Journal
ACS ENERGY LETTERS
Volume 3, Issue 9, Pages 2223-2229Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.8b01287
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Funding
- U.S. Department of Energy (DOE) [DE-AC36-08GO28308]
- Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, Solar Photochemistry Program
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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 photo-excitation. 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.
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