Surface-Plasmon-Assisted Photoelectrochemical Reduction of CO2 and NO3– on Nanostructured Silver Electrodes

Kim, Youngsang; Creel, Erin B.; Corson, Elizabeth R.; McCloskey, Bryan D.; Urban, Jeffrey J.; Kostecki, Robert

doi:10.1002/aenm.201800363

Surface-Plasmon-Assisted Photoelectrochemical Reduction of CO₂ and NO₃^– on Nanostructured Silver Electrodes

Journal Article · Sun May 27 00:00:00 EDT 2018 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.201800363· OSTI ID:1630604

Kim, Youngsang ^[1]; Creel, Erin B. ^[2]; Corson, Elizabeth R. ^[3]; McCloskey, Bryan D. ^[4]; Urban, Jeffrey J. ^[5]; Kostecki, Robert ^[6]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Artificial Photosynthesis
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Artificial Photosynthesis and Molecular Foundry; Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Artificial Photosynthesis; Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Artificial Photosynthesis and Energy Storage and Distributed Resources Division; Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Artificial Photosynthesis and Molecular Foundry
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Artificial Photosynthesis and Energy Storage and Distributed Resources Division

Electrochemical reduction of carbon dioxide (CO₂) typically suffers from low selectivity and poor reaction rates that necessitate high overpotentials, which impede its possible application for CO₂ 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. Here, this study demonstrates surface-plasmon-enhanced photoelectrochemical reduction of CO₂ and nitrate (NO₃^-) 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 CO₂, NO₃^-, or their reductive intermediates. The observed differences in the resonant effects at the Ag electrode with respect to electrode potential and photon energy for CO₂ versus NO₃^- reduction suggest that plasmonic hot-carriers interact selectively with specific MO acceptor energy levels of adsorbed surface species such as CO₂, NO₃^-, 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.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; SC0004993

OSTI ID:: 1630604

Alternate ID(s):: OSTI ID: 1439256

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 22 Vol. 8; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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The Development of Cocatalysts for Photoelectrochemical CO ₂ Reduction Chang, Xiaoxia; Wang, Tuo; Yang, Piaoping Advanced Materials, Vol. 31, Issue 31 https://doi.org/10.1002/adma.201804710	journal	December 2018
Heterogeneous Photocatalyzed C−C Cross-coupling Reactions Under Visible-light and Near-infrared Light Irradiation Gu, Quan; Jia, Qiaohui; Long, Jinlin ChemCatChem, Vol. 11, Issue 2 https://doi.org/10.1002/cctc.201801616	journal	December 2018
Site-selective growth of Ag nanoparticles controlled by localized surface plasmon resonance of nanobowl arrays Zhu, Aonan; Gao, Renxian; Zhao, Xiaoyu Nanoscale, Vol. 11, Issue 14 https://doi.org/10.1039/c8nr10277e	journal	January 2019

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Related Subjects

36 MATERIALS SCIENCE
Ag electrodes
CO2
NO3 − reduction
photo-electrocatalysis
surface plasmons