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[Display omitted] • A hydrogen-bond binding strategy is proposed to fabricate iCOF nanosheets (iCONs) and tannic acid (TA) composite membranes. • TA nanoaggregates were synthesized as hydrogen-bond binders. • Abundant hydrogen-bond interactions enable flexible connection between iCONs. • Highly interconnected hydrogen-bond networks facilitate rapid proton transport. • The membranes showed both enhanced mechanical properties and proton conductivity. Robust and highly conductive proton exchange membrane (PEM) is the unremitting pursuit of numerous electrochemical energy technologies such as fuel cell and the emerging electrochemical hydrogen compression. Ionic covalent organic framework nanosheets (iCONs) with long-range ordered nanochannels and abundant ionic groups show substantial potential as next-generation PEM materials. However, it is challenging to assemble iCONs into membranes with both robustness and flexibility due to the electrostatic repulsion and rigid framework. Herein, we propose a hydrogen-bond binding strategy to fabricate sulfonic iCON (SCON) composite membranes by co-assembling tannic acid (TA) nanoaggregates and SCONs. The abundant and dynamically reversible hydrogen-bond interactions introduced by TA nanoaggregates establish effective linkage between SCONs and allow some restricted movements, endowing membranes with remarkably improved mechanical properties. The stacked SCONs construct long-range ordered nanochannels with well-arranged sulfonic groups in membranes, and the hydrogen-bond networks further facilitate the proton transport through Grotthuss mechanism. Consequently, TA/SCON composite membranes displays significantly enhanced tensile strength of 101.9 MPa, good flexibility and high proton conductivity of 490.1 mS cm−1 at 80 °C and 100 % RH simultaneously. This hydrogen-bond binding strategy offers a promising approach to fabricate robust and highly conductive PEMs for various proton-conducting applications. [ABSTRACT FROM AUTHOR]

Developing effective organic solvent nanofiltration (OSN) membranes to separate molecular solutes from organic solvents is highly desired yet requires a suitable material platform and an in-depth investigation of membrane selectivity. Herein, an oriented ionic covalent organic framework membrane (oi -COM) was fabricated, which features well-ordered channels that are vertically aligned towards the membrane surface and lined with abundant sulfonate groups. Filtration experiments of multifarious organic solvents and solutes with different charges and molecular sizes were conducted. The oi -COM exhibited above 99% rejection for negatively charged dye (Evans blue), much higher than that for positively charged dye with similar molecular size, while maintaining high solvent permeance for ethanol of 63 L m−2 h−1 bar−1. These results demonstrated the significance of electrostatic repulsion effect in membrane selectivity, providing insights for the design of high-performance OSN membranes. Oriented ionic COF nanosheet membranes are fabricated, which demonstrate high organic solvent nanofiltration performance and charge-controlled molecular separation. [Display omitted] • Oriented ionic COF nanosheet membranes were fabricated and applied to organic solvent nanofiltration. • The membranes displayed well-defined, vertically aligned and high-density charged channels. • The membranes exhibited excellent solvent permeance for ethanol of 63 L m−2 h−1 bar−1. • The membranes exhibited <99% rejection of anionic dyes, much higher than cationic dyes. • The effect of electrostatic repulsion on membrane selectivity in organic solvents has been demonstrated. [ABSTRACT FROM AUTHOR]