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| Open AccessGas–solid interfacial modification of oxygen activity in layered oxide cathodes for lithium-ion batteries
Oxygen activity can play a vital role in determining charge transport properties of materials. Here, the authors demonstrate a method to create oxygen vacancies on layered oxides via a gas-solid interface reaction, leading to materials with enhanced energy and power densities for Li-ion batteries.
- Bao Qiu
- , Minghao Zhang
- & Ying Shirley Meng
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Article
| Open AccessArray of nanosheets render ultrafast and high-capacity Na-ion storage by tunable pseudocapacitance
Sodium ion batteries are a promising alternative to lithium ion technology, however their sluggish sodiation kinetics currently hinder performance. Here the authors fabricate ultrathin layered tin(II) sulfide nanostructures displaying a pseudocapacitance contribution for high capacity sodium ion anodes.
- Dongliang Chao
- , Changrong Zhu
- & Ze Xiang Shen
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Article
| Open AccessSuperconcentrated electrolytes for a high-voltage lithium-ion battery
Electrode degradation due to metal-ion dissolution in conventional electrolyte hampers the performance of 5 V-class lithium ion batteries. Here, the authors employ a high concentration electrolyte to inhibit metal-ion dissolution and realize a stable high voltage LiNi0.5Mn1.5O4/graphite battery.
- Jianhui Wang
- , Yuki Yamada
- & Atsuo Yamada
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Article
| Open AccessWater-mediated cation intercalation of open-framework indium hexacyanoferrate with high voltage and fast kinetics
Rechargeable aqueous metal-ion batteries are promising for large-scale applications, but performance and stability issues still remain. Here the authors utilize open-framework indium hexacyanoferrate cathodes to improve performance, showing that water-mediated cation intercalation occurs at the cathode.
- Liang Chen
- , Hezhu Shao
- & Zhaoping Liu
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Article
| Open AccessFailure mechanisms of single-crystal silicon electrodes in lithium-ion batteries
Long-term durability is crucial for heavy-duty usage of lithium ion batteries; however, electrode failure mechanisms are still unknown. Here, the authors reveal the fracture mechanisms of single crystal silicon electrodes over extended cycling, and show how electrolyte additives can heal electrode cracks.
- Feifei Shi
- , Zhichao Song
- & Kyriakos Komvopoulos
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Article
| Open AccessStabilizing lithium metal using ionic liquids for long-lived batteries
Suppressing dendrite formation at lithium anodes during cycling is critical to development of lithium battery technology. Here, the authors show that immersion of lithium electrodes in ionic liquid electrolytes prior to battery assembly produces a durable and lithium ion permeable solid-electrolyte interphase.
- A. Basile
- , A. I. Bhatt
- & A. P. O’Mullane
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Article
| Open AccessA stable room-temperature sodium–sulfur battery
Rechargeable sodium-sulfur batteries able to operate stably at room temperature are sought-after platforms as they can achieve high storage capacity from inexpensive electrode materials. Here, the authors use rationally selected cathode and electrolyte materials to design a room temperature Na-S battery.
- Shuya Wei
- , Shaomao Xu
- & Lynden A. Archer
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Article
| Open AccessAvoiding short circuits from zinc metal dendrites in anode by backside-plating configuration
Zinc-based aqueous battery chemistries allow for attractive cost and energy densities, but are susceptible to zinc dendrite formation during plating and internal shorting. Here, the authors show that by plating only on the side away from the counter-electrode, internal shorts can be circumvented.
- Shougo Higashi
- , Seok Woo Lee
- & Yi Cui
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Article
| Open AccessFreestanding three-dimensional core–shell nanoarrays for lithium-ion battery anodes
Degradation and low conductivity of transition metal oxide anodes cause capacity fading in lithium ion batteries. Here the authors make freestanding 3D copper oxide/carbon nitride core-shell nanoarrays which accommodate volume change, provide electro-active zones and facilitate rapid charge transport.
- Guoqiang Tan
- , Feng Wu
- & Khalil Amine
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Article
| Open AccessIntegrating a dual-silicon photoelectrochemical cell into a redox flow battery for unassisted photocharging
Technologies for in situ capture and storage of intermittent solar energy are an important research goal. Here the authors report a solar rechargeable flow cell based on a dual-silicon photoelectrochemical cell and a quinone/bromine redox flow battery for in situsolar energy conversion and storage.
- Shichao Liao
- , Xu Zong
- & Can Li
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Article
| Open AccessIntermediate honeycomb ordering to trigger oxygen redox chemistry in layered battery electrode
Sodium-excess metal oxides Na2MO3 are appealing cathode materials for sodium-ion batteries. Here, the authors demonstrate that honeycomb-type cation ordering in Na2RuO3 triggers the oxygen redox reaction via frontier orbital reorganization, increasing the capacity by 1/3 compared with disordered Na2RuO3.
- Benoit Mortemard de Boisse
- , Guandong Liu
- & Atsuo Yamada
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Article
| Open AccessBalancing surface adsorption and diffusion of lithium-polysulfides on nonconductive oxides for lithium–sulfur battery design
Metal oxides can suppress detrimental polysulfide shuttling in lithium-sulfur batteries, however selection criteria for oxide materials are still lacking. Here, the authors investigate polysulfide adsorption and diffusion on metal oxides and propose selection criteria based on balancing these two effects.
- Xinyong Tao
- , Jianguo Wang
- & Yi Cui
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Article
| Open AccessSilicon oxycarbide glass-graphene composite paper electrode for long-cycle lithium-ion batteries
Most high-loading silicon-based anodes for lithium-ion batteries suffer from low efficiency and volumetric capacity. Here, the authors show that a paper-like electrode of silicon oxycarbide glass and graphene at mass loading of >2 mg cm−2can efficiently deliver high energy density for over 1,000 cycles.
- Lamuel David
- , Romil Bhandavat
- & Gurpreet Singh
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Article
| Open AccessCalcium-based multi-element chemistry for grid-scale electrochemical energy storage
Calcium is an attractive but poorly studied material for the negative electrode in a rechargeable battery. Here, the authors use a multi-cation binary electrolyte along with an alloyed negative electrode to make a calcium-based rechargeable battery with enhanced stability and reduced operating temperature.
- Takanari Ouchi
- , Hojong Kim
- & Donald R. Sadoway
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Article
| Open AccessLi(V0.5Ti0.5)S2 as a 1 V lithium intercalation electrode
Lithium sulfides have been previously investigated as 1 V anodes for Li-ion batteries, but suffered from significant performance issues. Here, the authors report on a 1 V lithium sulfide electrode with noteworthy performance, demonstrating that sulfide-based electrodes may merit further exploration.
- Steve J. Clark
- , Da Wang
- & Peter G. Bruce
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Article
| Open AccessDesign and synthesis of the superionic conductor Na10SnP2S12
Solid electrolytes are an attractive alternative to the flammable organic solvents typically used in intercalation batteries. Here, the authors report the computation-assisted discovery and synthesis of Na10SnP2S12, a sodium electrolyte with room temperature conductivity of 0.4 mS cm−1.
- William D. Richards
- , Tomoyuki Tsujimura
- & Gerbrand Ceder
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Article
| Open AccessDissolution and ionization of sodium superoxide in sodium–oxygen batteries
Sodium-oxygen batteries are promising energy storage devices but the nature of their discharge products remains unresolved. Here, the authors reveal that the dissolution and ionization of sodium superoxide leads to the formation of other phases, which increases the charge overpotential of the cell.
- Jinsoo Kim
- , Hyeokjun Park
- & Kisuk Kang
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Article
| Open AccessAdvanced intermediate temperature sodium–nickel chloride batteries with ultra-high energy density
Sodium metal halide batteries are attractive technologies for stationary electrical energy storage. Here, the authors report that planar sodium-nickel chloride batteries operated at an intermediate temperature of 190 °C display larger energy densities than tubular batteries operated at higher temperatures.
- Guosheng Li
- , Xiaochuan Lu
- & Vincent L. Sprenkle
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| Open AccessThree-dimensional porous carbon composites containing high sulfur nanoparticle content for high-performance lithium–sulfur batteries
Lithium–sulfur batteries have high theoretical capacities but their performance is limited by poor conductivity and low stability. Here, the authors fabricate three-dimensional porous graphitic carbon composites containing sulfur nanoparticles and probe the effect of sulfur content on battery performance.
- Guoxing Li
- , Jinhua Sun
- & Jianxin Geng
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Article
| Open AccessInsertion compounds and composites made by ball milling for advanced sodium-ion batteries
New sodium-ion battery technology requires better control over solid electrolyte interface formation. Here, the authors report a series of ball-milled sodium alloys and enriched insertion electrodes, which act as sodium reservoirs compensating for sodium loss during solid electrolyte interface formation.
- Biao Zhang
- , Romain Dugas
- & Jean-Marie Tarascon
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| Open AccessA highly reversible room-temperature lithium metal battery based on crosslinked hairy nanoparticles
There is intensive research effort in suppressing lithium dendrite growth in lithium batteries. Here, the authors report the use of a crosslinked nanoparticle-polymer composite membrane with high mechanical strength and ionic conductivity which enables stable cycling of lithium metal batteries.
- Snehashis Choudhury
- , Rahul Mangal
- & Lynden A. Archer
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Article
| Open AccessPie-like electrode design for high-energy density lithium–sulfur batteries
Lithium-sulfur batteries are a promising candidate for next-generation battery technologies. Here, the authors report a pie-like structured electrode in which sulfur is confined in multichannel carbon nanofibers which is then coated by amino-functionalized graphene, leading to good balance between electrochemical performance and cell energy density.
- Zhen Li
- , Jin Tao Zhang
- & Xiong Wen (David) Lou
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Article
| Open AccessInward lithium-ion breathing of hierarchically porous silicon anodes
Porous silicon is highly promising as an anode material in lithium ion batteries, but its volume change upon lithiation has deleterious effects upon efficiency. Here, the authors demonstrate porous shell/hollow core Si nanospheres which exhibit negligible outward expansion and maintain performance.
- Qiangfeng Xiao
- , Meng Gu
- & Mei Cai
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Article
| Open AccessUniform yolk-shell iron sulfide–carbon nanospheres for superior sodium–iron sulfide batteries
There is intensive research into the development of sodium–metal sulfide batteries. Here, the authors report a yolk-shell-like iron sulfide–carbon nanosphere structure as the cathode material which displays exceptionally high performance.
- Yun-Xiao Wang
- , Jianping Yang
- & Shi Xue Dou
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| Open AccessEvidence of covalent synergy in silicon–sulfur–graphene yielding highly efficient and long-life lithium-ion batteries
Silicon anodes are promising for lithium-ion battery development, but suffer from problems such as undesired volume expansion and solid-electrolyte interface formation. Here, the authors report a hierarchical silicon-sulfur-graphene composite anode which mitigates the problems leading to high performance.
- Fathy M. Hassan
- , Rasim Batmaz
- & Zhongwei Chen
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Article
| Open AccessHigh damage tolerance of electrochemically lithiated silicon
Mechanical degradation is an undesired behaviour for battery electrode materials such as lithiated silicon. Here, the authors performin situnanomechanical experiments and atomistic modelling to reveal the damage tolerance of electrochemically lithiated silicon.
- Xueju Wang
- , Feifei Fan
- & Shuman Xia
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Article
| Open AccessDirect view on the phase evolution in individual LiFePO4 nanoparticles during Li-ion battery cycling
Understanding phase transitions in electrodes under realistic conditions is important for future battery design. Here, the authors use synchrotron micro-beam diffraction to reveal the phase transition mechanism within individual particles of LiFePO4, revealing a cycling rate transformation mechanism.
- Xiaoyu Zhang
- , Martijn van Hulzen
- & Marnix Wagemaker
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Article
| Open AccessCombined operando X-ray diffraction–electrochemical impedance spectroscopy detecting solid solution reactions of LiFePO4 in batteries
A clear understanding of the phase behaviour of lithium-ion electrode materials is essential for the development of the field. Here, the authors report a combined X-ray diffraction–electrochemical impedance spectroscopy method to detect solid solution reactions of LiFePO4.
- Michael Hess
- , Tsuyoshi Sasaki
- & Petr Novák
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Article
| Open AccessEfficiently photo-charging lithium-ion battery by perovskite solar cell
Photo-charged battery devices are an attractive technology but suffer from low photo-electric storage conversion efficiency and poor cycling stability. Here, the authors demonstrate the use of perovskite solar cells in conjunction with a lithium ion battery which displays excellent properties.
- Jiantie Xu
- , Yonghua Chen
- & Liming Dai
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Article
| Open AccessAccommodating lithium into 3D current collectors with a submicron skeleton towards long-life lithium metal anodes
A major problem with the use of lithium metal as the battery anode is the undesired lithium dendrite formation during cycling. Here, the authors show that the problem can be mitigated with a carefully designed three-dimensional porous current collector.
- Chun-Peng Yang
- , Ya-Xia Yin
- & Yu-Guo Guo
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| Open AccessVisualizing nanoscale 3D compositional fluctuation of lithium in advanced lithium-ion battery cathodes
It is challenging to quantitatively diagnose the lithium-ion distribution in batteries. Here, the authors use laser-assisted atom probe tomography to probe the nanoscale compositional fluctuations of lithium ions in two popular lithium-ion battery cathodes before and after electrochemical cycling.
- A. Devaraj
- , M. Gu
- & S. Thevuthasan
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| Open AccessRETRACTED ARTICLE: High-rate aluminium yolk-shell nanoparticle anode for Li-ion battery with long cycle life and ultrahigh capacity
Aluminium offers an attractive alternative anode for lithium-ion batteries, but its practical performance falls far short of the theoretical promise. Here, the authors present a yolk-shell structured nanocomposite anode of aluminium core and titanium oxide shell which displays outstanding electrochemical properties.
- Sa Li
- , Junjie Niu
- & Ju Li
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Article
| Open AccessFlexible lithium–oxygen battery based on a recoverable cathode
Flexible energy storage systems usually have limited energy densities. Here the authors report a flexible lithium–oxygen battery with the cathode consisting of titanium dioxide nanowire arrays grown on carbon textiles, which displays high mechanical strength as well as promising electrochemical performance.
- Qing-Chao Liu
- , Ji-Jing Xu
- & Xin-Bo Zhang
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Article
| Open AccessUnlocking the energy capabilities of micron-sized LiFePO4
Nanonization of battery electrode particles is a usual way to enhance their conductivity, but the decreased tap density is detrimental to battery performance. Here, the authors coat micron-sized lithium iron phosphate with a conducting polymer layer and demonstrate some excellent electrochemical properties.
- Limin Guo
- , Yelong Zhang
- & Zhangquan Peng
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| Open AccessLong-life Li/polysulphide batteries with high sulphur loading enabled by lightweight three-dimensional nitrogen/sulphur-codoped graphene sponge
There is intensive research underway into the cathode development of lithium–sulphur batteries. Here, the authors report a lithium–sulphur battery using nitrogen/sulphur codoped graphene structure which displays excellent electrochemical performance with high sulphur loading.
- Guangmin Zhou
- , Eunsu Paek
- & Arumugam Manthiram
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| Open AccessProbing three-dimensional sodiation–desodiation equilibrium in sodium-ion batteries by in situ hard X-ray nanotomography
In situ3D visualization of sodium-ion battery processes is challenging due to the highly active sodium metal and the sluggish kinetics. Here, the authors present a X-ray tomography technique, which enables tracking the sodiation–desodiation process of a Sn anode in battery operation.
- Jiajun Wang
- , Christopher Eng
- & Jun Wang
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Article
| Open AccessKinetics and fracture resistance of lithiated silicon nanostructure pairs controlled by their mechanical interaction
It is imperative to understand how individual Si nanostructures interact in battery operations. Here, the authors design well-defined crystalline Si nanopillars and show how mechanical interactions of neighbouring Si structures affect their reaction kinetics and fracture resistance during electrochemical lithiation.
- Seok Woo Lee
- , Hyun-Wook Lee
- & Yi Cui
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Article
| Open AccessSilicon carbide-free graphene growth on silicon for lithium-ion battery with high volumetric energy density
The volume expansion of silicon is a big problem in lithium-ion batteries with silicon anodes. Here, the authors report direct graphene growth on silicon nanoparticles, which effectively mitigates the problem, leading to excellent electrochemical performance.
- In Hyuk Son
- , Jong Hwan Park
- & Hyuk Chang
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The synergetic effect of lithium polysulfide and lithium nitrate to prevent lithium dendrite growth
Lithium dendrite growth is a serious hazard in battery operations. Here, the authors show that when using lithium polysulfide and lithium nitrate as additives in ether-based electrolyte, a stable and uniform solid electrolyte interphase forms on the lithium surface, which prevents dendrite growth.
- Weiyang Li
- , Hongbin Yao
- & Yi Cui
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Article
| Open AccessSynthesis of three-dimensionally interconnected sulfur-rich polymers for cathode materials of high-rate lithium–sulfur batteries
There is intensive research underway into the cathode development of lithium–sulphur batteries. Here, the authors present a battery with organosulfur-containing polymers as the cathode active materials which displays promising electrochemical performance.
- Hoon Kim
- , Joungphil Lee
- & Moon Jeong Park
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Article
| Open AccessPhase and composition controllable synthesis of cobalt manganese spinel nanoparticles towards efficient oxygen electrocatalysis
It is challenging to synthesize cobalt manganese spinels with controlled phase and composition. Here the authors present a solution-based synthesis method for the spinels, which show potential in catalysing oxygen reduction reactions.
- Chun Li
- , Xiaopeng Han
- & Jun Chen
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Article
| Open AccessSelf-assembled three-dimensional and compressible interdigitated thin-film supercapacitors and batteries
It is challenging to construct three-dimensional thin-film energy-storage devices. Here the authors present supercapacitors and batteries based on layer-by-layer self-assembly of interdigitated thin films inside aerogels, demonstrating energy storage as well as compressibility in three-dimensional devices.
- Gustav Nyström
- , Andrew Marais
- & Mahiar M. Hamedi
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Article
| Open AccessIn-operando high-speed tomography of lithium-ion batteries during thermal runaway
It is important to understand the mechanisms of thermally induced battery degradation and any safety hazards. Here, the authors use high-speed synchrotron radiation X-ray computed tomography to shed light on the structural and thermal dynamics associated with thermal runaway and failure of commercial Li-ion batteries.
- Donal P. Finegan
- , Mario Scheel
- & Paul R. Shearing
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Article
| Open AccessRadiolysis as a solution for accelerated ageing studies of electrolytes in Lithium-ion batteries
The degradation of organic solvents used in lithium-ion batteries reduces battery performance. Here, the authors present a radiolysis technique which is not only more efficient than conventional thermally activated ageing methods, but also allows mechanistic analysis of the degradation process.
- Daniel Ortiz
- , Vincent Steinmetz
- & Sophie Le Caër
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Article
| Open AccessP2-Na0.6[Cr0.6Ti0.4]O2 cation-disordered electrode for high-rate symmetric rechargeable sodium-ion batteries
Sodium-containing layered oxides are promising battery cathodes, but their performance suffers from the formation of sodium ion-vacancy ordered superstructures. Here, the authors present a P2-Na0.6[Cr0.6Ti0.4]O2layered oxide with disordered cations, leading to high battery performance.
- Yuesheng Wang
- , Ruijuan Xiao
- & Liquan Chen
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Na+ intercalation pseudocapacitance in graphene-coupled titanium oxide enabling ultra-fast sodium storage and long-term cycling
There are intensive efforts in developing anode materials for sodium-ion batteries. Here, the authors present a graphene-titanium dioxide composite as an anode material and show that sodium ion intercalation pseudocapacitance charge storage leads to excellent electrochemical properties.
- Chaoji Chen
- , Yanwei Wen
- & Yunhui Huang
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Article
| Open AccessVisualization of electrochemically driven solid-state phase transformations using operando hard X-ray spectro-imaging
Hard X-ray spectro-imaging using synchrotron radiation can be used to monitor electrochemical reactions. Here, the authors present X-ray absorption data and resolve phase evolution for the conversion of iron fluoride, a high-capacity Li-ion battery conversion cathode, with nanoscale resolution.
- Linsen Li
- , Yu-chen Karen Chen-Wiegart
- & Song Jin
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Radially aligned hierarchical columnar structure as a cathode material for high energy density sodium-ion batteries
There are intensive efforts in developing cathode materials for sodium-ion batteries. Here, the authors present a spherical particle with a radially aligned hierarchical columnar structure as a cathode material which leads to good performance of capacity, retention, rate capability and thermal stability.
- Jang-Yeon Hwang
- , Seung-Min Oh
- & Yang-Kook Sun
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Article
| Open AccessTernary metal fluorides as high-energy cathodes with low cycling hysteresis
Transition metal fluorides have high theoretical specific capacities as cathodes for lithium ion batteries, but low working potentials and poor energy efficiency limit their practical applications. Here, the authors report a group of ternary metal fluorides, which may overcome these problems.
- Feng Wang
- , Sung-Wook Kim
- & Jason Graetz