Promoter Effects of Alkali Metal Cations on the Electrochemical Reduction of Carbon Dioxide

Resasco, Joaquin; Chen, Leanne D.; Clark, Ezra; Tsai, Charlie; Hahn, Christopher; Jaramillo, Thomas F.; Chan, Karen; Bell, Alexis T.

doi:10.1021/jacs.7b06765

Title: Promoter Effects of Alkali Metal Cations on the Electrochemical Reduction of Carbon Dioxide

Journal Article · Mon Jul 24 00:00:00 EDT 2017 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.7b06765· OSTI ID:1390621

Resasco, Joaquin ^[1]; Chen, Leanne D. ^[2]; Clark, Ezra ^[1]; Tsai, Charlie ^[2];

^[2];

^[1]

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)

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.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division

Grant/Contract Number:: AC02-76SF00515; DGE-0802270; AC02-05CH11231; SC0004993

OSTI ID:: 1390621

Alternate ID(s):: OSTI ID: 1418306

Journal Information:: Journal of the American Chemical Society, Vol. 139, Issue 32; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 527 works

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Quantification of Interfacial pH Variation at Molecular Length Scales Using a Concurrent Non-Faradaic Reaction Ryu, Jaeyune; Wuttig, Anna; Surendranath, Yogesh Angewandte Chemie, Vol. 130, Issue 30 https://doi.org/10.1002/ange.201802756	journal	July 2018
FeNC catalysts for CO ₂ electroreduction to CO: effect of nanostructured carbon supports Karapinar, Dilan; Tran, Ngoc-Huan; Giaume, Domitille Sustainable Energy & Fuels, Vol. 3, Issue 7 https://doi.org/10.1039/c9se00214f	journal	January 2019
Role of the Adsorbed Oxygen Species in the Selective Electrochemical Reduction of CO ₂ to Alcohols and Carbonyls on Copper Electrodes Le Duff, Cécile S.; Lawrence, Matthew J.; Rodriguez, Paramaconi Angewandte Chemie International Edition, Vol. 56, Issue 42 https://doi.org/10.1002/anie.201706463	journal	September 2017
Carbon‐Nanotube‐Supported Copper Polyphthalocyanine for Efficient and Selective Electrocatalytic CO ₂ Reduction to CO Karapinar, Dilan; Zitolo, Andrea; Huan, Tran Ngoc ChemSusChem, Vol. 13, Issue 1 https://doi.org/10.1002/cssc.201902859	journal	November 2019
Understanding the Heterogeneous Electrocatalytic Reduction of Carbon Dioxide on Oxide-Derived Catalysts Pander, James E.; Ren, Dan; Huang, Yun ChemElectroChem, Vol. 5, Issue 2 https://doi.org/10.1002/celc.201701100	journal	December 2017
Atomic‐Scale Spacing between Copper Facets for the Electrochemical Reduction of Carbon Dioxide Jeong, Hyung Mo; Kwon, Youngkook; Won, Jong Ho Advanced Energy Materials, Vol. 10, Issue 10 https://doi.org/10.1002/aenm.201903423	journal	March 2020
Hydroxide Is Not a Promoter of C ₂₊ Product Formation in the Electrochemical Reduction of CO on Copper Li, Jing; Wu, Donghuan; Malkani, Arnav S. Angewandte Chemie, Vol. 132, Issue 11 https://doi.org/10.1002/ange.201912412	journal	March 2020
Lateral Adsorbate Interactions Inhibit HCOO ⁻ while Promoting CO Selectivity for CO ₂ Electrocatalysis on Silver Bohra, Divya; Ledezma-Yanez, Isis; Li, Guanna Angewandte Chemie, Vol. 131, Issue 5 https://doi.org/10.1002/ange.201811667	journal	December 2018
Defining a Materials Database for the Design of Copper Binary Alloy Catalysts for Electrochemical CO ₂ Conversion Lee, Chan Woo; Yang, Ki Dong; Nam, Dae-Hyun Advanced Materials, Vol. 30, Issue 42 https://doi.org/10.1002/adma.201704717	journal	January 2018
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) Li, Jing; Wu, Donghuan; Malkani, Arnav S. Angewandte Chemie International Edition, Vol. 59, Issue 11 https://doi.org/10.1002/anie.202000873	journal	January 2020
Competition between H and CO for Active Sites Governs Copper-Mediated Electrosynthesis of Hydrocarbon Fuels Schreier, Marcel; Yoon, Youngmin; Jackson, Megan N. Angewandte Chemie International Edition, Vol. 57, Issue 32 https://doi.org/10.1002/anie.201806051	journal	July 2018
Lateral Adsorbate Interactions Inhibit HCOO ⁻ while Promoting CO Selectivity for CO ₂ Electrocatalysis on Silver Bohra, Divya; Ledezma‐Yanez, Isis; Li, Guanna Angewandte Chemie International Edition, Vol. 58, Issue 5 https://doi.org/10.1002/anie.201811667	journal	January 2019
Titelbild: Hydroxide Is Not a Promoter of C ₂₊ Product Formation in the Electrochemical Reduction of CO on Copper (Angew. Chem. 11/2020) Li, Jing; Wu, Donghuan; Malkani, Arnav S. Angewandte Chemie, Vol. 132, Issue 11 https://doi.org/10.1002/ange.202000873	journal	March 2020
Plasma-Modified Dendritic Cu Catalyst for CO₂Electroreduction Scholten, Fabian; Sinev, Ilya; Bernal, Miguel ACS Catalysis, Vol. 9, Issue 6 https://doi.org/10.1021/acscatal.9b00483	journal	April 2019
In Situ Infrared Spectroscopy Reveals Persistent Alkalinity near Electrode Surfaces during CO ₂ Electroreduction Yang, Kailun; Kas, Recep; Smith, Wilson A. Journal of the American Chemical Society, Vol. 141, Issue 40 https://doi.org/10.1021/jacs.9b07000	journal	September 2019
Operando Insight into the Correlation between the Structure and Composition of CuZn Nanoparticles and Their Selectivity for the Electrochemical CO ₂ Reduction Jeon, Hyo Sang; Timoshenko, Janis; Scholten, Fabian Journal of the American Chemical Society, Vol. 141, Issue 50 https://doi.org/10.1021/jacs.9b10709	journal	November 2019
Theoretical insights into selective electrochemical conversion of carbon dioxide Lee, Chan Woo; Kim, Chanyeon; Min, Byoung Koun Nano Convergence, Vol. 6, Issue 1 https://doi.org/10.1186/s40580-019-0177-2	journal	March 2019

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