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| Open AccessDual fluorination of polymer electrolyte and conversion-type cathode for high-capacity all-solid-state lithium metal batteries
The practical use of all-solid-state batteries is hindered by inadequate cycling performance. Here, the authors propose a fluorination strategy for the positive electrode and polymeric electrolyte to develop all-solid-state Li||FeF3 pouch cells with high discharge capacity and long cycle life.
- Jiulin Hu
- , Chuanzhong Lai
- & Chilin Li
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Article
| Open AccessSlight compositional variation-induced structural disorder-to-order transition enables fast Na+ storage in layered transition metal oxides
In layered transition metal oxides as cathode active materials for Na-ion batteries, Na+ diffusion kinetics are impacted by Na+/vacancy ordering. Here, the authors suggest that the P2-type Na2/3Ni1/3Mn2/3O2 with large zigzag ordering exhibits high Na+ mobility and thus superior rate capability.
- Yuansheng Shi
- , Pengfeng Jiang
- & Xia Lu
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Article
| Open AccessLithiated Prussian blue analogues as positive electrode active materials for stable non-aqueous lithium-ion batteries
Prussian blue analogues (PBAs) are appealing materials for aqueous Na- and K- ion batteries but are limited for non-aqueous Li-ion storage. Here, the authors report the synthesis of various lithiated PBAs and discuss critical factors for improving the non-aqueous electrochemical storage of Li ions.
- Ziheng Zhang
- , Maxim Avdeev
- & Guang He
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Article
| Open AccessUnlocking the hidden chemical space in cubic-phase garnet solid electrolyte for efficient quasi-all-solid-state lithium batteries
Conventional compositions of garnet solid electrolytes have limited access to the cubic phase for a high Li content of 7.0, which is beneficial for stability against Li metals. Here, the authors unlock the hidden chemical space via a high entropy strategy, enabling stable long-term battery cycling.
- Sung-Kyun Jung
- , Hyeokjo Gwon
- & Ju-Sik Kim
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Article
| Open AccessEffect of current density on the solid electrolyte interphase formation at the lithium∣Li6PS5Cl interface
The interface between the Li metal electrode and inorganic solid electrolyte is crucial for developing reliable all-solid-state Li batteries. Here, the authors show that the Li plating current density distinctly affects the chemistry and morphology of interphase components formed at the interface.
- Sudarshan Narayanan
- , Ulderico Ulissi
- & Mauro Pasta
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Article
| Open AccessOnboard early detection and mitigation of lithium plating in fast-charging batteries
Fast-charging is highly desired for lithium-ion batteries but is hindered by potential hazardous lithium plating and the associated parasitic reactions. Here, the authors report a nondestructive differential pressure sensing method for early detection and mitigation of lithium plating in fast-charging batteries.
- Wenxiao Huang
- , Yusheng Ye
- & Yi Cui
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Article
| Open AccessLithium hexamethyldisilazide as electrolyte additive for efficient cycling of high-voltage non-aqueous lithium metal batteries
High-voltage non-aqueous lithium metal batteries suffer from poor cycling stability due to the presence of impurities in the electrolyte solution. Here, the authors report lithium hexamethyldisilazide to scavenge HF and H2O, prevent the Ni dissolution and suppress side reactions during cycling.
- Danfeng Zhang
- , Ming Liu
- & Yan-Bing He
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Comment
| Open AccessError, reproducibility and uncertainty in experiments for electrochemical energy technologies
The authors provide a metrology-led perspective on best practice for the electrochemical characterisation of materials for electrochemical energy technologies. Such electrochemical experiments are highly sensitive, and their results are, in practice, often of uncertain quality and challenging to reproduce quantitatively.
- Graham Smith
- & Edmund J. F. Dickinson
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Article
| Open AccessAn improved 9 micron thick separator for a 350 Wh/kg lithium metal rechargeable pouch cell
Thin separators can improve batteries’ energy densities but increase cell shortcircuit risks. Here, the authors report an improved thin metal-organic frameworks separator to improve the dendrite formation resistance and cycling stability of high-voltage lithium battery in carbonate electrolytes.
- Zhi Chang
- , Huijun Yang
- & Haoshen Zhou
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Article
| Open AccessDevelopment of long lifespan high-energy aqueous organic||iodine rechargeable batteries
Aqueous I2-based batteries are a promising system for cost-effective and environmentally-friendly electricity storage. Here, the authors propose a high-capacity and long-lasting aqueous I2 battery system using an electrochemically active organic molecule at the negative electrode.
- Zishuai Zhang
- , Yilong Zhu
- & Yan Huang
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Article
| Open AccessSurface chemical heterogeneous distribution in over-lithiated Li1+xCoO2 electrodes
Over-lithiation often causes structural transformation in electrodes and may lead to safety issues in Li-ion batteries. Here, authors investigate the over-discharged mechanism of LiCoO2/graphite pouch cells, and spatially resolve the morphological, surface phase, and local electronic structure of LiCoO2 electrode.
- Gang Sun
- , Fu-Da Yu
- & Zhenbo Wang
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Article
| 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 AccessA medium-entropy transition metal oxide cathode for high-capacity lithium metal batteries
Structural instability is a major drawback of high-capacity lithium-based battery cathodes. Here, the authors report a cathode active material with a medium-entropy state created by partial cation disordering capable of restraining the structural evolution in the high-capacity operated spinel phase.
- Yi Pei
- , Qing Chen
- & Cheng-Yan Xu
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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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Matters Arising
| Open AccessCritical evaluation of (110) texture in lithium electrodeposits on isotropic Cu polycrystals
- Chaojing Lu
- & Zongta Luo
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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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Article
| Open AccessUnconventional interfacial water structure of highly concentrated aqueous electrolytes at negative electrode polarizations
Water-in-salt electrolytes can be useful for future electrochemical energy storage systems. Here, the authors investigate the potential-dependent double-layer structures at the interface between a gold electrode and a highly concentrated aqueous electrolyte solution via in situ Raman measurements.
- Chao-Yu Li
- , Ming Chen
- & Tianquan Lian
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Article
| Open AccessTransition metal migration and O2 formation underpin voltage hysteresis in oxygen-redox disordered rocksalt cathodes
The oxygen-redox mechanism in lithium-rich disordered rocksalt cathode materials is still not well understood. Here, the authors show that in Li2MnO2F, molecular oxygen forms in the bulk during charge and is re-incorporated into the structure as oxygen anions on discharge, but this process is associated with irreversible Mn migration, causing voltage hysteresis.
- Kit McColl
- , Robert A. House
- & M. Saiful Islam
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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 AccessVisualizing the failure of solid electrolyte under GPa-level interface stress induced by lithium eruption
The mechanism of lithium dendrites penetrating solid electrolytes remains elusive. Herein, the authors reveal the Li deposition dynamics and the associated failure mechanism of solid electrolyte by visualizing the Li|LLZO interface evolution via in situ transmission electron microscopy.
- Haowen Gao
- , Xin Ai
- & Ming-Sheng Wang
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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 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 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 AccessUnderstanding the lithium–sulfur battery redox reactions via operando confocal Raman microscopy
The complex redox processes in lithium–sulfur batteries are not yet fully understood at the fundamental level. Here, the authors report operando confocal Raman microscopy measurements to provide mechanistic insights into polysulfide evolution and sulfur deposition during battery cycling.
- Shuangyan Lang
- , Seung-Ho Yu
- & Héctor D. Abruña
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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 AccessThe role of solid solutions in iron phosphate-based electrodes for selective electrochemical lithium extraction
Lithium extraction from dilute sources could help solve the lithium supply security issue. Here, the authors investigate the Li- and Na- ion co-intercalation behavior in iron phosphate electrodes and demonstrate the lithium selectivity control through intercalation kinetic manipulations.
- Gangbin Yan
- , George Kim
- & Chong Liu
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Article
| Open AccessNon-fluorinated non-solvating cosolvent enabling superior performance of lithium metal negative electrode battery
Localised high-concentration electrolyte is key to prevent uneven growth of lithium metal by forming a mechanically stable solid-electrolyte interphase. Here, the authors identify the suitable physicochemical properties for non-solvating co-solvents that improve the performance of lithium metal battery.
- Junyeob Moon
- , Dong Ok Kim
- & Jongwoo Lim
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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 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 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 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 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