Promoter Effects of Alkali Metal Cations on the Electrochemical Reduction of Carbon Dioxide
Abstract
The electrochemical reduction of CO2 is known to be influenced by the identity of the alkali metal cation in the electrolyte; however, a satisfactory explanation for this phenomenon has not been developed. Here we present the results of experimental and theoretical studies aimed at elucidating the effects of electrolyte cation size on the intrinsic activity and selectivity of metal catalysts for the reduction of CO2. Experiments were conducted under conditions where the influence of electrolyte polarization is minimal in order to show that cation size affects the intrinsic rates of formation of certain reaction products, most notably for HCOO–, C2H4, and C2H5OH over Cu(100)- and Cu(111)-oriented thin films, and for CO and HCOO– over polycrystalline Ag and Sn. Interpretation of the findings for CO2 reduction was informed by studies of the reduction of glyoxal and CO, key intermediates along the reaction pathway to final products. Density functional theory calculations show that the alkali metal cations influence the distribution of products formed as a consequence of electrostatic interactions between solvated cations present at the outer Helmholtz plane and adsorbed species having large dipole moments. As a result, the observed trends in activity with cation size are attributed to an increase inmore »
- Authors:
-
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
- OSTI Identifier:
- 1390621
- Alternate Identifier(s):
- OSTI ID: 1418306
- Grant/Contract Number:
- AC02-76SF00515; DGE-0802270; AC02-05CH11231; SC0004993
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 139; Journal Issue: 32; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; electrochemical reduction; CO2; copper; silver
Citation Formats
Resasco, Joaquin, Chen, Leanne D., Clark, Ezra, Tsai, Charlie, Hahn, Christopher, Jaramillo, Thomas F., Chan, Karen, and Bell, Alexis T. Promoter Effects of Alkali Metal Cations on the Electrochemical Reduction of Carbon Dioxide. United States: N. p., 2017.
Web. doi:10.1021/jacs.7b06765.
Resasco, Joaquin, Chen, Leanne D., Clark, Ezra, Tsai, Charlie, Hahn, Christopher, Jaramillo, Thomas F., Chan, Karen, & Bell, Alexis T. Promoter Effects of Alkali Metal Cations on the Electrochemical Reduction of Carbon Dioxide. United States. https://doi.org/10.1021/jacs.7b06765
Resasco, Joaquin, Chen, Leanne D., Clark, Ezra, Tsai, Charlie, Hahn, Christopher, Jaramillo, Thomas F., Chan, Karen, and Bell, Alexis T. Mon .
"Promoter Effects of Alkali Metal Cations on the Electrochemical Reduction of Carbon Dioxide". United States. https://doi.org/10.1021/jacs.7b06765. https://www.osti.gov/servlets/purl/1390621.
@article{osti_1390621,
title = {Promoter Effects of Alkali Metal Cations on the Electrochemical Reduction of Carbon Dioxide},
author = {Resasco, Joaquin and Chen, Leanne D. and Clark, Ezra and Tsai, Charlie and Hahn, Christopher and Jaramillo, Thomas F. and Chan, Karen and Bell, Alexis T.},
abstractNote = {The electrochemical reduction of CO2 is known to be influenced by the identity of the alkali metal cation in the electrolyte; however, a satisfactory explanation for this phenomenon has not been developed. Here we present the results of experimental and theoretical studies aimed at elucidating the effects of electrolyte cation size on the intrinsic activity and selectivity of metal catalysts for the reduction of CO2. Experiments were conducted under conditions where the influence of electrolyte polarization is minimal in order to show that cation size affects the intrinsic rates of formation of certain reaction products, most notably for HCOO–, C2H4, and C2H5OH over Cu(100)- and Cu(111)-oriented thin films, and for CO and HCOO– over polycrystalline Ag and Sn. Interpretation of the findings for CO2 reduction was informed by studies of the reduction of glyoxal and CO, key intermediates along the reaction pathway to final products. Density functional theory calculations show that the alkali metal cations influence the distribution of products formed as a consequence of electrostatic interactions between solvated cations present at the outer Helmholtz plane and adsorbed species having large dipole moments. As a result, the observed trends in activity with cation size are attributed to an increase in the concentration of cations at the outer Helmholtz plane with increasing cation size.},
doi = {10.1021/jacs.7b06765},
journal = {Journal of the American Chemical Society},
number = 32,
volume = 139,
place = {United States},
year = {Mon Jul 24 00:00:00 EDT 2017},
month = {Mon Jul 24 00:00:00 EDT 2017}
}
Web of Science
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- Bohra, Divya; Ledezma-Yanez, Isis; Li, Guanna
- Angewandte Chemie, Vol. 131, Issue 5
Defining a Materials Database for the Design of Copper Binary Alloy Catalysts for Electrochemical CO 2 Conversion
journal, January 2018
- Lee, Chan Woo; Yang, Ki Dong; Nam, Dae-Hyun
- Advanced Materials, Vol. 30, Issue 42
Cover Picture: Hydroxide Is Not a Promoter of C 2+ Product Formation in the Electrochemical Reduction of CO on Copper (Angew. Chem. Int. Ed. 11/2020)
journal, January 2020
- Li, Jing; Wu, Donghuan; Malkani, Arnav S.
- Angewandte Chemie International Edition, Vol. 59, Issue 11
Competition between H and CO for Active Sites Governs Copper-Mediated Electrosynthesis of Hydrocarbon Fuels
journal, July 2018
- Schreier, Marcel; Yoon, Youngmin; Jackson, Megan N.
- Angewandte Chemie International Edition, Vol. 57, Issue 32
Lateral Adsorbate Interactions Inhibit HCOO − while Promoting CO Selectivity for CO 2 Electrocatalysis on Silver
journal, January 2019
- Bohra, Divya; Ledezma‐Yanez, Isis; Li, Guanna
- Angewandte Chemie International Edition, Vol. 58, Issue 5
Titelbild: Hydroxide Is Not a Promoter of C 2+ Product Formation in the Electrochemical Reduction of CO on Copper (Angew. Chem. 11/2020)
journal, March 2020
- Li, Jing; Wu, Donghuan; Malkani, Arnav S.
- Angewandte Chemie, Vol. 132, Issue 11
Lateral Adsorbate Interactions Inhibit HCOO − while Promoting CO Selectivity for CO 2 Electrocatalysis on Silver
journal, January 2019
- Bohra, Divya; Ledezma‐Yanez, Isis; Li, Guanna
- Angewandte Chemie International Edition, Vol. 58, Issue 5
Plasma-Modified Dendritic Cu Catalyst for CO2Electroreduction
journal, April 2019
- Scholten, Fabian; Sinev, Ilya; Bernal, Miguel
- ACS Catalysis, Vol. 9, Issue 6
In Situ Infrared Spectroscopy Reveals Persistent Alkalinity near Electrode Surfaces during CO 2 Electroreduction
journal, September 2019
- Yang, Kailun; Kas, Recep; Smith, Wilson A.
- Journal of the American Chemical Society, Vol. 141, Issue 40
Operando Insight into the Correlation between the Structure and Composition of CuZn Nanoparticles and Their Selectivity for the Electrochemical CO 2 Reduction
journal, November 2019
- Jeon, Hyo Sang; Timoshenko, Janis; Scholten, Fabian
- Journal of the American Chemical Society, Vol. 141, Issue 50
Tuning the activity and selectivity of electroreduction of CO2 to synthesis gas using bimetallic catalysts
journal, August 2019
- Lee, Ji Hoon; Kattel, Shyam; Jiang, Zhao
- Nature Communications, Vol. 10, Issue 1
Theoretical insights into selective electrochemical conversion of carbon dioxide
journal, March 2019
- Lee, Chan Woo; Kim, Chanyeon; Min, Byoung Koun
- Nano Convergence, Vol. 6, Issue 1