Hydrogen evolution enhancement of ultra-low loading, size-selected molybdenum sulfide nanoclusters by sulfur enrichment

Daniel Escalera-lópez; Yubiao Niu; Sung Jin Park; Mark Isaacs; Karen Wilson; Richard E. Palmer; Neil V. Rees

doi:10.1016/j.apcatb.2018.04.068

Hydrogen evolution enhancement of ultra-low loading, size-selected molybdenum sulfide nanoclusters by sulfur enrichment

Daniel Escalera-lópez, Yubiao Niu, Sung Jin Park, Mark Isaacs, Karen Wilson, Richard E. Palmer, Neil V. Rees

College of Engineering and Physical Sciences

Research output: Contribution to journal › Article › peer-review

Abstract

Size-selected molybdenum sulfide (MoSx) nanoclusters obtained by magnetron sputtering and gas condensation on glassy carbon substrates are typically sulfur-deficient (x = 1.6 ± 0.1), which limits their crystallinity and electrocatalytic properties. Here we demonstrate that a sulfur-enriching method, comprising sulfur evaporation and cluster annealing under vacuum conditions, significantly enhances their activity towards the hydrogen evolution reaction (HER). The S-richness (x = 4.9 ± 0.1) and extended crystalline order obtained in the sulfur-treated MoSx nanoclusters lead to consistent 200 mV shifts to lower HER onset potentials, along with two-fold and more-than 30-fold increases in turnover frequency and exchange current density values respectively. The high mass activities (~111 mA mg-1 @ 400 mV) obtained at ultra-low loadings (~100 ng cm-2, 5 % surface coverage) are comparable to the best reported MoS2 catalysts in the literature.

Original language	English
Pages (from-to)	84-91
Journal	Applied Catalysis B: Environmental
Volume	235
Early online date	27 Apr 2018
DOIs	https://doi.org/10.1016/j.apcatb.2018.04.068
Publication status	Published - 5 Nov 2018

Bibliographical note

Creative Commons Attribution 4.0 International (CC BY 4.0)

Funding: EPSRC for support through funding for the Centre for Doctoral Training in Fuel Cells and their fuels (D.E.L., N.V.R., EP/G037116/1) and a fellowship grant (R.E.P., EP/L015749/1 and EP/K006061/2) and the European Commission for the Marie-Curie ITN project “Catsense” (Y.N.)

Keywords

molybdenum disulfide
nanoclusters
sulfur-rich
hydrogen evolution
magnetron sputtering deposition

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Hydrogen evolution enhancement of ultra-low loading, size-selected molybdenum sulfide nanoclusters by sulfur enrichment
Creative Commons Attribution 4.0 International (CC BY 4.0)
Accepted author manuscript, 0.99 MBLicence: CC BY 3.0

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title = "Hydrogen evolution enhancement of ultra-low loading, size-selected molybdenum sulfide nanoclusters by sulfur enrichment",

abstract = "Size-selected molybdenum sulfide (MoSx) nanoclusters obtained by magnetron sputtering and gas condensation on glassy carbon substrates are typically sulfur-deficient (x = 1.6 ± 0.1), which limits their crystallinity and electrocatalytic properties. Here we demonstrate that a sulfur-enriching method, comprising sulfur evaporation and cluster annealing under vacuum conditions, significantly enhances their activity towards the hydrogen evolution reaction (HER). The S-richness (x = 4.9 ± 0.1) and extended crystalline order obtained in the sulfur-treated MoSx nanoclusters lead to consistent 200 mV shifts to lower HER onset potentials, along with two-fold and more-than 30-fold increases in turnover frequency and exchange current density values respectively. The high mass activities (~111 mA mg-1 @ 400 mV) obtained at ultra-low loadings (~100 ng cm-2, 5 % surface coverage) are comparable to the best reported MoS2 catalysts in the literature.",

keywords = "molybdenum disulfide, nanoclusters, sulfur-rich, hydrogen evolution, magnetron sputtering deposition",

author = "Daniel Escalera-l{\'o}pez and Yubiao Niu and Park, {Sung Jin} and Mark Isaacs and Karen Wilson and Palmer, {Richard E.} and Rees, {Neil V.}",

note = "Creative Commons Attribution 4.0 International (CC BY 4.0) Funding: EPSRC for support through funding for the Centre for Doctoral Training in Fuel Cells and their fuels (D.E.L., N.V.R., EP/G037116/1) and a fellowship grant (R.E.P., EP/L015749/1 and EP/K006061/2) and the European Commission for the Marie-Curie ITN project “Catsense” (Y.N.) ",

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doi = "10.1016/j.apcatb.2018.04.068",

language = "English",

volume = "235",

pages = "84--91",

journal = "Applied Catalysis B: Environmental",

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T1 - Hydrogen evolution enhancement of ultra-low loading, size-selected molybdenum sulfide nanoclusters by sulfur enrichment

AU - Escalera-lópez, Daniel

AU - Niu, Yubiao

AU - Park, Sung Jin

AU - Isaacs, Mark

AU - Wilson, Karen

AU - Palmer, Richard E.

AU - Rees, Neil V.

N1 - Creative Commons Attribution 4.0 International (CC BY 4.0) Funding: EPSRC for support through funding for the Centre for Doctoral Training in Fuel Cells and their fuels (D.E.L., N.V.R., EP/G037116/1) and a fellowship grant (R.E.P., EP/L015749/1 and EP/K006061/2) and the European Commission for the Marie-Curie ITN project “Catsense” (Y.N.)

PY - 2018/11/5

Y1 - 2018/11/5

N2 - Size-selected molybdenum sulfide (MoSx) nanoclusters obtained by magnetron sputtering and gas condensation on glassy carbon substrates are typically sulfur-deficient (x = 1.6 ± 0.1), which limits their crystallinity and electrocatalytic properties. Here we demonstrate that a sulfur-enriching method, comprising sulfur evaporation and cluster annealing under vacuum conditions, significantly enhances their activity towards the hydrogen evolution reaction (HER). The S-richness (x = 4.9 ± 0.1) and extended crystalline order obtained in the sulfur-treated MoSx nanoclusters lead to consistent 200 mV shifts to lower HER onset potentials, along with two-fold and more-than 30-fold increases in turnover frequency and exchange current density values respectively. The high mass activities (~111 mA mg-1 @ 400 mV) obtained at ultra-low loadings (~100 ng cm-2, 5 % surface coverage) are comparable to the best reported MoS2 catalysts in the literature.

AB - Size-selected molybdenum sulfide (MoSx) nanoclusters obtained by magnetron sputtering and gas condensation on glassy carbon substrates are typically sulfur-deficient (x = 1.6 ± 0.1), which limits their crystallinity and electrocatalytic properties. Here we demonstrate that a sulfur-enriching method, comprising sulfur evaporation and cluster annealing under vacuum conditions, significantly enhances their activity towards the hydrogen evolution reaction (HER). The S-richness (x = 4.9 ± 0.1) and extended crystalline order obtained in the sulfur-treated MoSx nanoclusters lead to consistent 200 mV shifts to lower HER onset potentials, along with two-fold and more-than 30-fold increases in turnover frequency and exchange current density values respectively. The high mass activities (~111 mA mg-1 @ 400 mV) obtained at ultra-low loadings (~100 ng cm-2, 5 % surface coverage) are comparable to the best reported MoS2 catalysts in the literature.

KW - molybdenum disulfide

KW - nanoclusters

KW - sulfur-rich

KW - hydrogen evolution

KW - magnetron sputtering deposition

UR - https://www.sciencedirect.com/science/article/pii/S0926337318303977

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DO - 10.1016/j.apcatb.2018.04.068

M3 - Article

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JO - Applied Catalysis B: Environmental

JF - Applied Catalysis B: Environmental

ER -

Hydrogen evolution enhancement of ultra-low loading, size-selected molybdenum sulfide nanoclusters by sulfur enrichment

Abstract

Bibliographical note

Keywords

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