催化作用
Boosting(机器学习)
电化学
化学
氧还原反应
氧气
还原(数学)
氧还原
材料科学
化学工程
电极
工程类
有机化学
计算机科学
物理化学
数学
几何学
机器学习
作者
Xiaoxiao Li,Yushan Yan,Xiaonan Zheng,Yuan Yao,Yang Liu
标识
DOI:10.1016/j.cej.2022.136363
摘要
• V-N-C SAC was designed for electrocatalytic ORR using biomimetic strategy. • Abnormal saturated coordination effect boosts ORR activity of V-N-C SAC. • V-N-C SAC shows innate Fenton nonreactivity to improve ORR stability. Single atom catalysts (SACs) exhibit impressive catalytic activity for various reactions due to low coordination environment and tunable electronic structures, attracting increasing attention. However, it is big challenge to develop transition-metal-based SACs for oxygen reduction reaction (ORR) with high stability. Bioinspired by the structure and mechanism of vanadium-dependent haloperoxidase, we herein demonstrate that saturated coordination could boost ORR activity of atomically dispersed V-N-C catalyst combining DFT prediction and experimental verification. Spontaneous axial OH coordination to V-N-C catalyst in alkaline electrolyte not only optimizes the adsorption interaction for key intermediates to boost ORR activity, but also keeps vanadium atom at the highest valence against Fenton activity to improve the stability. The as-designed catalyst exhibits half-wave potential of 0.858 V vs . RHE for ORR, comparable to the commercial Pt/C benchmark. This work provides a proof-of-concept design of SACs and broadens the horizon of its potential applications.
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