The role of electronic coupling between substrate and 2D MoS2 nanosheets in electrocatalytic production of hydrogen

Damien Voiry, Raymond Fullon, Jieun Yang, Cecilia de Carvalho Castro e Silva, Rajesh Kappera, Ibrahim Bozkurt, Daniel Kaplan, Maureen J. Lagos, Philip E. Batson, Gautam Gupta, Aditya D. Mohite, Liang Dong, Dequan Er, Vivek B. Shenoy, Teddy Asefa, Manish Chhowalla

Research output: Contribution to journalArticle

259 Citations (Scopus)

Abstract

The excellent catalytic activity of metallic MoS2 edges for the hydrogen evolution reaction (HER) has led to substantial efforts towards increasing the edge concentration. The 2H basal plane is less active for the HER because it is less conducting and therefore possesses less efficient charge transfer kinetics. Here we show that the activity of the 2H basal planes of monolayer MoS2 nanosheets can be made comparable to state-of-the-art catalytic properties of metallic edges and the 1T phase by improving the electrical coupling between the substrate and the catalyst so that electron injection from the electrode and transport to the catalyst active site is facilitated. Phase-engineered low-resistance contacts on monolayer 2H-phase MoS2 basal plane lead to higher efficiency of charge injection in the nanosheets so that its intrinsic activity towards the HER can be measured. We demonstrate that onset potentials and Tafel slopes of ∼−0.1 V and ∼50 mV per decade can be achieved from 2H-phase catalysts where only the basal plane is exposed. We show that efficient charge injection and the presence of naturally occurring sulfur vacancies are responsible for the observed increase in catalytic activity of the 2H basal plane. Our results provide new insights into the role of contact resistance and charge transport on the performance of two-dimensional MoS2 nanosheet catalysts for the HER.

Original languageEnglish
JournalNature Materials
DOIs
Publication statusAccepted/In press - Jun 13 2016

Fingerprint

Nanosheets
Hydrogen
catalysts
Charge injection
Catalysts
Substrates
hydrogen
Contact resistance
injection
electronics
catalytic activity
Charge transfer
Monolayers
Catalyst activity
Electron injection
low resistance
contact resistance
Sulfur
Vacancies
sulfur

ASJC Scopus subject areas

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

Cite this

The role of electronic coupling between substrate and 2D MoS2 nanosheets in electrocatalytic production of hydrogen. / Voiry, Damien; Fullon, Raymond; Yang, Jieun; de Carvalho Castro e Silva, Cecilia; Kappera, Rajesh; Bozkurt, Ibrahim; Kaplan, Daniel; Lagos, Maureen J.; Batson, Philip E.; Gupta, Gautam; Mohite, Aditya D.; Dong, Liang; Er, Dequan; Shenoy, Vivek B.; Asefa, Teddy; Chhowalla, Manish.

In: Nature Materials, 13.06.2016.

Research output: Contribution to journalArticle

Voiry, D, Fullon, R, Yang, J, de Carvalho Castro e Silva, C, Kappera, R, Bozkurt, I, Kaplan, D, Lagos, MJ, Batson, PE, Gupta, G, Mohite, AD, Dong, L, Er, D, Shenoy, VB, Asefa, T & Chhowalla, M 2016, 'The role of electronic coupling between substrate and 2D MoS2 nanosheets in electrocatalytic production of hydrogen', Nature Materials. https://doi.org/10.1038/nmat4660
Voiry, Damien ; Fullon, Raymond ; Yang, Jieun ; de Carvalho Castro e Silva, Cecilia ; Kappera, Rajesh ; Bozkurt, Ibrahim ; Kaplan, Daniel ; Lagos, Maureen J. ; Batson, Philip E. ; Gupta, Gautam ; Mohite, Aditya D. ; Dong, Liang ; Er, Dequan ; Shenoy, Vivek B. ; Asefa, Teddy ; Chhowalla, Manish. / The role of electronic coupling between substrate and 2D MoS2 nanosheets in electrocatalytic production of hydrogen. In: Nature Materials. 2016.
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