The rational design of highly efficient, low-cost, and durable electrocatalysts to replace platinum-based electrodes for oxygen reduction reaction (ORR) is highly desirable. Although atomically dispersed supported metal catalysts often exhibit excellent catalytic performance with maximized atom efficiency, the fabrication of single-atom catalysts remains a great challenge because of their easy aggregation. Herein, a simple ionothermal method was developed to fabricate atomically dispersed Fe–N_x species on porous porphyrinic triazine-based frameworks (FeSAs/PTF) with high Fe loading up to 8.3 wt %, resulting in highly reactive and stable single-atom ORR catalysts for the first time. Owing to the high density of single-atom Fe–N₄ active sites, highly hierarchical porosity, and good conductivity, the as-prepared catalyst FeSAs/PTF-600 exhibited highly efficient activity, methanol tolerance, and superstability for oxygen reduction reaction (ORR) under both alkaline and acidic conditions. This work will bring new inspiration to the design of highly efficient noble-metal-free catalysts at the atomic scale for energy conversion.

中文翻译：

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碱性和酸性介质中基于卟啉三嗪的骨架中原子分散的铁氮活性位点，用于氧还原反应

迫切需要高效，低成本和耐用的电催化剂来代替用于氧还原反应（ORR）的铂基电极的合理设计。尽管原子分散的负载型金属催化剂通常表现出优异的催化性能和最大的原子效率，但是单原子催化剂的制造由于其易于聚集而仍然是一个巨大的挑战。本文中，开发了一种简单的电热方法，以在多孔卟啉三嗪基骨架（FeSAs / PTF）上制备原子分散的Fe–N _x物种，其中Fe的载量高达8.3 wt％，从而产生了高反应性和稳定的单原子ORR催化剂首次。由于单原子Fe–N ₄的高密度制备的催化剂FeSAs / PTF-600具有活性位点，高度分层的孔隙率和良好的电导率，在碱性和酸性条件下均表现出高效的活性，甲醇耐受性和氧还原反应（ORR）的超稳定性。这项工作将为设计用于原子转化的高效无贵金属催化剂带来新的灵感。