高等学校化学学报 ›› 2022, Vol. 43 ›› Issue (9): 20220341.doi: 10.7503/cjcu20220341

• 研究论文 • 上一篇    下一篇

S掺杂Fe-N-C高活性氧还原反应催化剂

程前, 杨博龙, 吴文依, 向中华()   

  1. 北京化工大学有机无机复合材料国家重点实验室, 北京 100029
  • 收稿日期:2022-05-14 出版日期:2022-09-10 发布日期:2022-06-24
  • 通讯作者: 向中华 E-mail:xiangzh@mail.buct.edu.cn
  • 基金资助:
    国家重点研发计划项目(2017YFA0206500)

S-doped Fe-N-C as Catalysts for Highly Reactive Oxygen Reduction Reactions

CHENG Qian, YANG Bolong, WU Wenyi, XIANG Zhonghua()   

  1. State Key Laboratory of Organic?Inorganic Composites,Beijing University of Chemical Technology,Beijing 100029,China
  • Received:2022-05-14 Online:2022-09-10 Published:2022-06-24
  • Contact: XIANG Zhonghua E-mail:xiangzh@mail.buct.edu.cn
  • Supported by:
    the National Key Research and Development Program of China(2017YFA0206500)

摘要:

采用微波加热和高温碳化技术, 以ZIF-8为前驱体, 在甲醇-水双溶剂体系中先后引入Fe(NO3)3·9H2O和KSCN, 制备了一系列S掺杂的Fe-N-C催化剂(Fe3C/Fe-SAS@SNC), 并通过X射线粉末衍射、 扫描透射电子显微镜和氮气吸附-脱附测试等表征手段进行分析. 结果表明, Fe和S两种元素的合理掺杂使Fe3C/Fe-SAS@SNC催化剂具有明显的分级多孔结构, 比表面积达到673 m2/g, 在酸、 碱电解质中均表现出了优异的氧还原催化性能. 在0.1 mol/L KOH中, Fe3C/Fe-SAS@SNC催化剂的半波电位达到0.880 V(vs. RHE), 高于商业Pt/C催化剂, 且表现出了比商业Pt/C更优的稳定性. 在0.5 mol/L H2SO4中, Fe3C/Fe-SAS@SNC电催化氧还原的性能也与商业Pt/C催化剂相当.

关键词: 非贵金属催化剂, 杂原子掺杂, 氧还原反应

Abstract:

In this paper, a series of S-doped Fe-N-C catalysts were prepared by introducing Fe(NO33·9H2O and KSCN in a methanol-water two-solvent system using microwave heating and high-temperature pyrolysis techniques with ZIF-8 as the precursor. The results were analyzed by several characterization means such as X-ray powder diffraction, scanning transmission electron microscopy, and nitrogen adsorption and desorption tests. The results indicated that the reasonable introduction of both Fe and S resulted in Fe3C/Fe-SAS@SNC catalysts with obvious graded porous structure and specific surface area of 673 m2/g, which exhibited excellent catalytic performance for oxygen reduction in both acid and alkaline electrolytes. In 0.1 mol/L KOH, the half-wave potential of the Fe3C/Fe-SAS@SNC was 0.880 V(vs. RHE), which is higher than that of commercial Pt/C catalysts, and exhibited better stability than commercial Pt/C. In addition, the Fe3C/Fe-SAS@SNC electrocatalytic oxygen reduction performance in 0.5 mol/L H2SO4 is similarly comparable to that of commercial Pt/C catalysts.

Key words: Nonnoble metal catalyst, Heteroatom doping, Oxygen reduction reaction

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