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Giuffredi G, Mezzetti A, Perego A, et al. Non-Equilibrium Synthesis of Highly Active Nanostructured, Oxygen-Incorporated Amorphous Molybdenum Sulfide HER Electrocatalyst. Small. 2020;e2004047doi: 10.1002/smll.202004047.
Giuffredi, G., Mezzetti, A., Perego, A., Mazzolini, P., Prato, M., Fumagalli, F., Lin, Y. C., Liu, C., Ivanov, I. N., Belianinov, A., Colombo, M., Divitini, G., Ducati, C., Duscher, G., Puretzky, A. A., Geohegan, D. B., & Di Fonzo, F. (2020). Non-Equilibrium Synthesis of Highly Active Nanostructured, Oxygen-Incorporated Amorphous Molybdenum Sulfide HER Electrocatalyst. Small (Weinheim an der Bergstrasse, Germany), e2004047. https://doi.org/10.1002/smll.202004047
Giuffredi, Giorgio, et al. "Non-Equilibrium Synthesis of Highly Active Nanostructured, Oxygen-Incorporated Amorphous Molybdenum Sulfide HER Electrocatalyst." Small (Weinheim an der Bergstrasse, Germany) vol. (2020): e2004047. doi: https://doi.org/10.1002/smll.202004047
Giuffredi G, Mezzetti A, Perego A, Mazzolini P, Prato M, Fumagalli F, Lin YC, Liu C, Ivanov IN, Belianinov A, Colombo M, Divitini G, Ducati C, Duscher G, Puretzky AA, Geohegan DB, Di Fonzo F. Non-Equilibrium Synthesis of Highly Active Nanostructured, Oxygen-Incorporated Amorphous Molybdenum Sulfide HER Electrocatalyst. Small. 2020 Oct 08;e2004047. doi: 10.1002/smll.202004047. Epub 2020 Oct 08. PMID: 33090682.
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Small. 2020 Oct 08;e2004047. doi: 10.1002/smll.202004047. Epub 2020 Oct 08.

Non-Equilibrium Synthesis of Highly Active Nanostructured, Oxygen-Incorporated Amorphous Molybdenum Sulfide HER Electrocatalyst.

Small (Weinheim an der Bergstrasse, Germany)

Giorgio Giuffredi, Alessandro Mezzetti, Andrea Perego, Piero Mazzolini, Mirko Prato, Francesco Fumagalli, Yu-Chuan Lin, Chenze Liu, Ilia N Ivanov, Alex Belianinov, Massimo Colombo, Giorgio Divitini, Caterina Ducati, Gerd Duscher, Alexander A Puretzky, David B Geohegan, Fabio Di Fonzo

Affiliations

  1. Center for Nano Science and Technology, Istituto Italiano di Tecnologia, Via Pascoli 70/3, Milano, 20133, Italy.
  2. Department of Energy, Politecnico di Milano, Via Lambruschini 4, Milano, 20156, Italy.
  3. Materials Characterization Facility, Istituto Italiano di Tecnologia, Via Morego 30, Genova, 16163, Italy.
  4. Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA.
  5. Department of Material Science and Engineering, University of Tennessee, Knoxville, TN, 37996, USA.
  6. Nanochemistry Department, Istituto Italiano di Tecnologia, Via Morego 30, Genova, 16130, Italy.
  7. Department of Materials Science & Metallurgy, University of Cambridge, 27 Charles Babbage Road, Cambridge, CB3 0FS, UK.

PMID: 33090682 DOI: 10.1002/smll.202004047

Abstract

Molybdenum sulfide emerged as promising hydrogen evolution reaction (HER) electrocatalyst thanks to its high intrinsic activity, however its limited active sites exposure and low conductivity hamper its performance. To address these drawbacks, the non-equilibrium nature of pulsed laser deposition (PLD) is exploited to synthesize self-supported hierarchical nanoarchitectures by gas phase nucleation and sequential attachment of defective molybdenum sulfide clusters. The physics of the process are studied by in situ diagnostics and correlated to the properties of the resulting electrocatalyst. The as-synthesized architectures have a disordered nanocrystalline structure, with nanodomains of bent, defective S-Mo-S layers embedded in an amorphous matrix, with excess sulfur and segregated molybdenum particles. Oxygen incorporation in this structure fosters the creation of amorphous oxide/oxysulfide nanophases with high electrical conductivity, enabling fast electron transfer to the active sites. The combined effect of the nanocrystalline pristine structure and the surface oxidation enhances the performance leading to small overpotentials, very fast kinetics (35.1 mV dec

© 2020 Wiley‐VCH GmbH.

Keywords: a‐MoSx; electrocatalysis; hydrogen evolution reaction; non‐equilibrium synthesis; pulsed laser deposition

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