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碱性介质中Fe/N/C催化剂的氧气还原反应催化性能研究
  • ISSN号:0567-7351
  • 期刊名称:《化学学报》
  • 时间:0
  • 分类:O621.254.2[理学—有机化学;理学—化学]
  • 作者机构:[1]华东交通大学化学化工系,南昌330013
  • 相关基金:国家自然科学基金(Nos.20965003, 21163007, 21165009, 21210102011)资助.
中文摘要:

以氧化石墨烯(GO)为碳载体,K3Fe(CN)6同时作为N源和Fe源,经热处理后构建了新型Fe/N/C结构的氧气还原催化剂.在热处理过程中,氧化石墨烯上的官能团分解脱离形成活性中心,Fe元素和N元素的同时掺杂是通过氧化石墨烯与K3Fe(CN)6之间的相互作用而实现的.通过傅立叶变换红外光谱(FTIR)和X射线光电子能谱(XPS)表征证明了这种非贵金属催化剂中N元素和Fe元素的成功掺杂,在催化剂中N元素主要是以吡啶式氮、吡咯式氮和石墨式氮的形式存在,Fe(II)和Fe(III)则与其中的吡啶式氮配位形成Fe-Nx结构.采用循环伏安法(CV)和旋转圆盘电极(RDE)技术,研究其在碱性介质中对氧气还原反应(ORR)的电催化性能.实验结果显示:Fe/N/C催化剂具有良好的ORR电催化活性,在碱性溶液中的起始电位为-0.15 V,同时有着良好的稳定性和抗甲醇性能.

英文摘要:

Fuel cells have been recognized as one of the most promising power sources due to their high efficiency and low emissions.However,the high cost and scarcity of traditional Pt-based catalyst limit their commercialization.More intensive research have been focused on the development of non-noble-metal catalysts in order to replace Pt for catalyzing oxygen reduction reaction(ORR).Recently,it was reported that the Fe/N/C catalyst have high activity toward ORR.Chemical vapor deposition(CVD) is the most common method for the preparation of the Fe/N/C catalyst.However,the cost of CVD method is much higher.Here we report a facile method for the preparation of Fe/N/C catalyst for ORR in alkaline electrolyte.The catalyst is prepared by using graphene oxide as carbon support,and K3Fe(CN)6 as both nitrogen and iron sources.The precursors are then treated thermally at 800 ℃ under nitrogen atmosphere.In the process of heat treatment,the functional groups of graphene oxide are decomposed to form active center.Simultaneous doping of N and Fe can be realized by the interaction between graphene oxide and K3Fe(CN)6.The non-noble-metal catalyst is further characterized by Fourier transform infrared spectroscopy(FTIR) and X-ray photoelectron spectroscopy(XPS).It shows that N and Fe elements are successively doped into the graphene substrate.In the catalyst,N elements exist mainly in the forms of pyridine N,pyrrole N and graphite N.Fe(II) and Fe(III) are coordinated with pyridine N to form Fe-Nxstructure.The electrocatalytic activity of catalyst is evaluated by cyclic voltammetry(CV) and rotating disk electrode(RDE) experiments.The Fe/N/C catalyst shows high electrocatalytic activity toward ORR in an alkaline solution with an onset potential of-0.15 V vs.Ag/AgCl reference electrode.CVs of consecutive sweep for 2000 cycles are conducted to study the stability of the catalyst.The Fe/N/C catalyst exhibits excellent stability and methanol-tolerant ability.

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期刊信息
  • 《化学学报》
  • 北大核心期刊(2014版)
  • 主管单位:中国科学院
  • 主办单位:中国化学会 中国科学院上海有机化学研究所
  • 主编:周其林
  • 地址:上海市零陵路345号
  • 邮编:200032
  • 邮箱:hxxb@sioc.ac.cn
  • 电话:021-54925085
  • 国际标准刊号:ISSN:0567-7351
  • 国内统一刊号:ISSN:31-1320/O6
  • 邮发代号:4-209
  • 获奖情况:
  • 首届国家期刊奖,第二届国家期刊奖提名奖,中国期刊方阵“双高期刊”
  • 国内外数据库收录:
  • 俄罗斯文摘杂志,美国化学文摘(网络版),荷兰文摘与引文数据库,美国科学引文索引(扩展库),日本日本科学技术振兴机构数据库,中国中国科技核心期刊,中国北大核心期刊(2004版),中国北大核心期刊(2008版),中国北大核心期刊(2011版),中国北大核心期刊(2014版),英国英国皇家化学学会文摘,中国北大核心期刊(2000版)
  • 被引量:28694