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Progress in Chemistry 2022, Vol. 34 Issue (10): 2190-2201 DOI: 10.7536/PC220214 Previous Articles   Next Articles

• Review •

Enhancing the Performance of Atomically Dispersed Carbon-Based Catalysts Through Metallic/Nonmetallic Elements Co-Doping Towards Oxygen Reduction

Meng Pengfei1, Zhang Xiaorong1, Liao Shijun1(), Deng Yijie2()   

  1. 1 School of Chemistry and Chemical Engineering, South China University of Technology,Guangzhou 510641, China
    2 School of Resource Environment and Safety Engineering, University of South China,Hengyang 421001, China
  • Received: Revised: Online: Published:
  • Contact: Liao Shijun, Deng Yijie
  • Supported by:
    National Key Research and Development Program of China(2017YFB0102900); National Key Research and Development Program of China(2016YFB0101201); National Natural Science Foundation of China(51971094); National Natural Science Foundation of China(21476088); National Natural Science Foundation of China(21776104); Guangdong Provincial Department of Science and Technology(2015A030312007)
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Metal-nitrogen-carbon (M-Nx-C), possessing prominent advantages of high reactivity, high selectivity, facile synthesis, have presented potential to replace the conventional platinum-based catalysts. However, when these catalysts are used in the oxygen reduction process of fuel cells, the low active site density and insufficient durability restrict application. It is found that modulating the electronic structure and spatial configuration of the active site by doping with various metal/nonmetal elements can significantly enhance the oxygen reduction activity and stability of M-Nx-C catalysts, which has become a popular research topic in the field. This article reviews the main research works in recent years at home and abroad on the doping of various metal/nonmetal elements to enhance the performance of M-Nx-C carbon-based catalysts, including the studies on doping of metal elements and doping of nonmetal elements. The article also summarizes and points out the problems and challenges faced by M-Nx-C carbon-based catalysts, and gives an outlook on their development prospects and future research directions.

Key words: non-platinum catalyst, carbon catalyst, oxygen reduction, co-doping, single-atom catalyst
Fig. 1 Schematic illustration of the hard template method for preparation of Fe—N—C HNS[22]
Fig. 2 Illustration of synthesis of Cr-N-C[21]
Fig. 3 Plots of catalytic activities for the ORR in alkaline media[44]
Fig. 4 Dynamic transformation process of active site[47]
Fig. 5 LSV curves of Fe-N-C and Pt1@Fe-N-C measured after 10 000 voltage cycles in the air-saturated electrolyte,0.5 mol/L H2S O 4 [ 60 ]
Fig. 6 (a) ORR LSV curves for different catalysts in 0.1 mol/L HClO4 solution. (b) H2/O2 fuel cell polarization plots[63]
Fig. 7 (a) ORR LSV curves for different catalysts in 0.1 mol/L KOH solution.(b) ORR LSV curves for different catalysts in 0.1 mol/L HClO4 solution.[67]
Fig. 8 (a) Schematic illustration of the synthesis of FeNSC. (b) ORR LSV curves for different catalysts in 0.1 mol/L KOH solution (rotation rate: 1600 r/min). Inset shows corresponding half-wave potentials and the number of transferred electrons[68]
Fig. 9 Schematic of the synthesis process of the Fe-N/P-C[73]
Fig. 10 Polarization and power density curves for a H2-O2 PEMFC with Fe-N-C-P/N,P-C, Fe-N-C/N-C, and Pt/C as the cathode catalysts[74]
Fig. 11 ORR free energy profiles of a Co-N2P2 site in PSTA-Co-1000 as compared with a Co-N4 site at zero potential and equilibrium potential (U=1.23 V)[75]
Fig. 12 (a) Synthetic procedure of the Co/N-B-doped carbon nanosheet. (b) ORR polarization curves in O2-saturated 0.1 mol/L KOH[79]
Table 1 Summary of electrochemical performance of M-Nx-C electrocatalysts
Catalysts type structure Carbon carrier Acidic media Alkaline media ref
Eonesetvs
RHE(V)		 E1/2vs
RHE(V)		 Eonesetvs
RHE(V)		 E1/2vs
RHE(V)
Non-doped
M-Nx-C		 Fe-N-C histidine - - 1.046 0.87 22
Fe-N-C block co-polymer - - 1.00 0.901 28
Co-N-C the mixture of polystyrene,
polyacrylonitrile		 - - 0.95 0.86 88
Co-N-C Zn/Co-ZIF - - 0.982 0.881 30
Cr-N-C ZIF-8 - 0.773 - - 32
Cu-N-C ZIF-8 0.83 - 0.99 0.895 36
Fe-N-C 2-MeIm 0.963 0.835 - - 38
Fe-N-C ZIF-8 - 0.78 - 0.864 34
Mn-N-C ZIF-8 - - - 0.90 35
Non-metal elements
doped M-Nx-C		 Fe-N/S-C UIO-66—NH2 - 0.785 0.97 0.87 67
Fe-N/S-C formamide - 0.78 1.09 0.92 68
Fe-N/S-C porphyra - - 0.96 0.84 72
ZnCo-N/S-C chitosan - - 1.07 0.893 51
FeN3P1 - 0.89 0.72 0.941 0.867 73
FeN4P2 - 0.80 1.06 0.87 74
Co-N2P2 - - - - 0.878 75
FeCl1N4/CNS - - - - 0.921 77
Fe-N/S/P-C ZIF-8 - 0.791 - 0.912 69
Co-N/B-C - - - - 0.83 79
Mn-N/O-C Mn-BTC - - - 0.86 70
Multi-metal elements
doped M-Nx-C		 Fe/Ni-N-C ZIF-8 - - - 0.02* 56
Fe/Mn-N-C ZIF-8 - - - 0.904 57
Fe/Cu-N-C PVP - - 0.96 0.86 58
Pt1-O2-Fe-N4 - 0.93 0.80 - - 60
FeNi-N-C polydopamine - - 0.95 0.82 87
Fe/Co-N-C ZIF-8 - - 0.995 0.920 89
Fe/Co-N-C Co/Zn-ZIF 1.02 0.86 - - 61
Zn/Co-N-C Zn/Co-ZIF - 0.796 - - 63
Co/Ni-N-C CoNi-NCNT - - 0.88 0.81 64
Co/Cu-N-C DCDA - - 0.98 0.88 65
Fe/Ni-N-C polystyrene spheres,ZIF-8 - 0.840 - 0.938 90
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