期刊
ADVANCED SCIENCE
卷 3, 期 10, 页码 -出版社
WILEY
DOI: 10.1002/advs.201600189
关键词
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资金
- Ontario Ministry of Research Innovation (MRI)
- Ministry of Economic Development, Employment and Infrastructure (MEDI)
- Ministry of the Environment and Climate Change
- Connaught Innovation Fund
- Connaught Global Challenge Fund
- Natural Sciences and Engineering Research Council of Canada (NSERC)
- Masri institute fund [102882]
- Kamal A. Shair CRSL Research Fund at the American University of Beirut (AUB) [102847]
- DOE Office of Basic Energy Sciences Materials Sciences and Engineering Division
The reverse water gas shift (RWGS) reaction driven by Nb2O5 nanorod-supported Pd nanocrystals without external heating using visible and near infrared (NIR) light is demonstrated. By measuring the dependence of the RWGS reaction rates on the intensity and spectral power distribution of filtered light incident onto the nanostructured Pd@Nb2O5 catalyst, it is determined that the RWGS reaction is activated photothermally. That is the RWGS reaction is initiated by heat generated from thermalization of charge carriers in the Pd nanocrystals that are excited by interband and intraband absorption of visible and NIR light. Taking advantage of this photothermal effect, a visible and NIR responsive Pd@Nb2O5 hybrid catalyst that efficiently hydrogenates CO2 to CO at an impressive rate as high as 1.8 mmol gcat(-1) h(-1) is developed. The mechanism of this photothermal reaction involves H-2 dissociation on Pd nanocrystals and subsequent spillover of H to the Nb2O5 nanorods whereupon adsorbed CO2 is hydrogenated to CO. This work represents a significant enhancement in our understanding of the underlying mechanism of photothermally driven CO2 reduction and will help guide the way toward the development of highly efficient catalysts that exploit the full solar spectrum to convert gas-phase CO2 to valuable chemicals and fuels.
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