Progress in Chemistry

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Research on the Construction Strategy and Interface Control of Electrocatalytic Carbon Dioxide Reduction Electrodes

Zheng Zhang, Xiaoqiang Guo, Xiaoming Zhang, Shuangjie Liu

Progress in Chemistry, DOI: 10.7536/PC20250708

Product	Reaction equation	Number of electrons transferred
CO	CO₂ + 2H⁺ + 2e⁻ → CO + H₂O	2
HCOOH	CO₂ + 2H⁺ + 2e⁻ → HCOOH	2
CH₃OH	CO₂ + 6H⁺ + 6e⁻ → CH₃OH + H₂O	6
CH₄	CO₂ + 8H⁺ + 8e⁻ → CH₄ + 2H₂O	8
C₂H₄	2CO₂ + 12H⁺ + 12e⁻ → C₂H₄+ 4H₂O	12
C₂H₅OH	2CO₂ + 12H⁺ + 12e⁻ → C₂H₅OH + 3H₂O	12

Table 2 Cathode complete reaction (using CO₂ as the starting material)

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Table 1 Typical reaction mechanism framework (CO pathway as an example)
Fig. 1 Electrode configurations of Cu-based materials: (A) Catalytic mechanism of Cu electrode. (B) Scanning electron microscope images (SEM) of 0.5-UiO/Cu. (C) SEM and EDS elemental mapping of cross-section. (D) FE vs. potential of CO₂RR and HER products^[26]. (E) FE vs. potential of C₂₊ products on Cu and 0.5-UiO/Cu. (F) FE vs. potential of HER and CO₂RR product distributions on Cu, UiO-66, 0.5-UiO/Cu, and 0.5-UiO/Cu-bare electrodes. (G) Schematic diagram of the microfluidic electrolyzer. (H) Typical SEM images of the nanoporous Cu catalysts, (I) cross-sectional SEM images of the nanoporous Cu catalysts on GDL, and (J) typical HRTEM images. (K) Timing current profiles of CO₂RR on nanoporous Cu at different potentials, (L) electrolytic C₂₊ fractional current density, and (M) corresponding FE^[48]
Fig. 2 Electrode configurations of Zn, Ag, and Sn-based materials: (A) Porous Zn electrode can convert CO₂ to CO at -0.95 V (relative to the RHE electrode) with high FE (∼95%) and current density (27 mA cm⁻²). (B) SEM images of Cu lattice and (C) P-Zn. (D) Potential-dependent current densities of P-Zn and Zn foils. (E) FE of CO. (F) Schematic representation of the local pH effect in CO₂RR^[4]. (G) Schematic representation of the synthesis process of Ag/Sn-SnO₂ nanosheets electrocatalyzing the conversion of CO₂ to pure HCOOH solution. (H, I) Typical TEM images of Ag/Sn-SnO₂ NSs. (J) Particle size distribution of Sn-SnO₂ in Ag/Sn-SnO₂ NSs. (K) Particle size distribution of Ag/HRTEM images and corresponding FFT maps of Sn-SnO₂ NSs with integrated pixel intensities of Ag, Sn, and SnO₂. (L) HAADF-STEM images and EDX mapping images of Ag/Sn-SnO₂ NSs. (M) Electrocatalytic LSV curves. (N) FEs of formate CO and H₂. (O) Reduction of CO₂ in PSE cell to pure HCOOH with accompanying OER reaction. (P) Concentration of HCOOH under deionized water as a diffusion carrier, and the FE of the corresponding HCOOH^[18]
Fig. 3 Carbon paper electrode construction: (A) Catalytic mechanism of metal phthalocyanine loaded on carbon nanotube buckypaper. (B) TEM images of FePc/BP, (C) FePc/BP_f, (D) CoPc/BP and (E) CoPc/BP_f. (F) LSV of FePc/BP and FePc/BP_f, (G) CoPc/BP and CoPc/BP_f^[60]
Fig. 4 Graphene and carbon nanotube thin-film electrode constructs: (A) Synthesis procedures of RGOL@PPS/CNT+RGO thin films. (B, C) SEM images of Cu₂O nanocrystals on RGOL@PPS/CNT+RGO thin films at 15 s and (D, E) 90 s electrodeposition times. (F) Polarization curves of (PPS/CNT+RGO)-Cu₂O, RGOL@PPS/CNT+RGO and PPS/CNT+RGO substrates with polarization curves^[20]. (G) Schematic of Co/MnO@N-C synthesis. (H) Typical TEM images of Co/MnO@N-C^[22]. (I) SEM photographs of cross sections of NCS/EG and top views of (J) NCS/EG/CNT-H. (K) Corresponding elemental mappings of C, S, Co and Ni. (L) CV curves and capacitance contributions of NCS/EG/CNT-H^[65]
Fig. 5 Carbon aerogel versus carbon foam electrode constructs: (A) Schematic representation of the active sites of Zn-750 and Zn-950. (B) SEM images of Zn-650 and (C) Zn-750. (D) ECSA curves and (E) LSV curves of Zn-T. (F) FE stability of Zn-750 after 8 h of continuous operation at −1.0 V vs. RHE^[23]
Fig. 6 Emerging structures with 3D printed electrodes: (A) 3D printed electrodes with different shapes and optimal 3Dp-PNCE catalytic electrodes. (B) TEM images of the optimal 3Dp-PNCE. (C) Comparison of current densities on 3Dp-CE, 3Dp-NCE, and 3Dp-PNCE. (D) CO₂RR stability test of 3Dp-PNCE at −0.7 V^[21]. (E) Schematic of the complete electrochemical flow cell (left), gaseous CO₂ reactants and target product C₂H₄ flow pattern (center), and surface morphology at the GDL/catalyst interface (right). (F) SEM image of H-PFPE. (G) Complete product distribution and total current density of H-Δ-PFPE-2.4 at 5 applied potentials^[13]
Fig. 7 Surface and interface engineering: (A) Schematic representation of CO₂conversion to formate mediated on a GC electrode in a liquid-phase electrolyzer and CO₂RR mediated on a GDE modified by [EMIM]⁺ layer in a gas-phase electrolyzer. (B) Conformational and chemical characterization of pristine GC cathode and modified GC cathode obtained by immobilization of imidazolium cation by SEM and WCA. (C) On IM⁺_EE/GDE cathode with 9 successive electrolysis at different current densities, respectively. (D) Variation of the average full-cell energy efficiency and EC of formate generation with applied current density on bare carbon GDE and IM⁺_EE/GDE, respectively^[12]. (E) Schematic diagram of the preparation process and the reaction mechanism of Si-Bi@C photocathode. SEM images of (F) SiNWs, (G) BiMOF and (H) Si-Bi@C800. (I) FE of Si-Bi@C1000 photocathode at different potentials (left). Chemical generation rate versus potential for Si, Si-Bi@C600, Si-Bi@C800 and Si-Bi@C1000 photocathodes (middle). Comparison of the catalytic performance of the Si-Bi@C800 photocathode with that of the reported photocathodes for the formation of formate from CO₂(right)^[9].
Table 3 Electrode test condition table
Fig. 8 Future and Prospects

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