Metal oxides are widely employed in heterogeneous catalysis, but it remains challenging to determine their exact structure and understand the reaction mechanisms at the molecular level due to their structural complexity, in particular for binary oxides. This paper describes the observation of the strong electronic interaction between InO and monoclinic ZrO (m-ZrO) by XPS experiments combined with theoretical studies, which leads to support-dependent methanol selectivity. InO/m-ZrO exhibits methanol selectivity up to 84.6% with a CO conversion of 12.1%. Moreover, at a wide range of temperatures, the methanol yield of InO/m-ZrO is much higher than that of InO/t-ZrO (t-: tetragonal), which is due to the high dispersion of the In-O-In structure over m-ZrO as determined by Raman spectra. The electron transfer from m-ZrO to InO is confirmed by XPS and DFT calculations and improves the electron density of InO, which promotes H dissociation and hydrogenation of formate intermediates to methanol. The concept of the electronic interaction between an oxide and a support provides guidelines to develop hydrogenation catalysts.
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