Zheng Wei, Wang Changlai, Chen Jing, Chen Shi, Lin Zhiyu, Huang Minxue, Huang Hao, Qu Yafei, Wang Peichen, Hu Lin, Chen Qianwang
Hefei National Research Center for Physical Sciences at the Microscale and Department of Materials Science & Engineering, University of Science and Technology of China, Hefei 230026, China.
The High Magnetic Field Laboratory, Chinese Academy of Sciences, Hefei 230031, China.
Dalton Trans. 2024 Mar 5;53(10):4617-4623. doi: 10.1039/d3dt04342h.
The electrochemical reduction of CO to HCOOH is considered one of the most appealing routes to alleviate the energy crisis and close the anthropogenic CO cycle. However, it remains challenging to develop electrocatalysts with high activity and selectivity towards HCOOH in a wide potential window. In this regard, Ag/BiOCO was prepared by an electrochemical transformation from Ag/BiO. The Ag/BiOCO catalyst achieves a faradaic efficiency (FE) of over 90% for HCOOH in a wide potential window between -0.8 V and -1.3 V the reversible hydrogen electrode (RHE). Moreover, a maximum FE of 95.8% and a current density of 15.3 mA cm were achieved at a low applied potential of -1.1 V. Density functional theory (DFT) calculations prove that the high catalytic activity of Ag/BiOCO is ascribed to the fact that Ag can regulate the electronic structure of Bi, thus facilitating the adsorption of *OCHO and hindering the adsorption of *COOH. This work expands the electrochemical derivatization strategy for the preparation of electrocatalysts.
将CO电化学还原为HCOOH被认为是缓解能源危机和闭合人为CO循环的最具吸引力的途径之一。然而，开发在宽电位窗口内对HCOOH具有高活性和选择性的电催化剂仍然具有挑战性。在这方面，通过从Ag/BiO进行电化学转变制备了Ag/BiOCO。Ag/BiOCO催化剂在相对于可逆氢电极（RHE）为-0.8 V至-1.3 V的宽电位窗口内对HCOOH实现了超过90%的法拉第效率（FE）。此外，在-1.1 V的低施加电位下实现了95.8%的最大FE和15.3 mA cm的电流密度。密度泛函理论（DFT）计算证明，Ag/BiOCO的高催化活性归因于Ag可以调节Bi的电子结构，从而促进OCHO的吸附并阻碍COOH的吸附。这项工作扩展了用于制备电催化剂的电化学衍生策略。
