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Title: Determination of Hydrogen Oxidation Reaction Mechanism Based on Pt-H ad Energetics in Alkaline Electrolyte

Abstract

The understanding of the sluggish hydrogen oxidation reaction (HOR) kinetics in alkaline electrolyte is crucial for designing high performance electrocatalysts. Here, we report a clear and convincing result on this problem by investigating the relationship between the HOR kinetics and Pt-adsorbate energetics. Using electrochemical analysis for well-modified Pt surfaces with distinct Pt-adsorbate interactions, we establish a clear trend in activity for HOR in alkaline electrolyte, that is, the activity changes in the order Au@Pt < Pt < Pd@Pt < Ru@Pt. A decisive role of Pt-H ad energetics in the HOR kinetics on Pt surfaces is determined, while no favorable effects of Pt-OH ad energetics in the HOR kinetics were found. The nature of strong Pt-H ad interaction for Pt/C catalyst in alkaline electrolyte is revealed by in-situ X-ray absorption near-edge structure (XANES) analysis. These insights play an important role for better understanding the mechanism and structure sensitivity for Pt catalyzed hydrogen oxidation reactions.

Authors:
 [1];  [2]; ORCiD logo [2]; ORCiD logo [3];  [2]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States); Kunming Univ. of Science and Technology (China)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Kunming Univ. of Science and Technology (China)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1485438
Report Number(s):
BNL-209670-2018-JAAM
Journal ID: ISSN 0013-4651
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 165; Journal Issue: 15; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY

Citation Formats

Hu, Jue, Kuttiyiel, Kurian A., Sasaki, Kotaro, Zhang, Chengxu, and Adzic, Radoslav R. Determination of Hydrogen Oxidation Reaction Mechanism Based on Pt-Had Energetics in Alkaline Electrolyte. United States: N. p., 2018. Web. doi:10.1149/2.0471815jes.
Hu, Jue, Kuttiyiel, Kurian A., Sasaki, Kotaro, Zhang, Chengxu, & Adzic, Radoslav R. Determination of Hydrogen Oxidation Reaction Mechanism Based on Pt-Had Energetics in Alkaline Electrolyte. United States. doi:10.1149/2.0471815jes.
Hu, Jue, Kuttiyiel, Kurian A., Sasaki, Kotaro, Zhang, Chengxu, and Adzic, Radoslav R. Tue . "Determination of Hydrogen Oxidation Reaction Mechanism Based on Pt-Had Energetics in Alkaline Electrolyte". United States. doi:10.1149/2.0471815jes. https://www.osti.gov/servlets/purl/1485438.
@article{osti_1485438,
title = {Determination of Hydrogen Oxidation Reaction Mechanism Based on Pt-Had Energetics in Alkaline Electrolyte},
author = {Hu, Jue and Kuttiyiel, Kurian A. and Sasaki, Kotaro and Zhang, Chengxu and Adzic, Radoslav R.},
abstractNote = {The understanding of the sluggish hydrogen oxidation reaction (HOR) kinetics in alkaline electrolyte is crucial for designing high performance electrocatalysts. Here, we report a clear and convincing result on this problem by investigating the relationship between the HOR kinetics and Pt-adsorbate energetics. Using electrochemical analysis for well-modified Pt surfaces with distinct Pt-adsorbate interactions, we establish a clear trend in activity for HOR in alkaline electrolyte, that is, the activity changes in the order Au@Pt < Pt < Pd@Pt < Ru@Pt. A decisive role of Pt-Had energetics in the HOR kinetics on Pt surfaces is determined, while no favorable effects of Pt-OHad energetics in the HOR kinetics were found. The nature of strong Pt-Had interaction for Pt/C catalyst in alkaline electrolyte is revealed by in-situ X-ray absorption near-edge structure (XANES) analysis. These insights play an important role for better understanding the mechanism and structure sensitivity for Pt catalyzed hydrogen oxidation reactions.},
doi = {10.1149/2.0471815jes},
journal = {Journal of the Electrochemical Society},
number = 15,
volume = 165,
place = {United States},
year = {2018},
month = {11}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Figures / Tables:

Figure 1 Figure 1: HOR activities on different Pt core-shell catalysts in alkaline solution. (a) Ohmic loss corrected HOR/HER polarization curves on Pt catalysts in a H2-saturated 0.1 M KOH solution at 2500 rpm with a potential scan rate of 10 mV s–1. Pt loading for Pt/C, Ru@Pt/C, Pd@Pt/C and Au@Pt/C catalystsmore » were 21.9, 19.0, 15.8 and 16.4 μg cm–2, respectively. (b) HOR polarization curves normalized to the limiting current 5 density. The diffusion overpotential curve (grey line) is also shown in (b).« less

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    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.