Photoinducing different mechanisms on a co-ni bimetallic alloy in catalytic dry reforming of methane
Abstract
Photothermal catalytic dry reforming of methane (DRM) is a promising process for simultaneous solar energy conversion and fossil fuel upgrading; however, its mechanistic difference from thermocatalysis has not been much investigated. Herein, we report a comprehensive mechanistic investigation of bimetal NiCo/SiO2 in photothermo- and thermocatalytic DRM. Co substitution in Ni/SiO2 poses a suppressing effect on thermocatalysis, while a promotion effect emerges after light irradiation. In situ diffuse reflectance infrared Fourier transform spectroscopy and theoretical simulations reveal that Co substitution thermodynamically inhibits the cleavage of C-H in methane, CO2 dissociation, and CO desorption in thermal catalysis. While energetic hot carriers are evidenced in the NiCo alloy under light irradiation, they directly activate reactant molecules and overcome the thermodynamic barriers to selectively promote the generation of *CHO to CO instead of *C to coke. Thus, NiCo/SiO2 achieves higher photo-to-thermal efficiency and prominent performance in photothermal catalytic DRM. This work unveils the intrinsic photo effects on non-noble bimetallic catalysts in photothermal catalytic DRM for developing robust photothermal DRM catalysts for practical applications.
RAS ID
62001
Document Type
Journal Article
Date of Publication
1-1-2023
Funding Information
scientific and technological innovation project of carbon emission peak and carbon neutrality of Jiangsu Province / National Natural Science Foundation of China / Australian Research Council / ECU Vice-Chancellor's Professional Research Fellowship
School
School of Science
Grant Number
ARC Numbers : DP200103206, DP190103548
Grant Link
http://purl.org/au-research/grants/arc/DP200103206 http://purl.org/au-research/grants/arc/DP190103548
Copyright
subscription content
Publisher
ACS Publications
Recommended Citation
Zhang, J., Xie, K., Jiang, Y., Li, M., Tan, X., Yang, Y., Zhao, X., Wang, L., Wang, Y., Wang, X., Zhu, Y., Chen, H., Wu, M., Sun, H., & Wang, S. (2023). Photoinducing different mechanisms on a co-ni bimetallic alloy in catalytic dry reforming of methane. DOI: https://doi.org/10.1021/acscatal.3c02525
Comments
Zhang, J., Xie, K., Jiang, Y., Li, M., Tan, X., Yang, Y., . . . Wang, S. (2023). Photoinducing different mechanisms on a co-ni bimetallic alloy in catalytic dry reforming of methane. ACS Catalysis, 13(16), 10855-10865. https://doi.org/10.1021/acscatal.3c02525