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Hierarchically Macro–Microporous Covalent Organic Frameworks for Efficient Proton Conduction

机译：Hierarchically Macro–Microporous Covalent Organic Frameworks for Efficient Proton Conduction

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摘要

Assembling molecular proton carriers into crosslinked networks is widelyused to fabricate proton conductors, but they often suffer losses in conductionefficiency and stability accompanied by unclear causes. Covalent organicframeworks (COFs), with well-defined crystal frameworks and excellentstability, offer a platform for exploring the proton transfer process. Herein, astrategy to construct proton conductors that induce conductivity and stabilityby introducing bottom-up hierarchical structure, mass transport interfaces,and host–guest interactions into the COFs is proposed. The proton-transportplatforms are designed to possess hierarchically macro–microporous structurefor proton storage and mass transport. The protic ionic liquids, with lowproton dissociation energies investigated by DFT calculation, are installedat open channel walls for faster proton motion. As expected, the resultantproton conductors based on a covalent organic framework (PIL0.5@m-TpPa-SO_3H) with hierarchical pores increase conductivity by approximatelythree orders of magnitude, achieving the value of 1.02 × 10~(?1) S cm~(?1) (90 ℃,100 RH), and maintain excellent stability. In addition, molecular dynamicssimulations reveal the mechanism of “hydrogen-bond network” for protonconduction. This work offers a fresh perspective on COF-based materialmanufacturing for high-performance proton conductors via a protocol ofmacro-micropores.

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