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

John, Samuel St.; Atkinson, Robert W.; Roy, Asa; Unocic, Raymond R.; Papandrew, Alexander B.; Zawodzinski, Thomas A.

doi:10.1149/2.1071603jes

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

Journal Article · Mon Jan 11 00:00:00 EST 2016 · Journal of the Electrochemical Society

DOI:https://doi.org/10.1149/2.1071603jes· OSTI ID:1335336

John, Samuel St. ^[1]; Atkinson, Robert W. ^[1]; Roy, Asa ^[1]; Unocic, Raymond R. ^[2]; Papandrew, Alexander B. ^[1]; Zawodzinski, Thomas A. ^[3]

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

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.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-06CH11357; AC05-00OR22725

OSTI ID:: 1335336

Journal Information:: Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Journal Issue: 3 Vol. 163; ISSN 0013-4651

Publisher:: The Electrochemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Origin of Superior HOR/HER Activity of Bimetallic Pt-Ru Catalysts in Alkaline Media Identified via Ru@Pt Core-Shell Nanoparticles Schwämmlein, Jan N.; Stühmeier, Björn M.; Wagenbauer, Klaus Journal of The Electrochemical Society, Vol. 165, Issue 5 https://doi.org/10.1149/2.0791805jes	journal	January 2018
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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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carbonate
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oxygen reduction
platinum
ruthenium

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

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