期刊
ACS CATALYSIS
卷 -, 期 -, 页码 7748-7759出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c01996
关键词
CO2 hydrogenation; methanol; zinc; zirconia; solid solution; calculation
资金
- Uncharted Territory Challenge 2050, New Energy and Industrial Technology Development Organization, Japan [19101608-0]
- Japan Society for the Promotion of Science (JSPS) KAKENHI, Japan [21K04988]
- Advanced Characterization Nanotechnology Platform, Nanotechnology Platform Program of the Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan [JPMXP09A21OS0012]
This study investigated the effect of Zn content on the CO2-to-methanol hydrogenation over ZnxZr1-xO2-x catalysts and determined the active-site structure through calculations and experiments. The results showed that Zn species in the catalysts were unevenly distributed and formed clusters and nanoparticles near the surface. The Zn-O-Zr sites derived from the clusters exhibited specific activity for CO2 conversion.
Recently, ZnxZr1-xO2-x catalysts have attracted catalysts. In this study, we examined the effect of the Zn content on CO2-to-methanol hydrogenation over ZnxZr1-xO2-x catalysts and determined the active-site structure through both calculations and experiments. When the Zn content was low, ZnxZr1-xO2-x contained Zn clusters (isolated [ZnOa] clusters and [ZnbOc] oligomers). The presence of clusters indicates the formation of Zn-O-Zr sites. Interestingly, our calculations revealed that the Zn species in the clusters are easily exposed on the ZnxZr1-xO2-x surface. This result is in line with the experimental results, suggesting that Zn species were unevenly distributed on the ZnxZr1-xO2-x surface and deposited near the surface. The addition of excess Zn to ZrO2 led to the formation of both Zn-containing clusters and ZnO nanoparticles. During the reactions, the Zn-O- Zr sites derived from the clusters showed specific activity for CO2-to-methanol hydrogenation. Understanding the active-site structure will lead to the future development of ZnxZr1-xO2-x catalysts.
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