期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 48, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202213024
关键词
CO2; Cu; ZnO; Methanol; Single-Atom Catalysis; Water
资金
- National Key Research and Development Program of China [2021YFA1500500, 2019YFA0405600, 2017YFA0204904]
- CAS Project for Young Scientists in Basic Research [YSBR-051]
- National Science Fund for Distinguished Young Scholars [21925204]
- NSFC [U19A2015, 11904353, 22204158]
- Fundamental Research Funds for the Central Universities, Provincial Key Research and Development Program of Anhui [202004a05020074]
- K. C. Wong Education [GJTD-2020-15]
- DNL Cooperation Fund, CAS [DNL202003]
- China Postdoctoral Science Foundation [2020M682007, 2019TQ0347]
- China Postdoctoral Program for Innovative Talents [BX20200323]
- Guangdong Basic and Applied Basic Research Foundation [2020A1515110743]
- Natural Science Foundation of Anhui Province [2208085QB42]
- Hefei National Synchrotron Radiation Laboratory [KY2340000157]
The hydrogenation of CO2 using renewable power-generated hydrogen is a promising way to achieve a sustainable carbon cycle. However, the role of water in CO2 hydrogenation is still debated. This study found that both too low and too high water contents hindered the synthesis of methanol over Cu/ZnO catalysts. The optimal water content was 0.11 vol. %, resulting in high methanol selectivity and CO2 conversion.
The hydrogenation of CO2 by renewable power-generated hydrogen offers a promising approach to a sustainable carbon cycle. However, the role of water during CO2 hydrogenation is still under debate. Herein, we demonstrated that either too low or too high contents of water hampered the methanol synthesis over Cu/ZnO based catalysts. For Cu single atoms on ZnO supports, the optimal content of water was 0.11 vol. % under 30 bar (CO2 : H-2=1 : 3) at 170 degrees C. Upon the introduction of optimal-content water, the methanol selectivity immediately became 99.1 %, meanwhile the conversion of CO2 underwent a volcano-type trend with the maximum of 4.9 %. According to mechanistic studies, water acted as a bridge between H atoms and CO2/intermediates, facilitating the transformation of COOH* and CH2O*. The enhanced activity induced the generation of more water to react with CO via water-gas shift reaction, resulting in the increase in methanol selectivity.
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