北京大学徐冰君团队研究发现C-C偶联不太可能是铜催化CO电化学还原中C2+产物形成的速率决定步骤。相关研究成果于2021年11月15日发表在《德国应用化学》。

Author: Xiaoxia Chang, Jing Li, Haocheng Xiong, Haochen Zhang, Yifei Xu, Hai Xiao, Qi Lu, Bingjun Xu

Issue&Volume: 2021-11-15

Abstract: The identity of the rate-determining step (RDS) in the electrochemical CO reduction reaction (CORR) on Cu catalysts remains unresolved because: 1) the presence of mass transport limitation of CO; and 2) the absence of quantitative correlation between CO partial pressure (  p  CO  ) and surface CO coverage. In this work, we determined CO adsorption isotherms on Cu in a broad pH range of 7.2-13.9. Together with electrokinetic data, we demonstrate that the reaction orders of adsorbed CO at  p  CO  < 0.4 and > 0.6 atm are 1  st  and 0  th  , respectively, on three Cu catalysts. These results indicate that the C-C coupling is unlikely to be the RDS in the formation of C2+ products in the CORR. We propose that the hydrogenation of CO with adsorbed water is the RDS, and the site competition between CO and water leads to the observed transition of the CO reaction order.

DOI: 10.1002/anie.202111167

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202111167