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Title: Monolayer-enriched production of Au-decorated WS2 Nanosheets via Defect Engineering

Journal Article · · MRS Advances
DOI:https://doi.org/10.1557/adv.2018.350· OSTI ID:1433603
 [1];  [2];  [2];  [3];  [4];  [5];  [4];  [5];  [2];  [2]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. Ruprecht-Karls Univ. Heidelberg (Germany)
  3. Army Research Lab., Adelphi, MD (United States)
  4. Univ. of Arkansas, Fayetteville, AR (United States)
  5. Trinity College, Dublin (Ireland)
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Layered transition metal dichalcogenides (TMDs) represent a diverse, emerging source of two-dimensional (2D) nanostructures with broad application in optoelectronics and energy. Chemical functionalization has evolved into a powerful tool to tailor properties of these 2D TMDs; however, functionalization strategies have been largely limited to the metallic 1T-polytype. The work herein illustrates that 2H-semiconducting liquid-exfoliated tungsten disulfide (WS2) undergoes a spontaneous redox reaction with gold (III) chloride (AuCl3). Au nanoparticles (NPs) predominantly nucleate at nanosheet edges with tuneable NP size and density. AuCl3 is preferentially reduced on multi-layer WS2 and resulting large Au aggregates are easily separated from the colloidal dispersion by simple centrifugation. This process may be exploited to enrich the dispersions in laterally large, monolayer nanosheets. It is proposed that thiol groups at edges and defects sides reduce the AuCl3 to Au0 and are in turn oxidized to disulfides. Optical emission, i.e. photoluminescence, of the monolayers remained pristine, while the electrocatalytic activity towards the hydrogen evolution reaction is significantly improved. Taken together, these improvements in functionalization, fabrication, and catalytic activity represent an important advance in the study of these emerging 2D nanostructures.

Research Organization:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC36-08GO28308
OSTI ID:
1433603
Report Number(s):
NREL/JA-5900-71314; applab
Journal Information:
MRS Advances, Vol. 3, Issue 41; ISSN 2059-8521
Publisher:
Materials Research Society (MRS)Copyright Statement
Country of Publication:
United States
Language:
English

References (7)

Electrochemical Applications of Two-Dimensional Nanosheets: The Effect of Nanosheet Length and Thickness journal April 2016
Liquid Exfoliation of Layered Materials journal June 2013
Electronics and optoelectronics of two-dimensional transition metal dichalcogenides journal November 2012
Identification of Active Edge Sites for Electrochemical H2 Evolution from MoS2 Nanocatalysts journal July 2007
Comparison of liquid exfoliated transition metal dichalcogenides reveals MoSe 2 to be the most effective hydrogen evolution catalyst journal January 2016
Production of Highly Monolayer Enriched Dispersions of Liquid-Exfoliated Nanosheets by Liquid Cascade Centrifugation journal December 2015
Edge and confinement effects allow in situ measurement of size and thickness of liquid-exfoliated nanosheets journal August 2014

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