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Title: Low pressure CO₂ hydrogenation to methanol over gold nanoparticles activated on a CeO x/TiO₂ interface

Capture and recycling of CO 2 into valuable chemicals such as alcohols could help mitigate its emissions into the atmosphere. Due to its inert nature, the activation of CO 2 is a critical step in improving the overall reaction kinetics during its chemical conversion. Although pure gold is an inert noble metal and cannot catalyze hydrogenation reactions, it can be activated when deposited as nanoparticles on the appropriate oxide support. In this combined experimental and theoretical study, it is shown that an electronic polarization at the metal-oxide interface of Au nanoparticles anchored and stabilized on a CeO x/TiO 2 substrate generates active centers for CO 2 adsorption and its low pressure hydrogenation, leading to a higher selectivity towards methanol. As a result, this study illustrates the importance of localized electronic properties and structure in catalysis for achieving higher alcohol selectivity from CO 2 hydrogenation.
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [2] ;  [3] ;  [1] ;  [1] ;  [1] ;  [4]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Dalian Univ. of Technology, Liaoning Province (China)
  3. Univ. of Seville, Seville (Spain)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States); Columbia Univ., New York, NY (United States)
Publication Date:
Report Number(s):
BNL-108284-2015-JA; BNL-108338-2015-JA
Journal ID: ISSN 0002-7863; R&D Project: 16083; KC0403020
Grant/Contract Number:
SC00112704
Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 137; Journal Issue: 32; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1213389
Alternate Identifier(s):
OSTI ID: 1214528

Yang, Xiaofang, Boscoboinik, J. Anibal, Kattel, Shyam, Senanayake, Sanjaya D., Nie, Xiaowa, Graciani, Jesus, Rodriguez, Jose A., Liu, Ping, Stacchiola, Dario J., and Chen, Jingguang G.. Low pressure CO₂ hydrogenation to methanol over gold nanoparticles activated on a CeOx/TiO₂ interface. United States: N. p., Web. doi:10.1021/jacs.5b06150.
Yang, Xiaofang, Boscoboinik, J. Anibal, Kattel, Shyam, Senanayake, Sanjaya D., Nie, Xiaowa, Graciani, Jesus, Rodriguez, Jose A., Liu, Ping, Stacchiola, Dario J., & Chen, Jingguang G.. Low pressure CO₂ hydrogenation to methanol over gold nanoparticles activated on a CeOx/TiO₂ interface. United States. doi:10.1021/jacs.5b06150.
Yang, Xiaofang, Boscoboinik, J. Anibal, Kattel, Shyam, Senanayake, Sanjaya D., Nie, Xiaowa, Graciani, Jesus, Rodriguez, Jose A., Liu, Ping, Stacchiola, Dario J., and Chen, Jingguang G.. 2015. "Low pressure CO₂ hydrogenation to methanol over gold nanoparticles activated on a CeOx/TiO₂ interface". United States. doi:10.1021/jacs.5b06150. https://www.osti.gov/servlets/purl/1213389.
@article{osti_1213389,
title = {Low pressure CO₂ hydrogenation to methanol over gold nanoparticles activated on a CeOx/TiO₂ interface},
author = {Yang, Xiaofang and Boscoboinik, J. Anibal and Kattel, Shyam and Senanayake, Sanjaya D. and Nie, Xiaowa and Graciani, Jesus and Rodriguez, Jose A. and Liu, Ping and Stacchiola, Dario J. and Chen, Jingguang G.},
abstractNote = {Capture and recycling of CO2 into valuable chemicals such as alcohols could help mitigate its emissions into the atmosphere. Due to its inert nature, the activation of CO2 is a critical step in improving the overall reaction kinetics during its chemical conversion. Although pure gold is an inert noble metal and cannot catalyze hydrogenation reactions, it can be activated when deposited as nanoparticles on the appropriate oxide support. In this combined experimental and theoretical study, it is shown that an electronic polarization at the metal-oxide interface of Au nanoparticles anchored and stabilized on a CeOx/TiO2 substrate generates active centers for CO2 adsorption and its low pressure hydrogenation, leading to a higher selectivity towards methanol. As a result, this study illustrates the importance of localized electronic properties and structure in catalysis for achieving higher alcohol selectivity from CO2 hydrogenation.},
doi = {10.1021/jacs.5b06150},
journal = {Journal of the American Chemical Society},
number = 32,
volume = 137,
place = {United States},
year = {2015},
month = {7}
}