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A Multiscale, Dynamic Elucidation of Li Solubility in the Alloy and Metallic Plating Process
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).ORCID iD: 0000-0001-7286-1211
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Number of Authors: 72023 (English)In: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, Vol. 35, no 47, article id 2306826Article in journal (Refereed) Published
Abstract [en]

Li-containing alloys and metallic deposits offer substantial Li+ storage capacities as alternative anodes to commercial graphite. However, the thermodynamically in sequence, yet kinetically competitive mechanism between Li solubility in the solid solution and intermediate alloy-induced Li deposition remains debated, particularly across the multiple scales. The elucidation of the mechanism is rather challenging due to the dynamic alloy evolution upon the non-equilibrium, transient lithiation processes under coupled physical fields. Here, influential factors governing Li solubility in the Li-Zn alloy are comprehensively investigated as a demonstrative model, spanning from the bulk electrolyte solution to the ion diffusion within the electrode. Through real-time phase tracking and spatial distribution analysis of intermediate alloy/Li metallic species at varied temperatures, current densities and particle sizes, the driving force of Li solubility and metallic plating along the Li migration pathway are probed in-depth. This study investigates the correlation between kinetics (pronounced concentration polarization, miscibility gap in lattice grains) and rate-limiting interfacial charge transfer thermodynamics in dedicating the Li diffusion into the solid solution. Additionally, the lithiophilic alloy sites with the balanced diffusion barrier and Li adsorption energy are explored to favor the homogeneous metal plating, which provides new insights for the rational innovation of high-capacity alloy/metallic anodes.

Place, publisher, year, edition, pages
2023. Vol. 35, no 47, article id 2306826
Keywords [en]
decoupled physical fields, dynamic phasic change, lithiophilic alloys, multiscale Li+ migration pathways, operando characterization
National Category
Materials Chemistry Physical Chemistry
Identifiers
URN: urn:nbn:se:su:diva-223749DOI: 10.1002/adma.202306826ISI: 001084858600001PubMedID: 37769145Scopus ID: 2-s2.0-85174214723OAI: oai:DiVA.org:su-223749DiVA, id: diva2:1812773
Available from: 2023-11-17 Created: 2023-11-17 Last updated: 2024-01-11Bibliographically approved

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Tai, Cheuk-Wai

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