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Molten-salt/oxalate mediating Fe and N-doped mesoporous carbon sheet nanostructures towards highly efficient and durable oxygen reduction electrocatalysis
Microporous and Mesoporous Materials ( IF 4.8 ) Pub Date : 2020-04-28 , DOI: 10.1016/j.micromeso.2020.110281
Chaozhong Guo , Rong Zhou , Zhaoxu Li , Yujun Si , Wenli Liao , Wei Sun , Shijie Xiang , Xinyi Luo , Meifang Luo , Zhongli Luo

Designer Fe-N/C-type oxygen reduction electrocatalysts with ultrahigh active-sites density and distinctive physical properties are recently considered to be a new frontier in energy technology. In this work, we creatively propose a new strategy for the controllable synthesis of iron and nitrogen co-doped mesoporous Fe-N/C-type graphene-like carbon nanosheet structures via NaCl template-assisted two-step calcination of iron coordinated with triazine compounds using potassium oxalate as a pore-activator. The synthesized Fe-N/C electrocatalyst exhibits unexpectedly ORR catalytic performance with a half-wave potential of ca. 0.846 V and an onset potential of ca. 1.02 V that compare favourably with the best Pt/C catalyst, but its electrochemical stability and methanol-tolerant property are more excellent. It is found that the unique mesoporous structure, the excellent electro-conductivity and the full exposure of N-doped catalytic sites (e.g., pyridinic-N, graphitic-N and Fe-Nx) of the gained Fe-N/C catalyst can facilitate the transport of electrolyte ions, reaction intermediates and products, maintain continuous electron-transport pathways, and minimize the agglomeration of catalytic sites to further boost the reaction rate and ORR activity. This study provides a new avenue to design high-performance and low-cost nanocarbon-based catalytic materials with dense active sites for some important reactions in new energy devices.



中文翻译:

熔融盐/草酸盐介导Fe和N掺杂的中孔碳片纳米结构,以实现高效,持久的氧还原电催化

具有超高活性位点密度和独特物理性能的专业Fe-N / C型氧还原电催化剂最近被认为是能源技术的一个新领域。在这项工作中,我们创造性地提出了一种新的策略,该方法通过NaCl模板辅助的铁与三嗪化合物的两步煅烧来可控合成铁和氮共掺杂的介孔Fe-N / C型石墨烯样碳纳米片结构用草酸钾作为孔活化剂。合成的Fe-N / C电催化剂具有出乎意料的ORR催化性能,其半波电势约为。0.846 V,起始电位约为1.02 V可以与最佳的Pt / C催化剂相比,但其电化学稳定性和耐甲醇性更优异。发现所获得的Fe-N / C催化剂具有独特的介孔结构,优异的导电性和N掺杂的催化位点(例如吡啶-N,石墨-N和Fe-N x)的完全暴露。促进电解质离子,反应中间体和产物的传输,保持连续的电子传输路径,并使催化位点的聚集最小化,从而进一步提高反应速率和ORR活性。这项研究为设计高性能,低成本的纳米碳基催化材料提供了一条新途径,该催化材料具有密集的活性位,可用于新能源设备中的一些重要反应。

更新日期:2020-04-28
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