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arXiv · 2403.01198

Organic solvent boosts charge storage and charging dynamics of conductive MOF supercapacitors

Ming Chen·Taizheng Wu·Liang Niu·Ting Ye·Wenlei Dai·Liang Zeng·Alexei A. Kornyshev·Zhenxiang Wang·Zhou Liu·Guang Feng
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Abstract

Conductive metal-organic frameworks (c-MOFs) and ionic liquids (ILs) have emerged as auspicious combinations for high-performance supercapacitors. However, the nanoconfinement from c-MOFs and high viscosity of ILs slow down the charging process. This hindrance can, however, be resolved by adding solvent. Here, we performed constant-potential molecular simulations to scrutinize the solvent impact on charge storage and charging dynamics of MOF-IL-based supercapacitors. We find conditions for >100% enhancement in capacity and ~6 times increase in charging speed. These improvements were confirmed by synthesizing near-ideal c-MOFs and developing multiscale models linking molecular simulations to electrochemical measurements. Fundamentally, our findings elucidate that the solvent acts as an ionophobic agent to induce a substantial enhancement in charge storage, and as an ion traffic police to eliminate convoluted counterion and co-ion motion paths and create two distinct ion transport highways to accelerate charging dynamics. This work paves the way for the optimal design of MOF supercapacitors.

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Ming Chen, Taizheng Wu, Liang Niu, Ting Ye, Wenlei Dai, Liang Zeng, Alexei A. Kornyshev, Zhenxiang Wang, Zhou Liu, Guang Feng. 2024-03-02. Organic solvent boosts charge storage and charging dynamics of conductive MOF supercapacitors. https://arxiv.org/abs/2403.01198

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