Probing the Active Surface Sites for CO Reduction on Oxide-Derived Copper Electrocatalysts

Verdaguer-Casadevall, Arnau; Li, Christina W.; Johansson, Tobias P.; Scott, Soren B.; McKeown, Joseph T.; Kumar, Mukul; Stephens, Ifan E.  L.; Kanan, Matthew W.; Chorkendorff, Ib

doi:10.1021/jacs.5b06227

Title: Probing the Active Surface Sites for CO Reduction on Oxide-Derived Copper Electrocatalysts

Journal Article · Thu Jul 30 00:00:00 EDT 2015 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.5b06227· OSTI ID:1234582

Verdaguer-Casadevall, Arnau ^[1]; Li, Christina W. ^[2]; Johansson, Tobias P. ^[1]; Scott, Soren B. ^[1]; McKeown, Joseph T. ^[3]; Kumar, Mukul ^[4]; Stephens, Ifan E. L. ^[1]; Kanan, Matthew W. ^[2]; Chorkendorff, Ib ^[1]

Technical Univ. of Denmark, Lyngby (Denmark). Center for Individual Nanoparticle Functionality, Dept. of Physics
Stanford Univ., CA (United States). Dept. of Chemistry
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Materials Science Division
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Materials Engineering Division

CO electroreduction activity on oxide-derived Cu (OD-Cu) was found to correlate with metastable surface features that bind CO strongly. OD-Cu electrodes prepared by H₂ reduction of Cu₂O precursors reduce CO to acetate and ethanol with nearly 50% Faradaic efficiency at moderate overpotential. Temperature-programmed desorption of CO on OD-Cu revealed the presence of surface sites with strong CO binding that are distinct from the terraces and stepped sites found on polycrystalline Cu foil. After annealing at 350 °C, the surface-area corrected current density for CO reduction is 44-fold lower and the Faradaic efficiency is less than 5%. These changes are accompanied by a reduction in the proportion of strong CO binding sites. Here, we propose that the active sites for CO reduction on OD-Cu surfaces are strong CO binding sites that are supported by grain boundaries. Uncovering these sites is a first step toward understanding the surface chemistry necessary for efficient CO electroreduction.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1234582

Report Number(s):: LLNL-JRNL-672859

Journal Information:: Journal of the American Chemical Society, Vol. 137, Issue 31; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 604 works

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Microfabricated electrodes unravel the role of interfaces in multicomponent copper-based CO2 reduction catalysts Larrazábal, Gastón O.; Shinagawa, Tatsuya; Martín, Antonio J. ETH Zurich https://doi.org/10.3929/ethz-b-000260950	text	January 2018
Nitride-Derived Copper Modified with Indium as a Selective and Highly Stable Catalyst for the Electroreduction of Carbon Dioxide Veenstra, Florentine L. P.; Martín, Antonio J.; Pérez-Ramírez, Javier ETH Zurich https://doi.org/10.3929/ethz-b-000366265	text	January 2019
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
Selective $CO_{2}$ Electroreduction to Ethylene and Multicarbon Alcohols via Electrolyte-Driven Nanostructuring Gao, Dunfeng; Sinev, Ilya; Scholten, Fabian Deutsches Elektronen-Synchrotron, DESY, Hamburg https://doi.org/10.3204/pubdb-2020-00548	text	January 2019
Stability of Residual Oxides in Oxide‐Derived Copper Catalysts for Electrochemical CO ₂ Reduction Investigated with ¹⁸ O Labeling Lum, Yanwei; Ager, Joel W. Angewandte Chemie, Vol. 130, Issue 2 https://doi.org/10.1002/ange.201710590	journal	December 2017
Acetaldehyde as an Intermediate in the Electroreduction of Carbon Monoxide to Ethanol on Oxide-Derived Copper Bertheussen, Erlend; Verdaguer-Casadevall, Arnau; Ravasio, Davide Angewandte Chemie International Edition, Vol. 55, Issue 4 https://doi.org/10.1002/anie.201508851	journal	December 2015
A Direct Grain-Boundary-Activity Correlation for CO Electroreduction on Cu Nanoparticles Feng, Xiaofeng; Jiang, Kaili; Fan, Shoushan ACS Central Science, Vol. 2, Issue 3 https://doi.org/10.1021/acscentsci.6b00022	journal	March 2016
Tracking a Common Surface-Bound Intermediate during CO ₂ -to-Fuels Catalysis Wuttig, Anna; Liu, Can; Peng, Qiling ACS Central Science, Vol. 2, Issue 8 https://doi.org/10.1021/acscentsci.6b00155	journal	August 2016
Supramolecular Porphyrin Cages Assembled at Molecular–Materials Interfaces for Electrocatalytic CO Reduction Gong, Ming; Cao, Zhi; Liu, Wei ACS Central Science, Vol. 3, Issue 9 https://doi.org/10.1021/acscentsci.7b00316	journal	September 2017
Quantitatively Unraveling the Redox Shuttle of Spontaneous Oxidation/Electroreduction of CuO _x on Silver Nanowires Using in Situ X-ray Absorption Spectroscopy Chang, Chia-Jui; Hung, Sung-Fu; Hsu, Chia-Shuo ACS Central Science, Vol. 5, Issue 12 https://doi.org/10.1021/acscentsci.9b01142	journal	December 2019
The Importance of Cannizzaro-Type Reactions during Electrocatalytic Reduction of Carbon Dioxide Birdja, Yuvraj Y.; Koper, Marc T. M. Journal of the American Chemical Society, Vol. 139, Issue 5 https://doi.org/10.1021/jacs.6b12008	journal	January 2017
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
Correction: Corrigendum: Highly selective plasma-activated copper catalysts for carbon dioxide reduction to ethylene Mistry, Hemma; Varela, Ana Sofia; Bonifacio, Cecile S. Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms12945	journal	September 2016
Origin of the selective electroreduction of carbon dioxide to formate by chalcogen modified copper Rodrigo, García-Muelas,; Federico, Dattila,; Tatsuya, Shinagawa, ETH Zurich https://doi.org/10.3929/ethz-b-000384043	text	January 2018

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