Fullerene-based materials are promising electrodes for various electrochemistry applications due to their specific electronic properties, easy functionalization, and self-assembly capability. To achieve good catalytic performance, fullerenes are always converted into unfolded fullerenes in the derived carbon electrodes. However, the potential of fullerene-based electrodes with closed-cage fullerenes, which may further reflect the fullerene's uniqueness, still needs to be explored. Here, we fabricated a new fullerene C₆₀-based electrode (C₆₀–FePc_500) by the co-assembly of C₆₀ and iron-phthalocyanine (FePc) and pyrolysis under the low temperature of 500 °C for the oxygen reduction reaction (ORR). C₆₀–FePc_500 could maintain the buckyball structure of C₆₀ with the binding of active Fe–N₄ derived from FePc. For the first time, this buckyball C₆₀/Fe–N₄ superstructured electrode with complete C₆₀s exhibited higher catalytic ORR performance than the unfolded C₆₀s electrodes from 900 °C heat treatment (C₆₀–FePc_900). Based on the structural analysis and the simulations, the excellent catalytic activity of C₆₀–FePc_500 is estimated due to the improvement of the closed-cage C₆₀s on the electronic density states of Fe–N₄ catalytic sites. This work may bring new insights into understanding the driven mechanism of fullerenes and the development of superior fullerene-based electrodes for electrocatalytic processes.

中文翻译：

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用于高效氧还原反应的 Buckyball C60/Fe–N4 超结构电极


富勒烯基材料由于其特定的电子特性、易于功能化和自组装能力，是各种电化学应用的有前途的电极。为了获得良好的催化性能，富勒烯总是在衍生的碳电极中转化为未折叠的富勒烯。然而，具有闭笼富勒烯的富勒烯基电极的潜力仍有待探索，这可能进一步反映富勒烯的独特性。在这里，我们通过 C₆₀ 和铁酞菁 （FePc） 的共组装并在 500 °C 的低温下热解氧还原反应 （ORR） 制造了一种新的富勒烯 C₆₀ 基电极 （C_{60-FePc_500}）。C_{60-FePc_500} 可以通过结合源自 FePc 的活性 Fe-N₄ 来维持 C₆₀ 的布基球结构。这种具有完整 C₆₀s 的布基球 C₆₀/Fe-N₄ 超结构电极首次表现出比 900 °C 热处理 （C₆₀–FePc_900） 后展开的 C₆₀s 电极更高的催化 ORR 性能。基于结构分析和模拟，由于闭笼 C₆₀s 对 Fe-N₄ 催化位点电子密度态的改进，估计了 C_{60-FePc_500} 的优异催化活性。这项工作可能为理解富勒烯的驱动机制和开发用于电催化过程的优质富勒烯基电极带来新的见解。