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

Jeong, Hyung Mo; Kwon, Youngkook; Won, Jong Ho; Lum, Yanwei; Cheng, Mu‐Jeng; Kim, Kwang Ho; Head‐Gordon, Martin; Kang, Jeung Ku

doi:10.1002/aenm.201903423

Title: Atomic‐Scale Spacing between Copper Facets for the Electrochemical Reduction of Carbon Dioxide

Journal Article · Thu Jan 30 00:00:00 EST 2020 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.201903423· OSTI ID:1596183

Jeong, Hyung Mo ^[1]; Kwon, Youngkook ^[2]; Won, Jong Ho ^[3]; Lum, Yanwei ^[4]; Cheng, Mu‐Jeng ^[5]; Kim, Kwang Ho ^[6]; Head‐Gordon, Martin ^[7];

^[8]

School of Mechanical Engineering Sungkyunkwan University 2066 Seubu‐ro, Jangan‐gu Suwon 16419 Republic of Korea
School of Energy and Chemical Engineering Ulsan National Institute of Science and Technology 50 Unist‐gil Ulsan 44919 Republic of Korea
Graduate School of Energy, Environment, Water and Sustainability (EEWS) Department of Materials Science &, Engineering Korea Advanced Institute of Science and Technology 291 Daehak‐ro Yuseong‐gu Daejeon 34141 Republic of Korea
Department of Materials Science and Engineering University of California Berkeley CA 94720 USA
Department of Materials Science and Engineering University of California Berkeley CA 94720 USA, Department of Chemistry National Cheng Kung University No. 1 University Road Tainan 701 Taiwan
School of Materials Science &, Engineering Pusan National University Busandaehak‐ro 63 beon‐gil, Geumjeong‐gu Pusan 609735 Republic of Korea
Department of Materials Science and Engineering University of California Berkeley CA 94720 USA, Department of Chemistry University of California Berkeley CA 94720 USA
Graduate School of Energy, Environment, Water and Sustainability (EEWS) Department of Materials Science &, Engineering Korea Advanced Institute of Science and Technology 291 Daehak‐ro Yuseong‐gu Daejeon 34141 Republic of Korea, Department of Chemistry California Institute of Technology 1200 East California Blvd. Pasadena CA 91125 USA

Abstract Copper (Cu) offers a means for producing value‐added fuels through the electrochemical reduction of carbon dioxide (CO ₂ ), i.e., the CO ₂ reduction reaction (CO ₂ RR), but designing Cu catalysts with significant Faradaic efficiency to C ₂₊ products remains as a great challenge. This work demonstrates that the high activity and selectivity of Cu to C ₂₊ 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 CO ₂ RR. 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 C ₂₊ . Density functional theory calculations support that d _s of 5–6 Å maximizes the binding energies of CO ₂ 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 C ₂₊ product selectivity for the CO ₂ RR.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: DE‐SC0004993

OSTI ID:: 1596183

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Vol. 10 Journal Issue: 10; ISSN 1614-6832

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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Cited by: 35 works

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