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One-pot synthesis of Fe/Cu/N-doped carbon materials derived from shale oil for efficient oxygen reduction reaction
Molecular Catalysis ( IF 3.9 ) Pub Date : 2020-12-17 , DOI: 10.1016/j.mcat.2020.111330
Xiaobo Chen , Rumeng Qin , Zhiqiang Li , Shengjie Shan , Yibin Liu , Chaohe Yang

In this study, the nitrogen compounds in shale oil were extracted using a metal complexation method with FeCl3·6H2O as the chelating agent. Subsequently, with complexes as raw materials, carbon materials doped with metals and nitrogen were successfully prepared using the one-pot method. The performances of the prepared Fe/Cu/N-doped carbon materials in the electrocatalytic oxygen reduction reaction (ORR) were investigated. Adding Cu to Fe@NC produced a new Fe4N species in addition to pyrrolic N-M, thereby improving the ORR performance of FeCu@NC. FeCu1.0@NC exhibited the largest content of pyrrolic-N and the highest ORR activity (initial potential = 0.8883 V, limiting current density = 6.59 mA cm−2). Its stability and methanol poisoning resistance were superior to those of commercial Pt/C electrodes. Fumed silica was used as a hard template to introduce mesopores and macropores into FeCu1.0@NC (FeCu1.0@NC-SK) and further improve its ORR activity (initial potential = 0.8973 V, limiting current density = 8.0 mA cm−2). The half-wave potential of FeCu1.0@NC-SK was 0.79 V and the electron transfer number was ∼3.99, which is close to that of commercial Pt/C catalysts. This method therefore solves the issues related to treating the complexing denitrogenation residues of shale oil, while also producing Fe/Cu/N-doped carbon materials exhibiting good ORR performances.



中文翻译:

页岩油一锅法合成Fe / Cu / N掺杂碳材料可有效进行氧还原反应

在这项研究中,使用FeCl 3 ·6H 2 O作为螯合剂的金属络合方法提取了页岩油中的氮化合物。随后,以配合物为原料,通过一锅法成功地制备了金属和氮掺杂的碳材料。研究了制备的Fe / Cu / N掺杂碳材料在电催化氧还原反应(ORR)中的性能。除吡咯NM外,向Fe @ NC中添加Cu还产生了新的Fe 4 N物质,从而改善了FeCu @ NC的ORR性能。FECU 1.0 @NC表现出吡咯-N最大含量和最高ORR活性(初始电位= 0.8883 V,极限电流密度=6.59毫安厘米-2)。其稳定性和抗甲醇中毒性优于市售Pt / C电极。使用气相二氧化硅作为硬模板,将中孔和大孔引入FeCu 1.0 @NC(FeCu 1.0 @ NC-SK)中,并进一步提高其ORR活性(初始电势= 0.8973 V,极限电流密度= 8.0 mA cm -2)。FeCu 1.0 @ NC-SK的半波电势为0.79 V,电子转移数为〜3.99,接近于商用Pt / C催化剂。因此,该方法解决了与处理页岩油的络合脱氮残余物有关的问题,同时还生产了具有良好ORR性能的Fe / Cu / N掺杂碳材料。

更新日期:2020-12-17
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