ZIFs材料对Fe/N/C催化剂氧还原性能的影响

doi:10.11896/cldb.22100278

材料导报

2024, Vol. 38

Issue (10): 22100278-7 https://doi.org/10.11896/cldb.22100278

无机非金属及其复合材料

ZIFs材料对Fe/N/C催化剂氧还原性能的影响

宋冬梅^1,2, 郑秋燕^1,2, 潘廷仙^1,2, 胡长刚^1,2, 同鑫^1,2, 田娟^1,2,*

1 贵州师范大学化学与材料科学学院,贵阳 550001
2 贵州省功能材料化学重点实验室,贵阳 550001

Effect of ZIFs Materials on the Oxygen Reduction Performance of Fe/N/C Catalysts

SONG Dongmei^1,2, ZHENG Qiuyan^1,2, PAN Tingxian^1,2, HU Changgang^1,2, TONG Xin^1,2, TIAN Juan^1,2,*

1 School of Chemistry and Material Science, Guizhou Normal University, Guiyang 550001, China
2 Key Laboratory for Functional Materials Chemistry of Guizhou Province, Guiyang 550001, China

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摘要过渡金属/氮/碳(M/N/C)催化剂是替代铂基催化剂用于氧还原反应(ORR)的理想材料。沸石咪唑骨架(ZIFs)材料结合了无机沸石的高稳定性和MOFs材料的高比表面积、高孔隙率及可调孔结构等特点,是制备M/N/C催化剂的优良前驱体。本工作以FeSO₄·7H₂O为铁源,1,10-菲啰啉为氮源,探究不同ZIFs材料对FeN/C-Z_x催化剂ORR性能的影响。通过X射线衍射、比表面积和孔径分布测试、透射电子显微镜等对催化剂进行结构表征,使用线性扫描伏安法对催化剂ORR催化活性进行测试。结果表明:FeN/C-Z₈催化剂表现出最佳的ORR活性,具有较小的Tafel斜率(64.98 mV/dec)且反应过程是近四电子过程;在经过25 000次循环后,FeN/C-Z₈催化剂的半波电位仅有20 mV的负移,表现出良好的稳定性。FeN/C-Z₈催化剂中存在的Fe₃C化合物可有效提高催化剂的催化性能;Zn²⁺在碳化过程中挥发使FeN/C-Z₈催化剂具有较高比表面积(550.09 m²/g)、孔体积(1.36 cm³/g)及丰富的微孔、介孔结构,并促进了过渡金属在ZIFs材料上的均匀分布,使FeN/C-Z₈催化剂颗粒较小、分散均匀,这是该催化剂表现出较好的ORR催化性能的可能原因。

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	宋冬梅
	郑秋燕
	潘廷仙
	胡长刚
	同鑫
	田娟

关键词: 氧还原反应非贵金属催化剂沸石咪唑骨架 FeN掺杂

Abstract: Transition metal/nitrogen/carbon (M/N/C) catalysts are the most promising candidates to replace platinum-based catalysts for oxygen reduction reaction (ORR). Zeolitic imidazolate frameworks (ZIFs) are ideal precursors for the preparation of M/N/C catalysts since they combine the high stability of inorganic zeolites and the high specific surface area, high porosity, and tunable pore structure of MOFs materials. In this work, FeN/C-Z_x catalysts were synthesized using FeSO₄·7H₂O, 1, 10-phenanthroline, and ZIFs as iron, nitrogen, and carbon precursors, respectively. The effect of using different ZIFs as carbon precursors on the ORR activity of FeN/C-Z_x catalysts were investigated. The structure of the catalyst was characterized by X-ray diffraction, specific surface area and pore size distribution test, and transmission electron microscope. The catalytic activity of the catalyst for ORR was tested by linear scanning voltammetry. The results show that the FeN/C-Z₈ catalyst exhibits the best ORR activity, a small Tafel slope (64.98 mV/dec) with a nearly four-electron reaction process, and a good stability with only 20 mV negative shift in half-wave potential after 25 000 cycles of accelerated degradation tests. The Fe₃C compound, which can effectively improve the catalytic activity, present in the FeN/C-Z₈ catalyst;the high specific surface area (550.09 m²/g) and pore volume (1.36 cm³/g), the abundant micropore and mesoporous structure, as well as the uniform distribution of transition metals on the ZIFs materials and the small catalyst particles size due to the volatilization of Zn²⁺ during the carbonization process, are the possible reasons to increase the ORR catalytic performance of FeN/C-Z₈ catalyst.

Key words: oxygen reduction reaction (ORR) non-precious metal catalyst zeolitic imidazolate frameworks (ZIFs) FeN doping

出版日期: 2024-05-25 发布日期: 2024-05-28

ZTFLH:

O643.36

基金资助: 国家自然科学基金(21965006;22005072);中国科学院燃料电池及复合电能源重点实验室开放课题(KLFC201703)

通讯作者: *田娟,贵州师范大学化学与材料科学学院副教授、硕士研究生导师。2002年7月毕业于武汉大学化学与分子科学学院,获应用化学学士学位;2008年11月毕业于中国科学院大连化学物理研究所,获物理化学专业博士学位;2009年2月至2013年7月分别于加拿大魁北克大学国立科学研究院能源材料及通信研究中心和美国俄亥俄州立大学从事博士后研修。主要从事质子交换膜燃料电池铂基贵金属、非贵金属电催化剂的研究,发表论文20余篇。tianjuan@gznu.edu.cn

作者简介: 宋冬梅,2020年毕业于安徽省淮南师范学院,获得理学化学学士学位。现为贵州师范大学化学与材料科学学院硕士研究生,在田娟老师的指导下进行研究,目前主要研究领域为质子交换膜燃料电池非贵金属电催化剂。

引用本文:

宋冬梅, 郑秋燕, 潘廷仙, 胡长刚, 同鑫, 田娟. ZIFs材料对Fe/N/C催化剂氧还原性能的影响[J]. 材料导报, 2024, 38(10): 22100278-7.
SONG Dongmei, ZHENG Qiuyan, PAN Tingxian, HU Changgang, TONG Xin, TIAN Juan. Effect of ZIFs Materials on the Oxygen Reduction Performance of Fe/N/C Catalysts. Materials Reports, 2024, 38(10): 22100278-7.

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http://www.mater-rep.com/CN/10.11896/cldb.22100278 或 http://www.mater-rep.com/CN/Y2024/V38/I10/22100278

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