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| Open AccessUltrahigh loading dry-process for solvent-free lithium-ion battery electrode fabrication
Scalable dry electrode process is essential for the sustainable manufacturing of the lithium based batteries. Here, the authors propose a dry press-coating technique to fabricate a robust and flexible high loading electrode for lithium pouch cells.
- Minje Ryu
- , Young-Kuk Hong
- & Jong Hyeok Park
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Article
| Open AccessNanoarchitecture factors of solid electrolyte interphase formation via 3D nano-rheology microscopy and surface force-distance spectroscopy
Characterization of the solid electrolyte interphase formed on Li-ion battery electrodes presents significant experimental challenges. Here the authors use atomic force microscopy-based force-spectroscopy techniques to depict the initial interphase formation in two different electrolyte classes.
- Yue Chen
- , Wenkai Wu
- & Oleg V. Kolosov
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Article
| Open AccessUnderstanding the evolution of lithium dendrites at Li6.25Al0.25La3Zr2O12 grain boundaries via operando microscopy techniques
Lithium metal penetration into solid-state electrolytes is a major drawback for developing all-solid-state batteries. Here, authors, via operando force microscopy, demonstrate that the trapping of electrons in garnet-type solid-state electrolyte grain boundaries is the origin of cell failure.
- Chao Zhu
- , Till Fuchs
- & Rüdiger Berger
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Article
| Open AccessNaked metallic skin for homo-epitaxial deposition in lithium metal batteries
The oxide passivation layer on the lithium metal surface causes uneven deposition and stripping in lithium metal batteries. Here authors introduce uniform homo-epitaxial lithium deposition on the metal surface to alleviate this issue and improve the cycle stability of the lithium metal batteries.
- Minsung Baek
- , Jinyoung Kim
- & Jang Wook Choi
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Article
| Open AccessHeterovalent-doping-enabled atom-displacement fluctuation leads to ultrahigh energy-storage density in AgNbO3-based multilayer capacitors
AgNbO3 has a potential for high power capacitors due to its antiferroelectric characteristics. Here, the authors achieve multilayer capacitors with energy-storage density of 14 J·cm−3 by heterovalent-doping-enabled atom-displacement fluctuation.
- Li-Feng Zhu
- , Shiqing Deng
- & Jing-Feng Li
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Article
| Open AccessA monofluoride ether-based electrolyte solution for fast-charging and low-temperature non-aqueous lithium metal batteries
The energy content of non-aqueous lithium batteries is limited by the electrochemical stability window of the electrolyte solution. Here, the authors report a monofluoride ether-based electrolyte to stabilize high-voltage lithium metal batteries at high current rates and low temperatures.
- Guangzhao Zhang
- , Jian Chang
- & Jun Lu
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Article
| Open AccessAnion-enrichment interface enables high-voltage anode-free lithium metal batteries
The implementation of Li metal anode with high-voltage Ni/Co rich cathode is plagued by low coulombic efficiency and inferior cycling stability. Here authors propose an anion-enriched interface to facilitate the columnar-structure of Li deposits to solve this issue.
- Minglei Mao
- , Xiao Ji
- & Liumin Suo
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Article
| Open AccessElectrolyte design principles for developing quasi-solid-state rechargeable halide-ion batteries
State-of-the-art electrolytes limit the cycle life of halide-ion batteries. Here, the authors report a fluorinated low-polar gel polymer electrolyte capable of improving the stability of the electrolyte and electrode interphases to boost battery performance.
- Xu Yang
- , Bao Zhang
- & Guoxiu Wang
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Article
| Open AccessNon-polar ether-based electrolyte solutions for stable high-voltage non-aqueous lithium metal batteries
Ether solvents have poor anodic stabilities in lithium metal batteries. Here, the authors propose a non-aqueous electrolyte solution with a non-polar and non-fluorinated ether solvent. The electrolyte enables stable cycling of high-voltage Li metal batteries in pouch cell configuration.
- Zheng Li
- , Harsha Rao
- & Vilas G. Pol
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Article
| Open AccessInvestigating microstructure evolution of lithium metal during plating and stripping via operando X-ray tomographic microscopy
Understanding the plating and stripping behaviours of lithium metal is crucial for high-energy battery development. Here, authors track these electrochemical processes in real time by an operando synchrotron X-ray tomographic microscopy, revealing the formation of inactive lithium microstructures.
- Matthew Sadd
- , Shizhao Xiong
- & Aleksandar Matic
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Article
| Open AccessSurface engineering of inorganic solid-state electrolytes via interlayers strategy for developing long-cycling quasi-all-solid-state lithium batteries
Lithium metal batteries (LMBs) with inorganic solid-state electrolytes suffer from lithium dendrites propagation. Here, the authors demonstrate the production of stable lab-scale LMBs using an Ag-coated Li6.4La3Zr1.7Ta0.3O12 inorganic solid electrolyte in combination with a silver-carbon interlayer.
- Ju-Sik Kim
- , Gabin Yoon
- & Dongmin Im
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Article
| Open AccessUltrathin positively charged electrode skin for durable anion-intercalation battery chemistries
The application of graphite as anodes for anion-intercalation chemistry-based batteries suffers from durability issues. Here authors demonstrate that a positively charged two-dimensional poly(pyridinium salt) membrane can work as the artificial skin of the graphite electrode to enable long-term cycling stability.
- Davood Sabaghi
- , Zhiyong Wang
- & Xinliang Feng
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Article
| Open AccessSelf-organized hetero-nanodomains actuating super Li+ conduction in glass ceramics
The development of Li2S-P2S5 glass ceramics is greatly hampered by the low room temperature lithium conductivity. Here, the authors propose a nanocrystallization strategy to fabricate super lithium conductive glass ceramics.
- Yantao Wang
- , Hongtao Qu
- & Liquan Chen
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Article
| Open AccessPhase-engineered cathode for super-stable potassium storage
The large radius of potassium ions inevitably destabilizes the crystal structure of the cathode material in potassium-ion batteries, leading to capacity degradation. Here, authors demonstrate that phase-engineered amorphous vanadium oxide alleviates large volume variation and improves electrochemical behaviour.
- Lichen Wu
- , Hongwei Fu
- & Bingan Lu
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Article
| Open AccessGradient design of imprinted anode for stable Zn-ion batteries
Zinc metal anodes suffer from electrolyte corrosion and dendrite growth issues during electrochemical cycling. Here, the authors propose a gradient design to imprint the zinc anode, which both prohibits side reactions and alleviates zinc deposition behaviour.
- Qinghe Cao
- , Yong Gao
- & Cao Guan
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Article
| Open AccessDispersed surface Ru ensembles on MgO(111) for catalytic ammonia decomposition
Ruthenium-based materials show promising performance for ammonia decomposition, yet the underlying mechanism remains to be further explored. Here the authors investigate atomically dispersed Ru atoms on polar (111) on MgO facets to show synergistic metal sites in close proximity are required for the stepwise dehydrogenation of ammonia to N2/H2.
- Huihuang Fang
- , Simson Wu
- & Shik Chi Edman Tsang
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Article
| Open AccessDirect regeneration of degraded lithium-ion battery cathodes with a multifunctional organic lithium salt
Sustainable recycle of spent Li ion batteries is an effective strategy to alleviate environmental concerns and support resource conservation. Here, authors report the direct regeneration of LiFePO4 cathode using multifunctional organic lithium salts, leading to high environmental and economic benefits.
- Guanjun Ji
- , Junxiong Wang
- & Hui-Ming Cheng
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Article
| Open AccessTailoring water structure with high-tetrahedral-entropy for antifreezing electrolytes and energy storage at −80 °C
The anti-freezing property of electrolyte is crucial for aqueous batteries under extreme conditions. Here authors explore the relationship between tetrahedral entropy and the freezing behavior of aqueous electrolyte, and further develop anti-freezing electrolyte for aqueous zinc ion batteries.
- Meijia Qiu
- , Peng Sun
- & Wenjie Mai
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Article
| Open AccessBinuclear Cu complex catalysis enabling Li–CO2 battery with a high discharge voltage above 3.0 V
Li–CO2 batteries following Li2CO3-product route suffer from low output voltage and severe parasitic reactions. Herein, a soluble binuclear copper(I) complex is introduced as the liquid catalyst to achieve Li2C2O4 products in Li–CO2 batteries, which increases their output voltage to higher than 3.0 V.
- Xinyi Sun
- , Xiaowei Mu
- & Haoshen Zhou
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Article
| Open AccessTailoring polymer electrolyte ionic conductivity for production of low- temperature operating quasi-all-solid-state lithium metal batteries
Low-temperature batteries are detrimentally affected by the sluggish kinetics of the electrolyte. Here, the authors propose a quasi-solid-state polymer electrolyte capable of improving interfacial charge transfer and enabling stable Li metal cell operation even at −30 °C.
- Zhuo Li
- , Rui Yu
- & Xin Guo
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Article
| Open AccessHigh entropy liquid electrolytes for lithium batteries
Electrolytes, function as an ion conducting membrane between battery electrodes, are essential for rechargeable batteries. Here, the authors report high-entropy liquid electrolytes and reveal substantial impact of the increasing entropy on lithium-ion solvation structures for highly reversible lithium batteries.
- Qidi Wang
- , Chenglong Zhao
- & Marnix Wagemaker
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Perspective
| Open AccessA non-academic perspective on the future of lithium-based batteries
In the field of lithium-based batteries, there is often a divide between academic research and industrial needs. Here, the authors present a view on applied research to help bridge academia and industry, focusing on metrics and challenges to be considered for the development of practical batteries.
- James T. Frith
- , Matthew J. Lacey
- & Ulderico Ulissi
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Article
| Open AccessIsolation of pseudocapacitive surface processes at monolayer MXene flakes reveals delocalized charging mechanism
MXenes are two-dimensional nanomaterials that can be used as supercapacitors to store electrical energy. Here, the authors isolated chemical response from a single MXene flake and provide a new understanding of the surface chemistry of MXenes.
- Marc Brunet Cabré
- , Dahnan Spurling
- & Kim McKelvey
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Article
| Open AccessIsolated Fe-Co heteronuclear diatomic sites as efficient bifunctional catalysts for high-performance lithium-sulfur batteries
The slow redox kinetics of polysulfides and the difficulties in decomposition of Li2S are two serious obstacles to lithium-sulfur batteries. Here, the authors report an isolated Fe-Co heteronuclear diatomic catalyst to achieve high efficiency bifunctional catalysis for lithium-sulfur batteries.
- Xun Sun
- , Yue Qiu
- & Naiqing Zhang
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Article
| Open AccessElectrolyte engineering via ether solvent fluorination for developing stable non-aqueous lithium metal batteries
Fluorination of solvents, useful for non-aqueous lithium-based batteries, improves the electrochemical stability but decreases the ionic conductivity. Here, the authors report a targeted functionalization of an ether solvent to balance the electrolyte ionic conductivity and oxidative stability.
- Yan Zhao
- , Tianhong Zhou
- & Ali Coskun
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Article
| Open AccessUnderstanding the failure process of sulfide-based all-solid-state lithium batteries via operando nuclear magnetic resonance spectroscopy
All-solid-state lithium batteries performance is affected by the solid electrolyte interphase (SEI) and electrically disconnected (“dead”) Li metal. Here, via operando NMR measurements, the authors quantify the Li metal in the SEI and “dead” regions using various inorganic solid-state electrolytes.
- Ziteng Liang
- , Yuxuan Xiang
- & Yong Yang
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Article
| Open AccessElectric vehicle batteries alone could satisfy short-term grid storage demand by as early as 2030
Renewable energy and electric vehicles will be required for the energy transition, but the global electric vehicle battery capacity available for grid storage is not constrained. Here the authors find that electric vehicle batteries alone could satisfy short-term grid storage demand by as early as 2030.
- Chengjian Xu
- , Paul Behrens
- & Bernhard Steubing
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Article
| Open AccessGas induced formation of inactive Li in rechargeable lithium metal batteries
The formation of electrochemically inactive, or “dead”, lithium limits the reversibility of lithium metal batteries. Here the authors elucidate the (electro)chemical roles of ethylene gas produced from electrolyte decomposition on the formation of inactive lithium.
- Yuxuan Xiang
- , Mingming Tao
- & Yong Yang
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Article
| Open AccessSiO-induced thermal instability and interplay between graphite and SiO in graphite/SiO composite anode
SiO is an adequate anode material for next generation lithium-ion batteries, but little is known about its aging mechanism. Here, the authors report thermal instability of the graphite/SiO composite anode induced by the accelerated loss of lithium from SiO and have elucidated the interplay between graphite and SiO.
- Ban Seok Lee
- , Sang-Hwan Oh
- & Seung-Ho Yu
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Article
| Open AccessA gradient oxy-thiophosphate-coated Ni-rich layered oxide cathode for stable all-solid-state Li-ion batteries
Layered oxide cathode active materials suffer from interfacial structural instability when coupled with sulfide solid-state electrolytes. Here, the authors propose a gradient coating with a lithium oxythiophosphate layer that can stabilize the cathode|solid-state electrolyte interface.
- Jianwen Liang
- , Yuanmin Zhu
- & Xueliang Sun
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Article
| Open AccessConstructing robust heterostructured interface for anode-free zinc batteries with ultrahigh capacities
The development of dendrite-free, Zn-free anodes is challenging. Here, the authors design a two-dimensional antimony/antimony-zinc alloy heterostructured interface to achieve dendrite-free Zn deposition with areal capacity of 200 mAh cm−2, and energy density of around 270 Wh kg−1 for anode-free zinc-bromine battery.
- Xinhua Zheng
- , Zaichun Liu
- & Wei Chen
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Article
| Open AccessHigh-strength and machinable load-bearing integrated electrochemical capacitors based on polymeric solid electrolyte
High-strength composite materials for electrochemical energy storage is attractive for mobile systems. Here the authors demonstrate high-performance load-bearing integrated electrochemical capacitors, which show high strength, large capacitance, and good machinability.
- Jinmeng Zhang
- , Jianlong Yan
- & Hua Bai
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Article
| Open AccessSurface-redox sodium-ion storage in anatase titanium oxide
Sodium ion storage remains relatively unexplored in comparison with well-understood lithium ion storage mechanisms. Here, the authors systematically investigate the surface-redox sodium ion storage properties of anatase titanium dioxide, which delivers excellent rate capability, cycling stability and low overpotentials.
- Qiulong Wei
- , Xiaoqing Chang
- & Bruce Dunn
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Article
| 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 AccessThree-dimensional Zn-based alloys for dendrite-free aqueous Zn battery in dual-cation electrolytes
The dual-cations electrochemical system was considered to be a promising strategy to facilitate sluggish diffusion kinetics. Here the authors prepare zinc-based alloy anode with three-dimensional interface, thus to improve the interfacial stability, achieve high-performing battery system in the aqueous electrolytes containing dual cations.
- Huajun Tian
- , Guangxia Feng
- & Yang Yang
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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 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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Article
| Open Access4D printing of MXene hydrogels for high-efficiency pseudocapacitive energy storage
2D MXene hydrogels are promising for diverse applications. Here, the authors report a universal 4D printing technology to manufacture MXene hydrogels with customizable geometry, high conductivity, and efficient pseudocapacitive energy storage ability.
- Ke Li
- , Juan Zhao
- & Valeria Nicolosi
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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 AccessAqueous hybrid electrochemical capacitors with ultra-high energy density approaching for thousand-volts alternating current line filtering
Filtering capacitors are essential to smooth high voltage alternating current lines but are typically limited to hundreds of volts. Here, the authors demonstrate an aqueous hybrid electrochemical capacitor that can exhibit an operating voltage of 1,000 V when assembled into a device of 670 units.
- Zhou Li
- , Xiaopeng Wang
- & Liangti Qu
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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 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