期刊
ADVANCED ENERGY MATERIALS
卷 11, 期 10, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.202003118
关键词
batteries; dendrites; in situ TEM; Li electroplating; metal anodes
类别
资金
- DCCEM, at the Materials Department, Oxford [EP/R010145/1]
- 111 project of China [D17003]
- EPSRC [EP/P001645/1]
- Engineering and Physical Sciences Research Council (EPSRC)
- SUPERGEN Energy Storage Hub [EP/L019469/1]
- Enabling Next Generation Lithium Batteries [EP/M009521/1]
- Henry Royce Institute for Advanced Materials [EP/R010145/1, EP/R00661X/1, EP/S019367/1]
- Faraday Institution All-Solid-State Batteries with Li and Na Anodes [FIRG007, FIRG008]
- Research and Development Program of Korea Institute of Energy Research [KIER/C0-2459]
- Royal Society
- EPSRC [EP/L019469/1, EP/S003053/1, EP/M009521/1, EP/P001645/1] Funding Source: UKRI
The study investigates the nanoscale structural evolution of lithium electrodeposition and dissolution at the electrode surface across fluoride-poor and fluoride-rich interphases, showing that a fluoride-rich SEI can suppress lithium detachment and isolation, reduce dead Li formation, and prevent electrolyte decomposition, ultimately improving lithium cycling efficiency.
The solid electrolyte interphase (SEI), a complex layer that forms over the surface of electrodes exposed to battery electrolyte, has a central influence on the structural evolution of the electrode during battery operation. For lithium metallic anodes, tailoring this SEI is regarded as one of the most effective avenues for ensuring consistent cycling behavior, and thus practical efficiencies. While fluoride-rich interphases in particular seem beneficial, how they alter the structural dynamics of lithium plating and stripping to promote efficiency remains only partly understood. Here, operando liquid-cell transmission electron microscopy is used to investigate the nanoscale structural evolution of lithium electrodeposition and dissolution at the electrode surface across fluoride-poor and fluoride-rich interphases. The in situ imaging of lithium cycling reveals that a fluoride-rich SEI yields a denser Li structure that is particularly amenable to uniform stripping, thus suppressing lithium detachment and isolation. By combination with quantitative composition analysis via mass spectrometry, it is identified that the fluoride-rich SEI suppresses overall lithium loss through drastically reducing the quantity of dead Li formation and preventing electrolyte decomposition. These findings highlight the importance of appropriately tailoring the SEI for facilitating consistent and uniform lithium dissolution, and its potent role in governing the plated lithium's structure.
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