Using a 3D Porous Flow-Through Electrode Geometry for High-Rate Electrochemical Reduction of CO2 to CO in Ionic Liquid
Abstract
Three-dimensional porous flow-through electrodes promise the realization of higher current densities in the electrochemical carbon dioxide reduction reaction (CO2RR) by overcoming mass-transport limitations associated with the diffusion of dissolved CO2 in the bulk electrolyte. Using an ionic-liquid-based electrolyte, [EMIM]BF4, offers the additional benefit of higher CO2 solubility compared to water-based electrolytes. Here, we quantitatively evaluated the effects of flow-driven reactant transport on electrode activity and selectivity for the electrochemical CO2RR in [EMIM]BF4. High-surface-area porous flow-through electrodes were fabricated by wet-chemical deposition of Ag nanoflowers on commercial macroporous Al foams. At the highest electrolyte flow-through rate of 100 mL min–1, we observed a 70-fold increase in partial CO current density, and a 7-fold increase in the Faradaic efficiency toward CO, from 10% without flow to 75% with flow. At the same time, the selectivity changed from oxalate as the main product without flow to CO in the electrolyte flow-through configuration. These results demonstrate that the flow-through approach provides a promising path forward to control selectivity and to overcome mass-transport limitations of the electrochemical CO2RR.
- Authors:
-
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1630811
- Report Number(s):
- LLNL-JRNL-782157
Journal ID: ISSN 2155-5435; 976694
- Grant/Contract Number:
- AC52-07NA27344
- Resource Type:
- Journal Article: Accepted Manuscript
- Journal Name:
- ACS Catalysis
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 12; Journal ID: ISSN 2155-5435
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; flow-through electrochemistry; ionic liquid; CO2 reduction; porous electrode
Citation Formats
Vedharathinam, Vedasri, Qi, Zhen, Horwood, Corie, Bourcier, Bill, Stadermann, Michael, Biener, Juergen, and Biener, Monika. Using a 3D Porous Flow-Through Electrode Geometry for High-Rate Electrochemical Reduction of CO2 to CO in Ionic Liquid. United States: N. p., 2019.
Web. doi:10.1021/acscatal.9b03201.
Vedharathinam, Vedasri, Qi, Zhen, Horwood, Corie, Bourcier, Bill, Stadermann, Michael, Biener, Juergen, & Biener, Monika. Using a 3D Porous Flow-Through Electrode Geometry for High-Rate Electrochemical Reduction of CO2 to CO in Ionic Liquid. United States. https://doi.org/10.1021/acscatal.9b03201
Vedharathinam, Vedasri, Qi, Zhen, Horwood, Corie, Bourcier, Bill, Stadermann, Michael, Biener, Juergen, and Biener, Monika. 2019.
"Using a 3D Porous Flow-Through Electrode Geometry for High-Rate Electrochemical Reduction of CO2 to CO in Ionic Liquid". United States. https://doi.org/10.1021/acscatal.9b03201. https://www.osti.gov/servlets/purl/1630811.
@article{osti_1630811,
title = {Using a 3D Porous Flow-Through Electrode Geometry for High-Rate Electrochemical Reduction of CO2 to CO in Ionic Liquid},
author = {Vedharathinam, Vedasri and Qi, Zhen and Horwood, Corie and Bourcier, Bill and Stadermann, Michael and Biener, Juergen and Biener, Monika},
abstractNote = {Three-dimensional porous flow-through electrodes promise the realization of higher current densities in the electrochemical carbon dioxide reduction reaction (CO2RR) by overcoming mass-transport limitations associated with the diffusion of dissolved CO2 in the bulk electrolyte. Using an ionic-liquid-based electrolyte, [EMIM]BF4, offers the additional benefit of higher CO2 solubility compared to water-based electrolytes. Here, we quantitatively evaluated the effects of flow-driven reactant transport on electrode activity and selectivity for the electrochemical CO2RR in [EMIM]BF4. High-surface-area porous flow-through electrodes were fabricated by wet-chemical deposition of Ag nanoflowers on commercial macroporous Al foams. At the highest electrolyte flow-through rate of 100 mL min–1, we observed a 70-fold increase in partial CO current density, and a 7-fold increase in the Faradaic efficiency toward CO, from 10% without flow to 75% with flow. At the same time, the selectivity changed from oxalate as the main product without flow to CO in the electrolyte flow-through configuration. These results demonstrate that the flow-through approach provides a promising path forward to control selectivity and to overcome mass-transport limitations of the electrochemical CO2RR.},
doi = {10.1021/acscatal.9b03201},
url = {https://www.osti.gov/biblio/1630811},
journal = {ACS Catalysis},
issn = {2155-5435},
number = 12,
volume = 9,
place = {United States},
year = {Fri Oct 11 00:00:00 EDT 2019},
month = {Fri Oct 11 00:00:00 EDT 2019}
}
Web of Science
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