材料科学
化学吸附
成核
过电位
电流密度
阳极
纳米技术
化学物理
电化学
化学工程
金属
镁
吸附
电极
冶金
物理化学
热力学
工程类
化学
物理
量子力学
作者
Zihao Song,Zhonghua Zhang,Aobing Du,Shanmu Dong,Guicun Li,Guanglei Cui
标识
DOI:10.1002/adma.202100224
摘要
Abstract 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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