Electro-chemo-mechanics of lithium in solid state lithium metal batteries

Tang, Yongfu; Zhang, Liqiang; Chen, Jingzhao; Sun, Haiming; Yang, Tingting; Liu, Qiunan; Huang, Qiao; Zhu, Ting; Huang, Jianyu

doi:10.1039/d0ee02525a

Cited by 107 publications

(85 citation statements)

References 285 publications

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“…Much research is devoted to combining solid electrolytes and lithium metal electrodes. 4,5 However, liquid electrolytes as used in lithium-ion batteries offer a high ionic conductivity and can stay in contact with the moving surface of a metal, 6 as demonstrated, for example, in commercial zinc metal batteries. 7 Moreover, liquid electrolytes for lithium-ion batteries have been studied for decades and have better compatibility with the current manufacturing process than solid-state electrolytes.…”

Section: Introductionmentioning

confidence: 99%

Strategies towards enabling lithium metal in batteries: interphases and electrodes

Horstmann

Shi

Amine

et al. 2021

Energy Environ. Sci.

187

189

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Section: Introductionmentioning

confidence: 99%

Strategies towards enabling lithium metal in batteries: interphases and electrodes

Horstmann

Shi

Amine

et al. 2021

Energy Environ. Sci.

187

189

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“…How the mechanical response and electrochemical performance correlates is yet to be answered. [ 37–40 ] Especially, since the stress is generated locally during lithium deposition, its characteristic effective length may well go down to nanometers. This leads to difficulty in direct measurements using conventional macroscopic electrochemical setups as shown in Figure 1 a,b.…”

Section: Introductionmentioning

confidence: 99%

Modulating Nanoinhomogeneity at Electrode–Solid Electrolyte Interfaces for Dendrite‐Proof Solid‐State Batteries and Long‐Life Memristors

Yang

et al. 2021

Advanced Energy Materials

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Dendrite penetration in ceramic lithium conductors severely constrains the development of solid‐state batteries (SSBs) while its nanoscale origin remains unelucidated. An in situ nanoscopic electrochemical characterization technique is developed based on conductive‐atomic force microscopy (c‐AFM) to reveal the local dendrite growth kinetics. Using Li7La3Zr2O12 (LLZO) as a model system, significant local inhomogeneity is observed with a hundredfold decrease in the dendrite triggering bias at grain boundaries compared with that at grain interiors. The origin of the local weakening is assigned to the nanoscale variation of elastic modulus and lithium flux detouring. An ionic‐conductive polymeric homogenizing layer is designed which achieves a high critical current density of 1.8 mA cm–2 and a low interfacial resistance of 14 Ω cm2. Practical SSBs based on LiFePO4 cathodes can be stably cycled over 300 times. Beyond this, highly reversible electrochemical dendrite healing in LLZO is discovered using the c‐AFM electrode, based on which a model memristor with a high on/off ratio of ≈105 is demonstrated for >200 cycles. This work not only provides a novel tool to investigate and design interfaces in SSBs but also offers opportunities for solid electrolytes beyond energy applications.

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“…[ 5 , 6 , 7 ] Li dendrites growing with high crystal orientation would penetrate into the separators and cause a short circuit in the batteries, which would induce serious safety hazards. [ 8 , 9 ] During Li deposition/exfoliation, the volume expansion is uncontrollable, resulting in the breakages of unstable SEI layer, as well as the Coulomb efficiency and reversible capacity decaying closely with the repeated fractures of SEI and continuous electrolyte consumption. [ 6 ] In addition, isolated Li‐dendrites are formed after cycling and gradually turn into the dead Li, which easily accumulated on the electrode surfaces and intensified the polarization of Li electrodes.…”

Section: Introductionmentioning

confidence: 99%

Effectively Regulating More Robust Amorphous Li Clusters for Ultrastable Dendrite‐Free Cycling

Huang

Yang

et al. 2021

Advanced Science

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A disordered phase in Li-deposit nanostructure is greatly attractive, but plagued by the uncontrollable and unstable growth, and the nanoscale characterization in the structure. Here, fully characterized in cryogenic transmission electron microscopy (cryo-TEM), more robust amorphous-Li (ALi) clusters are revealed and effectively regulated on heteroatom-activating electronegative sites and an advanced solid electrolyte interphase (SEI) layer. Heteroatom-activating electronegative sites capably enhance the electrostatic interaction of Li + and heteroatom-doping graphene-like film (HDGs), meaning lower Li diffusion barrier and larger binding energy that is confirmed by small nucleation overpotentials of 13.9 and 10 mV at 0.1 mA cm −2 in the fluoroethylene carbonate-adding ester-based (FEC-ester) and LiNO 3 -adding ether-based (LiNO 3 -ether) electrolytes. Orderly multilayer SEI structure comprised of inorganic-rich components enables fast ion transports and durable capabilities to construct highly reversible and long-term plating/stripping cycling. ALi cluster anodes exhibit non-crystalline morphologies and perform ultrastable dendrite-free cycling over 2800 times. Stable ALi clusters are also grown in LiFePO 4 (LFP) (LFP-ALi-HDGs-N||LiFePO 4 [LFP]) full cells with advantageous capacities up to 165.5 and 164.3 mAh g −1 in these optimized electrolytes at 0.1 C; the remarkable capacity retentions maintain to 93% and 91% after 150 cycles at 0.2 C. Structure viability, electrochemical reversibility, and excellent performance in ALi clusters are effectively regulated.

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Electro-chemo-mechanics of lithium in solid state lithium metal batteries

Abstract: Using lithium as the anode to achieve high energy density of lithium-ion/metal batteries is the ultimate goal of energy storage technology. Recent development of solid state electrolytes (SSEs) with high...

Cited by 107 publications

References 285 publications

Strategies towards enabling lithium metal in batteries: interphases and electrodes

Strategies towards enabling lithium metal in batteries: interphases and electrodes

Modulating Nanoinhomogeneity at Electrode–Solid Electrolyte Interfaces for Dendrite‐Proof Solid‐State Batteries and Long‐Life Memristors

Effectively Regulating More Robust Amorphous Li Clusters for Ultrastable Dendrite‐Free Cycling

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