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Comparative Study on Proton Conductivity and Mechanism Analysis of Two Imidazole Modified Imine‐Based Covalent Organic Frameworks

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The effect of intramolecular hydrogen bonding on the proton conductivity of COFs was investigated. It was shown that the extrinsic proton carriers could increase the proton conductivity of DaTta, which originally had negligible proton conductivity due to intramolecular hydrogen bonds, to 0.91×10−2 S cm−1 at 100 °C/98 % RH by breaking the intramolecular H-bonds.


This work elucidates the potential impact of intramolecular H-bonds within the pore walls of covalent organic frameworks (COFs) on proton conductivity. Employing DaTta and TaTta as representative hosts, it was observed that their innate proton conductivities (σ) are both unsatisfactory and σ(DaTta)<σ(TaTta). Intriguingly, the performance of both imidazole-loaded products, Im@DaTta and Im@TaTta is greatly improved, and the σ of Im@DaTta (0.91×10−2 S cm−1) even surpasses that of Im@TaTta (3.73×10−3 S cm−1) under 100 °C and 98 % relative humidity. The structural analysis, gas adsorption tests, and activation energy calculations forecast the influence of imidazole on the H-bonded system within the framework, leading to observed changes in proton conductivity. It is hypothesized that intramolecular H-bonds within the COF framework impede efficient proton transmission. Nevertheless, the inclusion of an imidazole group disrupts these intramolecular bonds, leading to the formation of an abundance of intermolecular H-bonds within the pore channels, thus contributing to a dramatic increase in proton conductivity. The related calculation of Density Functional Theory (DFT) provides further evidence for this inference.

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