Dynamics of Photocatalytic Hydrogen Production in Aqueous Dispersions of Monolayer-Rich Tungsten Disulfide
Abstract
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.
- Authors:
-
- 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. 2018.
"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 = {Tue Aug 21 00:00:00 EDT 2018},
month = {Tue Aug 21 00:00:00 EDT 2018}
}
Web of Science
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