Abstract

This work proposed a novel strategy for synthesizing highly efficient non-precious metal oxygen reduction reaction (ORR) electrocatalysts. Fe complexes were homogeneously deposited (HD) on graphene oxide through in situ hydrolysis of urea, followed by two-step pyrolysis under Ar and NH3 atmospheres, resulting in formation of Fe- and N-functionalized graphene (HD-FeN/G). The morphology, crystalline structure and elemental composition of HD-FeN/G were characterized. ORR activity was evaluated by using a rotary disk electrode (RDE) electrochemical system. HD improved the loading and distribution of the Fe–Nx composites on graphene. The ORR activity of the as-prepared HD-FeN/G in neutral medium was comparable to that of the state-of-the-art commercial Pt/C and significantly superior to a FeN/G counterpart produced via traditional approach. The ORR electron transfer number of HD-FeN/G was as high as 3.83±0.08, which suggested that ORR catalysis proceeds through a four-electron pathway. HD-FeN/G was used as a cathodic electrocatalyst in microbial fuel cells (MFCs), and the resultant HD-FeN/G-MFC showed comparable voltage output and maximum power density to those of Pt/C-MFC. The HD-FeN/G-MFC achieved a maximum power density of 885mWm−2, which was much higher than that of FeN/G-MFC (708mWm−2). These findings demonstrate that HD-FeN/G produced through the novel synthesis strategy proposed in this work would be a good candidate as cathodic electrocatalyst in MFCs.

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