无机材料学报

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蜂窝状碳负载铁基单原子催化剂的制备及ORR催化性能研究

刘自若, 刘炜, 郝策, 胡金文, 史彦涛   

  1. 大连理工大学化工学院化学系,大连 116024
  • 收稿日期:2020-11-04 修回日期:2020-12-07 出版日期:2021-01-07 发布日期:2020-12-30
  • 作者简介:刘自若(1996-),女,硕士研究生.E-mail:lzr@mail.dlut.edu.cn.
  • 基金资助:
    国家自然科学基金面上项目(51773025)

Honeycomb-Like Carbon-Supported Fe Single Atom Catalyst: Preparation and Electrocatalytic Performance in Oxygen Reduction Reaction

LIU Ziruo, LIUWei, HAOCe, HU Jinwen, SHI Yantao   

  1. Department of Chemistry, School of Chemical Engineering, Dalian University of Technology, Dalian116024, China
  • Received:2020-11-04 Revised:2020-12-07 Online:2021-01-07 Published:2020-12-30
  • About author:LIUZiruo (1996-), female, Master candidate. E-mail: lzr@mail.dlut.edu.cn
  • Supported by:
    General Program of National Natural Science Foundation of China(51773025)

摘要: 单原子催化剂(SACs)以近100%的原子利用率以及优秀的催化活性等,在促进多相催化方面受到广泛关注。然而,由于金属原子在高温下易烧结,SACs的合成仍然具有挑战性。本研究利用熔融盐(MS)提供的强极性环境,制备了以氮掺杂碳为载体的铁基单原子催化剂(FeSA-NC)。结果表明,FeSA-NC显示出蜂窝状的多孔形貌,比表面积高达2072.5m2g-1,其中Fe元素的含量为0.57wt%。通过球差电镜直接观察到了孤立存在的Fe单原子,并通过X射线吸收精细结构(XAFS)分析确定Fe单原子以Fe-N4配位体形式分散在碳基材料上。Fe SA-NC催化剂在0.1 mol/L KOH 溶液中半波电位为0.85V,极限电流密度为5.79mA cm-2,超过商业Pt/C催化剂。Fe SA-NC催化剂不仅对ORR四电子途径显示出高选择性(H2O2产率嗯嗯嗯2%,转移电子数为3.9),同时表现出优秀的抗甲醇性能。 Abstract: Single atom catalysts (SACs) have emerged as an attractive concept for promoting heterogeneous reactionsdue to the unique properties, such as high activity and nearly 100% atom utilization. However, the synthesis ofSACs remains a challengedue tothe sintering of metal atoms at high temperature. In this study, Fe single atom on N doped porouscarbon (Fe SA-NC)catalyst was obtained by the ultrastrong polarity of molten salt (MS). Fe SA-NC shows honeycomb-like porous morphology and possesses a high specific surface areaof 2072.5 m2 g -1.The content of Fe element in FeSA-NC is 0.57wt%. The isolated Fe atomsare observed by AC HAADF-STEM, and the X-ray absorption fine structure (XAFS) analysis confirms that Fe atomsare dispersed in the form of Fe-N4 on the carbonsubstrate.Fe SA-NC shows 0.85 V half-wave potential and 5.79mA cm-2maximum current density for ORR in 0.1 mol/L KOH solution. Fe SA-NCdemonstrates highselectivityforORR four electron pathway (H2O2 yield 嗯嗯嗯2%, electron transfer number is 3.9), outstanding stability, and good methanol tolerance.

关键词: 单原子催化剂, 多孔, 氮掺杂碳, 氧还原反应

Key words: single atom catalysts, porous, nitrogen-doped carbons, oxygen reduction reaction

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