Single atom electrocatalysts with typical metal–nitrogen–carbon sites possess good oxygen reduction reaction (ORR) activity, yet challenges remain in fabricating rechargeable zinc–air batteries (ZABs) due to their poor oxygen evolution reaction (OER) performance. Herein, we demonstrated the in situ anchoring of indium clusters on a carbon matrix with iron–nitrogen–carbon sites via the pyrolysis of supermolecule aggregates coordinated with indium and iron ions, aimed to prepare advanced bifunctional electrocatalysts for the ORR and OER. A detailed atomic structure analysis reveals that the modulation of the coordination environment between the indium cluster and iron–nitrogen–carbon sites induces asymmetrical charge distribution to reduce the reaction barrier via the p–d orbital hybridization, thus achieving superior bifunctional electrocatalytic activity. Consequently, the rechargeable ZABs demonstrated a cycling durability of 1650 h. Moreover, the solid-state batteries also exhibited a large power density of 220.0 mW cm⁻². This work provides a feasible guidance for rational incorporation of metal clusters with single atom sites to enhance bifunctional electrocatalysis.

中文翻译：

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铟簇与原子 Fe-N4 在碳上的耦合，用于长期可充电 Zn-air 电池


具有典型金属-氮-碳位点的单原子电催化剂具有良好的氧还原反应 （ORR） 活性，但由于其析氧反应 （OER） 性能不佳，制造可充电锌-空气电池 （ZAB） 仍然存在挑战。在此，我们展示了通过与铟和铁离子配位的超分子聚集体的热解，将铟簇原位锚定在具有铁-氮-碳位点的碳基体上，旨在制备用于 ORR 和 OER 的先进双功能电催化剂。详细的原子结构分析表明，铟簇和铁-氮-碳位点之间的配位环境的调制诱导了不对称的电荷分布，从而通过 p-d 轨道杂化减少了反应势垒，从而实现了优异的双功能电催化活性。因此，可充电 ZAB 表现出 1650 小时的循环耐久性。此外，固态电池还表现出 220.0 mW ^cm-2 的大功率密度。这项工作为合理掺入具有单个原子位点的金属团簇以增强双功能电催化提供了可行的指导。