Luo Zhuyu, He Linfeng, Wu Jinfeng, Tian Yue, Yang Menghua, Liu Xiaoyan, Zheng Ru, Zhang Dieqing
The Education Ministry Key Lab of Resource Chemistry, Joint International Research Laboratory of Resource Chemistry, Shanghai Key Laboratory of Rare Earth Functional Materials, Shanghai Frontiers Science Center of Biomimetic Catalysis, College of Chemistry and Materials Science, Shanghai Normal University, Shanghai, 200234, China.
ChemSusChem. 2025 Jan 14;18(2):e202401552. doi: 10.1002/cssc.202401552. Epub 2024 Oct 22.
Fe single atoms (Fe SAs) based catalysts have received much attention in electrocatalytic oxygen reduction reaction (ORR) due to its low-cost and high activity. Yet, the facile synthesis of efficient and stable Fe SAs catalysts is still challenging. Here, we reported a Fe SAs anchored on N-doped mesoporous carbon microspheres (NC) catalyst via spraying drying and pyrolysis processes. The highly active Fe SAs are uniformly distributed on the NC matrix, which prevented the aggregation benefiting from the enhanced Fe-N bonds. Also, the mesoporous carbon structure is favorable for fast electron and mass transfer. The optimized Fe@NC-2-900 catalyst shows positive half wave potential (E=0.86 V vs reversible hydrogen electrodes (RHE)) and starting potential (E=0.98 V vs RHE) in ORR, which is comparable to the commercial Pt/C catalyst (E=0.87 V, E=1.08 V vs RHE). Outstanding stability with a current retention rate of 92.5 % for 9 hours and good methanol tolerance are achieved. The assembled zinc-air batteries showed good stability up to 500 hours at a current density of 5 mA cm. This work shows potentials of Fe SAs based catalysts for the practical application in ORR and pave a new avenue for promoting their catalytic performances.
基于铁单原子（Fe SAs）的催化剂因其低成本和高活性，在电催化氧还原反应（ORR）中受到了广泛关注。然而，高效且稳定的Fe SAs催化剂的简便合成仍然具有挑战性。在此，我们报道了一种通过喷雾干燥和热解过程制备的、锚定在氮掺杂介孔碳微球（NC）上的Fe SAs催化剂。高活性的Fe SAs均匀分布在NC基体上，由于增强的Fe-N键，这防止了团聚。此外，介孔碳结构有利于快速的电子和质量传递。优化后的Fe@NC-2-900催化剂在ORR中显示出正的半波电位（E = 0.86 V vs可逆氢电极（RHE））和起始电位（E = 0.98 V vs RHE），与商业Pt/C催化剂（E = 0.87 V，E = 1.08 V vs RHE）相当。实现了出色的稳定性，在9小时内电流保留率为92.5%，并且具有良好的甲醇耐受性。组装的锌空气电池在5 mA cm的电流密度下显示出高达500小时的良好稳定性。这项工作展示了基于Fe SAs的催化剂在ORR实际应用中的潜力，并为提高其催化性能开辟了一条新途径。
