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 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.
- Authors:
-
- Univ. of Tennessee, Knoxville, TN (United States). Chemical and Biomolecular Engineering
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences
- 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)
- 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. https://doi.org/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. https://doi.org/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 = {Mon Jan 11 00:00:00 EST 2016},
month = {Mon Jan 11 00:00:00 EST 2016}
}
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Works referencing / citing this record:
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