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| 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 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 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 AccessLaser maskless fast patterning for multitype microsupercapacitors
Miniature asymmetric supercapacitors have higher voltage and energy density but are often limited by a complex manufacturing process and difficulties in further miniaturization. Here, the authors demonstrate a maskless method for the patterned fabrication of submicron-scale symmetric and asymmetric supercapacitors.
- Yongjiu Yuan
- , Xin Li
- & Liangti Qu
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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 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 AccessCarbon neutral hydrogen storage and release cycles based on dual-functional roles of formamides
The search for new carbon-based hydrogen storage materials attracts scientists from various disciplines. Now, carbon-neutral hydrogen storage-release is reported based on dual-functional roles of formamides and uses non-noble, Fe-based catalyst.
- Duo Wei
- , Xinzhe Shi
- & Matthias Beller
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Article
| Open AccessA fluorinated cation introduces new interphasial chemistries to enable high-voltage lithium metal batteries
Fluorides have been identified as a key ingredient in interphases supporting aggressive battery chemistries. Here, the authors show a positive charged organic cation carrying fluorine populates at the inner Helmholtz layer of the electrode and contributes to the interphasial chemistry.
- Qian Liu
- , Wei Jiang
- & Zhengcheng Zhang
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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 AccessFe/Cu diatomic catalysts for electrochemical nitrate reduction to ammonia
Nitrate electroreduction to ammonia can decrease pollutants and produce high-value ammonia. Here, the authors design a Fe/Cu diatomic catalyst on nitrogen-doped graphene, which exhibits high catalytic activities of and selectivity for ammonia.
- Shuo Zhang
- , Jianghua Wu
- & Jun Lu
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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 AccessHigh-rate and selective conversion of CO2 from aqueous solutions to hydrocarbons
Electrochemical CO2 conversion to methane offers a promising solution for the large-scale storage of renewable electricity, yet the catalytic selectivity at high current density still needs to be refined. Here the authors report to use both dissolved CO2 and in-situ generated CO2 from bicarbonate to sustain high local CO2 concentration around Cu electrode and thus achieve selective CO2 conversion to methane.
- Cornelius A. Obasanjo
- , Guorui Gao
- & Cao-Thang Dinh
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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 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 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 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 AccessDesigning tailored combinations of structural units in polymer dielectrics for high-temperature capacitive energy storage
Polymer dielectrics face huge challenges in the harsh environments of emergent applications. Now, increased energy storage of polymer dielectrics at temperatures up to 250 °C by designing tailored combinations of structural units is reported.
- Rui Wang
- , Yujie Zhu
- & Qi Li
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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 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 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 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 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 AccessUltrahigh loading dry-process for solvent-free lithium-ion battery electrode fabrication
Scalable dry electrode process is essential for the sustainable manufacturing of the lithium based batteries. Here, the authors propose a dry press-coating technique to fabricate a robust and flexible high loading electrode for lithium pouch cells.
- Minje Ryu
- , Young-Kuk Hong
- & Jong Hyeok Park
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Article
| Open AccessNanoarchitecture factors of solid electrolyte interphase formation via 3D nano-rheology microscopy and surface force-distance spectroscopy
Characterization of the solid electrolyte interphase formed on Li-ion battery electrodes presents significant experimental challenges. Here the authors use atomic force microscopy-based force-spectroscopy techniques to depict the initial interphase formation in two different electrolyte classes.
- Yue Chen
- , Wenkai Wu
- & Oleg V. Kolosov
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Article
| Open AccessUnderstanding the evolution of lithium dendrites at Li6.25Al0.25La3Zr2O12 grain boundaries via operando microscopy techniques
Lithium metal penetration into solid-state electrolytes is a major drawback for developing all-solid-state batteries. Here, authors, via operando force microscopy, demonstrate that the trapping of electrons in garnet-type solid-state electrolyte grain boundaries is the origin of cell failure.
- Chao Zhu
- , Till Fuchs
- & Rüdiger Berger
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Article
| Open AccessNaked metallic skin for homo-epitaxial deposition in lithium metal batteries
The oxide passivation layer on the lithium metal surface causes uneven deposition and stripping in lithium metal batteries. Here authors introduce uniform homo-epitaxial lithium deposition on the metal surface to alleviate this issue and improve the cycle stability of the lithium metal batteries.
- Minsung Baek
- , Jinyoung Kim
- & Jang Wook Choi