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Title: Dynamics of Photocatalytic Hydrogen Production in Aqueous Dispersions of Monolayer-Rich Tungsten Disulfide

Abstract

Two-dimensional tungsten disulfide (WS 2) is an emerging semiconducting photocatalyst featuring high optical absorption, carrier mobility, and catalytic activity toward hydrogen evolution. While characterization of its optical and electrocatalytic properties has advanced, less is known about its ultrafast carrier dynamics and intrinsic photocatalytic activity in aqueous systems producing hydrogen. This work removed extraneous variables often found in photoelectrochemical systems, thereby allowing the intrinsic proton reduction rate for monolayer-rich WS2 nanosheets to be estimated via transient absorption lifetimes and a developed kinetic scheme. Addition of a hole scavenger, ascorbic acid (AA), resulted in a 3-fold increase in carrier lifetimes following photoexcitation. Longer electron lifetimes with AA yielded a 14-fold increase in hydrogen production. An intrinsic proton reduction rate constant was extracted that may be extended to any photoelectrochemical or electrochemical hydrogen evolution scheme involving small, monolayer-rich WS 2 catalysts. This represents an important step in better understanding catalytic systems utilizing TMD catalysts.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1468392
Report Number(s):
NREL/JA-5900-71560
Journal ID: ISSN 2380-8195
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Energy Letters
Additional Journal Information:
Journal Volume: 3; Journal Issue: 9; Journal ID: ISSN 2380-8195
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; tungsten disulfide; semiconductors; photocatalysts; photoelectrochemical systems

Citation Formats

Dunklin, Jeremy R., Zhang, Hanyu, Yang, Ye, Liu, Jun, and van de Lagemaat, Jao. Dynamics of Photocatalytic Hydrogen Production in Aqueous Dispersions of Monolayer-Rich Tungsten Disulfide. United States: N. p., 2018. Web. doi:10.1021/acsenergylett.8b01287.
Dunklin, Jeremy R., Zhang, Hanyu, Yang, Ye, Liu, Jun, & van de Lagemaat, Jao. Dynamics of Photocatalytic Hydrogen Production in Aqueous Dispersions of Monolayer-Rich Tungsten Disulfide. United States. https://doi.org/10.1021/acsenergylett.8b01287
Dunklin, Jeremy R., Zhang, Hanyu, Yang, Ye, Liu, Jun, and van de Lagemaat, Jao. Tue . "Dynamics of Photocatalytic Hydrogen Production in Aqueous Dispersions of Monolayer-Rich Tungsten Disulfide". United States. https://doi.org/10.1021/acsenergylett.8b01287. https://www.osti.gov/servlets/purl/1468392.
@article{osti_1468392,
title = {Dynamics of Photocatalytic Hydrogen Production in Aqueous Dispersions of Monolayer-Rich Tungsten Disulfide},
author = {Dunklin, Jeremy R. and Zhang, Hanyu and Yang, Ye and Liu, Jun and van de Lagemaat, Jao},
abstractNote = {Two-dimensional tungsten disulfide (WS2) is an emerging semiconducting photocatalyst featuring high optical absorption, carrier mobility, and catalytic activity toward hydrogen evolution. While characterization of its optical and electrocatalytic properties has advanced, less is known about its ultrafast carrier dynamics and intrinsic photocatalytic activity in aqueous systems producing hydrogen. This work removed extraneous variables often found in photoelectrochemical systems, thereby allowing the intrinsic proton reduction rate for monolayer-rich WS2 nanosheets to be estimated via transient absorption lifetimes and a developed kinetic scheme. Addition of a hole scavenger, ascorbic acid (AA), resulted in a 3-fold increase in carrier lifetimes following photoexcitation. Longer electron lifetimes with AA yielded a 14-fold increase in hydrogen production. An intrinsic proton reduction rate constant was extracted that may be extended to any photoelectrochemical or electrochemical hydrogen evolution scheme involving small, monolayer-rich WS2 catalysts. This represents an important step in better understanding catalytic systems utilizing TMD catalysts.},
doi = {10.1021/acsenergylett.8b01287},
url = {https://www.osti.gov/biblio/1468392}, journal = {ACS Energy Letters},
issn = {2380-8195},
number = 9,
volume = 3,
place = {United States},
year = {2018},
month = {8}
}

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Works referencing / citing this record:

Unique interfacial thermodynamics of few-layer 2D MoS 2 for (photo)electrochemical catalysis
journal, January 2019