摘要
Two-dimensional covalent organic framework nanosheets(CONs)with ultrathin thickness and porous crystalline nature show substantial potential as novel membrane materials.However,bringing CONs materials into flexible membrane form is a monumental challenge due to the limitation of weak interactions among CONs.Herein,one-dimensional silk nanofibrils(SNFs)from silkworm cocoon are designed as the nanobinder to link sulfonated CON(SCON)into robust SCON-based membrane through vacuum-filtration method.Ultrathin and large lateral-sized SCONs are synthesized via bottom-up interface-confined synthesis approach.Benefiting from high length-diameter ratio of SNF and rich functional groups in both SNF and SCON,two-dimensional(2D)SCONs are effectively connected together by physical entanglement and strong H-bond interactions.The resultant SCON/SNF membrane displays dense structure,high mechanical integrity and good stability.Importantly,the rigid porous nanochannels of SCON,high-concentration-SO3H groups insides the pores and H-bonds at SCON-SNF interfaces impart SCON/SNF membrane high-rate proton transfer pathways.Consequently,a superior proton conductivity of 365 mS cm^(-1)is achieved at 80C and 100%RH by SCON/SNF membrane.This work offers a promising approach for connecting 2D CON materials into flexible membrane as high-performance solid electrolyte for hydrogen fuel cell and may be applied in membrane-related other fields.