Journal
ACS ENERGY LETTERS
Volume 7, Issue 10, Pages 3666-3674Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.2c01755
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Funding
- Robert A. Welch Foundation [C-1220, C-1222]
- Air Force Office of Scientific Research [FA9550-15-1-0022]
- Defense Threat Reduction Agency [HDTRA 1-16-1-0042]
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Plasmonic metal nanostructures show highly efficient photocatalysis in the direct decomposition of hydrogen sulfide. Under visible light illumination, a 20-fold reactivity enhancement compared to thermocatalysis can be observed.
Plasmonic metal nanostructures have garnered rapidly increasing interest as heterogeneous photocatalysts, facilitating chemical bond activation and overcoming the high energy demands of conventional thermal catalysis. Here we report the highly efficient plasmonic photocatalysis of the direct decomposition of hydrogen sulfide into hydrogen and sulfur, an alternative to the industrial Claus process. Under visible light illumination and with no external heat source, up to a 20-fold reactivity enhancement compared to thermocatalysis can be observed. The substantially enhanced reactivity can be attributed to plasmon-mediated hot carriers (HCs) that modify the reaction energetics. With a shift in the rate-determining step of the reaction, a new reaction pathway is made possible with a lower apparent reaction barrier. Light-driven one-step decomposition of hydrogen sulfide represents an exciting opportunity for simultaneous high-efficiency hydrogen production and low-temperature sulfur recovery, important in many industrial processes.
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