The configuration of Auδ+-ZrO2δ− species induced activation enhances electrocatalytic CO2 to formate conversion

Electrochemical CO 2 conversion into value-added chemicals is a promising technology to solve the greenhouse effect and recycle chemical energy. However, the electrochemical CO 2 reduction reaction (e-CO 2 RR) is seriously compromised by weak CO 2 adsorption and a rough CO 2 activation process based...

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Veröffentlicht in:Nano research 2024-07, Vol.17 (7), p.6006-6015
Hauptverfasser: Jia, Yongjian, Zhang, Yadi, Lin, Mengque, Cheng, Yangyang, Xu, Yanjie
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Sprache:eng
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Zusammenfassung:Electrochemical CO 2 conversion into value-added chemicals is a promising technology to solve the greenhouse effect and recycle chemical energy. However, the electrochemical CO 2 reduction reaction (e-CO 2 RR) is seriously compromised by weak CO 2 adsorption and a rough CO 2 activation process based on the chemical inertness of the CO 2 molecule and the formed fragile metal–C/O bond. In this paper, we designed and fabricated Au particles embedded in ZrO 2 . The configuration of Au particles being of positive charge and ZrO 2 with negative charge is induced and generated by metal–support interactions (MSIs). As a result, Au/ZrO 2 @C presents a big difference in the CO 2 conversion compared with the known work, affording a formate yield of 112.5 µmol·cm −2 ·h −1 at −1.1 V vs. reversible hydrogen electrode (RHE), and a max formate Faradaic efficiency of up to 94.1% at −0.9 V vs. RHE. This superior performance was attributed to the activated Au–ZrO 2 interface to form the Au δ + species. Both in-situ Fourier transform infrared (FTIR) spectroscopy and theoretical calculations show that the MSIs configuration can be inclined to the *OCO intermediate generation on Au δ + species activating CO 2 molecules and then accelerate the formation of the *OCHO intermediate in e-CO 2 RR, thereby favoring the CO 2 conversion to formate.
ISSN:1998-0124
1998-0000
DOI:10.1007/s12274-024-6657-7