中科院化学所韩布兴团队报道了用于从甲酸盐转化为CO的CO2电还原产物的原子铟催化剂。 相关研究成果发表在2021年4月15日出版的国际学术期刊《美国化学会杂志》。

电化学还原二氧化碳为化学品和燃料是一个有趣的和有吸引力的减轻温室气体排放和能源短缺的方式。

该文中，研究人员报道了原子In催化剂在CO2电还原制CO中的应用。原子In催化剂通过In基金属有机骨架（MOFs）和双氰胺的热解固定在N掺杂碳（InA/NC）上。研究发现，InA/NC在离子液体/MeCN混合电解质中具有优异的选择性共生成性能。它不同于以甲酸/甲酸为主要产物的基体材料。CO的法拉第效率（FE）为97.2%，总电流密度为39.4mAcm-2，转换频率（TOF）为～40000h^-1。这是迄今为止所报道的所有催化剂中CO产品TOF最高的之一。

此外，催化剂具有显著的稳定性。研究表明，InA/NC具有较高的双层电容、较大的CO2吸附容量和较低的界面电荷转移电阻，具有较高的CO2还原活性。控制实验和理论计算表明，InA/NC的In-N位不仅有利于COOH*的解离生成CO，而且阻碍了甲酸盐的生成，对CO具有较高的选择性。

附：英文原文

Title: Atomic Indium Catalysts for Switching CO2 Electroreduction Products from Formate to CO

Author: Weiwei Guo, Xingxing Tan, Jiahui Bi, Liang Xu, Dexin Yang, Chunjun Chen, Qinggong Zhu, Jun Ma, Akhil Tayal, Jingyuan Ma, Yuying Huang, Xiaofu Sun, Shoujie Liu, Buxing Han

Issue&Volume: April 15, 2021

Abstract: Electrochemical reduction of CO2 to chemicals and fuels is an interesting and attractive way to mitigate greenhouse gas emissions and energy shortages. In this work, we report the use of atomic In catalysts for CO2 electroreduction to CO. The atomic In catalysts were anchored on N-doped carbon (InA/NC) through pyrolysis of In-based metal–organic frameworks (MOFs) and dicyandiamide. It was discovered that InA/NC had outstanding performance for selective CO production in the mixed electrolyte of ionic liquid/MeCN. It is different from those common In-based materials, in which formate/formic acid is formed as the main product. The faradaic efficiency (FE) of CO and total current density were 97.2% and 39.4 mA cm-2, respectively, with a turnover frequency (TOF) of ～40000 h–1. It is one of the highest TOF for CO production to date for all of the catalysts reported. In addition, the catalyst had remarkable stability. Detailed study indicated that InA/NC had higher double-layer capacitance, larger CO2 adsorption capacity, and lower interfacial charge transfer resistance, leading to high activity for CO2 reduction. Control experiments and theoretical calculations showed that the In–N site of InA/NC is not only beneficial for dissociation of COOH* to form CO but also hinders formate formation, leading to high selectivity toward CO instead of formate.

DOI: 10.1021/jacs.1c00151

Source: https://pubs.acs.org/doi/10.1021/jacs.1c00151