Abundant (110) Facets on PdCu3 Alloy Promote Electrochemical Conversion of CO2 to CO

Jianwu Dong; Ying Cheng; Ying Li; Xianyun Peng; Rui Zhang; Hsiao-Tsu Wang; Chunyang Wang; Xiaoyan Li; Pengfei Ou; Chih-Wen Pao; Lili Han; Way-Faung Pong; Zhang Lin; Jun Luo; Huolin L Xin

doi:10.1021/acsami.2c09615

Abundant (110) Facets on PdCu₃ Alloy Promote Electrochemical Conversion of CO₂ to CO

ACS Appl Mater Interfaces. 2022 Sep 21;14(37):41969-41977. doi: 10.1021/acsami.2c09615. Epub 2022 Sep 7.

Authors

Jianwu Dong^{1

2}, Ying Cheng², Ying Li³, Xianyun Peng², Rui Zhang⁴, Hsiao-Tsu Wang⁵, Chunyang Wang⁴, Xiaoyan Li⁶, Pengfei Ou⁶, Chih-Wen Pao⁷, Lili Han^{1

4}, Way-Faung Pong⁵, Zhang Lin⁸, Jun Luo², Huolin L Xin⁴

Affiliations

¹ State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, China.
² Institute for New Energy Materials and Low-Carbon Technologies and Tianjin Key Lab of Photoelectric Materials and Devices, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China.
³ School of Materials Science and Engineering, Hebei University of Technology, Tianjin 300130, China.
⁴ Department of Physics and Astronomy, University of California, Irvine, California 92697, United States.
⁵ Department of Physics, Tamkang University, New Taipei City 25137, Taiwan.
⁶ Department of Electrical and Computer Engineering, University of Toronto, 35 St. George Street, Toronto, Ontario M5S 1A4, Canada.
⁷ National Synchrotron Radiation Research Center, Hsinchu 30076, Taiwan.
⁸ School of Metallurgy and Environment, Central South University, Changsha 410083, China.

PMID: 36069363
DOI: 10.1021/acsami.2c09615

Abstract

Electrochemical conversion of CO₂ to high-value chemical fuels offers a promising strategy for managing the global carbon balance but faces huge challenges due to the lack of effective electrocatalysts. Here, we reported PdCu₃ alloy nanoparticles with abundant exposed (110) facets supported on N-doped three-dimensional interconnected carbon frameworks (PdCu₃/NC) as an efficient and durable electrocatalyst for electrochemical CO₂ reduction to CO. The catalyst exhibits extremely high intrinsic CO₂ reduction selectivity for CO production with a Faraday efficiency of nearly 100% at a mild potential of -0.5 V. Moreover, a rechargeable high-performance Zn-CO₂ battery with PdCu₃/NC as a cathode is developed to deliver a record-high energy efficiency of 99.2% at 0.5 mA cm^-2 and rechargeable stability of up to 133 h. Theoretical calculations elucidate that the exposed (110) facet over PdCu₃/NC is the active center for CO₂ activation and rapid formation of the key *COOH intermediate.

Keywords: CO product; CO2 reduction reaction; Zn−CO2 battery; alloy electrocatalyst; exposed facet.