Journal
ACS CATALYSIS
Volume 11, Issue 8, Pages 4730-4738Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c04826
Keywords
photothermal catalysis; dry reforming of methane; Ni/Ga2O3; nonthermal effect; H-2/CO ratio
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Funding
- Sichuan Provincial International Cooperation Project [2019YFH0164]
- Chengdu International Cooperation Project [2019-GH02-00056-HZ]
- National Natural Science Foundation of China [U1862111]
- JSPS Invitational Fellowships for Research in Japan
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-76SF00515]
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This study successfully manipulated the reaction paths by using light irradiation during photothermal dry reforming, promoting H-2 formation and suppressing the reverse water gas shift reaction. The increase in H-2/CO ratio from 0.55 to 0.94 was achieved through this method.
Photothermal catalysis, which couples both solar and thermal energies, has burgeoned as a promising approach to drive catalytic reactions. However, the utilization of light irradiation to tune the reaction paths to obtain ideal product distribution in photothermal catalysis is still of tremendous challenge. Herein, we successfully regulated the relationship between two core competition reactions through light irradiation during photothermal dry reforming of methane over Ni/Ga2O3, resulting in the promotion of H-2 formation and the suppression of the reverse water gas shift reaction. The increase in the H-2/CO ratio from 0.55 to 0.94 could be achieved. Furthermore, the combination of density functional calculations and X-ray photoelectron spectroscopy reveals that light irradiation impelled the direction of electron transfer to be reversed from Ga2O3 to Ni to form the Ni-0 sites, which provides the generation of abundant hot electrons from the electronic interband transition of Ni to boost the formation and desorption of H-2. This work promotes the understanding of nonthermal behaviors of light irradiation in light-driven photochemistry, which is significant for designing catalysts with high efficiency and controllable product distribution.
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