期刊
ACS NANO
卷 16, 期 6, 页码 9894-9907出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.2c04135
关键词
KEYWORDS; magnesium batteries; epitaxial growth; magnesiophilic hosts; lattice matching; electrostatic potential fi elds
类别
资金
- National Natural Science Foundation of China [51972187]
- China Postdoctoral Science Foundation [2021M701817]
- Natural Science Foundation of Shandong Province [ZR2021QE166]
- National Natural Science Foundation for Distinguished Young Scholars of China [51625204]
- Major Basic Research Program of Natural Science Foundation of Shandong Province [ZR2020ZD09]
Epitaxial electrocrystallization of Mg on a three-dimensional magnesiophilic host, achieved through the synergy of a magnesiophilic interface, lattice matching, and electrostatic confinement effects, can significantly improve the cycle life of rechargeable magnesium batteries.
Rechargeable magnesium batteries are particularly advantageous for renewable energy storage systems. However, the inhomogeneous Mg electrodeposits greatly shorten their cycle life under practical conditions. Herein, the epitaxial electrocrystallization of Mg on a three-dimensional magnesiophilic host is implemented via the synergy of a magnesiophilic interface, lattice matching, and electrostatic confinement effects. The vertically aligned nickel hydroxide nanosheet arrays grown on carbon cloth (abbreviated as Ni(OH)2@CC) have been delicately designed, which satisfy the essential prerequisite of a low lattice geometrical misfit with Mg (about 2.8%) to realize epitaxial electrocrystallization. Simultaneously, the ionic crystal nature of Ni(OH)2 displays a periodic and hillock-like electrostatic potential field over its exposed facets, which can precisely capture and confine the reduced Mg0 species onto the local electron-enriched sites at the atomic level. The Ni(OH)2@CC substrate undergoes sequential Mg-ion intercalation, underpotential deposition, and electrocrystallization processes, during which the uniform, lamellar Mg electrodeposits with a locked crystallographic orientation are formed. Under practical conditions (10 mA cm-2 and 10 mAh cm-2), the Ni(OH)2@ CC substrate exhibits stable Mg stripping/plating cycle performances over 600 h, 2 orders of magnitude longer than those of the pristine copper foil and carbon cloth substrates.
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