Autor: |
Tada, Shohei, Katagiri, Ayaka, Kiyota, Keiko, Honma, Tetsuo, Kamei, Hiromu, Nariyuki, Akane, Uchida, Sayaka, Satokawa, Shigeo |
Zdroj: |
The Journal of Physical Chemistry - Part C; February 2018, Vol. 122 Issue: 10 p5430-5442, 13p |
Abstrakt: |
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 ZrO2phase 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-ZrO2and Cu/t-ZrO2/KIT-6, copper-zirconium mixed oxide (CuxZryOz), not pure CuO, was formed on Cu/a-ZrO2and Cu/a-ZrO2/KIT-6, as evidenced by X-ray absorption spectroscopy (XAS) and the powder color. After reducing a-ZrO2-containing catalysts with H2at 300 °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-ZrO2than 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. |
Databáze: |
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