Water coordinated on Cu(I)-based catalysts is the oxygen source in CO2 reduction to CO

Yajun Zheng, Hedan Yao, Ruinan Di, Zhicheng Xiang, Qiang Wang (), Fangfang Lu, Yu Li, Guangxing Yang (), Qiang Ma and Zhiping Zhang ()
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Yajun Zheng: Xi’an Shiyou University
Hedan Yao: Xi’an Shiyou University
Ruinan Di: Nanjing Tech University
Zhicheng Xiang: Xi’an Shiyou University
Qiang Wang: Nanjing Tech University
Fangfang Lu: Xi’an Shiyou University
Yu Li: Xi’an Shiyou University
Guangxing Yang: South China University of Technology
Qiang Ma: Chinese Academy of Inspection and Quarantine
Zhiping Zhang: Xi’an Shiyou University

Nature Communications, 2022, vol. 13, issue 1, 1-11

Abstract: Abstract Catalytic reduction of CO2 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 CO2 to CO in the gas phase online. Our experimental observations reveal that the coordinated H2O on Cu(I)-based catalysts promotes CO2 adsorption and reduction to CO, and the resulting efficiencies are two orders of magnitude higher than those without H2O. Isotope-labeling studies render compelling evidence that the O atom in produced CO originates from the coordinated H2O on catalysts, rather than CO2 itself. Combining experimental observations and computational calculations with density functional theory, we propose a detailed reaction mechanism of CO2 reduction to CO over Cu(I)-based catalysts with coordinated H2O. This study offers an effective method to reveal the vital roles of H2O in promoting metal catalysts to CO2 reduction.

Date: 2022
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DOI: 10.1038/s41467-022-30289-5

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