Abstract
CO2 hydrogenation to methanol has been extensively studied over Cu-based catalysts. H2O is an inevitable by-product during this reaction process. The essential role of H2O in determining the catalytic performance remains controversial. Herein, three kinds of common Cu-based catalysts (Cu/ZnO, Cu/Al2O3, Cu/SiO2) were selected to investigate the effect of H2O on the reaction performance over the range of 190 °C–290 °C in detail. Of all catalysts tested, it was noted that adding H2O showed substantially different effects on the methanol selectivity compared with the normal reaction. The representative Cu/SiO2 catalyst was further selected to investigate the role of H2O through a series of characterizations including BET, XRD, TEM, H2-TPR and XPS, etc. Moreover, in situ FT-IR experiment was further conducted to understand the effect of H2O on the reaction pathways. The results indicated that H2O played the significant role on regulating the methanol selectivity by inhibiting and promoting the transformation from monodentate carbonate to bidentate formate over all the Cu-based catalysts at low (190–230 °C) and high (230–290 °C) temperature ranges, respectively. This preliminary study offers directions for the optimization of experimental conditions for the H2O involving reactions and provides referable experience for the further exploration and utilization of H2O effects on related fields as well.
Graphical Abstract
The addition of H2O shows a significant characteristic effect on methanol selectivity by inhibiting and promoting the conversion of monodentate carbonate to bidentate formate at low (190–230 ℃) and high (230–290 ℃) temperatures ranges, respectively.
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Acknowledgements
This work is supported by the National Natural Science Foundation of China (Grant No. 21676176), the Foundation of State Key Laboratory of Coal Conversion (Grant No. J20-21-610), the Natural Science Foundation of Shanxi Province, China (Grant No. 201601D011016), Graduate Innovation Program of Shanxi Province, China (Grant No. 2021Y180 and Grant No. 2021Y249 ) and the fund of State Key Laboratory of Catalysis in DICP, China (Grant No. N-15-05).
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Yan, Z., Wang, Y., Wang, X. et al. Unraveling the Role of H2O on Cu-Based Catalyst in CO2 Hydrogenation to Methanol. Catal Lett 153, 1046–1056 (2023). https://doi.org/10.1007/s10562-022-04047-7
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DOI: https://doi.org/10.1007/s10562-022-04047-7