Guanine-regulated proton transfer enhances CO2-to-CH4 selectivity over copper electrode

doi:10.1016/S1872-2067(22)64113-5

Abstract

Abstract:

Electrocatalytic CO₂ reduction has attracted growing attention as a promising route to realize artificial carbon recycling. Proton transfer plays an essential role in CO₂ reduction and dramatically impacts product distribution. However, the precise control of proton transfer during CO₂ reduction remains challenging. In this study, we present a well-controlled proton transfer through the modification of several purines with similar molecular structures, and reveal a direct correlation between surface proton transfer capability and CO₂ reduction selectivity over Cu electrode. With a moderate proton transfer capability, the guanine modification can remarkably boost CH₄ production and suppress C₂ products formation. In-situ ATR-SEIRAS suggests a weakened *CO intermediate adsorption and a relatively low local pH environment after the guanine modification, which facilitates the *CO protonation and detachment for CH₄ generation.

Key words: CO₂ electroreduction, Surface modification, Guanine, Proton transfer, Methane, Copper

Jun Gong, Jinmeng Li, Chang Liu, Fengyuan Wei, Jinlong Yin, Wenzheng Li, Li Xiao, Gongwei Wang, Juntao Lu, Lin Zhuang. Guanine-regulated proton transfer enhances CO₂-to-CH₄ selectivity over copper electrode[J]. Chinese Journal of Catalysis, 2022, 43(12): 3101-3106.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(22)64113-5

https://www.cjcatal.com/EN/Y2022/V43/I12/3101

Figures/Tables 3

Fig. 1. Gas product faradaic efficiencies (FE) of the blank Cu and Cu-purine electrodes toward CO2 reduction. (a) H2; (b) CO; (c) CH4; (d) C2H4. Lower insets are the molecular structures of these purines used for electrode surface modification.

Fig. 2. (a) CV curves of different purines (1.3 mmol/L) in 0.1 mol/L TBABF4 DMSO/H2O (15/1, v/v) electrolyte under Ar atmosphere at 100 mV/s. Inset is the definition of the enhancement factor (ε). The relationship between the H2 (b), CH4 (c), C2H4 (d) FEs at ?1.6 V vs. RHE and ε.

Fig. 3. In-situ ATR-SEIRAS of the blank Cu (a) and Cu-Gua (b). The peak positions of ν(*CO) band (c), δ(H2O) band (d), and the intensities of ν C=O) band (e) at different potentials.

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Guanine-regulated proton transfer enhances CO₂-to-CH₄ selectivity over copper electrode

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