Efficient CO2 fixation with acetophenone on Ag-CeO2 electrocatalyst by a double activation strategy

doi:10.1016/S1872-2067(22)64116-0

Abstract

Abstract:

The electrocarboxylation reaction is an attractive means to convert CO₂ into valuable chemicals under ambient conditions, while it still suffers from low efficiency due to the high stability of CO₂. In this work, we report a double activation strategy for simultaneously activating CO₂ and acetophenone by silver-doped CeO₂ (Ag-CeO₂) nanowires, featuring as an effective electrocatalyst for electrocarboxylation of acetophenone with CO₂. Compared to the Ag foil, Ag nanoparticles and CeO₂ nanowires, the Ag-CeO₂ nanowire catalyst allowed to reduce the onset potential difference between CO₂ and acetophenone activation, thus enabling efficient electrocarboxylation to form 2-phenyllactic acid. The Faradaic efficiency for producing 2-phenyllactic acid reached 91% at -1.8 V versus Ag/AgI. This double activation strategy of activating both CO₂ and organic substrate molecules can benefit the catalyst design to improve activities and selectivities in upgrading CO₂ fixation for higher-value electrocarboxylation.

Key words: Electrocarboxylation, CO₂ reduction, Electrocatalyst, Ag-CeO₂, Double activation strategy

Anxiang Guan, Yueli Quan, Yangshen Chen, Zhengzheng Liu, Junbo Zhang, Miao Kan, Quan Zhang, Haoliang Huang, Linping Qian, Linjuan Zhang, Gengfeng Zheng. Efficient CO₂ fixation with acetophenone on Ag-CeO₂ electrocatalyst by a double activation strategy[J]. Chinese Journal of Catalysis, 2022, 43(12): 3134-3141.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(22)64116-0

https://www.cjcatal.com/EN/Y2022/V43/I12/3134

Figures/Tables 5

Fig. 1. Schematic illustration of the synthesis procedure for the Ag-CeO2 NWs and the electrocarboxylation between acetophenone and CO2.

Fig. 2. (a) XRD patterns of CeO2 NWs (blue curve) and Ag-CeO2 NWs (red curve). (b) SEM image of Ag-CeO2 NWs. TEM (c) and high-resolution TEM (d) images of Ag-CeO2 NWs. (e) EDS elemental mapping of Ag-CeO2 NWs.

Fig. 3. XPS spectra of Ag-CeO2 NWs in the Ce 3d (a) and Ag 3d (b) regions. (c) XANES spectra of Ag K-edge for Ag-CeO2 NWs (red curve) and Ag foil (black curve). (d) First-derivatives of the XANES region for Ag-CeO2 NWs (upper panel) and Ag foil (low panel). (e) Wavelet-transform images of EXAFS data at Ag K-edge for Ag foil (upper panel) and Ag-CeO2 NWs (lower panel). (f) FT-EXAFS spectra of Ag K-edge for Ag-CeO2 NWs (red curve) and Ag foil (black curve).

Fig. 4. (a) Linear sweep voltammetry curves for Ag-CeO2 NWs sample in anhydrous acetonitrile with 0.2 mol L?1 tetrabutylammonium bromide under different reaction conditions: CO2 only (blue curve); acetophenone only (orange curve); and both CO2 and acetophenone (red curve). (b) Partial current densities (upper panel) and Faradaic efficiencies (lower panel) of 2-phenyllactic acid at different applied potentials when using the Ag-CeO2 NWs as catalyst. (c) Partial current densities (upper panel) and Faradaic efficiencies (lower panel) of 2-phenyllactic acid at -1.8 V vs. Ag/AgI for different catalysts. (d) The stability test of Ag-CeO2 NWs at -1.8 V vs. Ag/AgI.

Fig. 5. The proposed two formation mechanisms of electrocarboxylation between acetophenone and CO2 on the Ag-CeO2 NW catalyst.

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Efficient CO₂ fixation with acetophenone on Ag-CeO₂ electrocatalyst by a double activation strategy

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