Featured
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| Open AccessInterfacial friction enabling ≤ 20 μm thin free-standing lithium strips for lithium metal batteries
Thin, freestanding Li metal foils are key to improving the energy density of Li batteries but are difficult to manufacture. Here, authors achieve thin Li foils by mechanical rolling, exploiting tribochemistry to form a protective surface film that improves mechanical and electrochemical properties.
- Shaozhen Huang
- , Zhibin Wu
- & Libao Chen
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Article
| Open AccessA twelve-electron conversion iodine cathode enabled by interhalogen chemistry in aqueous solution
Enhancing energy density of batteries is a crucial focus within the field of energy storage. Here, the authors introduce a twelve-electron conversion iodine cathode (iodide/iodate) for high energy density zinc-iodine batteries, achieved through interhalogen chemistry in an acidic aqueous electrolyte.
- Wenjiao Ma
- , Tingting Liu
- & Xiao Liang
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Article
| Open AccessDiscovery of a three-proton insertion mechanism in α-molybdenum trioxide leading to enhanced charge storage capacity
The proton insertion mechanism in α-molybdenum trioxide remains incompletely elucidated. Herein, the authors uncover a three-proton intercalation mechanism within α-molybdenum trioxide using a specially designed electrolyte, which endows α-molybdenum trioxide with an improved specific discharge capacity.
- Yongjiu Lei
- , Wenli Zhao
- & Husam N. Alshareef
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Article
| Open AccessRegulating interfacial reaction through electrolyte chemistry enables gradient interphase for low-temperature zinc metal batteries
Zinc batteries have received intense attentions but suffer from inferior low-temperature performance. Here, the authors constructed a gradient phosphatized interphase in situ on zinc surface to accelerate zinc-ion desolvation and transport, greatly enhancing the cycling performance at subzero temperatures.
- Wei Wang
- , Shan Chen
- & Huan Wang
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Article
| Open AccessIntegration of microbattery with thin-film electronics for constructing an integrated transparent microsystem based on InGaZnO
In this work, authors demonstrate the full integration of miniaturized InGaZnO-based transparent energy device (lithium-ion battery), electronic device (thin-film transistor) and sensing device (photodetector) to form a monolithic integrated transparent microsystem with synergistic functions.
- Bin Jia
- , Chao Zhang
- & Xiaodong Huang
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Article
| Open AccessOperando monitoring of thermal runaway in commercial lithium-ion cells via advanced lab-on-fiber technologies
Operando monitoring of thermal runaway in Li-ion batteries is critical. Here, authors develop an optical fiber sensor capable of insertion into 18650 batteries to monitor internal temperature and pressure during thermal runaway, facilitating battery safety assessment and early warning capability.
- Wenxin Mei
- , Zhi Liu
- & Tuan Guo
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Article
| Open AccessTuning electron delocalization of hydrogen-bonded organic framework cathode for high-performance zinc-organic batteries
The practical use of zinc-organic batteries has been hindered by their low energy density and rapid capacity decay. Here, the authors introduce a super electron-delocalized hydrogen-bonded organic framework by tuning electron delocalization as a cathode material for high-performance zinc-organic batteries.
- Wenda Li
- , Hengyue Xu
- & Shaohua Liu
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Article
| Open AccessDesign principles for NASICON super-ionic conductors
Na Super Ionic Conductor (NASICON) materials are an important class of solid-state electrolytes. Here, authors combine calculations, experimental synthesis and testing, and text-mined historical data on NASICON ionic conductivity to understand how composition influences the Na-ion conductivity.
- Jingyang Wang
- , Tanjin He
- & Gerbrand Ceder
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Article
| Open AccessIdentifying and preventing degradation in flavin mononucleotide-based redox flow batteries via NMR and EPR spectroscopy
Aqueous organic redox-flow batteries are known to suffer capacity loss via degradation of the redox-active species. Here, the authors use in situ methods to study the electrolyte flavin mononucleotide, identifying a redox mediator mechanism that mitigates capacity loss and a route to prevent its degradation.
- Dominic Hey
- , Rajesh B. Jethwa
- & Clare P. Grey
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Article
| Open AccessMultiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling
Improved understanding of the spatial dynamics in graphite electrodes is needed to improve fast-charging protocols for Li-ion batteries. Here, authors highlight that lithiation heterogeneity leads to early lithium plating onset and find distinct relaxation behaviors at various states of charge.
- Xuekun Lu
- , Marco Lagnoni
- & Paul R. Shearing
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Article
| Open AccessAn aqueous electrolyte densified by perovskite SrTiO3 enabling high-voltage zinc-ion batteries
Conventional electrolytes of aqueous zinc-ion batteries suffer from serious side reactions. Here, the authors develop a densified electrolyte with perovskite additives to achieve reversible zinc plating/stripping with robust interface and improved performance of full cells at an extended voltage range.
- Rongyu Deng
- , Zhenjiang He
- & Feixiang Wu
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Perspective
| Open AccessA reflection on polymer electrolytes for solid-state lithium metal batteries
Polymer electrolytes are attractive candidates for rechargeable lithium metal batteries. Here, the authors give a personal reflection on the structural design of coupled and decoupled polymer electrolytes and possible routes to further enhance their performance in rechargeable batteries.
- Ziyu Song
- , Fangfang Chen
- & Heng Zhang
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Article
| Open AccessDevelopment of high-voltage and high-energy membrane-free nonaqueous lithium-based organic redox flow batteries
Redox flow batteries are promising energy storage systems but are limited in part due to high cost and low availability of membrane separators. Here, authors develop a membrane-free, nonaqueous 3.5 V all-organic lithium-based battery and demonstrate its operation in both static and flow conditions.
- Rajeev K. Gautam
- , Xiao Wang
- & Jianbing “Jimmy” Jiang
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Article
| Open AccessReaction-passivation mechanism driven materials separation for recycling of spent lithium-ion batteries
Separating active cathode materials from current collectors poses a critical challenge in battery recycling. Here, the authors develop a facile strategy that relies on a reaction-passivation mechanism to effectively separate the aluminum foil and cathode active material in spent lithium-ion batteries.
- Zihe Chen
- , Ruikang Feng
- & Yongming Sun
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Article
| Open AccessNon-flammable solvent-free liquid polymer electrolyte for lithium metal batteries
Although solid polymer electrolytes show promise as alternatives to organic liquid electrolytes, they are hampered by interface and ionic conduction issues. Here, the authors develop a solvent-free liquid polymer electrolyte to enhance the safety and electrochemical performance of lithium metal batteries.
- Guo-Rui Zhu
- , Qin Zhang
- & Yu-Zhong Wang
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Article
| Open AccessTemperature-dependent interphase formation and Li+ transport in lithium metal batteries
High-performance lithium metal batteries operating below −20 °C are desired but hindered by slow reaction kinetics. Here, the authors uncover the temperature-dependent Li+ behavior and interphase formation in liquid electrolytes and provide directions to enhance the low temperature performance.
- Suting Weng
- , Xiao Zhang
- & Xuefeng Wang
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Article
| Open AccessA recyclable biomass electrolyte towards green zinc-ion batteries
Functional hydrogel electrolytes show promising potential for enhancing the sustainability of aqueous zinc-ion batteries. Here, the authors introduce a biomass-based hydrogel electrolyte that not only prevents side reactions on the zinc anode but also enables easy retrieval from the zinc batteries.
- Hongyu Lu
- , Jisong Hu
- & Bingang Xu
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Article
| Open AccessAluminum foil negative electrodes with multiphase microstructure for all-solid-state Li-ion batteries
Aluminum-based negative electrodes could enable high-energy-density batteries, but their charge storage performance is limited. Here, the authors show that dense aluminum electrodes with controlled microstructure exhibit long-term cycling stability in all-solid-state lithium-ion batteries.
- Yuhgene Liu
- , Congcheng Wang
- & Matthew T. McDowell
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Article
| Open Access3D hierarchical graphene matrices enable stable Zn anodes for aqueous Zn batteries
Uncontrolled dendrite growth and severe side reactions at high capacities and rates impede its practical application for zinc metal anodes. Here, the authors propose a composite zinc anode with 3D hierarchical graphene matrix as a multifunctional host to regulate zinc deposition for aqueous zinc batteries.
- Yongbiao Mu
- , Zheng Li
- & Lin Zeng
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Article
| Open AccessProduction of gas-releasing electrolyte-replenishing Ah-scale zinc metal pouch cells with aqueous gel electrolyte
The production of large-format aqueous Zn batteries is hindered by electrolyte consumption, hydrogen gas evolution and Zn dendrites growth during cycling. Here, the authors propose a specific pouch cell design capable of releasing hydrogen gas and refilling the electrolyte components.
- Feifei Wang
- , Jipeng Zhang
- & Quan-Hong Yang
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Article
| Open AccessSlab gliding, a hidden factor that induces irreversibility and redox asymmetry of lithium-rich layered oxide cathodes
Lithium-rich layered oxides, promising high-energy-density cathode materials, face electrochemical degradation due to structural disordering. Here, the authors report that slab gliding is a key trigger of this disordering and a pivotal unexplored avenue for a reversible anionic redox reaction.
- Jun-Hyuk Song
- , Seungju Yu
- & Kisuk Kang
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Article
| Open AccessRealizing long-cycling all-solid-state Li-In||TiS2 batteries using Li6+xMxAs1-xS5I (M=Si, Sn) sulfide solid electrolytes
Stable inorganic solid-state electrolytes are crucial for reliable all-solid-state battery development. Here, the authors report a Li-In|Li6.8Si0.8As0.2S5I|Ti2S lab-scale cell with a long cycle life of almost 62500 cycles at 2.44 mA cm−2, 30 °C and 30 MPa.
- Pushun Lu
- , Yu Xia
- & Fan Wu
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Article
| Open AccessWeakly coordinated Li ion in single-ion-conductor-based composite enabling low electrolyte content Li-metal batteries
The reactivity between lithium and a liquid electrolyte leads to degradation of a lithium metal battery, resulting in the depletion of the liquid electrolyte. Here, authors develop a composite layer that can mitigate the reactivity and consequently enable long-cycling lithium metal batteries.
- Hyeokjin Kwon
- , Hyun-Ji Choi
- & Hee-Tak Kim
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Article
| Open AccessDynamic gel as artificial interphase layer for ultrahigh-rate and large-capacity lithium metal anode
Achieving stable lithium metal anodes under large current densities over 10 mA cm−2 and area capacities over 10 mAh cm−2 remains a critical challenge. Here, authors propose a dynamic gel as protect layer for lithium metal anode to facilitate with the Young’s modulus, flexibility and ionic conductivity, thus to stabilize the lithium metal anode.
- Chao Chen
- , Jiaming Zhang
- & Xunhui Xiong
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Article
| Open AccessA solution-to-solid conversion chemistry enables ultrafast-charging and long-lived molten salt aluminium batteries
Conventional solid-to-solid conversion cathodes in rechargeable aluminium batteries suffer from sluggish reaction kinetics and cumulative structural degradation. Here the authors disclose a solution-to-solid conversion chemistry using molten salt electrolytes to achieve fast-charging capability and good cycling stability.
- Jiashen Meng
- , Xuhui Yao
- & Quanquan Pang
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Article
| Open AccessLean-water hydrogel electrolyte for zinc ion batteries
Excess water in hydrogel-based zinc ion batteries causes side reactions, but reduced water content results in low conductivities. Here, authors develop a lean-water hydrogel based on molecular lubrication mechanism for fast ion transportation, extended stability, and reversible Zinc plating/stripping.
- Yanbo Wang
- , Qing Li
- & Chunyi Zhi
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Article
| Open AccessFundamental investigations on the ionic transport and thermodynamic properties of non-aqueous potassium-ion electrolytes
K-ion batteries may have rate advantages over Li-ion batteries due to the larger size of the cation. Here, the authors characterize the ionic transport and thermodynamic properties of non-aqueous K-ion electrolyte solutions demonstrating higher K-ion mobility than the Li-ion counterpart.
- Shobhan Dhir
- , Ben Jagger
- & Mauro Pasta
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Article
| Open AccessA cost-effective, ionically conductive and compressible oxychloride solid-state electrolyte for stable all-solid-state lithium-based batteries
Ionic conductivity > 1 mS cm−1 at 25 °C, compressibility enabling > 90% density at 250 − 350 MPa, and cost < $50/kg are desirable for inorganic solid-state electrolytes. Here, the authors report Li1.75ZrCl4.75O0.5 as a solid-state electrolyte capable of satisfying these requirements simultaneously.
- Lv Hu
- , Jinzhu Wang
- & Cheng Ma
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Article
| Open AccessA family of oxychloride amorphous solid electrolytes for long-cycling all-solid-state lithium batteries
Developing amorphous solid electrolytes for solid state lithium batteries is challenging due to limited understanding of disordered structures. Here, the authors report a family of oxychloride amorphous solid electrolytes with high ionic conductivities and promising electrochemical characteristics.
- Shumin Zhang
- , Feipeng Zhao
- & Xueliang Sun
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Article
| Open AccessBridging multiscale interfaces for developing ionically conductive high-voltage iron sulfate-containing sodium-based battery positive electrodes
Sluggish kinetics is a major challenge for iron-based sulfate electrode materials. Here, the authors report multiscale interface engineering to build continuous Na-ion transfer channels at all length scales by designing ionic conductors inside bulk and low-electron-density exposed crystal surfaces.
- Jiyu Zhang
- , Yongliang Yan
- & Weihua Chen
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Article
| Open AccessProduction of high-energy 6-Ah-level Li | |LiNi0.83Co0.11Mn0.06O2 multi-layer pouch cells via negative electrode protective layer coating strategy
Stable lithium metal electrodes are needed to produce high-energy batteries. Here, authors reported poly(2-hydroxyethyl acrylate-co-sodium benzenesulfonate) as a lithium metal protective layer and the production of a 490 Wh/kg class Li | |LiNi0.83Co0.11Mn0.06O2 pouch cell.
- Yangyang Feng
- , Yong Li
- & Yaobing Wang
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Article
| Open AccessUnderstanding capacity fade in organic redox-flow batteries by combining spectroscopy with statistical inference techniques
Organic redox-flow batteries have the potential to cheaply store renewable electricity at grid scale but require further development. Here, the authors show that combining spectroscopic measurements with statistical inference techniques can shed light on why these batteries lose capacity over time.
- Sanat Vibhas Modak
- , Wanggang Shen
- & David G. Kwabi
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Article
| Open AccessEnabling long-cycling aqueous sodium-ion batteries via Mn dissolution inhibition using sodium ferrocyanide electrolyte additive
Mn-based Prussian blue is an ideal positive electrode material for aqueous sodium-ion batteries but still suffers from Mn dissolution. Here, the authors introduce an Mn-ion trapping agent as an electrolyte additive to produce a 94 Wh kg−1 Na-ion aqueous battery with a long lifespan.
- Zhaoheng Liang
- , Fei Tian
- & Chengxin Wang
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Article
| Open AccessResolving nanostructure and chemistry of solid-electrolyte interphase on lithium anodes by depth-sensitive plasmon-enhanced Raman spectroscopy
The solid-electrolyte interphase is crucial for most batteries, but its characterization is challenging. Here, authors develop a depth-sensitive plasmon-enhanced Raman spectroscopy method to enable in-situ and nondestructive resolving of its structure and chemistry as well as formation mechanisms.
- Yu Gu
- , En-Ming You
- & Bing-Wei Mao
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Article
| Open AccessCoordination modulation of hydrated zinc ions to enhance redox reversibility of zinc batteries
Zinc-based batteries suffer from the dendrite growth and surface passivation of zinc derived from the unfavourable deposition and side reactions. Here, the authors modulate the coordination chemistry of hydrated zinc ions via electrolyte-design and gain insights into the reversible cycling of long-lived zinc electrode.
- Song Chen
- , Deluo Ji
- & Jintao Zhang
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Article
| Open AccessExtreme fast charging of commercial Li-ion batteries via combined thermal switching and self-heating approaches
A significant barrier to the mass adoption of electric vehicles is the long charge time (>30 min) of high-energy Li-ion batteries. Here, the authors propose a practical solution to enable fast charging of commercial Li-ion batteries by combining thermal switching and self-heating.
- Yuqiang Zeng
- , Buyi Zhang
- & Ravi S. Prasher
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Article
| Open AccessCross-linked polyaniline for production of long lifespan aqueous iron||organic batteries with electrochromic properties
Aqueous iron batteries are safe and cost-effective candidates for large-scale energy storage. However, their long-term cycling stability is inadequate. Here, the authors propose a crosslinked polyaniline-based positive electrode for high-power aqueous iron batteries with electrochromic properties.
- Haiming Lv
- , Zhiquan Wei
- & Hongfei Li
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Article
| Open AccessData-driven direct diagnosis of Li-ion batteries connected to photovoltaics
Li-ion batteries are used to store energy harvested from photovoltaics. However, battery use is sporadic and standard diagnostic methods cannot be applied. Here, the authors propose a methodology for diagnosing photovoltaics-connected Li-ion batteries that use trained machine learning algorithms.
- Matthieu Dubarry
- , Nahuel Costa
- & Dax Matthews
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Article
| Open AccessEnabling selective zinc-ion intercalation by a eutectic electrolyte for practical anodeless zinc batteries
Achieving high-performance aqueous Zn-metal batteries is a challenge. Here, authors report a eutectic electrolyte that concurrently enables selective Zn2+ intercalation at the cathode and highly reversible Zn metal plating/stripping, resulting in a benchmark high-areal capacity Zn anode-free cell.
- Chang Li
- , Ryan Kingsbury
- & Linda F. Nazar
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Article
| Open AccessBioinspired design of Na-ion conduction channels in covalent organic frameworks for quasi-solid-state sodium batteries
Quasi-solid-state polymer electrolytes are ideal candidates for practical secondary battery applications. Here, the authors propose a negatively charged (–COO–)-modified covalent organic framework as a Na-ion quasi-solid-state electrolyte with sub-nanometric Na-ion transport zones.
- Yingchun Yan
- , Zheng Liu
- & Zhuangjun Fan
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Article
| Open AccessLithium crystallization at solid interfaces
In solid-state lithium metal batteries, the crystallization of Li-ions deposited at interfaces remains unclear. Here, authors use molecular dynamics simulations to reveal lithium crystallization pathways and energy barriers, guiding improved interfacial engineering and accelerated crystal growth.
- Menghao Yang
- , Yunsheng Liu
- & Yifei Mo
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Article
| Open AccessAn asymmetric electrolyte to simultaneously meet contradictory requirements of anode and cathode
While Zinc anodes are thermodynamically unstable in aqueous solutions, the protons (H+) from the water favor the cathodes of Zinc batteries. Here, the authors address this contradiction by designing an asymmetric electrolyte composed of an inorganic solid-state electrolyte and a hydrogel electrolyte.
- Shengmei Chen
- , Yiran Ying
- & Chunyi Zhi
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Article
| Open AccessSurface modification using heptafluorobutyric acid to produce highly stable Li metal anodes
Development of lithium metal anodes is limited due to the dendritic growth and high reactivity of metal lithium. Here authors propose a surface modification strategy using heptafluorobutyric acid to form a lithiophilic interface, which enables uniform Li deposition and improving battery performance.
- Yuxiang Xie
- , Yixin Huang
- & Shigang Sun
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Article
| Open AccessMachine learning-guided discovery of ionic polymer electrolytes for lithium metal batteries
Ionic polymer electrolytes containing non-flammable ionic liquids and polyelectrolytes have the potential to create safe and high-energy batteries. Here, the authors propose a machine-learning approach to identify ionic liquids suitable for such electrolytes in lithium metal batteries.
- Kai Li
- , Jifeng Wang
- & Ying Wang
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Article
| Open AccessDeep learning to estimate lithium-ion battery state of health without additional degradation experiments
Estimation of Li-ion battery state of health is crucial but requires time- and resource-consuming degradation tests for development. Here, authors propose a deep-learning method that enables accurate estimations without additional tests, ensuring absolute errors of less than 3% for 89.4% of samples.
- Jiahuan Lu
- , Rui Xiong
- & Fengchun Sun
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Article
| Open AccessSolvent control of water O−H bonds for highly reversible zinc ion batteries
The electrochemical performance of aqueous zinc ion batteries is limited by water activity. Here, the authors propose a hybrid electrolyte that incorporate strongly polar molecules to strengthen the water O–H bonds, thus reduce water activity and improve the electrochemical performance of the batteries.
- Yanyan Wang
- , Zhijie Wang
- & Zaiping Guo
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Article
| Open AccessOrigin of dendrite-free lithium deposition in concentrated electrolytes
The origin of dendrite growth and lithium deposition behavior remains not well understood. Here, authors use a single-salt and single-solvent model electrolyte system to study the correlations between the electrolyte solvation structure, interphase structure and lithium deposition morphology.
- Yawei Chen
- , Menghao Li
- & Ruiguo Cao
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Article
| 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