Abstract Introducing mesopores into covalent organic frameworks (MesoCOFs) has been proven effective in optimizing ion transport for energy storage and related applications. Achieving precise mesopore-micropore structural control to concomitantly regulate interfacial reactions and flux uniformity remains a significant challenge. Herein, we report a versatile interfacial-energy-driven emulsion assembly strategy for the facile synthesis of MesoCOFs with diverse symmetries, mesophases and pore sizes. By tailoring the water/oil ratio in the meticulously designed water–mesitylene–dioxane–F127 system, the emulsion phases (positive and reverse), micelle structures (positive and reverse), and assembly behaviors (homogeneous and heterogeneous) can be systematically adjusted. Microanalysis reveals that the interfacial energy between water and the TMB phase increases with the amount of non-continuous phase in a given emulsion phase, which drives the swelling of micelles and then the transformation from homogeneous assembly to interfacial assembly, creating an emulsion assembly kaleidoscope. Given this, we construct a library of MesoCOF nanospheres with symmetries (from nanospheres to asymmetric cones and bowls), mesophases (spherical and dendritic) and pore sizes (13.2–48.5 nm). As a proof of concept, the dendritic MesoCOF nanospheres with abundant electron-rich C = N bonds and mesochannels are employed as functional ionic dividers to accelerate Zn2+ desolvation and homogenize the ion flux in Zn metal batteries, achieving a prolonged cycle life of over 1340 h at 1.0 mA cm−2.
Wan et al. (Fri,) studied this question.
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