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Title: Mg-Doped CuFeO 2 Photocathodes for Photoelectrochemical Reduction of Carbon Dioxide

Mg-doped CuFeO 2 delafossite is reported to be photoelectrochemically active for CO 2 reduction. The material was prepared via conventional solid-state methods, and subsequently assembled into an electrode as a pressed pellet. Addition of a Mg 2+ dopant is found to substantially improve the conductivity of the material, with 0.05% Mg-doped CuFeO 2 electrodes displaying photocathodic currents under visible irradiation. Photocurrent is found to onset at irradiation wavelengths of ~800 nm with the incident photon-to-current efficiency reaching a value of 14% at 340 nm using an applied electrode potential of –0.4 V vs SCE. Photoelectrodes were determined to have a –1.1 V vs SCE conduction band edge and were found capable of the reduction of CO 2 to formate at 400 mV of underpotential. The conversion efficiency is maximized at –0.9 V vs SCE, with H 2 production contributing as a considerable side reaction. Lastly, these results highlight the potential to produce Mg-doped p-type metal oxide photocathodes with a band structure tuned to optimize CO 2 reduction.
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1]
  1. Princeton Univ., Princeton, NJ (United States)
Publication Date:
Grant/Contract Number:
SC0002133
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 117; Journal Issue: 24; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Research Org:
Princeton Univ., NJ (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division
Contributing Orgs:
Princeton University
Country of Publication:
United States
Language:
English
Subject:
08 HYDROGEN; 14 SOLAR ENERGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; photoelectrochemistry; CO2 reduction to formate; CuFeO2 photocathode; doped CuFeO2; oxide photoelectrode; photoelectrochemical CO2 reduction; electrochemical band characterization
OSTI Identifier:
1418452

Gu, Jing, Wuttig, Anna, Krizan, Jason W., Hu, Yuan, Detweiler, Zachary M., Cava, Robert J., and Bocarsly, Andrew B.. Mg-Doped CuFeO2 Photocathodes for Photoelectrochemical Reduction of Carbon Dioxide. United States: N. p., Web. doi:10.1021/jp402007z.
Gu, Jing, Wuttig, Anna, Krizan, Jason W., Hu, Yuan, Detweiler, Zachary M., Cava, Robert J., & Bocarsly, Andrew B.. Mg-Doped CuFeO2 Photocathodes for Photoelectrochemical Reduction of Carbon Dioxide. United States. doi:10.1021/jp402007z.
Gu, Jing, Wuttig, Anna, Krizan, Jason W., Hu, Yuan, Detweiler, Zachary M., Cava, Robert J., and Bocarsly, Andrew B.. 2013. "Mg-Doped CuFeO2 Photocathodes for Photoelectrochemical Reduction of Carbon Dioxide". United States. doi:10.1021/jp402007z. https://www.osti.gov/servlets/purl/1418452.
@article{osti_1418452,
title = {Mg-Doped CuFeO2 Photocathodes for Photoelectrochemical Reduction of Carbon Dioxide},
author = {Gu, Jing and Wuttig, Anna and Krizan, Jason W. and Hu, Yuan and Detweiler, Zachary M. and Cava, Robert J. and Bocarsly, Andrew B.},
abstractNote = {Mg-doped CuFeO2 delafossite is reported to be photoelectrochemically active for CO2 reduction. The material was prepared via conventional solid-state methods, and subsequently assembled into an electrode as a pressed pellet. Addition of a Mg2+ dopant is found to substantially improve the conductivity of the material, with 0.05% Mg-doped CuFeO2 electrodes displaying photocathodic currents under visible irradiation. Photocurrent is found to onset at irradiation wavelengths of ~800 nm with the incident photon-to-current efficiency reaching a value of 14% at 340 nm using an applied electrode potential of –0.4 V vs SCE. Photoelectrodes were determined to have a –1.1 V vs SCE conduction band edge and were found capable of the reduction of CO2 to formate at 400 mV of underpotential. The conversion efficiency is maximized at –0.9 V vs SCE, with H2 production contributing as a considerable side reaction. Lastly, these results highlight the potential to produce Mg-doped p-type metal oxide photocathodes with a band structure tuned to optimize CO2 reduction.},
doi = {10.1021/jp402007z},
journal = {Journal of Physical Chemistry. C},
number = 24,
volume = 117,
place = {United States},
year = {2013},
month = {5}
}