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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]

[Display omitted] • COF-based membranes are utilized for C 3 H 6 /C 3 H 8 separation for the first time. • Large-sized COF pores can achieve maximum contact between Ag+ and C 3 H 6 molecules. • High-density Ag+ facilitates C 3 H 6 confined transport along nanochannel surface. • Density differences result in asymmetric structure and directional transport. • Confined mechanism with asymmetric structure provide superior separation performance. Energy-efficient membrane technology is sought to replace or integrate with conventional energy- and cost-intensive distillation for precise propylene/propane separation. Covalent organic framework (COF)-based composite membranes (CMs) are promising candidates for the representative difficult propylene/propane separation system. However, the large-size pore of COFs cannot achieve an effective separation of gas pairs with sub-angstrom (0.2 Å) size differences. Here, we design confined facilitated transport nanochannels within COFs as productive fillers to construct CMs. The anchored high-density Ag+ carriers facilitate C 3 H 6 monomolecular high-speed transport along the nanochannel surface. Under this confined transport mechanism, the problem of over-sized COF pores can be partially circumvented, and high selectivity obtained. Moreover, the obtained asymmetric configuration of SCOF-Ag/PI CMs results in directional gas transport. As the first work of COF-based membranes for olefin/paraffin separation, SCOF-Ag/PI CMs demonstrate a high propylene permeability of 75.16 barrer and good propylene/propane selectivity of 35.45, out-performing most of the polymer-based membranes and approaching the performance of ZIF-8 membranes. Furthermore, SCOF-Ag/PI CMs exhibit over one-month durability. The excellent separation performance combined with operating stability provides a promising alternative approach toward efficient C 3 H 6 /C 3 H 8 separation. [ABSTRACT FROM AUTHOR]