Recent Progress in the Mechanistic Understanding of Formic Acid Oxidation on Pt Electrode

本文综述了甲酸在铂电极上电催化氧化机理的实验和理论研究进展. 铂电极甲酸的电化学氧化主要有两种途径：1）间接途径，甲酸经由CO中间物氧化为最终产物CO2，室温下该途径对总电流贡献不超过1%；2）直接途径，甲酸直接氧化生成CO2. 作者课题组对文献中桥式吸附甲酸根是否是甲酸氧化反应直接途径的反应中间物的争论进行了详细的分析和探讨，认为桥式吸附的甲酸根不是间接途径中生成CO的前驱体，也不是甲酸直接氧化途径的中间物. 作者课题组还指出了支持甲酸根是甲酸直接氧化途径的反应中间物的推论的问题所在.This article reviews the recent progress in understanding of the mechanisms for formic acid oxidation on Pt electrode. There are two pathways for formic acid oxidation on Pt electrode: (1) Indirect Pathway through which HCOOH is oxidized to CO2 through COad intermediate. This pathway contributes only 1% of the total current; (2) Direct Pathway where HCOOH is oxidized directly to CO2. The results from IR Spectroscopy, single-crystal electrochemistry and DFT calculation all support that the bridge-bonded formate is neither the intermediate of direct pathway nor the precursor for COad formation in indirect pathway. Possible mechanism in the direct pathway for formic acid oxidation is discussed.国家自然基金面上项目（No. 21273215）资助作者联系地址：中国科技大学 化学物理系，合肥微尺度物质科学国家实验室（筹），安徽 合肥 230026Author's Address: Hefei National Laboratory for Physical Science at Microscale and Department of Chemical Physics, University of Science and Technology of China, Hefei, 230026, China通讯作者E-mail：[email protected]