Design of active and stable Co-Mo-Sx chalcogels as pH-universal catalysts for the hydrogen evolution reaction

Jakub Staszak-Jirkovský, Christos D. Malliakas, Pietro P. Lopes, Nemanja Danilovic, Subrahmanyam S. Kota, Kee Chul Chang, Bostjan Genorio, Dusan Strmcnik, Vojislav R. Stamenkovic, Mercouri G Kanatzidis, Nenad M. Markovic

Research output: Contribution to journalArticle

310 Citations (Scopus)

Abstract

Three of the fundamental catalytic limitations that have plagued the electrochemical production of hydrogen for decades still remain: low efficiency, short lifetime of catalysts and a lack of low-cost materials. Here, we address these three challenges by establishing and exploring an intimate functional link between the reactivity and stability of crystalline (CoS2 and MoS2) and amorphous (CoSx and MoSx) hydrogen evolution catalysts. We propose that Co2+ and Mo4+ centres promote the initial discharge of water (alkaline solutions) or hydronium ions (acid solutions). We establish that although CoSx materials are more active than MoSx they are also less stable, suggesting that the active sites are defects formed after dissolution of Co and Mo cations. By combining the higher activity of CoSx building blocks with the higher stability of MoSx units into a compact and robust CoMoSx chalcogel structure, we are able to design a low-cost alternative to noble metal catalysts for efficient electrocatalytic production of hydrogen in both alkaline and acidic environments.

Original languageEnglish
Pages (from-to)197-203
Number of pages7
JournalNature Materials
Volume15
Issue number2
DOIs
Publication statusPublished - Feb 1 2016

Fingerprint

Hydrogen
catalysts
Catalysts
hydrogen
hydronium ions
Precious metals
noble metals
Discharge (fluid mechanics)
Cations
Costs
dissolving
Dissolution
reactivity
Positive ions
Crystalline materials
cations
life (durability)
Defects
acids
Acids

ASJC Scopus subject areas

  • Mechanical Engineering
  • Mechanics of Materials
  • Condensed Matter Physics
  • Materials Science(all)
  • Chemistry(all)

Cite this

Staszak-Jirkovský, J., Malliakas, C. D., Lopes, P. P., Danilovic, N., Kota, S. S., Chang, K. C., ... Markovic, N. M. (2016). Design of active and stable Co-Mo-Sx chalcogels as pH-universal catalysts for the hydrogen evolution reaction. Nature Materials, 15(2), 197-203. https://doi.org/10.1038/nmat4481

Design of active and stable Co-Mo-Sx chalcogels as pH-universal catalysts for the hydrogen evolution reaction. / Staszak-Jirkovský, Jakub; Malliakas, Christos D.; Lopes, Pietro P.; Danilovic, Nemanja; Kota, Subrahmanyam S.; Chang, Kee Chul; Genorio, Bostjan; Strmcnik, Dusan; Stamenkovic, Vojislav R.; Kanatzidis, Mercouri G; Markovic, Nenad M.

In: Nature Materials, Vol. 15, No. 2, 01.02.2016, p. 197-203.

Research output: Contribution to journalArticle

Staszak-Jirkovský, J, Malliakas, CD, Lopes, PP, Danilovic, N, Kota, SS, Chang, KC, Genorio, B, Strmcnik, D, Stamenkovic, VR, Kanatzidis, MG & Markovic, NM 2016, 'Design of active and stable Co-Mo-Sx chalcogels as pH-universal catalysts for the hydrogen evolution reaction', Nature Materials, vol. 15, no. 2, pp. 197-203. https://doi.org/10.1038/nmat4481
Staszak-Jirkovský J, Malliakas CD, Lopes PP, Danilovic N, Kota SS, Chang KC et al. Design of active and stable Co-Mo-Sx chalcogels as pH-universal catalysts for the hydrogen evolution reaction. Nature Materials. 2016 Feb 1;15(2):197-203. https://doi.org/10.1038/nmat4481
Staszak-Jirkovský, Jakub ; Malliakas, Christos D. ; Lopes, Pietro P. ; Danilovic, Nemanja ; Kota, Subrahmanyam S. ; Chang, Kee Chul ; Genorio, Bostjan ; Strmcnik, Dusan ; Stamenkovic, Vojislav R. ; Kanatzidis, Mercouri G ; Markovic, Nenad M. / Design of active and stable Co-Mo-Sx chalcogels as pH-universal catalysts for the hydrogen evolution reaction. In: Nature Materials. 2016 ; Vol. 15, No. 2. pp. 197-203.
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