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| Open AccessBoosting the interfacial superionic conduction of halide solid electrolytes for all-solid-state batteries
Compositional tuning is a standard procedure to improve the ionic conductivity of inorganic superionic conductors. Here, the authors report (electro)chemical stable composite halide solid electrolytes applying a nanostructure approach that promotes interfacial superionic conductivity.
- Hiram Kwak
- , Jae-Seung Kim
- & Yoon Seok Jung
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Article
| Open AccessEffect of pulse-current-based protocols on the lithium dendrite formation and evolution in all-solid-state batteries
The practical use of all-solid-state batteries is hindered by lithium dendrites formed at current densities lower than the threshold suggested by industry research. Here, the authors propose a MHz-pulse-current protocol to circumvent the low-current cell failure and provide mechanistic analyses.
- V. Reisecker
- , F. Flatscher
- & D. Rettenwander
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Article
| Open AccessUnravelling rechargeable zinc-copper batteries by a chloride shuttle in a biphasic electrolyte
The zinc-copper (Zn-Cu) Daniell cell is regarded as primary battery due to the crossover of the copper species. Here, the authors report a rechargeable Zn-Cu battery with the combination of chloride shuttle chemistry in a ZnCl2 aqueous/organic biphasic electrolyte, delivering a high energy density with stable cycling performance
- Chen Xu
- , Chengjun Lei
- & Xiao Liang
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Article
| Open AccessBuilding electrode skins for ultra-stable potassium metal batteries
Metal potassium anodes show great potential in high energy density batteries. However, their practical application is hindered by the unstable nature of the highly active metal surface. Here, authors propose a “metal skin” approach that stabilizes the surface of the metal, resulting in improved cycle life of potassium metal anode-based batteries.
- Hongbo Ding
- , Jue Wang
- & Bingan Lu
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Article
| Open AccessPolyfluorinated crosslinker-based solid polymer electrolytes for long-cycling 4.5 V lithium metal batteries
Solid polymer electrolytes are commonly used in lithium-metal batteries, but their capacity and energy density cannot be easily increased beyond a charging cut-off voltage of 4.5 V due to the presence of easily oxidized oxygen-bearing polar groups. Here, authors apply a polyfluorinated crosslinker to enhance the oxidation resistance to solve this issue
- Lingfei Tang
- , Bowen Chen
- & Liwei Chen
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Article
| Open AccessElectronic signatures of Lorentzian dynamics and charge fluctuations in lithiated graphite structures
Lithium graphite intercalation compounds are important for developing Li-ion batteries. Here authors simulate the interaction of high energy X-rays with Li ions intercalated in graphite and show that Li ions behave in an unexpected non-Gaussian fashion, leading to increasingly chaotic behaviour as the ion concentration reduces.
- Sasawat Jamnuch
- & Tod A. Pascal
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Article
| Open AccessRapid determination of solid-state diffusion coefficients in Li-based batteries via intermittent current interruption method
The galvanostatic intermittent titration technique (GITT) is the state-of-the-art method for determining the Li+ diffusion coefficients in battery materials. Here, authors propose the intermittent current interruption method as a reliable, accurate and faster alternative to GITT-based methods.
- Yu-Chuan Chien
- , Haidong Liu
- & Matthew J. Lacey
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Article
| Open AccessExploiting nonaqueous self-stratified electrolyte systems toward large-scale energy storage
The use of energy-dense materials is inherently limited in biphasic self-stratified batteries due to the aqueous electrolyte environment. Here, the authors extended the concept of biphasic self-stratified batteries to non-aqueous systems, resulting in increased energy density and output voltage.
- Zhenkang Wang
- , Haoqing Ji
- & Chenglin Yan
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Article
| Open AccessA non-Newtonian fluid quasi-solid electrolyte designed for long life and high safety Li-O2 batteries
Lithium dendrite growth and liquid electrolyte volatilization limit the further development of lithium-oxygen batteries. Here, authors report a non-Newtonian fluid quasi-solid electrolyte to address those issues, which improve the life duration of the lithium-oxygen batteries.
- Guangli Zheng
- , Tong Yan
- & Huiyu Song
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Article
| Open AccessMultifunctional solvent molecule design enables high-voltage Li-ion batteries
The parasitic reactions at the electrolyte/electrode interfaces inhibit the increase of the charging cut-off voltage and the improvement of energy density. Herein, the authors design multifunctional solvent molecules and propose a practical design principle to stabilize the electrolyte/electrode interfaces for high-voltage Li ion batteries.
- Junbo Zhang
- , Haikuo Zhang
- & Xiulin Fan
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Article
| Open AccessAtomic-scale origin of the low grain-boundary resistance in perovskite solid electrolyte Li0.375Sr0.4375Ta0.75Zr0.25O3
Oxide solid electrolytes generally suffer from high grain boundary resistance. Here, the authors use advanced electron microscopy, along with an active learning moment tensor potential, to reveal the atomic-scale origin of low grain-boundary resistance in Li0.375Sr0.4375Ta0.75Zr0.25O3.
- Tom Lee
- , Ji Qi
- & Xiaoqing Pan
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Article
| Open AccessRealizing high-capacity all-solid-state lithium-sulfur batteries using a low-density inorganic solid-state electrolyte
Sulfur utilization in high-mass-loading positive electrodes is crucial for developing practical all-solid-state lithium-sulfur batteries. Here, authors propose a low-density inorganic solid-state electrolyte to improve the sulfur utilization in lab-scale Li-In||S all-solid-state cells.
- Daiwei Wang
- , Li-Ji Jhang
- & Donghai Wang
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Article
| Open AccessDevelopment of rechargeable high-energy hybrid zinc-iodine aqueous batteries exploiting reversible chlorine-based redox reaction
Cl-redox reactions cannot be fully exploited in batteries because of the Cl2 gas evolution. Here, reversible high-energy interhalogen reactions are demonstrated by using a iodine-based cathode in combination with a Zn anode and a Cl-containing aqueous electrolyte solution.
- Guojin Liang
- , Bochun Liang
- & Chunyi Zhi
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Article
| Open AccessSulfolane-containing aqueous electrolyte solutions for producing efficient ampere-hour-level zinc metal battery pouch cells
The negative electrode reversibility limits the lifespan of Zn metal batteries. Here, authors report an aqueous electrolyte with a reverse micelle structure that improves the reversibility of the Zn metal anode enabling the production of an ampere-hour-level pouch cell with five months lifetime.
- Yu Wang
- , Tairan Wang
- & Chunyi Zhi
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Article
| Open AccessAtomic-scale study clarifying the role of space-charge layers in a Li-ion-conducting solid electrolyte
Space-charge layers are believed to profoundly influence the interfaces in all-solid-state Li batteries. Here, the authors provide atomic scale insights into this phenomenon, and discover that its impact could be fundamentally different from commonly believed.
- Zhenqi Gu
- , Jiale Ma
- & Cheng Ma
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Article
| Open AccessSynergy of cations in high entropy oxide lithium ion battery anode
Though high entropy oxides have been explored as possible conversion-type negative electrodes for Li-ion batteries, the roles of the different elements remain unclear. Here the authors determine the behavior of each element during electrochemical cycling and connect it to the nanoscale structure.
- Kai Wang
- , Weibo Hua
- & Xiaoke Mu
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Article
| Open AccessHeterogeneous intercalated metal-organic framework active materials for fast-charging non-aqueous Li-ion capacitors
Ideal anode materials for Li-ion capacitors must demonstrate safety and fast-charging properties. Here, the authors propose intercalated metal-organic frameworks for fast-charging Li-ion capacitors using a combined machine learning design and spray-dry synthesis.
- Nobuhiro Ogihara
- , Masaki Hasegawa
- & Naoyuki Nagasako
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Article
| Open AccessLi3TiCl6 as ionic conductive and compressible positive electrode active material for all-solid-state lithium-based batteries
An ideal positive electrode for all-solid-state Li batteries should be ionic conductive and compressible. However, this is not possible with state-of-the-art metal oxides. Here, the authors demonstrate the use of an ionic conductive metal chloride as compressible positive electrode active material.
- Kai Wang
- , Zhenqi Gu
- & Cheng Ma
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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 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 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 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 AccessMetal-coordinated polybenzimidazole membranes with preferential K+ transport
Membranes with fast and selective ion transport are essential for electrochemical processes. Here the authors provide mechanistic insights into the structures of metal-ion coordinated polybenzimidazole membranes and the preferential K+ transport, and their application in an alkaline zinc-iron flow battery.
- Jine Wu
- , Chenyi Liao
- & Xianfeng Li
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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 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 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 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 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 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 AccessRecovery of oxidized two-dimensional MXenes through high frequency nanoscale electromechanical vibration
Despite their vast potential, the practical deployment of MXenes has been hampered by their tendency to be oxidized. Here, the authors show that simply vibrating MXene films in just a minute can remove the oxide layer formed and restore their electrochemical performance close to its original state.
- Heba Ahmed
- , Hossein Alijani
- & Leslie Y. Yeo