The development of new electrocatalysts for the hydrogen evolution reaction (HER) could reduce the dependence on Pt and other rare metals and enable large-scale production of hydrogen with near-zero carbon emissions. Mechanistic insight into the electrocatalytic activity of a material helps to accelerate the development of new electrocatalysts. Alternative electrocatalyst materials such as transition metal oxides and sulfides can undergo insertion reactions that change their properties. Recent reports indicate that the presence of inserted ions can influence the electrocatalytic activity. Here, we utilized a materials chemistry approach to understand the role of proton insertion in the HER activity of the layered tungsten oxide hydrates (WO3·xH2O, x = 1, 2). We synthesized a series of tungsten oxide hydrates along with an octylamine-pillared tungsten oxide (OA–WO3). We used cyclic voltammetry to study the electrochemical reactivity of each material and performed ex situ x-ray diffraction and Raman spectroscopy to understand bulk and surface structural changes during electrochemical cycling. We show an inverse relationship between the degree of proton insertion and HER overpotential in tungsten oxides: the lack of proton insertion leads to a high overpotential for the HER. We discuss three hypotheses for how proton insertion leads to the HER activity in WO3·xH2O: (1) proton insertion changes the electronic band structure of WO3·xH2O, (2) the presence of bulk protons can influence ΔGH,ads at the surface sites, and (3) the inserted protons may participate in the HER mechanism on WO3·xH2O. Overall, this work shows the critical role of proton insertion in enabling the high HER activity in tungsten oxides.
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14 February 2022
Research Article|
February 08 2022
Electrochemical proton insertion modulates the hydrogen evolution reaction on tungsten oxides
Special Collection:
The Chemical Physics of the Electrode-Electrolyte Interface
Michael A. Spencer
;
Michael A. Spencer
Department of Materials Science and Engineering, North Carolina State University
, Raleigh, North Carolina 27695, USA
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Jenelle Fortunato
;
Jenelle Fortunato
Department of Materials Science and Engineering, North Carolina State University
, Raleigh, North Carolina 27695, USA
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Veronica Augustyn
Veronica Augustyn
a)
Department of Materials Science and Engineering, North Carolina State University
, Raleigh, North Carolina 27695, USA
a)Author to whom correspondence should be addressed: [email protected]
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a)Author to whom correspondence should be addressed: [email protected]
Note: This paper is part of the JCP Special Topic on The Chemical Physics of the Electrode–Electrolyte Interface.
J. Chem. Phys. 156, 064704 (2022)
Article history
Received:
December 15 2021
Accepted:
January 23 2022
Citation
Michael A. Spencer, Jenelle Fortunato, Veronica Augustyn; Electrochemical proton insertion modulates the hydrogen evolution reaction on tungsten oxides. J. Chem. Phys. 14 February 2022; 156 (6): 064704. https://doi.org/10.1063/5.0082459
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