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A Unique Quadruple-Site System Integrating Fe-N4 Sites and Zn Atomic Clusters for Oxygen Reduction Reaction and
Ying Zhang1, Li Bo Chen1, Xu Liu1
1Key Laboratory of Automobile Materials (Jilin University), Ministry of Education, and School of Materials Science and Engineering, Jilin University, Changchun 130022, China.
Abstract:
Fe-N-C single-atom catalysts (SACs) featuring Fe-N4 configurations face challenges in the simultaneous enhancement of intrinsic oxygen reduction reaction (ORR) activity and long-term stability. Herein, we developed a unique quadruple-site cooperative system through a 90 s ultrafast thermal shock strategy, where most Zn atomic clusters are surrounded by two closely neighboring and a further Fe-N4 sites (FeSA/ZnAC-N-C). Density functional theory and molecular dynamics simulations jointly reveal that proximal Fe-N4-modified Zn atomic clusters mediate O2 adsorption/activation/hydrogenation, while distal Fe-N4 sites facilitate H2O formation/desorption. This synergistic dual-active-center configuration achieves a positive half-wave potential of 0.90 V and superb durability. The constructed aqueous FeSA/ZnAC-N-C-based Zn-air batteries demonstrate a large maximum power density of 161.5 mW cm-2, a high specific discharge capacity of 792.7 mAh g-1, and stable operation over 1500 cycles. In addition, the fabricated quasi-solid-state Zn-air batteries also maintain favorable operation across a wide temperature range (-30 to 60 °C) and at the ampere scale.
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