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Title: Visible and near-infrared photothermal catalyzed hydrogenation of gaseous CO 2 over nanostructured Pd@Nb 2O 5

Abstract

The reverse water gas shift (RWGS) reaction driven by Nb 2O 5 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@Nb 2O 5 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@Nb 2O 5 hybrid catalyst that efficiently hydrogenates CO 2 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 Nb 2O 5 nanorods whereupon adsorbed CO 2 is hydrogenated to CO. Here, this work represents a significant enhancement in our understanding of the underlying mechanism of photothermally driven CO 2 reduction and will help guide the way toward the development of highly efficient catalysts thatmore » exploit the full solar spectrum to convert gas-phase CO 2 to valuable chemicals and fuels.« less

Authors:
 [1];  [1];  [2];  [3];  [1];  [1];  [1];  [1];  [1];  [4];  [5];  [6];  [1];  [1];  [1];  [1]
  1. Univ. of Toronto, Toronto, ON (Canada)
  2. Soochow Univ., Jiangsu (China)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Univ. Complutense de Madrid, Madrid (Spain)
  5. National Univ. of Singapore (Singapore)
  6. American Univ. of Beirut, Beirut (Lebanon)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1329168
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Advanced Science
Additional Journal Information:
Journal Volume: 3; Journal Issue: 10; Journal ID: ISSN 2198-3844
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

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., and Ozin, Geoffrey A. Visible and near-infrared photothermal catalyzed hydrogenation of gaseous CO2 over nanostructured Pd@Nb2O5. United States: N. p., 2016. Web. doi:10.1002/advs.201600189.
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. Visible and near-infrared photothermal catalyzed hydrogenation of gaseous CO2 over nanostructured Pd@Nb2O5. United States. doi:10.1002/advs.201600189.
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., and Ozin, Geoffrey A. Tue . "Visible and near-infrared photothermal catalyzed hydrogenation of gaseous CO2 over nanostructured Pd@Nb2O5". United States. doi:10.1002/advs.201600189. https://www.osti.gov/servlets/purl/1329168.
@article{osti_1329168,
title = {Visible and near-infrared photothermal catalyzed hydrogenation of gaseous CO2 over nanostructured Pd@Nb2O5},
author = {Jia, Jia and O'Brien, Paul G. and He, Le and Qiao, Qiao and Fei, Teng and Reyes, Laura M. and Burrow, Timothy E. and Dong, Yuchan and Liao, Kristine and Varela, Maria and Pennycook, Stephen J. and Hmadeh, Mohamad and Helmy, Amr S. and Kherani, Nazir P. and Perovic, Doug D. and Ozin, Geoffrey A.},
abstractNote = {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.},
doi = {10.1002/advs.201600189},
journal = {Advanced Science},
issn = {2198-3844},
number = 10,
volume = 3,
place = {United States},
year = {2016},
month = {7}
}

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