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

Lu, Ziheng; Yang, Ziwei; Li, Cheng; Wang, Kai; Han, Jinlong; Tong, Peiqing; Li, Guoxiao; Vishnugopi, Bairav S.; Mukherjee, Partha P.; Yang, Chunlei; Li, Wenjie

doi:10.1002/aenm.202003811

Cited by 40 publications

(37 citation statements)

References 79 publications

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“…The ion transport in the model exhibits a uniform distribution, thus resulting in uniform nucleation and growth of Li, as we have observed with S‐99 sample. Our results are also consistent with recent simulations, [ 59,60 ] in which, however, the effect of heterogeneous ion current during nucleation and growth process has not been well‐linked. According to the Chazalviel–Rosso model, local cation concentration directly affects the nucleation and growth manners of lithium.…”

Section: Discussionsupporting

confidence: 93%

Linking the Defects to the Formation and Growth of Li Dendrite in All‐Solid‐State Batteries

Wang

Gao

Chen

et al. 2021

Advanced Energy Materials

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The nucleation and growth of Li metal during deposition and the associated dendrite penetration are the critical and fundamental issues influencing the safety and power density of solid‐state lithium metal batteries (SSLBs). However, investigations on Li metal deposition/dissolution especially the formation and growth of Li dendrites and their determining factors in the all‐solid‐state electrochemical systems are still lacking. In this work, in situ observations of the Li metal growth process, and defects induced heterogeneous deposition under cathodic load, are reported. By exploiting in situ scanning electron microscopy, along with electrochemical analytical approaches, the spatial distribution and morphological evolution of the deposited Li at the electrode|solid electrolyte interface are obtained and discussed. This investigation reveals that the formation of lithium whiskers is decided by the local Li ion flux and the deposition active sites, which are closely dependent on the content and types of defects in the polycrystalline electrolyte. Moreover, the defect regions exhibit faster Li deposition kinetics and higher nucleation tendency. These results can advance the fundamental understanding of the Li penetration mechanism in SSLBs.

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Section: Discussionsupporting

confidence: 93%

Linking the Defects to the Formation and Growth of Li Dendrite in All‐Solid‐State Batteries

Wang

Gao

Chen

et al. 2021

Advanced Energy Materials

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“…We further identified three different Li dendrite shapes: "needle," "mushroom," and "hemisphere" in different conditions. We finally proposed the concept of local current density (LCD) as a supplement to CCD to compensate for the contradiction in experimental observations (18,45). Thus, homogeneous distribution of LCD and high fluidity of Li are essential to trigger the two self-healing processes, which suppress dendrite formation.…”

Section: Introductionmentioning

confidence: 99%

Self‐Healing Mechanism of Lithium in Lithium Metal

et al. 2022

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Li metal as an ideal anode material meets the requirements of state-of-the-art secondary batteries. However, the dendrite growth of Li causes safety concerns and results in a low coulombic efficiency, which has significantly restricted the commercial applications of Li secondary batteries. Owing to the intrinsic limitations of even the most advanced experimental and computational techniques, a mechanistic understanding of Li deposition (growth) on the atomic scale is lacking.Here, we construct a Li potential model by machine learning with an accuracy of quantum mechanical computations. Our molecular dynamics simulations based on this potential model reveal two self-healing mechanisms in a large Li metal system, surface self-healing and bulk self-healing, and identify three Li dendrite morphologies in different conditions, "needle," "mushroom," and "hemisphere." We finally propose the concepts of local current density and variance of local current density as a supplement to critical current density to determine the probability of self-healing triggered.

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“…Direct correlation of local conductivity and topographical features of SSEs are very helpful in designing more reliable high energy density batteries when utilizing SSEs. [ 291 ] Intermittent contact alternating current scanning electrochemical microscopy (ic‐ac‐SECM) demonstrated its effectiveness in measuring the ionic conductivity while obtaining the local topographic images of SSE. [ 292 ] Figure 14 a,b show the topographic and impedance maps obtained at a large LLZO grain using ic‐ac‐SECM over 250 × 250 µm.…”

Section: Ec‐afm For the Understanding Of Libs And Their Materialsmentioning

confidence: 99%

Characterizing Batteries by In Situ Electrochemical Atomic Force Microscopy: A Critical Review

Zhang

Said

Smith

et al. 2021

Advanced Energy Materials

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Although lithium, and other alkali ion, batteries are widely utilized and studied, many of the chemical and mechanical processes that underpin the materials within, and drive their degradation/failure, are not fully understood. Hence, to enhance the understanding of these processes various ex situ, in situ and operando characterization methods are being explored. Recently, electrochemical atomic force microscopy (EC‐AFM), and related techniques, have emerged as crucial platforms for the versatile characterization of battery material surfaces. They have revealed insights into the morphological, mechanical, chemical, and physical properties of battery materials when they evolve under electrochemical control. This critical review will appraise the progress made in the understanding batteries using EC‐AFM, covering both traditional and new electrode–electrolyte material junctions. This progress will be juxtaposed against the ability, or inability, of the system adopted to embody a truly representative battery environment. By contrasting key EC‐AFM literature with conclusions drawn from alternative characterization tools, the unique power of EC‐AFM to elucidate processes at battery interfaces is highlighted. Simultaneously opportunities for complementing EC‐AFM data with a range of spectroscopic, microscopic, and diffraction techniques to overcome its limitations are described, thus facilitating improved battery performance.

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

Cited by 40 publications

References 79 publications

Linking the Defects to the Formation and Growth of Li Dendrite in All‐Solid‐State Batteries

Linking the Defects to the Formation and Growth of Li Dendrite in All‐Solid‐State Batteries

Self‐Healing Mechanism of Lithium in Lithium Metal

Characterizing Batteries by In Situ Electrochemical Atomic Force Microscopy: A Critical Review

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