Implanting Atomically Dispersed Fe Atoms with Dense Active Sites into Carbon Nanospheres for Efficient Oxygen Reduction Electrocatalysis in Anion Exchange Membrane Fuel Cells

作者：Chao Ge, Zhijuan Li, Jing Li, Yingna Chang, Bin He, Yunlan Gu, Yawen Tang, Tongfei Li · 发表于：ACS Sustainable Chemistry & Engineering · 年份：2025 · DOI：10.1021/acssuschemeng.5c01323 · 被引用次数：21 · 研究领域：Electrocatalysts for Energy Conversion、Fuel Cells and Related Materials、Advanced battery technologies research

Iron single-atom catalysts (SACs) featuring edge-located metal sites have attracted increasing attention as highly effective catalysts for the oxygen reduction reaction (ORR). However, it continues to be a significant challenge that their performance in practical devices, such as anion exchange membrane fuel cells (AEMFCs), is still unsatisfactory due to the sparse distribution of available active sites and prominent electrocatalytic performance. In this work, a facile and scalable SiO 2 hard-template approach is elaborately designed to fabricate an Fe SAC immobilized onto N,O-doped carbon nanospheres with highly dense active sites (Fe-N-CNS) for efficient ORR electrocatalysis. Experimental analyses affirm that the constructed Fe active sites are determined as an atomically dispersed FeN 4 coordination configuration, where the metal–support interaction between these two components involves electron transfer from FeN 4 to a N,O-doped carbon matrix, thereby modulating the electronic redistribution and binding energies of O-related intermediates for the improvement of ORR intrinsic activity. As anticipated, the optimal Fe-N-CNS showcases an exceptional ORR capability, encompassing notable ORR activity and featuring a strikingly higher half-wave potential value ( E 1/2, 0.85 V), a high density of accessible FeN 4 sites (20 μmol g –1 ), enhanced stability, and an impressive methanol tolerance. More excitingly, this integrated catalyst achieves an outstanding peak power density of ...