A Fe Single Atom Seed‐Mediated Strategy Toward Fe3C/FeNC Catalysts with Outstanding Bifunctional ORR/OER Activities

• Published in: Advanced science Vol. 10; no. 22
• Main Authors: Chang, Jiangwei, Zhang, Qi, Yu, Jingkun, Jing, Wen, Wang, Siyang, Yin, Guangchao, Waterhouse, Geoffrey I. N., Lu, Siyu
• Format: Journal Article
• Language: English
• Published: Weinheim John Wiley & Sons, Inc 01.08.2023; John Wiley and Sons Inc; Wiley
• Subjects: Adsorption; Carbon; carbon dots; Efficiency; Electrocatalysis; Energy storage; Fe3C; Fe3C oxygen reduction reaction (ORR); Fe‐N‐C single atom catalysts; Glucose; Graphene; oxygen evolution reaction (OER); Seeds; Spectrum analysis
• ISSN: 2198-3844; 2198-3844
• DOI: 10.1002/advs.202301656

The discovery of low‐cost and high‐performance bifunctional oxygen electrocatalysts is vital to the future commercialization of rechargeable zinc‐air batteries (ZABs). Herein, a Fe single atom seed‐mediated strategy is reported for the fabrication of Fe3C species closely surrounded by FeN4C active sites with strong electronic interactions built between them and more importantly, creating optimized coordination environment, via subtly adjusting their ratio, for favorable adsorption energies of oxygen intermediates formed during oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Concretely, the voltage difference (ΔE) between the ORR half‐wave and OER potential at a current density of 10 mA cm−2 for the compositionally‐optimized FeNC/Fe3C‐op electrocatalyst is only 0.668 V, endowing itself one of the best bifunctional OER/ORR benchmarks. As a demo, ZABs assembled with FeNC/Fe3C‐op as the air cathode deliver a remarkable specific capacity (818.1 mAh gZn−1) and a power density (1013.9 mWh gZn−1), along with excellent long‐term durability (>450 h). This work extends the methodology to modulate the activity of FeN4C atomic site, undoubtedly inspiring wide explorations on the precise design of bifunctional oxygen electrocatalysts. A Fe single atom seed‐mediated strategy is reported for constructing FeNC/Fe3C composites with optimized coordination environment (FeNC/Fe3C‐op), through subtle adjusting their ratio, for favorable adsorption‐desorption pathways of O‐containing key intermediates, thus exhibiting impressive performance with an activity descriptor ∆E of 0.668 V, endowing itself one of the best bifunctional oxygen evolution reaction/oxygen reduction reaction benchmarks.