期刊
GREEN ENERGY & ENVIRONMENT
卷 7, 期 4, 页码 807-817出版社
KEAI PUBLISHING LTD
DOI: 10.1016/j.gee.2021.05.004
关键词
Carbon dioxide; Hydrogenation; Methanol; Indium oxide; Silver
类别
资金
- National Key Research and Development Program of China [2016YFB0600902]
The feasibility of indium oxide supported silver catalyst for CO2 hydrogenation to methanol was investigated using density functional theoretical (DFT) study and experimental investigation. The study revealed the intense Ag-In2O3 interaction which positively charged the silver species and facilitated the activation and dissociation of carbon dioxide. The experimental study confirmed the high methanol selectivity of the Ag/In2O3 catalyst and demonstrated its potential as an efficient catalyst for CO2 hydrogenation.
Silver catalyst has been extensively investigated for photocatalytic and electrochemical CO2 reduction. However, its high activity for selective hydrogenation of CO2 to methanol has not been confirmed. Here, the feasibility of the indium oxide supported silver catalyst was investigated for CO2 hydrogenation to methanol by the density functional theoretical (DFT) study and then by the experimental investigation. The DFT study shows there exists an intense Ag-In2O3 interaction, which causes silver to be positively charged. The positively charged Ag species changes the electronic structure of the metal, facilitates the formation of the Ag-In2O3 interfacial site for activation and dissociation of carbon dioxide. The promoted CO2 dissociation leads to the enhanced methanol synthesis via the CO hydrogenation route as CO2* -> CO* -> HCO*-> H2CO*-> H3CO*-> H3COH*. The Ag/In2O3 catalyst was then prepared using the deposition-precipitation method. The experimental study confirms the theoretical prediction. The methanol selectivity of CO2 hydrogenation on Ag/In2O3 reaches 100.0% at reaction temperature of 200 degrees C. It remains more than 70.0% between 200 and 275 degrees C. At 300 degrees C and 5 MPa, the methanol selectivity still keeps 58.2% with a CO2 conversion of 13.6% and a space-time yield (STY) of methanol of 0.453 g(methanol) g(cat)(-1)h(-1), which is the highest methanol STY ever reported for silver catalyst. The catalyst characterization confirms the intense Ag-In2O3 interaction as well, which causes high Ag dispersion, increases and stabilizes the oxygen vacancies and creates the active Ag-In2O3 interfacial site for the enhanced CO2 hydrogenation to methanol. (C) 2021 Institute of Process Engineering, Chinese Academy of Sciences. Publishing services by Elsevier B.V. on behalf of KeAi Communications Co., Ltd.
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