The Effects of Exfoliation, Organic Solvents and Anodic Activation on Catalytic Hydrogen Evolution Reaction of Tungsten Disulfide

W Liu, J Benson, C Dawson, A Strudwick, APA Raju, Y Han, M Li, P Papakonstantinou

Research output: Contribution to journalArticle

9 Citations (Scopus)

Abstract

The rational design of transition metal dichalcogenide electrocatalysts for efficiently catalyzing hydrogen evolution reaction (HER) is believed to lead to the generation of a renewable energy carrier. To this end our work has made three main contributions. At first, we have demonstrated that exfoliation via ionic liquid assisted grinding combined with gradient centrifugation is an efficient method to exfoliate bulk WS2 to nanosheets with a thickness of a few atomic layers and lateral size dimensions in the range of 100 nm to 2 nm. These WS2 nanosheets decorated with scattered nanodots exhibited highly enhanced catalytic performance for HER with an onset potential of -130 mV vs. RHE, an overpotential of 337 mV at 10 mA cm-2 and a Tafel slope of 80 mV dec-1 in 0.5 M H2SO4. Secondly, we found a strong aging effect on the electrocatalytic performance of WS2 stored in high boiling point organic solvents such as dimethylformamide (DMF). Importantly, the HER ability could be recovered by removing the organic (DMF) residues, which obstructed the electron transport, with acetone. Thirdly, we established that the HER performance of WS2 nanosheets/nanodots could be significantly enhanced, by activating the electrode surface at a positive voltage for a very short time (60 s), decreasing the kinetic overpotential by more than 80 mV at 10 mA cm-2. The performance enhancement was found to arise primarily from the ability of a formed proton-intercalated amorphous tungsten trioxide (a-WO3) to provide additional active sites and favourably modify the immediate chemical environment of the WS2 catalyst, rendering it more favorable for local proton delivery and/or transport to the active edge site of WS2. Our results provide new insights into the effects of organic solvents and electrochemical activation on the catalytic performance of two-dimensional WS2 for HE
LanguageEnglish
Pages13515-13526
JournalNanoscale
Volume9
Issue number36
Early online date14 Aug 2017
DOIs
Publication statusPublished - 28 Sep 2017

Fingerprint

Tungsten
Disulfides
Organic solvents
Nanosheets
Hydrogen
Chemical activation
Dimethylformamide
Protons
Ionic Liquids
Centrifugation
Electrocatalysts
Boiling point
Acetone
Transition metals
Aging of materials
Electrodes
Catalysts
Kinetics
Electric potential

Keywords

  • hydrogen evolution reaction
  • tungsten disulfide
  • exfoliation
  • aging effect
  • electrochemical activation

Cite this

Liu, W ; Benson, J ; Dawson, C ; Strudwick, A ; Raju, APA ; Han, Y ; Li, M ; Papakonstantinou, P. / The Effects of Exfoliation, Organic Solvents and Anodic Activation on Catalytic Hydrogen Evolution Reaction of Tungsten Disulfide. In: Nanoscale. 2017 ; Vol. 9, No. 36. pp. 13515-13526.
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The Effects of Exfoliation, Organic Solvents and Anodic Activation on Catalytic Hydrogen Evolution Reaction of Tungsten Disulfide. / Liu, W; Benson, J; Dawson, C; Strudwick, A; Raju, APA; Han, Y; Li, M; Papakonstantinou, P.

In: Nanoscale, Vol. 9, No. 36, 28.09.2017, p. 13515-13526.

Research output: Contribution to journalArticle

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