Tuning the electrochemical and catalytic ORR performance of C60 by its encapsulation in ZIF-8: a solid-state analogue of dilute fullerene solution,Materials Chemistry Frontiers

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Tuning the electrochemical and catalytic ORR performance of C60 by its encapsulation in ZIF-8: a solid-state analogue of dilute fullerene solution
Materials Chemistry Frontiers ( IF 6.0 ) Pub Date : 2021-09-03 , DOI: 10.1039/d1qm00829c
Olivia Basu ₁ , Subhabrata Mukhopadhyay ₁ , Avik De ₂ , Anupam Das ₁ , Samar K. Das ₁

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Metal–organic frameworks (MOFs) with intrinsic electrochemical activity have received significant attention in the last two decades, mainly because of the high density of physically separated active sites. Yet, the potential of chemical tunability, spatial confinement and scope of heterogenization in the electrochemically inactive MOFs have been less explored. Here, we have shown that fullerene C₆₀, well-known for its rich reductive electrochemistry, when encapsulated inside zeolitic imidazolate framework-8 (ZIF-8) to prepare a heterogeneous composite (C₆₀Z), can act as a catalyst for the oxygen reduction reaction (ORR) at a lower overpotential with better selectivity than bare C₆₀ per se. Spectroscopic and electrochemical characterization methods prove significant interactions between the ZIF-8 host and the C₆₀ guest, which results in the modification of the electrochemical behavior of C₆₀ inside ZIF-8 and thereby causes an enhanced electrochemical ORR performance of the guest. The mono-confinement of C₆₀ inside ZIF-8 also results in spatial separation of C₆₀ molecules, which is highly effective for preserving its dilute solution-like behavior in solid-state inside the framework matrix. Furthermore, we have explored the scope of device processability of this solid-state analogue of dilute C₆₀ solution i.e., C₆₀Z, by its fabrication into a polymer membrane (C₆₀Z–PVA thin film) which could retain the physical properties of the C₆₀Z.

中文翻译：

通过封装在 ZIF-8 中调节 C60 的电化学和催化 ORR 性能：稀释富勒烯溶液的固态类似物

具有内在电化学活性的金属有机骨架（MOF）在过去的二十年中受到了极大的关注，主要是因为物理分离的活性位点的密度高。然而，电化学非活性 MOF 的化学可调性、空间限制和异质化范围的潜力尚未得到充分探索。在这里，我们已经证明富勒烯 C ₆₀以其丰富的还原电化学而闻名，当封装在沸石咪唑酯骨架-8（ZIF-8）中以制备多相复合材料（C ₆₀ Z）时，可以作为催化剂氧还原反应 (ORR) 在较低的过电位下具有比裸 C ₆₀ 本身更好的选择性. 光谱和电化学表征方法证明了 ZIF-8 主体和 C ₆₀客体之间的显着相互作用，这导致了ZIF-8 内部C ₆₀电化学行为的改变，从而提高了客体的电化学 ORR 性能。ZIF-8 内C ₆₀的单限制也导致 C ₆₀分子的空间分离，这对于在框架基质内保持其在固态中的稀溶液样行为非常有效。此外，我们已经探索稀的C此固态类似物的设备加工性的范围₆₀溶液即，Ç ₆₀ ž，通过将其制成聚合物膜（C ₆₀ Z-PVA薄膜），可以保留C ₆₀ Z的物理特性。

更新日期：2021-09-24

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