Operando time-resolved X-ray absorption spectroscopy reveals the chemical nature enabling highly selective CO2 reduction

Sheng Chih Lin, Chun Chih Chang, Shih Yun Chiu, Hsiao Tien Pai, Tzu Yu Liao, Chia Shuo Hsu, Wei Hung Chiang, Ming Kang Tsai, Hao Ming Chen

    Research output: Contribution to journalArticlepeer-review

    18 Citations (Scopus)

    Abstract

    Copper electrocatalysts have been shown to selectively reduce carbon dioxide to hydrocarbons. Nevertheless, the absence of a systematic study based on time-resolved spectroscopy renders the functional agent—either metallic or oxidative Copper—for the selectivity still undecidable. Herein, we develop an operando seconds-resolved X-ray absorption spectroscopy to uncover the chemical state evolution of working catalysts. An oxide-derived Copper electrocatalyst is employed as a model catalyst to offer scientific insights into the roles metal states serve in carbon dioxide reduction reaction (CO2RR). Using a potential switching approach, the model catalyst can achieve a steady chemical state of half-Cu(0)-and-half-Cu(I) and selectively produce asymmetric C2 products - C2H5OH. Furthermore, a theoretical analysis reveals that a surface composed of Cu-Cu(I) ensembles can have dual carbon monoxide molecules coupled asymmetrically, which potentially enhances the catalyst’s CO2RR product selectivity toward C2 products. Our results offer understandings of the fundamental chemical states and insights to the establishment of selective CO2RR.

    Original languageEnglish
    Article number3525
    JournalNature Communications
    Volume11
    Issue number1
    DOIs
    Publication statusPublished - 2020 Dec 1

    ASJC Scopus subject areas

    • Chemistry(all)
    • Biochemistry, Genetics and Molecular Biology(all)
    • Physics and Astronomy(all)

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