Carbon-based catalysts of the oxygen reduction reaction: Mechanistic understanding and porous structures

doi:10.1016/S1872-2067(23)64427-4

Chinese Journal of Catalysis ›› 2023, Vol. 48: 15-31.DOI: 10.1016/S1872-2067(23)64427-4

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Carbon-based catalysts of the oxygen reduction reaction: Mechanistic understanding and porous structures

Wenjing Zhang, Jing Li^*(), Zidong Wei^*()

School of Chemistry and Chemical Engineering, Chongqing University, Chongqing 401331, China

Received:2023-02-14 Accepted:2023-02-26 Online:2023-05-18 Published:2023-04-20
Contact: * E-mai: lijing@cqu.edu.cn (J. Li), zdwei@cqu.edu.cn (Z. Wei).
About author:Jing Li received her B.A. degree from Tianjin University in 1999, and Ph.D. degree from National University of Singapore in 2008. After postdoctoral research at the Fudan University, she joined the faculty of Tongji University as an associate professor in 2011 and Chongqing University as a professor in 2014. She has been in charge of 2 National Key Research and Development Program of China and 3 National Natural Science Foundation of China. Her research interests include porous materials, fuel cells and electrocatalysis. She has published more than 80 papers with citation over 8000 times.
Zidong Wei is Professor in School of Chemistry and Chemical Engineering, Chongqing University. He received Bachelor degree from Shaanxi University of Science & Technology (1984), and Ph.D. degree from Tianjin University (1994). He has been in the field of electrochemical catalysis for more than 30 years and has published more than 300 papers with citation over 22000 times. He has been the Chief Scientist of the National Key Research and Development Program and the Chief Scientist of the National Natural Science Foundation. He edited or participated in the compilation of "Electrochemical Catalysis", "Chemical Process Intensification", "Electrocatalysis", “Electrocatalytic Oxygen Reduction Reaction” and other books. He won the first, second and third prizes of provincial and ministerial level natural sciences and technological progress once each. He is a council member in the Chemical Industry and Engineering Society of China, and Chinese Chemical Society.
Supported by:
National Natural Science Foundation of China(22279012);Natural Science Foundation of Chongqing, China(CSTB2022NSCQ-MSX1167)

Abstract

Abstract:

Carbon-based catalysts are potential substitutes for noble-metal catalysts in the oxygen reduction reaction (ORR) owing to their excellent electrical conductivities and chemical stabilities. To rationally design and accelerate the identification of highly efficient carbon-based ORR catalysts, improving the design of the active sites and microstructures is necessary. In this review, strategies for improving the intrinsic performances, activities, stabilities, and anti-poisoning properties of catalysts are analyzed. As a critical component of the microstructure, the porous structures of catalysts significantly affect their distributions of active sites and levels of mass transfer, which are also extensively analyzed. Finally, based on the formation of active sites and the fabrication of porous structures, conclusions and perspectives regarding the future development of highly efficient carbon-based electrocatalysts are provided.

Key words: Carbon-based catalyst, Oxygen reduction reaction, Active site, Porous structure, Electrocatalyst

Wenjing Zhang, Jing Li, Zidong Wei. Carbon-based catalysts of the oxygen reduction reaction: Mechanistic understanding and porous structures[J]. Chinese Journal of Catalysis, 2023, 48: 15-31.

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Figures/Tables 15

Fig. 1. Mesoscale characteristics of ORR electrocatalysis.

Fig. 2. (a) Electrocatalytic mechanism of the oxygen reduction reaction. (b) Volcano plot of oxygen reduction activity as a function of the oxygen binding energies (ΔEO) of different metals. Reproduced with permission from Ref. [32]. Copyright 2004, American Chemical Society. (c) Volcano plot of log(j0) (A cm-2) as a function of adsorption free energy ΔGOOH*. Reproduced with permission from Ref. [29]. Copyright 2014, American Chemical Society.

Fig. 3. Schematic diagram of mass transfer between the cathode and anode in a PEMFC.

Fig. 4. (a) Schematic diagram of the Fe SAs-N/C-x composite. (b) Free energy diagram at U = 0.13 V (vs. the standard hydrogen electrode). (a,b) Reproduced with permission from Ref. [47]. Copyright 2018, American Chemical Society. (c) Mechanism of catalyst formation using CoCl2 and Co2+-SCN-. Reproduced with permission from Ref. [48]. Copyright 2019, Elsevier Inc.

Fig. 5. (a) Schematic diagram of the synthesis; transmission electron microscopy (TEM) (b), high-angle annular dark-field scanning TEM images (c,d) and the corresponding mappings (e-i) of atomically dispersed FeN2 on ordered mesoporous carbon in FeN2/NOMC-3. (a-i) Reproduced with permission from Ref. [49]. Copyright 2017, Elsevier Inc. (j) Schematic diagram of the syntheses of Co-N-C catalysts with different active site structures. Reproduced with permission from Ref. [50]. Copyright 2018, Elsevier Inc.

Fig. 6. (a) Preparation of NG@MMT. Reproduced with permission from Ref. [56]. Copyright 2013, Wiley-VCH. (b) Relationship between ORR overpotential and ΔG*OOH for all carbon active sites, with the ligand, charge, and spin effects indicated. The charge (c), ligand (d), and spin density (e) effects at each carbon active site shown separately in the distribution of ΔG*OOH. Reproduced with permission from Ref. [57]. Copyright 2018, Royal Society of Chemistry.

Fig. 7. (a) Different degradation mechanisms of an Fe-N-C catalyst. Reproduced with permission from Ref. [58]. Copyright 2021, The Royal Society of Chemistry. (b) Comparison of the polarization curves of Zn-N-C and Fe-N-C catalysts before and after aging. (c) Free energy diagram of the metal corrosion of different metal hydroxides based on the M-N4 (M = Zn/Fe) structure. (b,c) Reproduced with permission from Ref. [59]. Copyright 2019, Wiley-VCH.

Fig. 8. ORR polarization curves and mass activities of Pt/C (a,b) and BP-FeNC (c,d) catalysts in different electrolytes. Reproduced with permission from Ref. [65]. Copyright 2018, Elsevier Inc. (e) Synthesis of PNC. The ORR polarization curves of PNC (f) and Pt/C (g) in 0.1 mol L-1 HClO4 in the presence of NO2-, SO32-, and HPO42-. (e,f) Reproduced with permission from Ref. [66]. Copyright 2018, Wiley-VCH.

Fig. 9. (a) Schematic diagram of the macro-micropore morphologies and charge/mass transfer in Fe/N/FC nanofiber network catalysts. Reproduced with permission from Ref. [69]. Copyright 2015, National Academy of Sciences. (b) Schematic diagram of the synthesis of Fe/NC-NaCl. (c) Relationship between the site density (SD) of FeN4 sites and the micropore surface areas of the prepared catalysts. (d) Relationship between the Jk@0.83 V and the SD (in blue); the correlation between the peak power density and SD (in red) of the prepared catalysts. Reproduced with permission from Ref. [71]. Copyright 2021, Wiley-VCH. (e) Schematic diagram of the active sites within the micropores of the carbon support. Reproduced with permission from Ref. [70]. Copyright 2009, The American Association for the Advancement of Science.

Fig. 10. TEM (a,b) and scanning electron microscopy (SEM) (c) images of the Co-N/C catalysts prepared using different hard templates and their corresponding N2 adsorption-desorption isotherms (d). Reproduced with permission from Ref. [73]. Copyright 2013, American Chemical Society. (e) Schematic diagram of the preparation of an Fe-N-C catalyst with a 3D cubic carbon framework. Reproduced with permission from Ref. [75]. Copyright 2017, American Chemical Society. (f) Schematic diagram of the Fe-Nx-decorated CNT catalyst, with ZnO as the reaction template. Reproduced with permission from Ref. [76]. Copyright 2019, Wiley-VCH.

Fig. 11. (a) Schematic diagram of the preparation of the m-FePhen-C catalyst using F127 as the soft template. Reproduced with permission from Ref. [77]. Copyright 2018, Elsevier Inc. (b) Diagram of the syntheses of the FexNC-Ar700-NH3-y% catalysts. (c) Microstructure diagram of Fe/N/C catalysts with different pore structures and numbers of active sites. Reproduced with permission from Ref. [78]. Copyright 2017, American Chemical Society.

Fig. 12. (a) Synthetic procedures of hierarchically porous Fe-N-C nanotube catalysts. (b) ORR polarization curves of several catalysts. (c) Single-cell polarization curves of the Fe-N-C and Pt/C catalysts. Reproduced with permission from Ref. [80]. Copyright 2019, Elsevier Inc. (d) Schematic diagram of the synthesis of carbon nanotubes formed vertically on carbide metal oxide nanosheet catalysts. Half-wave potentials (e) and overpotentials (f) of the catalysts. Reproduced with permission from Ref. [81]. Copyright 2019, Elsevier Inc.

Fig. 13. (a) Schematic diagram of the hollow structure, stress-induced orientation contraction mechanism and the corresponding TEM images; ORR polarization curves (b) and the jk values (c) of all catalysts at 0.8 V. Reproduced with permission from Ref. [82]. Copyright 2018, Wiley-VCH.

Fig. 14. (a) Schematic diagram of the 3D hierarchically porous carbon catalysts. Reproduced with permission from Ref. [84]. Copyright 2018, The Royal Society of Chemistry. (b) Schematic diagram of the preparation of the Fe/N/C catalyst using the molten ZnCl2/KCl eutectic salt. ORR polarization plots of the catalysts in acidic (c) and alkaline (d) electrolytes. (e) Polarization plots of the Zn-O2 batteries. Reproduced with permission from Ref. [85]. Copyright 2018, The Royal Society of Chemistry.

Fig. 15. (a) Schematic diagram of the macroporous carbon catalysts prepared using the hard template method; ORR polarization curves (b) and onset and half-wave potentials (c) of all catalysts. Reproduced with permission from Ref. [86]. Copyright 2016, American Chemical Society. (d) Schematic diagram of the FeNC materials with 3D framework structures. LS voltammograms (e) and Jk values (f) at 0.9 V and E1/2 values of different catalysts; SEM (g) and TEM (h) images of FeNC-3. N2 adsorption-desorption isotherms (i) and pore size distribution lots (j) of the FeNC catalysts. Reproduced with permission from Ref. [87]. Copyright 2020, The Royal Society of Chemistry.

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Carbon-based catalysts of the oxygen reduction reaction: Mechanistic understanding and porous structures

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