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Title: Effect of Pressure and Temperature on Carbon Dioxide Reduction at a Plasmonically Active Silver Cathode

Abstract

Here, carbon dioxide reduction at a plasmonically active silver cathode was investigated by varying the pressure and temperature at multiple applied potentials under both dark and illuminated conditions to understand the mechanism of selectivity changes driven by plasmon-enhanced electrochemical conversion. Carbon dioxide partial pressures (PCo2) from 0.2 to 1 atm were studied during linear sweep voltammetry and chronoamperometry at -0.7, -0.9, and -1.1 VRHE. At a given applied overpotential the total current density increased with increasing PCo2 in both the dark and the light, but there were significant differences in the Tafel behavior between dark and illuminated conditions. The reduction of CO2 to carbon monoxide (CO) was found to have first-order behavior with respect to PCo2 at all applied potentials in both the dark and the light, likely indicating no change in the rate-determining step upon illumination. Activity for the hydrogen (H2) evolution reaction decreased with increasing PCo2 at slightly different rates in the dark and the light at each applied potential, making it unclear if light is influencing CO or H2 intermediate adsorbate coverage. Both formate and methanol production showed no dependence on PCo2 under any conditions, but the true reaction orders may be masked by the much highermore » activity for CO and H2 at the silver cathode. The investigation of product distribution with temperature at 14, 22, and 32°C at -0.7, -0.9, and -1.1 VRHE in both the dark and the light demonstrated that the selectivity changes observed upon illumination are not caused by local heating of the cathode surface.« less

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3];  [4];  [1]
  1. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry; Univ. of California, Berkeley, CA (United States)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry; California Institute of Technology (CalTech), Pasadena, CA (United States). Joint Center for Artificial Photosynthesis (JCAP); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1764559
Alternate Identifier(s):
OSTI ID: 1769239; OSTI ID: 1775754
Grant/Contract Number:  
AC02-05CH11231; SC0004993; AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Electrochimica Acta
Additional Journal Information:
Journal Volume: 374; Journal ID: ISSN 0013-4686
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Carbon dioxide reduction; Plasmon-enhanced electrocatalysis; Silver film; Carbon dioxide partial pressure; Reaction Order

Citation Formats

Corson, Elizabeth R., Creel, Erin B., Kostecki, Robert, Urban, Jeffrey J., and McCloskey, Bryan D.. Effect of Pressure and Temperature on Carbon Dioxide Reduction at a Plasmonically Active Silver Cathode. United States: N. p., 2021. Web. doi:10.1016/j.electacta.2021.137820.
Corson, Elizabeth R., Creel, Erin B., Kostecki, Robert, Urban, Jeffrey J., & McCloskey, Bryan D.. Effect of Pressure and Temperature on Carbon Dioxide Reduction at a Plasmonically Active Silver Cathode. United States. https://doi.org/10.1016/j.electacta.2021.137820
Corson, Elizabeth R., Creel, Erin B., Kostecki, Robert, Urban, Jeffrey J., and McCloskey, Bryan D.. Fri . "Effect of Pressure and Temperature on Carbon Dioxide Reduction at a Plasmonically Active Silver Cathode". United States. https://doi.org/10.1016/j.electacta.2021.137820. https://www.osti.gov/servlets/purl/1764559.
@article{osti_1764559,
title = {Effect of Pressure and Temperature on Carbon Dioxide Reduction at a Plasmonically Active Silver Cathode},
author = {Corson, Elizabeth R. and Creel, Erin B. and Kostecki, Robert and Urban, Jeffrey J. and McCloskey, Bryan D.},
abstractNote = {Here, carbon dioxide reduction at a plasmonically active silver cathode was investigated by varying the pressure and temperature at multiple applied potentials under both dark and illuminated conditions to understand the mechanism of selectivity changes driven by plasmon-enhanced electrochemical conversion. Carbon dioxide partial pressures (PCo2) from 0.2 to 1 atm were studied during linear sweep voltammetry and chronoamperometry at -0.7, -0.9, and -1.1 VRHE. At a given applied overpotential the total current density increased with increasing PCo2 in both the dark and the light, but there were significant differences in the Tafel behavior between dark and illuminated conditions. The reduction of CO2 to carbon monoxide (CO) was found to have first-order behavior with respect to PCo2 at all applied potentials in both the dark and the light, likely indicating no change in the rate-determining step upon illumination. Activity for the hydrogen (H2) evolution reaction decreased with increasing PCo2 at slightly different rates in the dark and the light at each applied potential, making it unclear if light is influencing CO or H2 intermediate adsorbate coverage. Both formate and methanol production showed no dependence on PCo2 under any conditions, but the true reaction orders may be masked by the much higher activity for CO and H2 at the silver cathode. The investigation of product distribution with temperature at 14, 22, and 32°C at -0.7, -0.9, and -1.1 VRHE in both the dark and the light demonstrated that the selectivity changes observed upon illumination are not caused by local heating of the cathode surface.},
doi = {10.1016/j.electacta.2021.137820},
journal = {Electrochimica Acta},
number = ,
volume = 374,
place = {United States},
year = {Fri Jan 29 00:00:00 EST 2021},
month = {Fri Jan 29 00:00:00 EST 2021}
}

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