期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 122, 期 10, 页码 5430-5442出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.7b11284
关键词
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资金
- Japan Synchrotron Radiation Research Institute (JASRI) [2017A1557]
- Japan Society for the Promotion of Science (JSPS) [15J10157, 16K18293]
- Grants-in-Aid for Scientific Research [16K05742] Funding Source: KAKEN
We prepared Cu/a-ZrO2 (a-ZrO2: amorphous ZrO2), Cu/m-ZrO2 (m-ZrO2: monoclinic ZrO2), Cu/a-ZrO2/KIT-6, and Cu/t-ZrO2/KIT-6 (t-ZrO2: tetragonal ZrO2) by a simple impregnation method and examined the effect of the ZrO2 phase on CO2-to-methanol hydrogenation. We discovered a-ZrO2-containing catalysts with high activity and selectivity in CO2-to-methanol hydrogenation. Next, we focused on Cu species formation on the above-described catalysts. While pure CuO was observed on Cu/m-ZrO2 and Cu/t-ZrO2/KIT-6, copper-zirconium mixed oxide (CuxZryOz), not pure CuO, was formed on Cu/a-ZrO2 and Cu/a-ZrO2/KIT-6, as evidenced by X-ray absorption spectroscopy (XAS) and the powder color. After reducing a-ZrO2-containing catalysts with H-2 at 300 degrees C, we observed highly dispersed Cu nanoparticles in close contact with a-ZrO2 (or CuxZryOz). In addition, methanol vapor sorption revealed that methanol adsorbed more weakly on a-ZrO2 than on m-ZrO2. Therefore, the high dispersion of Cu species and weak adsorption of methanol led to high activity and selectivity in CO2-to-methanol hydrogenation.
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