer to achieve a fast-charging and lowtemperature high voltage lithium metal batteries.
- Weili Zhang
- , Yang Lu
- & Kai Liu
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Article
| Open AccessRoom temperature all-solid-state lithium batteries based on a soluble organic cage ionic conductor
While solid-state batteries offer higher energy densities than liquid-based batteries, such devices require effective ion conduction pathways. Here, authors prepare porous organic cages as solution-processable catholytes that are enable excellent performances from various cathode active materials.
- Jing Li
- , Jizhen Qi
- & Liwei Chen
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Article
| Open AccessPromoting favorable interfacial properties in lithium-based batteries using chlorine-rich sulfide inorganic solid-state electrolytes
The interfacial stability of lithium metal is a crucial aspect for all-solid-state battery development. Here, authors report argyrodite solid electrolytes containing LiCl framework, where the Cl ions construct a LiCl-rich interphase capable of improving battery performances.
- Dewu Zeng
- , Jingming Yao
- & Lin Wang
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Article
| Open AccessEnabling fast-charging selenium-based aqueous batteries via conversion reaction with copper ions
Aqueous battery Se-based cathodes are based on a two-electron transfer electrochemical reaction and generally show inadequate rate capability behaviour. Here, the authors propose a four-electron Se chemistry with copper ions as charge carriers to enable fast-charging battery cycling.
- Chunlong Dai
- , Linyu Hu
- & Liangti Qu
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Article
| Open AccessHigh-energy and durable lithium metal batteries using garnet-type solid electrolytes with tailored lithium-metal compatibility
Lithium-metal batteries (LMBs) have attracted intense interest but the instability issues limit its practical deployment. Here, the authors report a durable LMB with high energy density using a garnet-type solid electrolyte with a tailored Li-metal compatibility.
- Sewon Kim
- , Ju-Sik Kim
- & Kisuk Kang
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Article
| Open AccessHollow-core optical fibre sensors for operando Raman spectroscopy investigation of Li-ion battery liquid electrolytes
New analytical tools are needed to identify chemical degradation and failure mechanisms in Li-ion batteries. Here, the authors report an operando Raman spectroscopy method, based on hollow-core optical fibres, that enables monitoring the chemistry of liquid electrolytes during battery cycling.
- Ermanno Miele
- , Wesley M. Dose
- & Tijmen G. Euser
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Article
| Open AccessEpitaxial growth of an atom-thin layer on a LiNi0.5Mn1.5O4 cathode for stable Li-ion battery cycling
Transition metal dissolution from cathode materials limits the cycle life of Li-ion batteries. Here, the authors report an atomic-thin protecting layer on the surface of a high-voltage cathode material, enabling long-term Li-ion battery cycling.
- Xiaobo Zhu
- , Tobias U. Schülli
- & Lianzhou Wang