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Title: Monolayer-enriched production of Au-decorated WS 2 Nanosheets via Defect Engineering

Abstract

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 (WS 2) undergoes a spontaneous redox reaction with gold (III) chloride (AuCl 3). Au nanoparticles (NPs) predominantly nucleate at nanosheet edges with tuneable NP size and density. AuCl 3 is preferentially reduced on multi-layer WS 2 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 AuCl 3 to Au 0 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.

Authors:
 [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)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1433603
Report Number(s):
NREL/JA-5900-71314
Journal ID: ISSN 2059-8521; applab
Grant/Contract Number:
AC36-08GO28308
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
MRS Advances
Additional Journal Information:
Journal Name: MRS Advances; Journal ID: ISSN 2059-8521
Publisher:
Materials Research Society (MRS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; self-assembly; functional; nanostructure

Citation Formats

Dunklin, Jeremy R., Lafargue, Paul, Higgins, Thomas M., Forcherio, Gregory T., Benamara, Mourad, McEvoy, Niall, Keith Roper, D., Coleman, Jonathan N., Vaynzof, Yana, and Backes, Claudia. Monolayer-enriched production of Au-decorated WS2 Nanosheets via Defect Engineering. United States: N. p., 2018. Web. doi:10.1557/adv.2018.350.
Dunklin, Jeremy R., Lafargue, Paul, Higgins, Thomas M., Forcherio, Gregory T., Benamara, Mourad, McEvoy, Niall, Keith Roper, D., Coleman, Jonathan N., Vaynzof, Yana, & Backes, Claudia. Monolayer-enriched production of Au-decorated WS2 Nanosheets via Defect Engineering. United States. doi:10.1557/adv.2018.350.
Dunklin, Jeremy R., Lafargue, Paul, Higgins, Thomas M., Forcherio, Gregory T., Benamara, Mourad, McEvoy, Niall, Keith Roper, D., Coleman, Jonathan N., Vaynzof, Yana, and Backes, Claudia. Fri . "Monolayer-enriched production of Au-decorated WS2 Nanosheets via Defect Engineering". United States. doi:10.1557/adv.2018.350.
@article{osti_1433603,
title = {Monolayer-enriched production of Au-decorated WS2 Nanosheets via Defect Engineering},
author = {Dunklin, Jeremy R. and Lafargue, Paul and Higgins, Thomas M. and Forcherio, Gregory T. and Benamara, Mourad and McEvoy, Niall and Keith Roper, D. and Coleman, Jonathan N. and Vaynzof, Yana and Backes, Claudia},
abstractNote = {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.},
doi = {10.1557/adv.2018.350},
journal = {MRS Advances},
number = ,
volume = ,
place = {United States},
year = {Fri Apr 06 00:00:00 EDT 2018},
month = {Fri Apr 06 00:00:00 EDT 2018}
}

Journal Article:
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