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Study of the mechanism of nitrogen doping in carbon supports on promoting electrocatalytic oxygen reduction reaction over platinum nanoparticles

SUN Xue-qin GAO Xin-hua WANG Ying-yong TONG Xi-li

孙雪琴, 高新华, 王英勇, 童希立. 氮掺杂碳载体促进铂纳米颗粒电催化氧还原反应的作用机制研究[J]. 燃料化学学报. doi: 10.1016/S1872-5813(22)60030-6
引用本文: 孙雪琴, 高新华, 王英勇, 童希立. 氮掺杂碳载体促进铂纳米颗粒电催化氧还原反应的作用机制研究[J]. 燃料化学学报. doi: 10.1016/S1872-5813(22)60030-6
SUN Xue-qin, GAO Xin-hua, WANG Ying-yong, TONG Xi-li. Study of the mechanism of nitrogen doping in carbon supports on promoting electrocatalytic oxygen reduction reaction over platinum nanoparticles[J]. Journal of Fuel Chemistry and Technology. doi: 10.1016/S1872-5813(22)60030-6
Citation: SUN Xue-qin, GAO Xin-hua, WANG Ying-yong, TONG Xi-li. Study of the mechanism of nitrogen doping in carbon supports on promoting electrocatalytic oxygen reduction reaction over platinum nanoparticles[J]. Journal of Fuel Chemistry and Technology. doi: 10.1016/S1872-5813(22)60030-6

氮掺杂碳载体促进铂纳米颗粒电催化氧还原反应的作用机制研究

doi: 10.1016/S1872-5813(22)60030-6
详细信息
  • 中图分类号: O643.3

Study of the mechanism of nitrogen doping in carbon supports on promoting electrocatalytic oxygen reduction reaction over platinum nanoparticles

Funds: The project was supported by National Natural Science Foundation of China (U1710112) and Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering (Grant No. 2022-K71).
More Information
  • 摘要: 氮掺杂碳通常被用作铂基催化剂电催化氧还原反应的功能载体,但是,掺杂的氮对分子氧在铂活性中心上的吸附和还原机理尚不清楚。本文采用氨气热解的方法制取氮掺杂纳米碳作为载体,并采用调节氨气热解温度进而控制不同种类氮掺杂的含量。可以使铂催化剂获得较高的零价铂含量、较大的电化学活性面积、合适的铂粒径 (2.10 nm)和电子快速传输能力从而提高电催化活性。研究发现,具有最佳氮含量掺杂的Pt/Nano-NC-800催化剂显示出优异的电催化氧还原性能(例如,半波电位为0.80 V vs RHE,极限扩散电流为5.37 mA/cm2),以及强的抗甲醇和一氧化碳中毒能力。该性能优于商业铂碳催化剂(20%.wt,JM)以及大多数沉积在碳纳米颗粒或其他载体上的铂催化剂,表现出优异的应用潜力。
  • Figure  1  (a) Raman spectra of carbon nanoparticles, Nano-NC-700, Nano-NC-800, and Nano-NC-900; (b) XRD patterns of Pt/C, Pt/Nano-NC-700, Pt/Nano-NC-800, and Pt/Nano-NC-900.

    Figure  2  TEM images of Pt/Nano-NC-700, Pt/Nano-NC-800, and Pt/Nano-NC-900 (a-c) and the corresponding size distribution of Pt nanoparticles of (d-f). The inset of a-c is the HRTEM image of three catalysts.

    Figure  3  XPS survey spectra (a) and HR-XPS spectra of (b), (c), and (d) N 1s obtained from Pt/Nano-NC-700, Pt/Nano-NC-800, and Pt/Nano-NC-900, and HR-XPS spectra Pt 4f (e) of Pt/Nano-C, Pt/Nano-NC-700, Pt/Nano-NC-800, and Pt/Nano-NC-900 catalysts.

    Figure  4  (a) RDE voltammogram of the Pt/Nano-NC-800, Pt/Nano-C, and JM Pt/C catalysts recorded in O2-saturated 0.1 mol/L HClO4 electrolyte at a scan rate of 5 mV/s at 1600 r/min; (b) corresponding Tafel plots; (c) LSVs in O2-saturated 0.1 mol/L HClO4 at different RDE rotation rates of Pt/Nano-NC-800;(d) The corresponding K-L plots of Pt/Nano-NC-800

    Figure  5  (a) Nyquist plots of the Pt/Nano-NC-800, Pt/Nano-C, and JM Pt/C catalysts and equivalent circuit model; (b) Endurance test of three catalysts tested at 0.756 V in O2-saturated 0.1 mol/L HClO4; (c) CO stripping experiments on three catalysts at 10 mV/s; (d) the addition of 4 mL of 3 mol/L methanol in O2-saturated solution at 1600 r/min

    Table  1  Results of the fits of the N 1s XPS For each single component, the binding energy (eV) and amount (%) values are given

    SamplePyridinic-N

    398.6 eV
    Pt-N

    399.4 eV
    Pyrrolic-N

    400.2 eV
    Graphitic-N

    401.1 eV
    Oxidized-N

    402.0 eV
    Pt/Nano-NC-7007.4%32.5%19.5%33.0%7.6%
    Pt/Nano-NC-8008.4%31.9%19.6%34.6%5.5%
    Pt/Nano-NC-90017.8%21.5%26.4%30.6%3.7%
    下载: 导出CSV
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  • 收稿日期:  2022-03-10
  • 录用日期:  2022-04-07
  • 修回日期:  2022-04-07
  • 网络出版日期:  2022-05-20

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