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

Daniel Escalera-López (), Christian Iffelsberger, Matej Zlatar, Katarina Novčić, Nik Maselj, Chuyen Pham, Primož Jovanovič, Nejc Hodnik, Simon Thiele, Martin Pumera and Serhiy Cherevko ()
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Daniel Escalera-López: Forschungszentrum Jülich GmbH
Christian Iffelsberger: Purkiňova 656/123
Matej Zlatar: Forschungszentrum Jülich GmbH
Katarina Novčić: Purkiňova 656/123
Nik Maselj: Hajdrihova 19
Chuyen Pham: Forschungszentrum Jülich GmbH
Primož Jovanovič: Hajdrihova 19
Nejc Hodnik: Hajdrihova 19
Simon Thiele: Forschungszentrum Jülich GmbH
Martin Pumera: Purkiňova 656/123
Serhiy Cherevko: Forschungszentrum Jülich GmbH

Nature Communications, 2024, vol. 15, issue 1, 1-13

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-47524-w

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