Zhang Da, Ding Ruixin, Zhang Chuanqi, Tang Yuanzheng, Yuan Tiejian, Dong Qianpeng, Bi Lansen, Shi Song, He Yan
College of Electromechanical Engineering, Shandong Engineering Laboratory for Preparation and Application of High-performance Carbon Materials, Qingdao University of Science and Technology, Qingdao 266061, China.
Langmuir. 2022 Aug 2;38(30):9310-9320. doi: 10.1021/acs.langmuir.2c01130. Epub 2022 Jul 21.
It is of significant implication to fabricate high-performance, durable and low-cost catalysts toward to oxygen reduction reaction (ORR) to drive commercial application of fuel cells. In our work, we synthesize the Fe/N-CNT catalyst via one-pot grinding combined with calcination using a mixture of carbamide, CNTs and iron salts as precursors, the as-synthesized catalysts show the structure that Fe nanoparticles are encapsulated in the tube of intertwined CNTs with abundant active sites. The catalyst is synthesized at 800 °C (Fe/N-CNT-800-20) obtain high graphitization degree and high N doped content, especially the high content and proportion of Fe-N and pyridinic-N, exhibiting outstanding ORR activity. Moreover, too high calcination temperature (850 °C) and high Fe content (25%) lead to the agglomeration of Fe during the calcination, which blocked some catalytic sites, leading to poor ORR activity. This facile synergy route will provide new thoughts for the fabrication and optimization of catalysts.
制备高性能、耐用且低成本的氧还原反应（ORR）催化剂以推动燃料电池的商业应用具有重要意义。在我们的工作中，我们以尿素、碳纳米管（CNTs）和铁盐的混合物为前驱体，通过一锅研磨结合煅烧的方法合成了Fe/N-CNT催化剂，所合成的催化剂呈现出Fe纳米颗粒被包裹在具有丰富活性位点的交织CNTs管中的结构。在800℃合成的催化剂（Fe/N-CNT-800-20）具有高石墨化程度和高氮掺杂含量，特别是Fe-N和吡啶氮的高含量及高比例，表现出优异的ORR活性。此外，过高的煅烧温度（850℃）和高Fe含量（25%）会导致煅烧过程中Fe的团聚，从而阻塞一些催化位点，导致ORR活性较差。这种简便的协同路线将为催化剂的制备和优化提供新思路。
