Water coordinated on Cu(I)-based catalysts is the oxygen source in CO2 reduction to CO
Ya‐Jun Zheng, Hedan Yao, Ruinan Di, Zhicheng Xiang, Qiang Wang, Fangfang Lu, Yu Li, Guangxing Yang, Qiang Ma, Zhiping Zhang
Abstract
Abstract Catalytic reduction of CO 2 over Cu-based catalysts can produce various carbon-based products such as the critical intermediate CO, yet significant challenges remain in shedding light on the underlying mechanisms. Here, we develop a modified triple-stage quadrupole mass spectrometer to monitor the reduction of CO 2 to CO in the gas phase online. Our experimental observations reveal that the coordinated H 2 O on Cu(I)-based catalysts promotes CO 2 adsorption and reduction to CO, and the resulting efficiencies are two orders of magnitude higher than those without H 2 O. Isotope-labeling studies render compelling evidence that the O atom in produced CO originates from the coordinated H 2 O on catalysts, rather than CO 2 itself. Combining experimental observations and computational calculations with density functional theory, we propose a detailed reaction mechanism of CO 2 reduction to CO over Cu(I)-based catalysts with coordinated H 2 O. This study offers an effective method to reveal the vital roles of H 2 O in promoting metal catalysts to CO 2 reduction.