Influence of Oxygen Dopants on the HER Catalytic Activity of Electrodeposited MoOxSyElectrocatalysts

Lee Kendall, Amir Chamaani, Zachary Piontkowski, Thomas E. Beechem, Mackenzie Ridley, Elizabeth J. Opila, Giovanni Zangari, Stephen J. McDonnell

Research output: Contribution to journalArticlepeer-review

6 Scopus citations

Abstract

Amorphous, polymeric molybdenum sulfide has attracted significant attention as a non-platinum group electrocatalyst for the hydrogen evolution reaction (HER). To elucidate the influence of oxygen incorporation on molybdenum sulfide catalysts, MoOxSy electrocatalysts were synthesized via a potentiostatic electrodeposition method. The presence of oxygen and the associated molybdenum oxidation state were modified by postsynthesis treatments of air exposure, annealing in an inert atmosphere, and annealing in a sulfur flux. The as deposited sample exhibited the best performance, requiring only 171 mV to reach a cathodic current density of 10 mA/cm2. While the modified films exhibited worse HER performance compared to the as deposited sample, by utilizing extensive X-ray photoelectron spectroscopy studies, we highlighted the importance of the Mo5+ oxidation state while identifying a previously unreported state within MoOxSy catalysts between Mo4+ and Mo5+.

Original languageEnglish
Pages (from-to)13676-13683
Number of pages8
JournalACS Applied Energy Materials
Volume4
Issue number12
DOIs
StatePublished - Dec 27 2021
Externally publishedYes

Funding

This work was supported by the University of Virginia’s Nanoscale Materials Characterization Facility and was partially funded by the Virginia Space Grant Consortium Graduate Research STEM Fellowship. Raman interpretation was aided by the Center for Integrated Nanotechnologies at Sandia National Laboratory. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology & Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International, Inc., for the U.S. DOE’s National Nuclear Security Administration under contract DE-NA-0003525. The views expressed in the article do not necessarily represent the views of the U.S. DOE or the United States Government.

FundersFunder number
U.S. Department of Energy
Virginia Space Grant Consortium
National Nuclear Security AdministrationDE-NA-0003525
University of Virginia

    Keywords

    • MoS
    • Raman spectroscopy
    • X-ray photoelectron spectroscopy
    • catalysis
    • electrodeposition
    • water splitting

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