Optical Excitation of a Nanoparticle Cu/p-NiO Photocathode Improves Reaction Selectivity for CO2 Reduction in Aqueous Electrolytes

DuChene, Joseph S.; Tagliabue, Giulia; Welch, Alex J.; Li, Xueqian; Cheng, Wen-Hui; Atwater, Harry A.

doi:10.1021/acs.nanolett.9b04895

Optical Excitation of a Nanoparticle Cu/p-NiO Photocathode Improves Reaction Selectivity for CO₂ Reduction in Aqueous Electrolytes

Journal Article · Wed Mar 04 23:00:00 EST 2020 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.9b04895· OSTI ID:1801628

^[1]; Tagliabue, Giulia ^[2]; ^[2]; Li, Xueqian ^[2]; ^[2]; ^[2]

California Institute of Technology (CalTech), Pasadena, CA (United States); OSTI
California Institute of Technology (CalTech), Pasadena, CA (United States)

We report the light-induced modification of catalytic selectivity for photoelectrochemical CO₂ reduction in aqueous media using copper (Cu) nanoparticles dispersed onto p-type nickel oxide (p-NiO) photocathodes. Optical excitation of Cu nanoparticles generates hot electrons available for driving CO₂ reduction on the Cu surface, while charge separation is accomplished by hot-hole injection from the Cu nanoparticles into the underlying p-NiO support. Photoelectrochemical studies demonstrate that optical excitation of plasmonic Cu/p-NiO photocathodes imparts increased selectivity for CO₂ reduction over hydrogen evolution in aqueous electrolytes. Specifically, we observed that plasmon-driven CO₂ reduction increased the production of carbon monoxide and formate, while simultaneously reducing the evolution of hydrogen. Our results demonstrate an optical route toward steering the selectivity of artificial photosynthetic systems with plasmon-driven photocathodes for photoelectrochemical CO₂ reduction in aqueous media.

View Accepted Manuscript (DOE)

Research Organization:: California Institute of Technology (CalTech), Pasadena, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: SC0004993

OSTI ID:: 1801628

Journal Information:: Nano Letters, Journal Name: Nano Letters Journal Issue: 4 Vol. 20; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Optical Excitation of a Nanoparticle Cu/p-NiO Photocathode Improves Reaction Selectivity for CO2 Reduction in Aqueous Electrolytes

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