Rong Yan, Huang Siping
College of Resources & Environment and Historical Culture, Xianyang Normal University, 43 Wenlin Road, Weicheng District, Xianyang 712000, China.
College of Chemistry and Chemical Engineering, Xianyang Normal University, 43 Wenlin Road, Weicheng District, Xianyang 712000, China.
Nanomaterials (Basel). 2022 Jun 19;12(12):2106. doi: 10.3390/nano12122106.
The development of low-cost, highly active, and stable oxygen reduction reaction (ORR) catalysts is of great importance for practical applications in numerous energy conversion devices. Herein, iron/nitrogen/phosphorus co-doped carbon electrocatalysts (NPFe-C) with multistage porous structure were synthesized by the self-template method using melamine, phytic acid and ferric trichloride as precursors. In an alkaline system, the ORR half-wave potential is 0.867 V (vs. RHE), comparable to that of platinum-based catalysts. It is noteworthy that NPFe-C performs better than the commercial Pt/C catalyst in terms of power density and specific capacity. Its unique structure and the feature of heteroatom doping endow the catalyst with higher mass transfer ability and abundant available active sites, and the improved performance can be attributed to the following aspects: (1) Fe-, N-, and P triple doping created abundant active sites, contributing to the higher intrinsic activity of catalysts. (2) Phytic acid was crosslinked with melamine to form hydrogel, and its carbonized products have high specific surface area, which is beneficial for a large number of active sites to be exposed at the reaction interface. (3) The porous three-dimensional carbon network facilitates the transfer of reactants/intermediates/products and electric charge. Therefore, Fe/N/P Co-doped 3D porous carbon materials prepared by a facile and scalable pyrolysis route exhibit potential in the field of energy conversion/storage.
开发低成本、高活性且稳定的氧还原反应(ORR)催化剂对于众多能量转换装置的实际应用至关重要。在此,以三聚氰胺、植酸和三氯化铁为前驱体,通过自模板法合成了具有多级多孔结构的铁/氮/磷共掺杂碳电催化剂(NPFe-C)。在碱性体系中,ORR半波电位为0.867 V(相对于可逆氢电极),与铂基催化剂相当。值得注意的是,NPFe-C在功率密度和比容量方面比商业Pt/C催化剂表现更好。其独特的结构和杂原子掺杂特性赋予催化剂更高的传质能力和丰富的可用活性位点,性能提升可归因于以下几个方面:(1)铁、氮和磷三重掺杂产生了丰富的活性位点,有助于提高催化剂的本征活性。(2)植酸与三聚氰胺交联形成水凝胶,其碳化产物具有高比表面积,有利于大量活性位点在反应界面暴露。(3)多孔三维碳网络促进了反应物/中间体/产物和电荷的转移。因此,通过简便且可扩展的热解路线制备的铁/氮/磷共掺杂三维多孔碳材料在能量转换/存储领域展现出潜力。