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Article
| Open AccessHigh dielectric barium titanate porous scaffold for efficient Li metal cycling in anode-free cells
The development of anode-free batteries requires current collectors able to deposit and remove Li metal upon cycling efficiently. Here, the authors report the use of high dielectric porous BaTiO3 to avoid the formation of inhomogeneous Li metal depositions during anode-free cell cycling.
- Chao Wang
- , Ming Liu
- & Marnix Wagemaker
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Article
| Open AccessStructural ceramic batteries using an earth-abundant inorganic waterglass binder
Structural batteries hold particular promise for decarbonizing the aviation industry. Here, the authors demonstrate that waterglass, an earth-abundant water-soluble silicate adhesive, can be used as a binder in structural batteries allowing them to both bear load and store electricity at the same time.
- Alan Ransil
- & Angela M. Belcher
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Article
| Open AccessEvolving contact mechanics and microstructure formation dynamics of the lithium metal-Li7La3Zr2O12 interface
All-solid-state batteries are promising alternatives to Li-ion batteries. Here, the authors investigate the chemo-mechanical changes at the lithium metal/solid electrolyte interface via operando acoustic transmission and magnetic resonance imaging.
- Wesley Chang
- , Richard May
- & Daniel Steingart
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Article
| Open AccessA Fe3N/carbon composite electrocatalyst for effective polysulfides regulation in room-temperature Na-S batteries
Room-temperature sodium-sulfur batteries are promising electrochemical energy storage systems. Here, the authors proposed a Fe3N/carbon composite to regulate the polysulfides chemistry and improve the performances of sodium-sulfur cells.
- Yuruo Qi
- , Qing-Jie Li
- & Maowen Xu
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Comment
| Open AccessThe importance of electrode interfaces and interphases for rechargeable metal batteries
Metal electrode interfaces and interphases are critical for the development of future high-energy metal batteries. Here, Dr Jelena Popovic-Neuber discusses the state of the art, issues and strategies to improve the stability of metal electrodes toward practical battery systems.
- Jelena Popovic
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Article
| Open AccessDeep learning-based segmentation of lithium-ion battery microstructures enhanced by artificially generated electrodes
Accurate 3D representations of lithium-ion battery electrodes can help in understanding and ultimately improving battery performance. Here, the authors report a methodology for using deep-learning tools to reliably distinguish the different electrode material phases where standard approaches fail.
- Simon Müller
- , Christina Sauter
- & Vanessa Wood
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Article
| Open AccessRational design of mechanically robust Ni-rich cathode materials via concentration gradient strategy
Mechanical integrity issues are one of the main causes of limited long-term cycle stability for Ni-rich cathode materials. Here the authors analyse the roles of cobalt and manganese and utilise a concentration gradient design to mitigate these issues.
- Tongchao Liu
- , Lei Yu
- & Khalil Amine
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Article
| Open AccessOn the crystallography and reversibility of lithium electrodeposits at ultrahigh capacity
Lithium metal batteries offer high-capacity electrical energy storage but suffer from poor reversibility of the metal anode. Here, the authors report that at very high capacities, lithium deposits as dense structures with a preferred crystallite orientation, yielding highly reversible lithium anodes.
- Qing Zhao
- , Yue Deng
- & Lynden A. Archer
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Article
| Open AccessQuantification of the Li-ion diffusion over an interface coating in all-solid-state batteries via NMR measurements
Development of all-solid-state batteries requires stable solid electrolyte-electrode interfaces. Here, via exchange-NMR measurements, the authors investigate the positive electrode-solid electrolyte interface, revealing the impact of an inorganic coating on the Li-ion transport properties.
- Ming Liu
- , Chao Wang
- & Marnix Wagemaker
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Article
| Open AccessUrban mining by flash Joule heating
Precious metals recovery from electronics wastes, termed urban mining, is significant for a circular economy. Here, the authors reported a solvent-free and ultrafast process based on flash Joule heating to recover precious metals and remove toxic heavy metals in electronic wastes.
- Bing Deng
- , Duy Xuan Luong
- & James M. Tour
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Article
| Open AccessAchieving stable Na metal cycling via polydopamine/multilayer graphene coating of a polypropylene separator
The development of future Na metal batteries relies on the cycling stability of the metallic anode. Here, the authors propose a polypropylene separator functionalized with polydopamine and multilayer graphene to enable stable and prolonged Na metal cell cycling.
- Jieqiong Qin
- , Haodong Shi
- & Zhong-Shuai Wu
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Article
| Open AccessSynthetic accessibility and stability rules of NASICONs
Sodium super ionic conductors are a class of promising energy storage materials owing to their high ionic conductivity. Here, the authors conducted high throughput calculations to understand the synthetic accessibility of NASICON-type materials and demonstrate an efficient paradigm for discovering new complex materials.
- Bin Ouyang
- , Jingyang Wang
- & Gerbrand Ceder
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Article
| Open AccessA synergistic exploitation to produce high-voltage quasi-solid-state lithium metal batteries
The energy content increase is of paramount importance for the development of future Li-based batteries. Here, the authors propose a gel polymer electrolyte in combination with a positive electrode comprising of a Li-rich oxide active material and graphite to produce a high-energy Li metal cell.
- Junru Wu
- , Xianshu Wang
- & Guoxiu Wang
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Article
| Open AccessReversible electrochemical oxidation of sulfur in ionic liquid for high-voltage Al−S batteries
The sulfur cathode in metal-sulfur batteries normally undergoes electrochemical reduction to form metal sulfides. Here, the authors demonstrate the electrochemical oxidation of sulfur in ionic liquid for high-voltage aluminium-sulfur batteries.
- Huan Li
- , Rongwei Meng
- & Shi-Zhang Qiao
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Article
| Open AccessAn electron-deficient carbon current collector for anode-free Li-metal batteries
The development of anode-free batteries requires fundamental investigations at the current collector/electrolyte interface. Here, the authors report an atomically defective carbon current collector to improve the electrochemical behaviour of an anode-free Li-based cell.
- Hyeokjin Kwon
- , Ju-Hyuk Lee
- & Hee-Tak Kim
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Article
| Open AccessActivation of anionic redox in d0 transition metal chalcogenides by anion doping
Activation of anionic redox in battery materials promises great benefits for battery materials, but remains an elusive phenomenon. Here, the authors present anion-doping as a novel strategy to unlock electrochemical activity in the cobalt/nickel free cathode material, Li2TiS3-xSex.
- Bernhard T. Leube
- , Clara Robert
- & Jean-Marie Tarascon
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Review Article
| Open AccessProduction of high-energy Li-ion batteries comprising silicon-containing anodes and insertion-type cathodes
Large-scale manufacturing of high-energy Li-ion cells is of paramount importance for developing efficient rechargeable battery systems. Here, the authors report in-depth discussions and evaluations on the use of silicon-containing anodes together with insertion-based cathodes.
- Gebrekidan Gebresilassie Eshetu
- , Heng Zhang
- & Egbert Figgemeier
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Article
| Open AccessA saccharide-based binder for efficient polysulfide regulations in Li-S batteries
The long-term cycling of Li-S batteries depends on the polysulfides shuttling regulation. Here, the authors present a saccharide-based binder system to control the polysulfides migration and improve the cycle life of a Li-S pouch cell.
- Yingyi Huang
- , Mahdokht Shaibani
- & Mainak Majumder
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Article
| Open AccessReaction inhomogeneity coupling with metal rearrangement triggers electrochemical degradation in lithium-rich layered cathode
Electrochemical degradation is the most critical challenge for Li-rich materials. Here, the authors reveal that manganese related phase reaction inhomogeneity coupling with transition metal rearrangement triggers electrochemical degradation in lithium-rich layered cathode.
- Liguang Wang
- , Tongchao Liu
- & Jun Lu
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Article
| Open AccessIn situ inorganic conductive network formation in high-voltage single-crystal Ni-rich cathodes
Single-crystal Ni-rich cathodes suffer from side reactions with the electrolyte and slow Li-ion transport during high-voltage cycling. Herein, a Li1.4Y0.4Ti1.6(PO4)3 coating is applied to facilitate the Li-ion transport and improve the cycling life of the cell.
- Xinming Fan
- , Xing Ou
- & Yong Yang
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Article
| Open AccessBoron-doped sodium layered oxide for reversible oxygen redox reaction in Na-ion battery cathodes
The irreversible oxygen redox reaction during charging to the high-voltage region causes cathode structural degradation and Na-ion cell capacity fading. Here, the authors report a B-doped cathode active material to mitigate the irreversible oxygen oxidation and increase the cell capacity.
- Yu-Jie Guo
- , Peng-Fei Wang
- & Yu-Guo Guo
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Article
| Open AccessLi-ion storage properties of two-dimensional titanium-carbide synthesized via fast one-pot method in air atmosphere
A facile and cost-effective synthesis of MXenes is not yet available. Here, the authors propose a one-pot molten salt-based method of MXenes synthesis from elemental precursors in an air atmosphere. Li-ion storage properties of the MXenes are also reported and discussed.
- Guoliang Ma
- , Hui Shao
- & Zifeng Lin
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Article
| Open AccessEngineering Na+-layer spacings to stabilize Mn-based layered cathodes for sodium-ion batteries
Suppressing phase transitions is crucial for the layered lithium/sodium transition metal oxide cathodes in batteries. Here, the authors report a water-mediated strategy to mitigate the phase transitions and boost electrochemical performances of manganese-based layered cathodes for cost-effective Na-ion batteries.
- Wenhua Zuo
- , Xiangsi Liu
- & Yong Yang
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Article
| Open AccessLong-life lithium-sulfur batteries with high areal capacity based on coaxial CNTs@TiN-TiO2 sponge
It is challenging to optimize catalytic heterostructures for lithium sulfur (Li-S) batteries. Here, authors prepare nanometer-scale TiN-TiO2 heterostructures via atomic layer deposition on carbon nanotube sponge to realize stable Li-S batteries with high areal capacity and improved rate capability.
- Hui Zhang
- , Luis K. Ono
- & Yabing Qi
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Article
| Open AccessMixed alkali-ion transport and storage in atomic-disordered honeycomb layered NaKNi2TeO6
Honeycomb layered oxides are an emerging class of materials with peculiar physicochemical properties. Here, the authors report the synthesis and electrochemical energy storage characterisations of a mixed-alkali honeycomb layered oxide material capable of storing Na and K ions simultaneously.
- Titus Masese
- , Yoshinobu Miyazaki
- & Tomohiro Saito
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Article
| Open AccessAtomic-scale unveiling of multiphase evolution during hydrated Zn-ion insertion in vanadium oxide
The detailed understanding of the structural variations during cycling in cathodes for Zn-ion aqueous rechargeable batteries is still limited. Here, the authors utilize atomic-column-resolved scanning transmission electron microscopy to elucidate multiphase evolution during hydrated Zn-Ion insertion in vanadium oxide.
- Pilgyu Byeon
- , Youngjae Hong
- & Sung-Yoon Chung
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Article
| Open AccessSurface enrichment and diffusion enabling gradient-doping and coating of Ni-rich cathode toward Li-ion batteries
The commercialisation of promising Ni-rich cathodes is limited by capacity fading and thermal runaway. Here, the authors design a gradient Al-doped and LiAlO2-coated LiNi0.9Co0.1O2 cathode, which addresses the crystal degradation and interfacial instability and thus improves the cycle and thermal stabilities.
- Haifeng Yu
- , Yueqiang Cao
- & Hao Jiang
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Article
| Open AccessA cost-effective and humidity-tolerant chloride solid electrolyte for lithium batteries
Stable inorganic solid electrolytes are instrumental in developing high-voltage Li metal batteries. Here, the authors present the synthesis and electrochemical energy storage properties of a cost-effective and humidity-tolerant chloride solid electrolyte.
- Kai Wang
- , Qingyong Ren
- & Cheng Ma
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Article
| Open AccessA high capacity small molecule quinone cathode for rechargeable aqueous zinc-organic batteries
The flexible structural design of organic materials make them promising candidates for cathode in rechargeable batteries. Here, the authors report a tetraamino-p-benzoquinone cathode which realizes facile proton conduction by the Grotthuss-type mechanism and shows excellent electrochemical performance.
- Zirui Lin
- , Hua-Yu Shi
- & Xiaoqi Sun
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Article
| Open AccessIn situ observation of thermal-driven degradation and safety concerns of lithiated graphite anode
The role of the lithiated graphite anode in battery thermal runaway failure remains under intense investigation. In this work, with multiple in situ synchrotron X-ray characterizations, the phase evolution, gas release, and lithium leaching of lithiated graphite anode are illustrated in detail.
- Xiang Liu
- , Liang Yin
- & Khalil Amine
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Article
| Open AccessAtomic-scale regulation of anionic and cationic migration in alkali metal batteries
An optimized transport of anions and cations is essential for the development of practical alkali metal batteries. Here, the authors report the use of Ti0.87O2 nanosheets as coating material of polypropylene separators for Li-S, Li-Se and Na-Se cells.
- Pan Xiong
- , Fan Zhang
- & Guoxiu Wang
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Article
| Open AccessCharacterising lithium-ion electrolytes via operando Raman microspectroscopy
The full characterisation of lithium-ion electrolytes is of paramount importance for the continued development and innovation of lithium ion and lithium metal batteries. Here, the authors present a new experimental setup to obtain all key electrolyte parameters using operando Raman microspectroscopy
- Jack Fawdon
- , Johannes Ihli
- & Mauro Pasta
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Article
| Open AccessEvolution and expansion of Li concentration gradient during charge–discharge cycling
Quantification of Li ions in local area is key to understand the degradation of Li ion batteries. Here the authors report Li compositional gradient evolution in the cathode after charge-discharge cycles using a complementary study via atom probe tomography and scanning transmission electron microscopy.
- Byeong-Gyu Chae
- , Seong Yong Park
- & Woo Sung Jeon
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Comment
| Open AccessCorrelating advanced microscopies reveals atomic-scale mechanisms limiting lithium-ion battery lifetime
The longevity of a lithium-ion battery is limited by cathode degradation. Combining atom probe tomography and scanning transmission electron microscopy reveals that the degradation results from atomic-scale irreversible structural changes once lithium leaves the cathode during charging, thereby inhibiting lithium intercalation back into the cathode as the battery discharges. This information unveils possible routes for improving the lifetime of lithium-ion batteries.
- Baptiste Gault
- & Jonathan D. Poplawsky
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Article
| Open AccessLayered double hydroxide membrane with high hydroxide conductivity and ion selectivity for energy storage device
Membranes with fast and selective ion transport are highly relevant for energy storage devices. Here, the authors report a layered double hydroxide membrane with high ionic selectivity and hydroxide ion conductivity for flow battery applications, and reveal the ions transport mechanism of the membrane.
- Jing Hu
- , Xiaomin Tang
- & Xianfeng Li
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Article
| Open AccessSub-nanometer confinement enables facile condensation of gas electrolyte for low-temperature batteries
Liquefied gas electrolytes (LGE) can enable the operation of electrochemical devices in cold conditions but their high vapour pressure poses safety concerns. Here, the authors show that the nano-confinement effect of metal-organic framework allows battery with LGE to work at low temperature and reduced pressure.
- Guorui Cai
- , Yijie Yin
- & Zheng Chen
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Article
| Open AccessA new high-voltage calcium intercalation host for ultra-stable and high-power calcium rechargeable batteries
Rechargeable calcium batteries are promising multivalent battery systems but the lack of suitable electrodes hampers their development. Here the authors report a cathode derived from polyanion framework that demonstrates uncommonly stable and fast intercalation behaviours of calcium ions.
- Zheng-Long Xu
- , Jooha Park
- & Kisuk Kang
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Article
| Open AccessArtificial dual solid-electrolyte interfaces based on in situ organothiol transformation in lithium sulfur battery
Lithium-sulfur batteries suffer from the shuttle effect of lithium polysulfides and interfacial instability of the lithium metal anode. Here, the authors use 1,3,5-benzenetrithiol as an electrolyte additive to protect sulfur cathode and lithium metal anode.
- Wei Guo
- , Wanying Zhang
- & Arumugam Manthiram
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Article
| Open AccessElectrosynthesis of 1,4-bis(diphenylphosphanyl) tetrasulfide via sulfur radical addition as cathode material for rechargeable lithium battery
Organic electrodes are promising energy storage materials owing to their chemical diversity and electrochemical specificity. Here, the authors report synthesis of phosphorous containing organopolysulfide 1,4-bis(diphenylphosphanyl)tetrasulfide material showing excellent performance in a rechargeable Li battery.
- Dan-Yang Wang
- , Yubing Si
- & Yongzhu Fu
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Article
| Open AccessManipulating anion intercalation enables a high-voltage aqueous dual ion battery
The interactions between water molecules, electrode materials and anions are essential yet challenging for aqueous dual ion batteries. Here, the authors demonstrate the voltage manipulation of dual ion batteries through matching intercalation energy and solvation energy of different anions.
- Zhaodong Huang
- , Yue Hou
- & Chunyi Zhi
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Article
| Open AccessAmorphization-induced surface electronic states modulation of cobaltous oxide nanosheets for lithium-sulfur batteries
Regulating the adsorption behaviour of the polysulfide species is the key to achieving highly stable Li-S batteries. Here, the authors show that amorphization-induced redistribution of d orbitals enable CoO to be a favourable candidate for polysulfide adsorption and conversion.
- Ruilong Li
- , Dewei Rao
- & Xun Hong
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Article
| Open AccessTwin boundary defect engineering improves lithium-ion diffusion for fast-charging spinel cathode materials
Defect modulation and understanding its impact on electrode materials remain challenging. Here, authors introduce twin boundaries into spinel cathode and demonstrate that their presence enables fast lithium ion diffusion.
- Rui Wang
- , Xin Chen
- & Yinguo Xiao
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Article
| Open AccessRealizing high-power and high-capacity zinc/sodium metal anodes through interfacial chemistry regulation
Zinc metal anodes suffer from severe dendrites’ growth. Herewith authors construct electrically conductive and zincophilic tin coating on separator to suppress dendrites initiation and eliminate the inevitably formed dendrites.
- Zhen Hou
- , Yao Gao
- & Biao Zhang
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Article
| Open AccessSub-micro droplet reactors for green synthesis of Li3VO4 anode materials in lithium ion batteries
The conventional solid-state reaction suffers from the low diffusivity, high energy consumption, and uncontrolled morphology. Here, the authors report a low-temperature solid-state reaction under water vapour for synthesis of various electrodes for lithium ions batteries.
- Ha Tran Huu
- , Ngoc Hung Vu
- & Won Bin Im
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Article
| Open AccessReversible formation of coordination bonds in Sn-based metal-organic frameworks for high-performance lithium storage
Tin-based alloying materials have been widely developed for lithium storage, but are limited by large volume variation. Herein, the authors created a new strategy of applying coordination chemistry to construct tin-based metal-organic frameworks which exhibited high-performance lithium storage property.
- Jingwei Liu
- , Daixi Xie
- & Peng Cheng
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Article
| Open AccessProbing the Na metal solid electrolyte interphase via cryo-transmission electron microscopy
The solid electrolyte interphase (SEI) strongly affects the cycling behaviour of rechargeable alkali metal cells. Here, the authors investigate via cryo-electron microscopy the SEI formed on a Na metal electrode using fluoroethylene carbonate-containing electrolyte.
- Bing Han
- , Yucheng Zou
- & Meng Gu
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Article
| Open AccessAddressing voltage decay in Li-rich cathodes by broadening the gap between metallic and anionic bands
Voltage fade is a critical issue for Li-rich transition metal oxide cathode. Here, the authors modulate the oxygen anionic redox chemistry and enlarges the gap between metallic and anionic states by constructing Li2ZrO3 slabs into Li2MnO3 domain in Li1.21Ni0.28Mn0.51O2 which fundamentally suppresses the voltage decay.
- Jicheng Zhang
- , Qinghua Zhang
- & Xiangfeng Liu
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Article
| Open AccessCovalency does not suppress O2 formation in 4d and 5d Li-rich O-redox cathodes
In this work, authors show that O-redox in 4d and 5d transition metal oxides involves the formation of molecular oxygen trapped in the particles. These results are in accord with observations in 3d oxides and show that the greater covalency of the 4d and 5d oxides does not stabilise peroxo-like species.
- Robert A. House
- , John-Joseph Marie
- & Peter G. Bruce
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Article
| Open AccessInorganic-organic competitive coating strategy derived uniform hollow gradient-structured ferroferric oxide-carbon nanospheres for ultra-fast and long-term lithium-ion battery
The gradient-structure is ideal nanostructure for conversion-type anodes with drastic volume change. Here, the authors demonstrate an inorganic-organic competitive coating strategy to construct gradient-structured Fe3O4@C nanospheres.
- Yuan Xia
- , Tiancong Zhao
- & Dongyuan Zhao