Fe nanoparticles embedded in N-doped porous carbon for enhanced electrocatalytic CO2 reduction and Zn-CO2 battery

doi:10.1016/S1872-2067(23)64415-8

Abstract

Abstract:

The selective electrochemical reduction of CO₂ to CO is a promising solution for the design of carbon-neutral, sustainable processes. Achieving a highly selective single reduction product is still challenging because of the energetically favorable competing hydrogen evolution reaction. We report the fabrication of N-doped sponge-like porous graphitic carbon structures embedded with Fe nanoparticles (Fe@NPC) via the pre-modification of a metal-organic framework (IRMOF-3(Zn)) with carboxyferrocene, followed by pyrolysis. The as-prepared Fe@NPC exhibited a 96.4% CO Faradaic efficiency at -0.5 V_RHE and good stability. The exceptional CO₂ reduction performance is attributed to the unique structure of the composite catalyst, which provides abundant hierarchical pores that increase CO₂ adsorption and mass transfer, and active Fe sites that synergistically accelerate the kinetics of CO generation. The in situ attenuated total reflectance-Fourier transform infrared analysis provided proof of the improved ability of Fe@NPC to accumulate the crucial intermediate *COOH compared with other pyrolyzed porous carbons. Fe@NPC was used in a Zn-CO₂ battery that delivered a maximum power density of 3.0 mW cm^-2, evidencing its potential for application in energy-converting devices.

Key words: Fe nanoparticles, Metal organic frameworks, N-doped porous carbon, CO₂ electroreduction, Zn-CO₂ battery

Wenqian Yang, Ziqian Xue, Jun Yang, Jiahui Xian, Qinglin Liu, Yanan Fan, Kai Zheng, Peiqin Liao, Hui Su, Qinghua Liu, Guangqin Li, Cheng-Yong Su. Fe nanoparticles embedded in N-doped porous carbon for enhanced electrocatalytic CO₂ reduction and Zn-CO₂ battery[J]. Chinese Journal of Catalysis, 2023, 48: 185-194.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64415-8

https://www.cjcatal.com/EN/Y2023/V48/I5/185

Figures/Tables 5

Fig. 1. (a) Schematic representation of the Fe@NPC preparation. SEM (b), TEM (c), HRTEM (d) images over Fe@NPC.

Fig. 2. High-resolution XPS N 1s spectra (a) and EPR spectra (b) of Fe@NPC and control samples. (c) Fe K-edge XANES spectra. (d) FT-EXAFS spectra of R space of Fe@NPC, Fe2O3, and Fe foil.

Fig. 3. LSV tests (a), FEco (b), and JCO (c) for different catalysts in the H-cell. FEs (d) and partial current densities (e) of reduction products using Fe@NPC in a GDE cell. (f) Stability of Fe@NPC in the flow cell.

Fig. 4. In situ ATR-FTIR spectra (a) and color contour map (b) of Fe@NPC collected at -0.6 VRHE using CO2-saturated 0.5 mol L-1 KHCO3 as electrolyte. (c) Proposed pathway for CO2 electroreduction using Fe@NPC.

Fig. 5. (a) Schematic configuration of ZCB with Fe@NPC cathode. (b) Photograph of a LED (~2.2 V) powered by Fe@NPC. (c) Polarization plot and power density. (d) Galvano-static discharge curve and corresponding FECO. (e) Galvanostatic discharge-charge cycling plots for 120 cycles of Fe@NPC.

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Fe nanoparticles embedded in N-doped porous carbon for enhanced electrocatalytic CO₂ reduction and Zn-CO₂ battery

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