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Title: Alcohol Oxidation at Platinum–Gas and Platinum–Liquid Interfaces: The Effect of Platinum Nanoparticle Size, Water Coadsorption, and Alcohol Concentration

Abstract

Platinum nanoparticles size range from 1 to 8 nm deposited on mesoporous silica MCF-17 catalyzed alcohol oxidations were studied in the gas and liquid phases. Among methanol, ethanol, 2- propanol and 2-butanol reactions, the turnover frequency increased with Pt nanoparticle size for all the alcohols utilized. The activation energies for the oxidations were almost same among all alcohol species, but higher in the gas phase than those in the liquid phase. Water coadsorption poisoned the reaction in the gas phase, while it increased the reaction turnover rates in the liquid phase. Sum frequency generation (SFG) vibrational spectroscopy studies and DFT calculations revealed that the alcohol molecules pack horizontally on the metal surface in low concentrations and stand up in high concentrations, which affect the dissociation of β-hydrogen of the alcohols as the critical step in alcohol oxidations.

Authors:
ORCiD logo [1];  [1];  [1];  [2]; ORCiD logo [1];  [2]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1393219
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 121; Journal Issue: 13; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Tatsumi, Hironori, Liu, Fudong, Han, Hui-Ling, Carl, Lindsay M., Sapi, Andras, and Somorjai, Gabor A. Alcohol Oxidation at Platinum–Gas and Platinum–Liquid Interfaces: The Effect of Platinum Nanoparticle Size, Water Coadsorption, and Alcohol Concentration. United States: N. p., 2017. Web. doi:10.1021/acs.jpcc.7b01432.
Tatsumi, Hironori, Liu, Fudong, Han, Hui-Ling, Carl, Lindsay M., Sapi, Andras, & Somorjai, Gabor A. Alcohol Oxidation at Platinum–Gas and Platinum–Liquid Interfaces: The Effect of Platinum Nanoparticle Size, Water Coadsorption, and Alcohol Concentration. United States. doi:10.1021/acs.jpcc.7b01432.
Tatsumi, Hironori, Liu, Fudong, Han, Hui-Ling, Carl, Lindsay M., Sapi, Andras, and Somorjai, Gabor A. Tue . "Alcohol Oxidation at Platinum–Gas and Platinum–Liquid Interfaces: The Effect of Platinum Nanoparticle Size, Water Coadsorption, and Alcohol Concentration". United States. doi:10.1021/acs.jpcc.7b01432. https://www.osti.gov/servlets/purl/1393219.
@article{osti_1393219,
title = {Alcohol Oxidation at Platinum–Gas and Platinum–Liquid Interfaces: The Effect of Platinum Nanoparticle Size, Water Coadsorption, and Alcohol Concentration},
author = {Tatsumi, Hironori and Liu, Fudong and Han, Hui-Ling and Carl, Lindsay M. and Sapi, Andras and Somorjai, Gabor A.},
abstractNote = {Platinum nanoparticles size range from 1 to 8 nm deposited on mesoporous silica MCF-17 catalyzed alcohol oxidations were studied in the gas and liquid phases. Among methanol, ethanol, 2- propanol and 2-butanol reactions, the turnover frequency increased with Pt nanoparticle size for all the alcohols utilized. The activation energies for the oxidations were almost same among all alcohol species, but higher in the gas phase than those in the liquid phase. Water coadsorption poisoned the reaction in the gas phase, while it increased the reaction turnover rates in the liquid phase. Sum frequency generation (SFG) vibrational spectroscopy studies and DFT calculations revealed that the alcohol molecules pack horizontally on the metal surface in low concentrations and stand up in high concentrations, which affect the dissociation of β-hydrogen of the alcohols as the critical step in alcohol oxidations.},
doi = {10.1021/acs.jpcc.7b01432},
journal = {Journal of Physical Chemistry. C},
number = 13,
volume = 121,
place = {United States},
year = {Tue Mar 21 00:00:00 EDT 2017},
month = {Tue Mar 21 00:00:00 EDT 2017}
}

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