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Surface‐Plasmon‐Assisted Photoelectrochemical Reduction of CO 2 and NO 3 − on Nanostructured Silver Electrodes
Author(s) -
Kim Youngsang,
Creel Erin B.,
Corson Elizabeth R.,
McCloskey Bryan D.,
Urban Jeffrey J.,
Kostecki Robert
Publication year - 2018
Publication title -
advanced energy materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.08
H-Index - 220
eISSN - 1614-6840
pISSN - 1614-6832
DOI - 10.1002/aenm.201800363
Subject(s) - photocurrent , materials science , photochemistry , electrochemistry , plasmon , adsorption , photoelectrochemistry , electrode , photocatalysis , surface plasmon resonance , surface plasmon , electrochemical reduction of carbon dioxide , acceptor , inorganic chemistry , optoelectronics , nanotechnology , catalysis , chemistry , carbon monoxide , nanoparticle , biochemistry , physics , condensed matter physics
Electrochemical reduction of carbon dioxide (CO 2 ) typically suffers from low selectivity and poor reaction rates that necessitate high overpotentials, which impede its possible application for CO 2 capture, sequestration, or carbon‐based fuel production. New strategies to address these issues include the utilization of photoexcited charge carriers to overcome activation barriers for reactions that produce desirable products. This study demonstrates surface‐plasmon‐enhanced photoelectrochemical reduction of CO 2 and nitrate (NO 3 − ) on silver nanostructured electrodes. The observed photocurrent likely originates from a resonant charge transfer between the photogenerated plasmonic hot electrons and the lowest unoccupied molecular orbital (MO) acceptor energy levels of adsorbed CO 2 , NO 3 − , or their reductive intermediates. The observed differences in the resonant effects at the Ag electrode with respect to electrode potential and photon energy for CO 2 versus NO 3 − reduction suggest that plasmonic hot‐carriers interact selectively with specific MO acceptor energy levels of adsorbed surface species such as CO 2 , NO 3 − , or their reductive intermediates. This unique plasmon‐assisted charge generation and transfer mechanism can be used to increase yield, efficiency, and selectivity of various photoelectrochemical processes.