Enhanced CO2 Electrochemical Reduction Performance over Cu@AuCu Catalysts at High Noble Metal Utilization Efficiency

Sheng Dai; Tzu-Hsi Huang; Wei-I Liu; Chia-Wei Hsu; Sheng-Wei Lee; Tsan-Yao Chen; Ya-Chen Wang; Jeng-Han Wang; Kuan-Wen Wang

doi:10.1021/acs.nanolett.1c03483

Enhanced CO₂ Electrochemical Reduction Performance over Cu@AuCu Catalysts at High Noble Metal Utilization Efficiency

Nano Lett. 2021 Nov 10;21(21):9293-9300. doi: 10.1021/acs.nanolett.1c03483. Epub 2021 Nov 1.

Authors

Sheng Dai¹, Tzu-Hsi Huang^{1

2}, Wei-I Liu², Chia-Wei Hsu², Sheng-Wei Lee², Tsan-Yao Chen^{3

4}, Ya-Chen Wang⁵, Jeng-Han Wang⁵, Kuan-Wen Wang^{2

6}

Affiliations

¹ Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Centre, Frontiers Science Center for Materiobiology and Dynamic Chemistry, Institute of Fine Chemicals, School of Chemistry and Molecular Engineering, East China University of Science & Technology, Shanghai 200237, China.
² Institute of Materials Science and Engineering, National Central University, Taoyuan 320, Taiwan.
³ Department of Engineering and System Science, National Tsing Hua University, Hsinchu 30013, Taiwan.
⁴ Hierarchical Green-Energy Materials (Hi-GEM) Research Center, National Cheng Kung University, Tainan 70101, Taiwan.
⁵ Department of Chemistry, National Taiwan Normal University, Taipei 116, Taiwan.
⁶ Department of Materials Science and Engineering, National Taiwan University of Science and Technology, Taipei 10607, Taiwan.

PMID: 34723555
DOI: 10.1021/acs.nanolett.1c03483

Abstract

The electrochemical CO₂ reduction reaction (CO₂RR) represents a viable alternative to help close the anthropogenic carbon cycle and convert intermittent electricity from renewable energy sources to chemical energy in the form of value-added chemicals. The development of economic catalysts possessing high faradaic efficiency (FE) and mass activity (MA) toward CO₂RR is critical in accelerating CO₂ utilization technology. Herein, an elaborate Au-Cu catalyst where an alloyed AuCu shell caps on a Cu core (Cu@AuCu) is developed and evaluated for CO₂-to-CO electrochemical conversion. Specific roles of Cu and Au for CO₂RR are revealed in the alloyed core-shell structure, respectively, and a compositional-dependent volcano-plot is disclosed for the Cu@AuCu catalysts toward selective CO production. As a result, the Au₂-Cu₈ alloyed core-shell catalyst (only 17% Au content) achieves an FE_CO value as high as 94% and an MA_CO of 439 mA/mg_Au at -0.8 V (vs RHE), superior to the values for pure Au, reflecting its high noble metal utilization efficiency.

Keywords: Au−Cu catalyst; CO selectivity; DFT calculation; core−shell structure; electrochemical CO2 reduction reaction.