过电位
甲酸
化学
格式化
催化作用
计时安培法
原位
无机化学
化学工程
物理化学
有机化学
电极
循环伏安法
电化学
工程类
作者
Zhijuan Niu,Yangyang Wan,Xin Li,Man Zhang,Biying Liu,Chen Zuo,Gang Lü,Kai Yan
标识
DOI:10.1016/j.jcat.2020.07.004
摘要
The capability to actively control chemical reactions has enormous implications for energy generation and conversion. By integrating theory and experiments, we achieved an in-situ regulation of formic acid oxidation on a Pt (1 1 1) surface via externally applied strains. The first-principles theory predicted that compressive strains can lower the reaction overpotential to boost the formate pathway and alleviate CO poisoning on the Pt surface, while tensile strains should have the opposite effects. The experimental observations confirmed the theoretical predictions. Compressive elastic strains (approximately -0.4%) could create over 75 mV overpotential decrease, far beyond what was achieved in previous works. A mass activity (~700 mA/mg) of Pt was achieved in a broad potential range of 0.4–0.85 V (vs RHE) under compressive strains. There was no evident activity loss during the chronoamperometry test at 0.6 V. The first-principles theory, controlled synthesis and in-situ measurements were combined to achieve active control, which represents important progress in tuning the electrocatalytic activity of formic acid oxidation.
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