In recent years, significant breakthroughs have been made in the direct conversion of syngas to high-value chemicals catalyzed by oxides. Understanding the physicochemical process of activation and adsorption of CO, CO2 and H2 on the catalyst surfaces at the atomic level is of great significance for screening and designing more efficient catalysts. Herein, we studied H2 activation and subsequent dehydration over pristine and substitutional ZnO and Cr2O3(001) by 3d transition metal atoms (3d-TMs) by extensive density functional theory (DFT) calculations. We found that the reactivity is directly related to the activity of surface O which could be regulated by the substituted 3d-TMs. Then the adsorption behavior of CO and CO2 on ZnO(10-10) surface at the atomic level under ambient conditions was studied by DFT combined with scanning tunnel microscope (STM). It is found that the lateral interaction between adsorbates would significantly affect the adsorption strength. The surface dipoles originating from CO2 molecules in different adsorption states cause a new ordered (3×1)-CO2 structure under ambient pressure, which contains two chemisorbed and one physisorbed CO2 molecules in a repeating unit. Our study has brought molecular insight into the fundamental chemistry and catalytic properties of ZnO surfaces under realistic reaction conditions.

Molecular insights of syngas adsorption and activation on oxide surfaces

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