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Title: Universal dependence of hydrogen oxidation and evolution reaction activity of platinum-group metals on pH and hydrogen binding energy

Abstract

An understanding how pH affects the activity of hydrogen oxidation reaction (HOR) and hydrogen evolution reaction (HER) is key to developing active, stable, and affordable HOR/HER catalysts for hydroxide exchange membrane fuel cells and electrolyzers. A common linear correlation between hydrogen binding energy (HBE) and pH is observed for four supported platinum-group metal catalysts (Pt/C, Ir/C, Pd/C, and Rh/C) over a broad pH range (0 to 13), suggesting that the pH dependence of HBE is metal-independent. A universal correlation between exchange current density and HBE is also observed on the four metals, indicating that they may share the same elementary steps and rate-determining steps and that the HBE is the dominant descriptor for HOR/HER activities. The onset potential of CO stripping on the four metals decreases with pH, indicating a stronger OH adsorption, which provides evidence against the promoting effect of adsorbed OH on HOR/HER.

Authors:
 [1];  [2];  [1];  [1];  [1]
  1. Univ. of Delaware, Newark, DE (United States). Dept. of Chemical and Biomolecular Engineering and Center for Catalytic Science and Technology
  2. Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering
Publication Date:
Research Org.:
Univ. of Delaware, Newark, DE (United States)
Sponsoring Org.:
USDOE Advanced Research Projects Agency - Energy (ARPA-E)
OSTI Identifier:
1466569
Grant/Contract Number:  
AR0000009
Resource Type:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 2; Journal Issue: 3; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; Hydrogen oxidation and evolution reaction; electrocatalysis; Pt-group metals; hydrogen binding energy

Citation Formats

Zheng, Jie, Sheng, Wenchao, Zhuang, Zhongbin, Xu, Bingjun, and Yan, Yushan. Universal dependence of hydrogen oxidation and evolution reaction activity of platinum-group metals on pH and hydrogen binding energy. United States: N. p., 2016. Web. doi:10.1126/sciadv.1501602.
Zheng, Jie, Sheng, Wenchao, Zhuang, Zhongbin, Xu, Bingjun, & Yan, Yushan. Universal dependence of hydrogen oxidation and evolution reaction activity of platinum-group metals on pH and hydrogen binding energy. United States. https://doi.org/10.1126/sciadv.1501602
Zheng, Jie, Sheng, Wenchao, Zhuang, Zhongbin, Xu, Bingjun, and Yan, Yushan. Fri . "Universal dependence of hydrogen oxidation and evolution reaction activity of platinum-group metals on pH and hydrogen binding energy". United States. https://doi.org/10.1126/sciadv.1501602. https://www.osti.gov/servlets/purl/1466569.
@article{osti_1466569,
title = {Universal dependence of hydrogen oxidation and evolution reaction activity of platinum-group metals on pH and hydrogen binding energy},
author = {Zheng, Jie and Sheng, Wenchao and Zhuang, Zhongbin and Xu, Bingjun and Yan, Yushan},
abstractNote = {An understanding how pH affects the activity of hydrogen oxidation reaction (HOR) and hydrogen evolution reaction (HER) is key to developing active, stable, and affordable HOR/HER catalysts for hydroxide exchange membrane fuel cells and electrolyzers. A common linear correlation between hydrogen binding energy (HBE) and pH is observed for four supported platinum-group metal catalysts (Pt/C, Ir/C, Pd/C, and Rh/C) over a broad pH range (0 to 13), suggesting that the pH dependence of HBE is metal-independent. A universal correlation between exchange current density and HBE is also observed on the four metals, indicating that they may share the same elementary steps and rate-determining steps and that the HBE is the dominant descriptor for HOR/HER activities. The onset potential of CO stripping on the four metals decreases with pH, indicating a stronger OH adsorption, which provides evidence against the promoting effect of adsorbed OH on HOR/HER.},
doi = {10.1126/sciadv.1501602},
journal = {Science Advances},
number = 3,
volume = 2,
place = {United States},
year = {Fri Mar 18 00:00:00 EDT 2016},
month = {Fri Mar 18 00:00:00 EDT 2016}
}

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Mechanistic Study of the Hydrogen Oxidation/Evolution Reaction over Bimetallic PtRu Catalysts
journal, January 2018

  • Nash, Jared; Zheng, Jie; Wang, Yan
  • Journal of The Electrochemical Society, Vol. 165, Issue 15
  • DOI: 10.1149/2.051181jes

Hydrogen Oxidation on Ni-Based Electrocatalysts: The Effect of Metal Doping
journal, October 2018

  • Davydova, Elena; Zaffran, Jérémie; Dhaka, Kapil
  • Catalysts, Vol. 8, Issue 10
  • DOI: 10.3390/catal8100454

Surface Modulation of Hierarchical MoS 2 Nanosheets by Ni Single Atoms for Enhanced Electrocatalytic Hydrogen Evolution
journal, October 2018

  • Zhang, Huabin; Yu, Le; Chen, Tao
  • Advanced Functional Materials, Vol. 28, Issue 51
  • DOI: 10.1002/adfm.201807086

Experimental Proof of the Bifunctional Mechanism for the Hydrogen Oxidation in Alkaline Media
journal, November 2017

  • Li, Jingkun; Ghoshal, Shraboni; Bates, Michael K.
  • Angewandte Chemie, Vol. 129, Issue 49
  • DOI: 10.1002/ange.201708484

Cover Picture: Hydroxide Is Not a Promoter of C 2+ Product Formation in the Electrochemical Reduction of CO on Copper (Angew. Chem. Int. Ed. 11/2020)
journal, January 2020

  • Li, Jing; Wu, Donghuan; Malkani, Arnav S.
  • Angewandte Chemie International Edition, Vol. 59, Issue 11
  • DOI: 10.1002/anie.202000873

Catalytic Surface Specificity of Ni(OH) 2 ‐Decorated Pt Nanocubes for the Hydrogen Evolution Reaction in an Alkaline Electrolyte
journal, August 2019

  • Hong, Youngmin; Choi, Chang Hyuck; Choi, Sang‐Il
  • ChemSusChem, Vol. 12, Issue 17
  • DOI: 10.1002/cssc.201901539

Facile synthesis of Pd@Ru nanoplates with controlled thickness as efficient catalysts for hydrogen evolution reaction
journal, January 2018

  • Han, Yu; Yan, Yucong; Wu, Zhemin
  • CrystEngComm, Vol. 20, Issue 30
  • DOI: 10.1039/c8ce00549d

The Nature of Hydrogen Adsorption on Platinum in the Aqueous Phase
journal, January 2019


Enhanced Electrocatalytic Hydrogen Oxidation on Ni/NiO/C Derived from a Nickel‐Based Metal–Organic Framework
journal, June 2019


Titelbild: Hydroxide Is Not a Promoter of C 2+ Product Formation in the Electrochemical Reduction of CO on Copper (Angew. Chem. 11/2020)
journal, March 2020


Niobium disulphide (NbS$_2$)-based (heterogeneous) electrocatalysts for an efficient hydrogen evolution reaction
text, January 2020


Mediator-Free SECM for Probing the Diffusion Layer pH with Functionalized Gold Ultramicroelectrodes
journal, December 2019


Interfacing nickel nitride and nickel boosts both electrocatalytic hydrogen evolution and oxidation reactions
journal, October 2018


Electrodeposition of Rhodium Nanowires Arrays and Their Morphology-Dependent Hydrogen Evolution Activity
journal, May 2017

  • Zhang, Liqiu; Liu, Lichun; Wang, Hongdan
  • Nanomaterials, Vol. 7, Issue 5
  • DOI: 10.3390/nano7050103