1. ZnZrOx Nanoparticles Derived from Metal–Organic Frameworks as Superior Catalysts to Boost CO2 Hydrogenation to Methanol.
- Author
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Song, Jialing, Chen, Bin, Bian, Juanjuan, Cai, Yanmei, Ali, Sajid, Cai, Dongren, Zheng, Bingyun, Huang, Jiale, and Zhan, Guowu
- Abstract
ZnZrO
x solid solution is a promising catalyst for the hydrogenation of CO2 to methanol, but precise design of the nanostructure to enhance catalytic performance remains a significant challenge. Herein, a ZnZrOx -based solid solution (ZnZrOx -MD) nanoparticle catalyst with uniform metal dispersion and remarkable CO2 activation ability was developed via calcination of metal–organic frameworks [MOFs, viz., PCN-223-(Zn)] with mixed metal (Zr and Zn) as solid precursors. It was found that the ZnZrOx -MD nanoparticle catalyst outperformed its counterparts prepared using a traditional deposition–precipitation method (ZnZrOx -TD). Furthermore, the effects of the micromorphology and crystal composition on the catalytic performance of ZnZrOx -MD were systematically investigated. Comprehensive characterization results reveal that ZnZrOx -MD contained abundant oxygen vacancies, large specific surface area, and uniform metal dispersion, which collectively contributed to its excellent CO2 hydrogenation performance, resulting in a high methanol selectivity of 77.2% at 320 °C. In situ DRIFTS experiments confirm the mechanism for the CO2 hydrogenation to methanol over the ZnZrOx nanoparticle catalysts involved the initial formation of HCOO* species, followed by subsequent hydrogenation to generate CH3 O* and ultimately produce methanol. Overall, this work highlights the potential benefits of MOFs as thermal decomposition precursors for the fabrication of solid-state catalysts with unique properties. [ABSTRACT FROM AUTHOR]- Published
- 2024
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