Visible and near-infrared photothermal catalyzed hydrogenation of gaseous CO2 over nanostructured Pd@Nb2O5

Jia, Jia; O'Brien, Paul G.; He, Le; Qiao, Qiao; Fei, Teng; Reyes, Laura M.; Burrow, Timothy E.; Dong, Yuchan; Liao, Kristine; Varela, Maria; Pennycook, Stephen J.; Hmadeh, Mohamad; Helmy, Amr S.; Kherani, Nazir P.; Perovic, Doug D.; Ozin, Geoffrey A.

doi:10.1002/advs.201600189

Title: Visible and near-infrared photothermal catalyzed hydrogenation of gaseous CO₂ over nanostructured Pd@Nb₂O₅

Journal Article · 05 July 2016 · Advanced Science

DOI: https://doi.org/10.1002/advs.201600189 · OSTI ID:1329168

Jia, Jia ^[1]; O'Brien, Paul G. ^[1]; He, Le ^[2]; Qiao, Qiao ^[3]; Fei, Teng ^[1]; Reyes, Laura M. ^[1]; Burrow, Timothy E. ^[1]; Dong, Yuchan ^[1]; Liao, Kristine ^[1]; Varela, Maria ^[4]; Pennycook, Stephen J. ^[5]; Hmadeh, Mohamad ^[6]; Helmy, Amr S. ^[1]; Kherani, Nazir P. ^[1]; Perovic, Doug D. ^[1]; Ozin, Geoffrey A. ^[1]

Univ. of Toronto, Toronto, ON (Canada)
Soochow Univ., Jiangsu (China)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. Complutense de Madrid, Madrid (Spain)
National Univ. of Singapore (Singapore)
American Univ. of Beirut, Beirut (Lebanon)

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 H₂ dissociation on Pd nanocrystals and subsequent spillover of H to the Nb₂O₅ nanorods whereupon adsorbed CO₂ is hydrogenated to CO. Here, 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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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1329168

Journal Information:: Advanced Science, Vol. 3, Issue 10; ISSN 2198-3844

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 113 works

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Title: Visible and near-infrared photothermal catalyzed hydrogenation of gaseous CO2 over nanostructured Pd@Nb2O5

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Title: Visible and near-infrared photothermal catalyzed hydrogenation of gaseous CO₂ over nanostructured Pd@Nb₂O₅