Abstract

Based on experimental and computational evidence, phthalocyanine (Pc) compounds in the form of quaternary bound metal-nitrogen (N) atoms are the most effective catalysts for oxygen reduction reaction (ORR). However, the heat treatment process used in their synthesis may compromise the ideal structure, causing the agglomeration of transition metals. To overcome this issue, we developed a novel method for synthesizing iron (Fe) single-atom catalysts with ideal structures supported by thermally exfoliated graphene oxide (GO). This was achieved through a short heat-treatment of only 2.5min involving FePc and N,N-dimethylformamide in the presence of GO. According to the synthesis mechanism revealed by this study, carbon monoxide acts as a strong linker between the single Fe atoms and graphene. It facilitates the formation of a structure containing oxygen species between FeN4 and graphene, which provides high activity and stability for the ORR. These catalysts possess an enormous number of active sites and exhibit enhanced activity towards the alkaline ORR. They have demonstrated excellent performance when applied to real electrochemical devices, such as zinc-air batteries and anion exchange membrane fuel cells. We expect that the instantaneous heat treatment method developed in our study will aid in the development of high-performing single-atom catalysts. This article is protected by copyright. All rights reserved.

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