Metal ion-bonded two-dimensional framework non-Van der Waals sandwich heterojunctions for fast mass transfer in flexible in-plane micro-supercapacitors

IF 52.9 Q1 ELECTROCHEMISTRY

eScience Pub Date : 2025-11-01 Epub Date: 2025-04-01 DOI:10.1016/j.esci.2025.100404

Xiaoyang Xu , Zhenni Zhang , Zihao Zhang , Xiaomi Tang , Hong Chen , Tian Li , Jia Zhang , Qingliang Feng , Shanlin Qiao

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Abstract

Two-dimensional (2D) reticular framework films featuring highly accessible surface areas, tunable active sites, and well-defined channels are promising candidates for flexible in-plane micro-supercapacitor (MSC) electrodes. However, the interlayer Van der Waals forces in 2D heterojunctions can limit mass/charge transport. Herein, we design a non-Van der Waals force bonded heterojunction of covalent organic frameworks (COFs) and metal–organic frameworks (MOFs) linked by metal-ion coordination. A COF@MOF monolithic nanofilm is constructed by growing MOF (M₃(HHTP)₂) in situ on the COF (COF_TD) surface, using nickel (Ni) as the optimal metal to connect the two layers and form a sandwich electrode. We further explore various transition metals in M₃(HHTP)₂, from manganese (Mn) to zinc (Zn), to adjust the electronic structure and charge redistribution. The optimal MSC-Ni-COF_TD@Co₃(HHTP)₂ device exhibits an impressive specific capacitance (1645.3 F cm⁻³ at 10 mV s⁻¹), a high energy density (146.3 mWh cm⁻³), as well as superior cycling and bending stability. This work offers an innovative perspective on overcoming the mass transfer and electron migration limitations of 2D reticular frameworks for miniaturization and wearable energy storage electronics.

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金属离子键合二维框架非范德华夹层异质结在柔性面内微型超级电容器中的快速传质

二维（2D）网状框架薄膜具有高度可接近的表面积、可调的活性位点和明确的通道，是柔性面内微超级电容器（MSC）电极的有希望的候选者。然而，二维异质结中的层间范德华力会限制质量/电荷输运。本文设计了共价有机骨架（COFs）和金属-有机骨架（MOFs）通过金属离子配位连接的非范德华力键异质结。通过在COF （COFTD）表面原位生长MOF (M3(HHTP)2)，以镍（Ni）作为连接两层的最佳金属，形成夹层电极，构建了COF@MOF单片纳米膜。我们进一步探索了M3(HHTP)2中的各种过渡金属，从锰（Mn）到锌（Zn），以调节电子结构和电荷再分配。最佳的MSC-Ni-COFTD@Co3(HHTP)2器件具有令人印象深刻的比电容（10mv s - 1时1645.3 F cm - 3），高能量密度（146.3 mWh cm - 3），以及优越的循环和弯曲稳定性。这项工作为克服小型化和可穿戴储能电子设备的二维网状框架的传质和电子迁移限制提供了一个创新的视角。

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来源期刊

eScience

CiteScore

33.70

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0.00%

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