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化学进展 2022, Vol. 34 Issue (10): 2190-2201 DOI: 10.7536/PC220214 前一篇   后一篇

• 综述与评论 •

金属/非金属元素掺杂提升原子级分散碳基催化剂的氧还原性能

孟鹏飞1, 张笑容1, 廖世军1,*(), 邓怡杰2,*()   

  1. 1 华南理工大学化学与化工学院 广州 510641
    2 南华大学资源环境与安全工程学院 衡阳 421001
  • 收稿日期:2022-02-17 修回日期:2022-05-04 出版日期:2022-10-24 发布日期:2022-06-25
  • 通讯作者: 廖世军, 邓怡杰
  • 基金资助:
    国家重点研发计划项目(2017YFB0102900); 国家重点研发计划项目(2016YFB0101201); 国家自然科学基金项目(51971094); 国家自然科学基金项目(21476088); 国家自然科学基金项目(21776104); 广东省自然科学基金项目(2015A030312007)
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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:2022-02-17 Revised:2022-05-04 Online:2022-10-24 Published:2022-06-25
  • 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)

原子级别分散的过渡金属和氮共掺杂碳基催化剂(M-Nx-C)具有反应活性好、选择性高、制备容易等优点,被认为是最有可能取代价格昂贵的铂催化剂用作燃料电池阴极的一类非贵金属催化剂。然而,该类催化剂在阴极侧氧还原反应过程中存在活性位点密度较低、耐久性不足的问题制约了其在燃料电池中的实际应用。研究表明,通过多种金属/非金属元素的掺杂调控活性位点的电子结构与空间构型可显著提升M-Nx-C催化剂的氧还原活性和稳定性,已成为掺杂碳基催化剂领域的热门研究课题。本文综述了近年来国内外在多种金属/非金属元素掺杂提升M-Nx-C碳基催化剂性能方面的主要研究工作,包括金属元素掺杂、非金属元素掺杂等研究。文章进一步总结和指出了M-Nx-C碳基催化剂面临的问题及挑战,并对其发展前景和未来研究方向进行了展望。

关键词： 非铂催化剂, 碳基催化剂, 氧还原, 共掺杂, 单原子催化剂

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
()
图1 硬模板合成Fe—N—C HNS[22]
Fig. 1 Schematic illustration of the hard template method for preparation of Fe—N—C HNS[22]
图2 合成Cr-N-C[21]
Fig. 2 Illustration of synthesis of Cr-N-C[21]
图3 碱性介质中ORR的催化活性图[44]
Fig. 3 Plots of catalytic activities for the ORR in alkaline media[44]
图4 活性中心的动态变化过程[47]
Fig. 4 Dynamic transformation process of active site[47]
图5 Fe-N-C和Pt1@Fe-N-C在空气饱和电解质中经过10 000次电压循环后测得的LSV曲线,0.5 mol/L H2S O 4 [ 60 ]
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 ]
图6 (a)不同催化剂在0.1 mol/L HClO4溶液中的ORR LSV曲线; (b) H2/O2燃料电池的极化图[63]
Fig. 6 (a) ORR LSV curves for different catalysts in 0.1 mol/L HClO4 solution. (b) H2/O2 fuel cell polarization plots[63]
图7 (a) 制备的样品在0.1 mol/L KOH 中的LSV曲线; (b)制备的样品在0.1 mol/L HClO4中的LSV 曲线[67]
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]
图8 (a) Fe-NSC的合成示意图;(b) 0.1 mol/L KOH 中的LSV 曲线(转速: 1600 r/min);插图为相应的半波电位和转移电子数[68]
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]
图9 Fe-N/P-C 催化剂的合成过程示意图[73]
Fig. 9 Schematic of the synthesis process of the Fe-N/P-C[73]
图10 以Fe-N-C-P/N,P-C、Fe-N-C/N-C和Pt/C为阴极催化剂的H2-O2质子交换膜燃料电池的极化和功率密度曲线图[74]
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]
图11 PSTA-Co-1000中Co-N2P2位点和Co-N4位点在零电势与平衡电势(U=1.23 V)时的ORR自由能图[75]
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]
图12 (a)Co/N-B掺杂的碳纳米片的合成流程图;(b) O2饱和的 0.1 mol/L KOH 中的ORR极化曲线[79]
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]
表1 近年M-Nx-C催化剂电化学性能汇总表
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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