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Atomic-Scale Spacing between Copper Facets for the Electrochemical Reduction of Carbon Dioxide

Jeong, Hyung Mo and Kwon, Youngkook and Won, Jong Ho and Lum, Yanwei and Cheng, Mu‐Jeng and Kim, Kwang Ho and Head‐Gordon, Martin and Kang, Jeung Ku (2020) Atomic-Scale Spacing between Copper Facets for the Electrochemical Reduction of Carbon Dioxide. Advanced Energy Materials, 10 (10). Art. No. 1903423. ISSN 1614-6832. doi:10.1002/aenm.201903423.

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Copper (Cu) offers a means for producing value‐added fuels through the electrochemical reduction of carbon dioxide (CO₂), i.e., the CO₂ reduction reaction (CO₂RR), but designing Cu catalysts with significant Faradaic efficiency to C₂₊ products remains as a great challenge. This work demonstrates that the high activity and selectivity of Cu to C₂₊ products can be achieved by atomic‐scale spacings between two facets of Cu particles. These spacings are created by lithiating CuO_x particles, removing lithium oxides formed, and electrochemically reducing CuO_x to metallic Cu. Also, the range of spacing (d_s) is confirmed via the 3D tomographs using the Cs‐corrected scanning transmission electron microscopy (3D tomo‐STEM), and the operando X‐ray absorption spectra show that oxidized Cu reduces to the metallic state during the CO₂RR. Moreover, control of d_s to 5–6 Å allows a current density exceeding that of unmodified CuO_x nanoparticles by about 12 folds and a Faradaic efficiency of ≈80% to C₂₊. Density functional theory calculations support that d_s of 5–6 Å maximizes the binding energies of CO₂ reduction intermediates and promotes C–C coupling reactions. Consequently, this study suggests that control of d_s can be used to realize the high activity and C₂₊ product selectivity for the CO₂RR.

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Kang, Jeung Ku0000-0003-3409-7544
Additional Information:© 2020 Wiley‐VCH Verlag GmbH & Co. KGaA, Weinheim. Received: October 18, 2019; Revised: December 5, 2019; Published online: 30 January 2020. H.M.J. and Y.K. contributed equally to this work. This work was mainly supported by the Global Frontier R&D Program on Center for Hybrid Interface Materials, the Korea Center for Artificial Photosynthesis (2009‐0093881), and the National Research Foundation of Korea (2017M2A2A6A01070673, 2018R1C1B6004358 and 2019M3E6A1104196) funded by the Ministry of Science and ICT, Republic of Korea. In addition, Y.K. was supported by the Next Generation Carbon Upcycling project (2017M1A2A2043122) through the National Research Foundation funded by the Ministry of Science and ICT, Republic of Korea. M.J.C. acknowledges financial support from the Ministry of Science and Technology of the Republic of China under MOST 107‐2113‐M‐006‐008‐MY2. Product analysis for electrochemical CO₂ reduction was carried out at the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award number DE‐SC0004993. The authors thank Mr. Hyung‐bin Bae at KAIST analysis center for research advancement (KARA) for technical assistance in TEM analysis. The authors declare no conflict of interest.
Funding AgencyGrant Number
Korea Center for Artificial Photosynthesis2009‐0093881
National Research Foundation of Korea2017M2A2A6A01070673
National Research Foundation of Korea2018R1C1B6004358
National Research Foundation of Korea2019M3E6A1104196
Ministry of Science and ICT (Korea)UNSPECIFIED
National Research Foundation of Korea2017M1A2A2043122
Ministry of Science and Technology (Taipei)MOST 107‐2113‐M‐006‐008‐MY2
Department of Energy (DOE)DE‐SC0004993
Subject Keywords:3D tomography; Cu nanoparticles; C2+ fuels; CO2 reduction, C–C coupling reactions
Issue or Number:10
Record Number:CaltechAUTHORS:20200206-111205774
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Official Citation:Jeong, H. M., Kwon, Y., Won, J. H., Lum, Y., Cheng, M.‐J., Kim, K. H., Head‐Gordon, M., Kang, J. K., Atomic‐Scale Spacing between Copper Facets for the Electrochemical Reduction of Carbon Dioxide. Adv. Energy Mater. 2020, 10, 1903423.
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:101157
Deposited By: Tony Diaz
Deposited On:06 Feb 2020 19:23
Last Modified:16 Nov 2021 18:00

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