Journal
JOURNAL OF CO2 UTILIZATION
Volume 41, Issue -, Pages -Publisher
ELSEVIER SCI LTD
DOI: 10.1016/j.jcou.2020.101215
Keywords
Cu-ZnO-ZrO2; Surfactant-assisted co-precipitation; Reaction mechanism; Methanol; CO2 hydrogenation
Funding
- FAPESP [2017/08293-8, 2018/05799-0, 2014/50279-4]
- U.S. Department of Energy (DOE) [DE-SC0012704]
- FAPESP-Shell Brazil through the Research Center for Gas Innovation
- National Council for Scientific and Technological Development -CNPq [304883/2016-6]
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In this study, we evaluated aspects of the CO2 hydrogenation mechanism, correlating structure-activity relationships of Cu-ZnO-ZrO2 catalysts prepared by one-pot surfactant-assisted co-precipitation with different surfactant ratios. Identifying the CO2 hydrogenation pathway intermediates is key to controlling the reaction selectivity. Experimental evidence shows that the CO2 is dissociating into CO* and O* onto the surface of the CuZnO-ZrO2 catalyst. The adsorption and dissociation of CO2 were evidenced by a combination of in situ ambient pressure X-ray Photoelectron Spectroscopy (AP-XPS) and Fourier Transform Infrared Spectroscopy (FTIR) with a transmission cell. AP-XPS showed that the catalysts are composed of a Cu2+, Zr3+, and Zr4+ mixture and two kinds of Zn2+ species. After the H-2 reduction process, only Cu2+ was reduced to Cu-0. The Zn and Zr species were oxidized by the dissociated O* species. In situ transmission FTIR showed that CO was adsorbed onto the Cu+/0 sites. The catalyst with the higher surfactant molar ratio exhibited the highest CO2 conversion close to the equilibrium conversion, as well as a good methanol formation rate.
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