| 1. |
- Jiao, Xingxing, et al.
(författare)
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Morphology evolution of electrodeposited lithium on metal substrates
- 2023
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Ingår i: Energy Storage Materials. - 2405-8297. ; 61
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Tidskriftsartikel (refereegranskat)abstract
- Lithium (Li) metal is deemed to be the high-energy-density anode material for next generation batteries, but its practical application is impeded by the uneven electrodeposition during charge of battery, which leads to the low Coulombic efficiency and potential safety issue. Here, multiscale modeling is fabricated to understand the morphology evolution of Li during electrodeposition process, from the self-diffusion of Li adatoms on electrode surface, to the nucleation process, and to the formation of Li microstructures, revealing the correlation between final morphology and deposition substrates. Energy batteries and self-diffusion of Li adatom on various substrates (lithium, copper, nickel, magnesium, and silver) result in the different nucleation size, which is calculated by kinetic Monte Carlo simulation based on classical nucleation theory. Formation of Li substructures that are grown from Li nuclei, is revealed by phase field modeling coupled with cellular automaton method. Our results show that larger Li nuclei is obtained under faster self-diffusion of Li adatom, leading to the low aspect ratio of Li substructures and the subsequent morphology evolution of electrodeposited Li. Furthermore, the electrodeposition of Li is strongly regulated by the selection of substrates, giving the practical guideline of anode design in rechargeable Li metal batteries. It is worthy to mention that this method to investigate the electro-crystallization process involving nucleation and growth can be transplanted to the other metallic anode, such as sodium, potassium, zinc, magnesium, calcium and the like.
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| 2. |
- Liu, Yangyang, et al.
(författare)
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Role of Interfacial Defects on Electro–Chemo–Mechanical Failure of Solid-State Electrolyte
- 2023
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Ingår i: Advanced Materials. - 0935-9648 .- 1521-4095. ; 35:24
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Tidskriftsartikel (refereegranskat)abstract
- High-stress field generated by electroplating of lithium (Li) in pre-existing defects is the main reason for mechanical failure of solid-state electrolyte because it drives crack propagation in electrolyte, followed by Li filament growth inside and even internal short-circuit if the filament reaches another electrode. To understand the role of interfacial defects on mechanical failure of solid-state electrolyte, an electro–chemo–mechanical model is built to visualize distribution of stress, relative damage, and crack formation during electrochemical plating of Li in defects. Geometry of interfacial defect is found as dominating factor for concentration of local stress field while semi-sphere defect delivers less accumulation of damage at initial stage and the longest failure time for disintegration of electrolyte. Aspect ratio, as a key geometric parameter of defect, is investigated to reveal its impact on failure of electrolyte. Pyramidic defect with low aspect ratio of 0.2–0.5 shows branched region of damage near interface, probably causing surface pulverization of solid-state electrolyte, whereas high aspect ratio over 3.0 will trigger accumulation of damage in bulk electrolyte. The correction between interfacial defect and electro–chemo–mechanical failure of solid-state electrolyte is expected to provide insightful guidelines for interface design in high-power-density solid-state Li metal batteries.
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| 3. |
- Xiong, Shizhao, 1985, et al.
(författare)
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Mechanical Failure of Solid-State Electrolyte Rooted in Synergy of Interfacial and Internal Defects
- 2023
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Ingår i: Advanced Energy Materials. - : Wiley. - 1614-6840 .- 1614-6832. ; 13:14
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Tidskriftsartikel (refereegranskat)abstract
- The mechanical failure of solid-state electrolytes induced by the growth of the lithium metal anode hinders the development of solid-state Li metal batteries with good safety and high energy density, and thus the understanding of the failure mechanism is of high importance for the application of solid-state lithium-metal batteries. Herein, a modified electro-chemo-mechanical model is built to bridge the dynamic relationship between the mechanical failure of solid-state electrolytes and the electrodeposition of lithium metal. The results, visualize evolution of local stress fields and the corresponding relative damage, and indicate that the generation of damage inside the solid-state electrolyte is rooted in a synergy of interfacial and internal defects. Compression by electrodeposited lithium inside interfacial defects and further transmission of stress inward in the electrolyte causes catastrophic damage, which is determined by the geometry of interfacial defects. Moreover, the internal defects of the solid-state electrolyte from sintering can influence the pathway of damage and work as the inner fountainhead for further damage propagation, and as such, the position and amount of the internal voids exhibit a more competitive role in the mechanical failure of solid-state electrolyte. Thus, the synergetic failure mechanism of solid-state electrolytes raised in this work provides a modeling framework to design effective strategies for state-of-the-art solid-state lithium-metal batteries.
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