Deciphering Local Structural Complexity in Zn/Ga-ZrO2 CO2 Hydrogenation Catalysts.

Davide Salusso, Pierfrancesco Ticali, Dragos Stoian, Sen Wang,Weibin Fan,Sara Morandi, Elisa Borfecchia,Silvia Bordiga

The journal of physical chemistry letters(2024)

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摘要
In the last few decades, massive effort has been expended in heterogeneous catalysis to develop new materials presenting high conversion, selectivity, and stability even under high-temperature and high-pressure conditions. In this context, CO2 hydrogenation is an interesting reaction where the catalyst local structure is strongly related to the development of an active and stable material under hydrothermal conditions at T/P > 300 °C/30 bar. In order to clarify the relationship between catalyst local ordering and its activity/stability, we herein report a combined laboratory and synchrotron investigation of aliovalent element (Ce/Zn/Ga)-containing ZrO2 matrixes. The results reveal the influence of similar average structures with different short-range orderings on the catalyst properties. Moreover, a further step toward the comprehension of the oxygen vacancy formation mechanism in Ce- and Ga-ZrO2 catalysts is reported. Finally, the reported results illustrate a robust method to guide local structure determination and ultimately help to avoid overuse of the "solid solution" definition.
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