期刊
ADVANCED MATERIALS
卷 33, 期 26, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202100224
关键词
chemisorption effect; current homogenization; geometric confinement; high areal capacity; magnesium batteries
类别
资金
- National Natural Science Foundation of China [51972187, 21805157]
- Key R&D project of Shandong Province [2019GGX103034]
- Development Program in Science and Technology of Qingdao [19-6-2-12-cg]
- National Key R&D Program of China [2018YFB0104300]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDA22010600]
- National Natural Science Foundation for Distinguished Young Scholars of China [51625204, 21975274]
- Youth Innovation Promotion Association of CAS [2016193]
- Natural Science Foundation of Shandong Province [ZR2019MEM043, ZR2019MB037]
- Major Basic Research Program of Natural Science Foundation of Shandong Province [ZR2020ZD09]
- Taishan Scholars of Shandong Province [ts201511063]
A comprehensive design matrix for 3D magnesiophilic hosts is reported to regulate the uniform Mg electrodeposition through a synergistic coupling of current distribution, geometric confinement, and chemisorptive interaction. The proposed VNCA@C host demonstrates reduced nucleation overpotential and an elongated Mg plating/stripping cycle life under high current density, with potential application in high-energy-density batteries with other metal anodes such as lithium and zinc.
Unevenly distributed magnesium (Mg) electrodeposits have emerged as a major obstacle for Mg-metal batteries. A comprehensive design matrix is reported for 3D magnesiophilic hosts, which regulate the uniform Mg electrodeposition through a synergistic coupling of homogenizing current distribution, geometric confinement, and chemisorptive interaction. Vertically aligned nitrogen- and oxygen-doped carbon nanofiber arrays on carbon cloth (denoted as VNCA@C) are developed as a proof of concept. The evenly arranged short nanoarray architecture helps to homogenize the surface current density and the microchannels built in this 3D host allow the preferential nucleation of Mg due to their geometrical confinement effect. Besides, the nitrogen-/oxygen-doped carbon species exhibit strong chemisorptive interaction toward Mg atoms, providing preferential nucleation sites as demonstrated by first-principle calculation results. Electrochemical analysis reveals a peculiar yet highly reversible microchannel-filling growth behavior of Mg metals, which empowers the delicately designed VNCA@C host with the ability to deliver a reduced nucleation overpotential of 429 mV at 10.0 mA cm(-2) and an elongated Mg plating/stripping cycle life (110 cycles) under high current density of 10.0 mA cm(-2). The proposed design matrix can be extended to other metal anodes (such as lithium and zinc) for high-energy-density batteries.
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