Atomic Pd-promoted ZnZrOx solid solution catalyst for CO2 hydrogenation to methanol
Lee, Kyungho 1Anjum, Uzma 1Mondelli, Cecilia 2He, Qian 1Furukawa, Shinya 3Perez-Ramirez, Javier 2Kozlov, Sergey M. 1Yan, Ning 1Arajo, Thaylan Pinheiro2
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作者信息
1. Natl Univ Singapore
2. Swiss Fed Inst Technol
3. Hokkaido Univ
折叠
Abstract
The development of efficient CO2 conversion catalysts is a long-lasting desire. Herein, we introduce an atomic Pd-promoted ZnZrOx solid solution catalyst (Pd-ZnZrOx), which shows markedly enhanced rate of methanol production compared to bare ZnZrOx, as well as excellent stability over 100 h on stream. Up to 0.8 at% (i.e. 0.6 wt%), Pd can be atomically dispersed in ZnZrOx, leading to more oxygen vacancies on the mixed oxide that foster methanol production. Kinetic analysis and in situ DRIFTS reveal that hydrogen activation is limited on ZnZrOx, but Pd doping facilitates H-2 dissociation as well as the consequent formation of HCOO*, thus boosting CO2 conversion to methanol. DFT analyses suggest that the presence of atomic Pd enables a more exothermic H2 dissociation, which increases the availability of surface H and facilitates CO2 hydrogenation on adjacent Zn sites, providing rationale on the high activity and robustness of Pd-ZnZrOx in CO2 hydrogenation.
NSTL
Elsevier