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Title: Correlating the chemical composition and size of various metal oxide substrates with the catalytic activity and stability of as-deposited Pt nanoparticles for the methanol oxidation reaction

Abstract

The performance of electrode materials in conventional direct alcohol fuel cells (DAFC) is constrained by (i) the low activity of the catalyst materials relative to their overall cost, (ii) the poisoning of the active sites due to the presence of partially oxidized carbon species (such as but not limited to CO, formate, and acetate) produced during small molecule oxidation, and (iii) the lack of catalytic stability and durability on the underlying commercial carbon support. Therefore, as a viable alternative, we have synthesized various metal oxide and perovskite materials of different sizes and chemical compositions as supports for Pt nanoparticles (NPs). Our results including unique mechanistic studies demonstrate that the SrRuO3 substrate with immobilized Pt NPs at its surface evinces the best methanol oxidation performance as compared with all of the other substrate materials tested herein, including commercial carbon itself. In addition, data from electron energy loss spectroscopy (EELS) and X-ray photoelectron spectroscopy (XPS) confirmed the presence of electron transfer from bound Pt NPs to surface Ru species within the SrRuO3 substrate itself, thereby suggesting that favorable metal support interactions are responsible for the increased methanol oxidation reaction (MOR) activity of Pt species with respect to the underlying SrRuO3 composite catalystmore » material.« less

Authors:
;  [1];  [2];  [2];  [3];  [3];  [2];  [2];  [3];  [3];  [3]
  1. State Univ. of New York at Stony Brook, Stony Brook, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. State Univ. of New York at Stony Brook, Stony Brook, NY (United States)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1235858
Report Number(s):
BNL-111608-2015-JA
Journal ID: ISSN 2044-4753; CSTAGD; R&D Project: PM037; KC0201030
Grant/Contract Number:  
SC00112704
Resource Type:
Accepted Manuscript
Journal Name:
Catalysis Science and Technology
Additional Journal Information:
Journal Volume: 137; Journal Issue: 48; Journal ID: ISSN 2044-4753
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; perovskite; electrocatalysis; catalyst supports; direct methanol fuel cell; platinum deposition; electron energy loss spectroscopy

Citation Formats

Megan E. Scofield, Wong, Stanislaus S., Koenigsmann, Christopher, Bobb-Semple, Dara, Tao, Jing, Tong, Xiao, Wang, Lei, Lewis, Crystal S., Vuklmirovic, Miomir, Zhu, Yimei, and Adzic, Radoslav R. Correlating the chemical composition and size of various metal oxide substrates with the catalytic activity and stability of as-deposited Pt nanoparticles for the methanol oxidation reaction. United States: N. p., 2015. Web. doi:10.1039/C5CY01444A.
Megan E. Scofield, Wong, Stanislaus S., Koenigsmann, Christopher, Bobb-Semple, Dara, Tao, Jing, Tong, Xiao, Wang, Lei, Lewis, Crystal S., Vuklmirovic, Miomir, Zhu, Yimei, & Adzic, Radoslav R. Correlating the chemical composition and size of various metal oxide substrates with the catalytic activity and stability of as-deposited Pt nanoparticles for the methanol oxidation reaction. United States. https://doi.org/10.1039/C5CY01444A
Megan E. Scofield, Wong, Stanislaus S., Koenigsmann, Christopher, Bobb-Semple, Dara, Tao, Jing, Tong, Xiao, Wang, Lei, Lewis, Crystal S., Vuklmirovic, Miomir, Zhu, Yimei, and Adzic, Radoslav R. Wed . "Correlating the chemical composition and size of various metal oxide substrates with the catalytic activity and stability of as-deposited Pt nanoparticles for the methanol oxidation reaction". United States. https://doi.org/10.1039/C5CY01444A. https://www.osti.gov/servlets/purl/1235858.
@article{osti_1235858,
title = {Correlating the chemical composition and size of various metal oxide substrates with the catalytic activity and stability of as-deposited Pt nanoparticles for the methanol oxidation reaction},
author = {Megan E. Scofield and Wong, Stanislaus S. and Koenigsmann, Christopher and Bobb-Semple, Dara and Tao, Jing and Tong, Xiao and Wang, Lei and Lewis, Crystal S. and Vuklmirovic, Miomir and Zhu, Yimei and Adzic, Radoslav R.},
abstractNote = {The performance of electrode materials in conventional direct alcohol fuel cells (DAFC) is constrained by (i) the low activity of the catalyst materials relative to their overall cost, (ii) the poisoning of the active sites due to the presence of partially oxidized carbon species (such as but not limited to CO, formate, and acetate) produced during small molecule oxidation, and (iii) the lack of catalytic stability and durability on the underlying commercial carbon support. Therefore, as a viable alternative, we have synthesized various metal oxide and perovskite materials of different sizes and chemical compositions as supports for Pt nanoparticles (NPs). Our results including unique mechanistic studies demonstrate that the SrRuO3 substrate with immobilized Pt NPs at its surface evinces the best methanol oxidation performance as compared with all of the other substrate materials tested herein, including commercial carbon itself. In addition, data from electron energy loss spectroscopy (EELS) and X-ray photoelectron spectroscopy (XPS) confirmed the presence of electron transfer from bound Pt NPs to surface Ru species within the SrRuO3 substrate itself, thereby suggesting that favorable metal support interactions are responsible for the increased methanol oxidation reaction (MOR) activity of Pt species with respect to the underlying SrRuO3 composite catalyst material.},
doi = {10.1039/C5CY01444A},
journal = {Catalysis Science and Technology},
number = 48,
volume = 137,
place = {United States},
year = {Wed Dec 09 00:00:00 EST 2015},
month = {Wed Dec 09 00:00:00 EST 2015}
}

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