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Title: The Effect of Carbonate and pH on Hydrogen Oxidation and Oxygen Reduction on Pt-Based Electrocatalysts in Alkaline Media

Abstract

In this paper, we investigated the performance of several carbon-supported Ru xPt y electrocatalysts for their alkaline hydrogen oxidation and oxygen reduction performance in the presence of carbonate and compared their performance with monometallic, carbon-supported Pt. Our results indicate a strong dependence of HOR upon pH for the monometallic Pt catalysts (22 mV/pH) and a weak dependence upon pH for the Ru-containing electrocatalysts (3.7, 2.5, and 4.7 mV/pH on Ru 0.2Pt 0.8, Ru 0.4Pt 0.6, and Ru 0.8Pt 0.2, respectively). These results are consistent with our previous findings that illustrate a change in rds from electron transfer (on monometallic Pt) to dissociative hydrogen adsorption (on Ru xPt y catalysts). Analysis of the kinetic currents to determine the rate-determining step via Tafel slope analysis provides additional data supporting this conclusion. There is no difference in the performance at comparable pH values in the presence or absence of carbonate on monometallic Pt indicating that water/hydroxide is the primary proton acceptor for alkaline HOR in 0.1 M KOH aqueous electrolyte. Finally, we observe no pH or carbonate dependence for the ORR on monometallic Pt.

Authors:
 [1];  [1];  [1];  [2];  [1];  [3]
  1. Univ. of Tennessee, Knoxville, TN (United States). Chemical and Biomolecular Engineering
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences
  3. Univ. of Tennessee, Knoxville, TN (United States). Chemical and Biomolecular Engineering; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1335336
Grant/Contract Number:  
AC05-00OR22725; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 163; Journal Issue: 3; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; alkaline; carbonate; hydrogen oxidation; oxygen reduction; platinum; ruthenium

Citation Formats

John, Samuel St., Atkinson, Robert W., Roy, Asa, Unocic, Raymond R., Papandrew, Alexander B., and Zawodzinski, Thomas A.. The Effect of Carbonate and pH on Hydrogen Oxidation and Oxygen Reduction on Pt-Based Electrocatalysts in Alkaline Media. United States: N. p., 2016. Web. doi:10.1149/2.1071603jes.
John, Samuel St., Atkinson, Robert W., Roy, Asa, Unocic, Raymond R., Papandrew, Alexander B., & Zawodzinski, Thomas A.. The Effect of Carbonate and pH on Hydrogen Oxidation and Oxygen Reduction on Pt-Based Electrocatalysts in Alkaline Media. United States. doi:10.1149/2.1071603jes.
John, Samuel St., Atkinson, Robert W., Roy, Asa, Unocic, Raymond R., Papandrew, Alexander B., and Zawodzinski, Thomas A.. Mon . "The Effect of Carbonate and pH on Hydrogen Oxidation and Oxygen Reduction on Pt-Based Electrocatalysts in Alkaline Media". United States. doi:10.1149/2.1071603jes. https://www.osti.gov/servlets/purl/1335336.
@article{osti_1335336,
title = {The Effect of Carbonate and pH on Hydrogen Oxidation and Oxygen Reduction on Pt-Based Electrocatalysts in Alkaline Media},
author = {John, Samuel St. and Atkinson, Robert W. and Roy, Asa and Unocic, Raymond R. and Papandrew, Alexander B. and Zawodzinski, Thomas A.},
abstractNote = {In this paper, we investigated the performance of several carbon-supported RuxPty electrocatalysts for their alkaline hydrogen oxidation and oxygen reduction performance in the presence of carbonate and compared their performance with monometallic, carbon-supported Pt. Our results indicate a strong dependence of HOR upon pH for the monometallic Pt catalysts (22 mV/pH) and a weak dependence upon pH for the Ru-containing electrocatalysts (3.7, 2.5, and 4.7 mV/pH on Ru0.2Pt0.8, Ru0.4Pt0.6, and Ru0.8Pt0.2, respectively). These results are consistent with our previous findings that illustrate a change in rds from electron transfer (on monometallic Pt) to dissociative hydrogen adsorption (on RuxPty catalysts). Analysis of the kinetic currents to determine the rate-determining step via Tafel slope analysis provides additional data supporting this conclusion. There is no difference in the performance at comparable pH values in the presence or absence of carbonate on monometallic Pt indicating that water/hydroxide is the primary proton acceptor for alkaline HOR in 0.1 M KOH aqueous electrolyte. Finally, we observe no pH or carbonate dependence for the ORR on monometallic Pt.},
doi = {10.1149/2.1071603jes},
journal = {Journal of the Electrochemical Society},
number = 3,
volume = 163,
place = {United States},
year = {2016},
month = {1}
}

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