An in Situ Sulfidation Approach for the Integration of MoS2 Nanosheets on Carbon Fiber Paper and the Modulation of Its Electrocatalytic Activity by Interfacing with nC60

Yun Hyuk Choi, Jongbok Lee, Abhishek Parija, Junsang Cho, Stanislav V. Verkhoturov, Mohammed Al-Hashimi, Lei Fang, Sarbajit Banerjee

Research output: Contribution to journalArticle

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Abstract

Molybdenum disulfide (MoS2) is a promising earth-abundant and low-cost electrocatalyst for the hydrogen evolution reaction (HER). In this study, we describe a stepwise synthetic approach comprising vapor transport, reduction, and topochemical sulfidation for creating 3D arrays of MoS2 nanosheets directly integrated onto carbon fiber paper (CFP) substrates. The sulfidation process results in a high density of edge sites along both the edges and the basal planes of MoS2. The obtained materials characterized by a high density of exposed edge sites exhibit promising electrocatalytic performance, including an overpotential (η10) of 245 mV at 10 mA/cm2, a Tafel slope of 81 mV/dec, and a turnover frequency (TOF) of 1.28 H2/s per active site at -0.2 V vs RHE in a 0.5 M acidic solution. The electrocatalytic properties of the MoS2 nanosheets are observed to be substantially enhanced by interfacing with solution-deposited buckminsterfullerene nanoclusters (nC60). A coverage of ca. 2% of nC60 yields a hybrid electrocatalyst exhibiting an η10 value of 172 mV, a Tafel slope of 60 mV/dec, and a TOF value of 2.33 H2/s per active site at -0.2 V vs RHE. The enhancement of electrocatalytic activity is found to derive from interfacial charge transfer at nC60/MoS2 p-n heterojunctions. The high conductivity of the interfacial layer formed as a result of charge transfer from nC60 to MoS2 is thought to substantially mitigate the limitations imposed by the poor basal plane conductivity of undoped MoS2. The hybrid catalysts illustrate an important design principle involving the use of structured interfaces to enhance the catalytic activity of low-dimensional materials.

Original languageEnglish
Pages (from-to)6246-6254
Number of pages9
JournalACS Catalysis
Volume6
Issue number9
DOIs
Publication statusPublished - 2 Sep 2016

Fingerprint

Nanosheets
Electrocatalysts
Carbon fibers
Charge transfer
Modulation
Fullerenes
Nanoclusters
Molybdenum
Heterojunctions
Hydrogen
Catalyst activity
Earth (planet)
Vapors
Catalysts
Substrates
Costs
carbon fiber
Buckminsterfullerene
molybdenum disulfide

Keywords

  • chemical vapor deposition
  • electrocatalyst
  • fullerene
  • hydrogen evolution reaction
  • molybdenum disulfide

ASJC Scopus subject areas

  • Catalysis

Cite this

An in Situ Sulfidation Approach for the Integration of MoS2 Nanosheets on Carbon Fiber Paper and the Modulation of Its Electrocatalytic Activity by Interfacing with nC60 . / Choi, Yun Hyuk; Lee, Jongbok; Parija, Abhishek; Cho, Junsang; Verkhoturov, Stanislav V.; Al-Hashimi, Mohammed; Fang, Lei; Banerjee, Sarbajit.

In: ACS Catalysis, Vol. 6, No. 9, 02.09.2016, p. 6246-6254.

Research output: Contribution to journalArticle

Choi, Yun Hyuk ; Lee, Jongbok ; Parija, Abhishek ; Cho, Junsang ; Verkhoturov, Stanislav V. ; Al-Hashimi, Mohammed ; Fang, Lei ; Banerjee, Sarbajit. / An in Situ Sulfidation Approach for the Integration of MoS2 Nanosheets on Carbon Fiber Paper and the Modulation of Its Electrocatalytic Activity by Interfacing with nC60 In: ACS Catalysis. 2016 ; Vol. 6, No. 9. pp. 6246-6254.
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abstract = "Molybdenum disulfide (MoS2) is a promising earth-abundant and low-cost electrocatalyst for the hydrogen evolution reaction (HER). In this study, we describe a stepwise synthetic approach comprising vapor transport, reduction, and topochemical sulfidation for creating 3D arrays of MoS2 nanosheets directly integrated onto carbon fiber paper (CFP) substrates. The sulfidation process results in a high density of edge sites along both the edges and the basal planes of MoS2. The obtained materials characterized by a high density of exposed edge sites exhibit promising electrocatalytic performance, including an overpotential (η10) of 245 mV at 10 mA/cm2, a Tafel slope of 81 mV/dec, and a turnover frequency (TOF) of 1.28 H2/s per active site at -0.2 V vs RHE in a 0.5 M acidic solution. The electrocatalytic properties of the MoS2 nanosheets are observed to be substantially enhanced by interfacing with solution-deposited buckminsterfullerene nanoclusters (nC60). A coverage of ca. 2{\%} of nC60 yields a hybrid electrocatalyst exhibiting an η10 value of 172 mV, a Tafel slope of 60 mV/dec, and a TOF value of 2.33 H2/s per active site at -0.2 V vs RHE. The enhancement of electrocatalytic activity is found to derive from interfacial charge transfer at nC60/MoS2 p-n heterojunctions. The high conductivity of the interfacial layer formed as a result of charge transfer from nC60 to MoS2 is thought to substantially mitigate the limitations imposed by the poor basal plane conductivity of undoped MoS2. The hybrid catalysts illustrate an important design principle involving the use of structured interfaces to enhance the catalytic activity of low-dimensional materials.",
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