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Allotrope-dependent activity-stability relationships of molybdenum sulfide hydrogen evolution electrocatalysts

Author

Listed:
  • Daniel Escalera-López

    (Forschungszentrum Jülich GmbH)

  • Christian Iffelsberger

    (Purkiňova 656/123)

  • Matej Zlatar

    (Forschungszentrum Jülich GmbH
    Egerlandstrasse 3)

  • Katarina Novčić

    (Purkiňova 656/123)

  • Nik Maselj

    (Hajdrihova 19
    Večna pot 113)

  • Chuyen Pham

    (Forschungszentrum Jülich GmbH)

  • Primož Jovanovič

    (Hajdrihova 19
    Večna pot 113)

  • Nejc Hodnik

    (Hajdrihova 19
    Večna pot 113)

  • Simon Thiele

    (Forschungszentrum Jülich GmbH
    Egerlandstrasse 3)

  • Martin Pumera

    (Purkiňova 656/123
    50 Nanyang Drive
    No. 91 Hsueh-Shih Road
    17. listopadu 2172/15)

  • Serhiy Cherevko

    (Forschungszentrum Jülich GmbH)

Abstract

Molybdenum disulfide (MoS2) is widely regarded as a competitive hydrogen evolution reaction (HER) catalyst to replace platinum in proton exchange membrane water electrolysers (PEMWEs). Despite the extensive knowledge of its HER activity, stability insights under HER operation are scarce. This is paramount to ensure long-term operation of Pt-free PEMWEs, and gain full understanding on the electrocatalytically-induced processes responsible for HER active site generation. The latter are highly dependent on the MoS2 allotropic phase, and still under debate. We rigorously assess these by simultaneously monitoring Mo and S dissolution products using a dedicated scanning flow cell coupled with downstream analytics (ICP-MS), besides an electrochemical mass spectrometry setup for volatile species analysis. We observe that MoS2 stability is allotrope-dependent: lamellar-like MoS2 is highly unstable under open circuit conditions, whereas cluster-like amorphous MoS3-x instability is induced by a severe S loss during the HER and undercoordinated Mo site generation. Guidelines to operate non-noble PEMWEs are therefore provided based on the stability number metrics, and an HER mechanism which accounts for Mo and S dissolution pathways is proposed.

Suggested Citation

  • Daniel Escalera-López & Christian Iffelsberger & Matej Zlatar & Katarina Novčić & Nik Maselj & Chuyen Pham & Primož Jovanovič & Nejc Hodnik & Simon Thiele & Martin Pumera & Serhiy Cherevko, 2024. "Allotrope-dependent activity-stability relationships of molybdenum sulfide hydrogen evolution electrocatalysts," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-47524-w
    DOI: 10.1038/s41467-024-47524-w
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    References listed on IDEAS

    as
    1. Julius Knöppel & Maximilian Möckl & Daniel Escalera-López & Kevin Stojanovski & Markus Bierling & Thomas Böhm & Simon Thiele & Matthias Rzepka & Serhiy Cherevko, 2021. "On the limitations in assessing stability of oxygen evolution catalysts using aqueous model electrochemical cells," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    2. Charlie Tsai & Hong Li & Sangwook Park & Joonsuk Park & Hyun Soo Han & Jens K. Nørskov & Xiaolin Zheng & Frank Abild-Pedersen, 2017. "Electrochemical generation of sulfur vacancies in the basal plane of MoS2 for hydrogen evolution," Nature Communications, Nature, vol. 8(1), pages 1-8, April.
    3. Thomas J. P. Hersbach & Alexei I. Yanson & Marc T. M. Koper, 2016. "Anisotropic etching of platinum electrodes at the onset of cathodic corrosion," Nature Communications, Nature, vol. 7(1), pages 1-7, November.
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