Copper/alkaline earth metal oxide interfaces for electrochemical CO2-to-alcohol conversion by selective hydrogenation

Aoni Xu, Sung Fu Hung, Ang Cao, Zhenbin Wang, Naiwrit Karmodak, Jianan Erick Huang, Yu Yan, Armin Sedighian Rasouli, Adnan Ozden, Feng Yi Wu, Zih Yi Lin, Hsin Jung Tsai, Tsung Ju Lee, Fengwang Li, Mingchuan Luo, Yuhang Wang, Xue Wang, Jehad Abed, Ziyun Wang, Dae Hyun NamYuguang C. Li, Alexander H. Ip, David Sinton, Chaofang Dong*, Edward H. Sargent*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

62 Scopus citations

Abstract

Multicarbon alcohols produced by electrochemical CO2 reduction (CO2RR) are attractive alternatives to fossil fuels; however, the selectivity towards alcohols in CO2RR remains low, a result of competing hydrocarbon (that is, ethylene) production. Here we report on Cu catalysts decorated with different alkaline earth metal oxides (MOs). We found that BaO delivers a Faradaic efficiency of 61% towards C2+ alcohols. At an industry-relevant current density of 400 mA cm−2, the ratio of alcohols to hydrocarbon reached 3:1. Mechanistic studies, including in operando X-ray absorption spectroscopy, in situ Raman spectroscopy and density functional theory calculations, suggested that the increased selectivity towards alcohols originates from sites at the MO/Cu interface. Furthermore, computational studies indicated that the incorporation of MOs favours a hydroxy-containing C2 intermediate (*HCCHOH) over the hydrocarbon intermediate (*HCC) at interfacial Cu sites on the path to alcohol products. We also propose that the relative bond strengths of Cu–COH and C–OH correlate with the selectivity for alcohol over hydrocarbon. [Figure not available: see fulltext.]

Original languageEnglish (US)
Pages (from-to)1081-1088
Number of pages8
JournalNature Catalysis
Volume5
Issue number12
DOIs
StatePublished - Dec 2022

ASJC Scopus subject areas

  • Catalysis
  • Bioengineering
  • Biochemistry
  • Process Chemistry and Technology

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