Journal
NANO LETTERS
Volume 20, Issue 4, Pages 2348-2358Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.9b04895
Keywords
artificial photosynthesis; photoelectrochemistry; hot holes; plasmonic photocathode; CO2 reduction
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Funding
- Office of Science of the U.S. Department of Energy [DE-SC0004993]
- Swiss National Science Foundation through the Early Postdoc Mobility Fellowship [P2EZP2_159101]
- Advanced Mobility Fellowship [P300P2_171417]
- Resnick Sustainability Institute at the California Institute of Technology
- National Science Foundation (NSF) Graduate Research Fellowship Program [1745301]
- Swiss National Science Foundation (SNF) [P2EZP2_159101, P300P2_171417] Funding Source: Swiss National Science Foundation (SNF)
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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 plasmondriven 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.
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