Crystal facet effect induced by different pretreatment of Cu2O nanowire electrode for enhanced electrochemical CO2 reduction to C2+ products

doi:10.1016/S1872-2067(21)63981-5

Abstract

Abstract:

Electrocatalytic CO₂ conversion has been considered as a promising way to recycle CO₂ and produce sustainable fuels and chemicals. However, the efficient and highly selective electrochemical reduction of CO₂ directly into multi-carbon (C₂₊) products remains a great challenge. Herein, we synthesized three type catalysts with different morphologies based on Cu₂O nanowires, and studied their morphology and crystal facet reconstruction during the pre-reduction process. Benefiting from abundant exposure of Cu (100) crystal facet, the nanosheet structure derived Cu catalyst showed a high faradaic efficiency (FE) of 67.5% for C₂₊ products. Additionally, electrocatalytic CO₂ reduction studies were carried out on Cu(100), Cu(110), and Cu(111) single crystal electrodes, which verified that Cu(100) crystal facets are favorable for the C₂₊products in electrocatalytic CO₂ reduction. Our work showed that catalysts would reconstruct during the CO₂ reduction process and the importance in morphology and crystal facet control to obtain desired products.

Key words: Electrocatalytic CO₂ reduction, Cu₂O, Multi-carbon products, Crystal facet reconstruction, Morphology

Yang Fu, Qixian Xie, Linxiao Wu, Jingshan Luo. Crystal facet effect induced by different pretreatment of Cu₂O nanowire electrode for enhanced electrochemical CO₂ reduction to C₂₊products[J]. Chinese Journal of Catalysis, 2022, 43(4): 1066-1073.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63981-5

https://www.cjcatal.com/EN/Y2022/V43/I4/1066

Figures/Tables 6

Fig. 1. (a) Schematic illustration of the preparation process of Cu-based nanowire, nanoparticle and nanosheet pre-catalysts. SEM images of NW (b-d), NP (e-g), NS (h-j) with different magnifications.

Fig. 2. (a) SEM image of NW-D Cu; TEM (b) and HRTEM (c) images of NW-D Cu with corresponding enlarged HRTEM image in the top right; (d) SEM image of NP-D Cu; (e) TEM image and the corresponding HRTEM image of NP-D Cu; (g) SEM image of NS-D Cu; (h,i) TEM and corresponding HRTEM of NS-D Cu with the enlarged HRTEM image in the top right.

Fig. 3. (a) XRD patterns of the NW-D Cu, NP-D Cu, and NS-D Cu; (b) Cu 2p1/2 and Cu 2p3/2 XPS spectra of the NW-D Cu, NP-D Cu, and NS-D Cu.

Fig. 4. CO2 reduction reaction performance in H-Cell. Faradaic efficiency of NW-D Cu (a), NP-D Cu (b) and NS-D Cu (c) in CO2-saturated 0.1 mol/L KHCO3 aqueous solution; Total current densities (d) and current densities of C1 (e), C2+ (f) and H2 (g) for NW, NP and NS; (h) The ratio of the C2+/C1 for NW-D Cu, NP-D Cu and NS-D Cu; (i) Long term stability and FE (C2H4) at -1.4 V (vs. RHE) of NS-D Cu electrode. All potential data were without iR-corrected.

Fig. 5. (a) CV curves in Ar-saturated 1.0 mol/L KOH of NW-D Cu, NP-D Cu and NS-D Cu at the scan rates of 50 mV s-1; Fitted OH-adsorption peaks of the NW-D Cu (b), NP-D Cu (c) and NS-D Cu (d) with the corresponding proportion of crystal planes in the inset.

Fig. 6. (a) XRD spectrum of the Cu (111), (200) and (220) single facets; Faradaic efficiency of Cu (111) (b), Cu (200) (c) and Cu (220) (d) in CO2-saturated 0.1 mol/L KHCO3 aqueous solution; (e) Faradaic efficiency of C2+ and C1 for Cu(111), Cu(220) and Cu(200) single facets; (f) The ratio of the C2+/C1 for Cu(111), Cu(220) and Cu(200) single facets.

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Crystal facet effect induced by different pretreatment of Cu₂O nanowire electrode for enhanced electrochemical CO₂ reduction to C₂₊products

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