open access

https://hdl.handle.net/2115/95829

High-pressure in situ X-ray absorption fine structure measurements for hydrogenation of CO2 to methanol over Zn-doped ZrO2

英語

2024-10-21

Royal Society of Chemistry

Catalysis science and technology

14(20)

5909-5917

Obtaining insights into the active-site structure of a catalyst during high-pressure and high-temperature catalytic reactions is extremely challenging. In this study, changes in the coordination structure of Zn species in Zn-doped ZrO2 catalysts (Zn/(Zn + Zr) atomic ratio = 9%) during CO2-to-methanol hydrogenation (cell temperature = 400 degrees C, pressure = 9 bars) was investigated using high-pressure in situ X-ray absorption fine structure measurements and density functional theory calculations. The formation of Zn-H species, which are considered the active sites for the reaction, was very limited, with most Zn species existing as [ZnOa] isolated clusters. Additionally, the adsorption of CO2 at the Zr4+ sites near the Zn species induced significant distortions in the coordination structure of the Zn species. This study provides new insights into the catalytic active-site structure.

学術雑誌論文

Accepted Manuscript

2044-4753