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

Journal Article · · Science Advances
 [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

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.

Research Organization:
Univ. of Delaware, Newark, DE (United States)
Sponsoring Organization:
USDOE Advanced Research Projects Agency - Energy (ARPA-E)
Grant/Contract Number:
AR0000009
OSTI ID:
1466569
Journal Information:
Science Advances, Vol. 2, Issue 3; ISSN 2375-2548
Publisher:
AAASCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 518 works
Citation information provided by
Web of Science

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A Roadmap to Low‐Cost Hydrogen with Hydroxide Exchange Membrane Electrolyzers journal December 2018
Recommended Practices and Benchmark Activity for Hydrogen and Oxygen Electrocatalysis in Water Splitting and Fuel Cells journal December 2018
Hydrogen Evolution and Oxidation: Mechanistic Studies and Material Advances journal December 2018
Structural‐Phase Catalytic Redox Reactions in Energy and Environmental Applications journal January 2020
Print-Light-Synthesis of Platinum Nanostructured Indium-Tin-Oxide Electrodes for Energy Research journal December 2017
The Effect of Residual Palladium Catalyst Contamination on the Photocatalytic Hydrogen Evolution Activity of Conjugated Polymers journal October 2018
Benchmarking the Activity, Stability, and Inherent Electrochemistry of Amorphous Molybdenum Sulfide for Hydrogen Production journal January 2019
3D Carbon Materials for Efficient Oxygen and Hydrogen Electrocatalysis journal November 2019
Ni 3 N as an Active Hydrogen Oxidation Reaction Catalyst in Alkaline Medium journal April 2019
Understanding the pH Dependence of Underpotential Deposited Hydrogen on Platinum journal October 2019
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Experimental Proof of the Bifunctional Mechanism for the Hydrogen Oxidation in Alkaline Media journal November 2017
The Hydrogen Evolution Reaction in Alkaline Solution: From Theory, Single Crystal Models, to Practical Electrocatalysts journal May 2018
The Nature of Hydrogen Adsorption on Platinum in the Aqueous Phase journal January 2019
Ni 3 N as an Active Hydrogen Oxidation Reaction Catalyst in Alkaline Medium journal May 2019
Enhanced Electrocatalytic Hydrogen Oxidation on Ni/NiO/C Derived from a Nickel-Based Metal-Organic Framework journal June 2019
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Co‐Mo‐P Based Electrocatalyst for Superior Reactivity in the Alkaline Hydrogen Evolution Reaction journal October 2018
Rhodium Phosphide: A New Type of Hydrogen Oxidation Reaction Catalyst with Non‐Linear Correlated Catalytic Response to pH journal March 2019
Recent Progress in Bifunctional Electrocatalysts for Overall Water Splitting under Acidic Conditions journal May 2019
The Effect of Ambient Carbon Dioxide on Anion-Exchange Membrane Fuel Cells journal March 2018
Facile electrochemical preparation of nonprecious Co‐Cu alloy catalysts for hydrogen production in proton exchange membrane water electrolysis journal December 2019
Ir‐Based Alloy Nanoflowers with Optimized Hydrogen Binding Energy as Bifunctional Electrocatalysts for Overall Water Splitting journal April 2019
Electrocatalysts for hydrogen oxidation and evolution reactions journal March 2016
The Hydrogen Oxidation Reaction in Alkaline Medium: An Overview journal March 2019
Interfacing nickel nitride and nickel boosts both electrocatalytic hydrogen evolution and oxidation reactions journal October 2018
Anomalous hydrogen evolution behavior in high-pH environment induced by locally generated hydronium ions journal October 2019
Identification of pH-dependent synergy on Ru/MoS 2 interface: a comparison of alkaline and acidic hydrogen evolution journal January 2017
Bronze alloys with tin surface sites for selective electrochemical reduction of CO 2 journal January 2018
Recent advances in metal sulfides: from controlled fabrication to electrocatalytic, photocatalytic and photoelectrochemical water splitting and beyond journal January 2019
CoO x (OH) y /C nanocomposites in situ derived from Na 4 Co 3 (PO 4 ) 2 P 2 O 7 as sustainable electrocatalysts for water splitting journal January 2018
Tuning the electrocatalytic activity of Pt by structurally ordered PdFe/C for the hydrogen oxidation reaction in alkaline media journal January 2018
Surface modification of Pt nanoparticles with other metals boosting the alkaline hydrogen oxidation reaction journal January 2019
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Breaking the volcano-plot limits for Pt-based electrocatalysts by selective tuning adsorption of multiple intermediates journal January 2019
Carbon vacancy defect-activated Pt cluster for hydrogen generation journal January 2019
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Hierarchical nanoporous intermetallic compounds with self-grown transition-metal hydroxides as bifunctional catalysts for the alkaline hydrogen evolution reaction journal January 2019
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Surface Modulation of Hierarchical MoS 2 Nanosheets by Ni Single Atoms for Enhanced Electrocatalytic Hydrogen Evolution journal October 2018
Experimental Proof of the Bifunctional Mechanism for the Hydrogen Oxidation in Alkaline Media journal November 2017
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
Catalytic Surface Specificity of Ni(OH) 2 ‐Decorated Pt Nanocubes for the Hydrogen Evolution Reaction in an Alkaline Electrolyte journal August 2019
Facile synthesis of Pd@Ru nanoplates with controlled thickness as efficient catalysts for hydrogen evolution reaction journal January 2018
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
Electrodeposition of Rhodium Nanowires Arrays and Their Morphology-Dependent Hydrogen Evolution Activity journal May 2017