Bifunctional Oxygen Electrocatalytic Performance of Atomically Dispersed Fe anchored on N doped Graphene

doi:10.15541/jim20250519

Abstract

Abstract: With the growing demand for efficient and environmentally friendly energy storage systems, zinc-air batteries have emerged as highly promising energy storage devices due to their high energy density, low cost, and environmental friendliness. The oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), which suffer from sluggish kinetics, are critical factors limiting battery performance. Therefore, the development of high-performance and low-cost bifunctional oxygen electrocatalysts is of great significance. In this work, Fe single atoms / clusters anchored graphene hybrid catalysts (Fe-N/Gra) were prepared via a ball-milling assisted pyrolysis method. A series of Fe-N/Gra catalysts were obtained by adjusting the mass ratio of the metal phthalocyanine precursor to graphene, and their bifunctional oxygen electrocatalytic performances were systematically investigated. The results demonstrate that the loading amount of different metal phthalocyanine precursors exerts a significant influence on the catalytic performance of the catalysts. When the loading amount of iron phthalocyanine was 0.02 g, the resulting Fe-N/Gra-0.02 catalyst exhibited the optimal bifunctional catalytic activity for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER): its ORR half-wave potential reached as high as 0.911 V, and the OER overpotential was 610 mV at a current density of 10 mA•cm^-2. The rechargeable zinc-air batteries assembled with this catalyst as the air electrode achieved a maximum power density of 315 mW•cm^-2 and could sustain stable discharge for 220 h at 10 mA•cm^-2. The excellent bifunctional oxygen catalytic activity of Fe-N/Gra-0.02 is mainly attributed to the atomically dispersed FeN_x active sites and the high electrical conductivity of graphene support. In addition, the agglomeration of active sites in the catalysts with excessive loading amounts is detrimental to the manifestation of their high-efficiency catalytic activity. This work provides an experimental basis for the controllable preparation of high-performance non-noble metal bifunctional oxygen catalysts and their practical applications in rechargeable zinc-air batteries.

Key words: iron-anchored nitrogen-doped graphene, single-atom/cluster, oxygen reduction reaction, oxygen evolution reaction, Zn-air battery

CLC Number:

TB383

WANG Jiahui, LIU Jingjing, QIU Yi, WANG Yongxia, CUI Xiangzhi. Bifunctional Oxygen Electrocatalytic Performance of Atomically Dispersed Fe anchored on N doped Graphene[J]. Journal of Inorganic Materials, DOI: 10.15541/jim20250519.

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