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Herein, according to the polydopamine (PDA)-based imprinting and thermal-induced imprinting methods, we reported on the development and applications of double-layer-imprinted mixed matrix membranes (DI-MMMs) through a dual-imprinted strategy, thereinto, the tetracycline (TC), one of the pollution-intensive pharmaceutical and personal care products, was chosen as template molecule. As to the first-TC-imprinted layer, the blended PDA-based TC-imprinted activated carbon (AC) and SiO 2 were both used for the preparation of membrane. Next, κ-carrageenan-modified graphene oxide (GO) nanosheets would be regarded as the surface-loaded layer to support the thermal-induced imprinting synthesis (second-TC-imprinted layer). Importantly, high adsorption capacity at around at 106.44 mg/g and fast adsorption rate (within 60 min) had been successfully obtained. Importantly, permselectivity rates (β) of our imprinting membranes were obtained as 3.60, 3.33 and 3.51, respectively. Overall, based the practical selective separation and scalability analysis, we believed that the as-prepared DI-MMMs with high-intensitive recognizability and permeability of template molecule would provide a possibility for breaking the permeability-selectivity trade-off of molecularly imprinted membrane materials. Porous&permeable double-layer-imprinted mixed-matrix membranes, in which TC was used as template molecule, were constructed based on our newly-developed synergetic synthesis strategy of double-TC-imprinted layers. [Display omitted] • PDA-based imprinting & thermal-induced imprinting methods were first proposed. • Double-layer-imprinted mixed-matrix membrane structures was successfully constructed. • Well-designed TC-imprinted membrane was applied as selective separation device. • High-performance flux and permselectivity of MIMs were obtained simultaneously. [ABSTRACT FROM AUTHOR]

Development of membrane-based molecularly imprinted material with rapid rebinding and high-permselectivity performance has become an urgent need in chemical separation and industrial production. Herein, the high-quality membrane-based designs were proposed for the preparation of SiO 2 @polydopamine blended nanocomposite imprinted membranes with hierarchical structure. The high-efficiency antimalarial drug, artemisinin, was used as template molecule during the newly-developed sol-gel artemisinin-imprinted strategy. Importantly in this work, instead of the direct construction of imprinting layers on membranes, the artemisinin-imprinted SiO 2 @polydopamine particles were initially synthesized followed by a phase conversion process to obtain the SPIMs. The SiO 2 -based artemisinin-imprinted polymers on PDA nanospheres would played imprinted-triggered roles for achieving specific artemisinin-imprinted sites. Meanwhile, amount of artemisinin-imprinted cavities and permselectivity were both optimized, high-permselectivity coefficients (more than 11.5), fast adsorption kinetics and enhanced rebinding capacity (45.89 mg g−1) could be obtained. That is to say, this new direction of the membrane's design would become the further design and guide for selective separation membrane materials. SiO 2 @PDA-blended nanocomposite imprinted membranes with multilevel synergistic integration structure were first proposed and developed for the selective recognition and separation of artemisinin. [Display omitted] • The sol-gel artemisinin-imprinted SiO 2 @PDA particles were first proposed. • A nanocomposite-blended synthesis strategy was developed instead of the direct modification of MIPs on membranes. • Well-designed multilevel/hierarchical SPIMs were used as selective separation membranes. • High rebinding capacity and permselectivity performance could be simultaneously obtained. [ABSTRACT FROM AUTHOR]

Porous&permselective dual-tetracycline-imprinted nanocomposite membranes based on twice-polymerization-based imprinting process were prepared for selective separation of tetracycline. [Display omitted] • Twice-PDA-based dual-TC-imprinted membrane was first proposed. • Dual-imprinted membrane with GO/SiO 2 -loaded structure was successfully constructed. • Well-designed TC-imprinted membrane was applied as selective separation device. • High-performance flux and permselectivity of MIMs were obtained simultaneously. Here, the graphene oxide (GO)/SiO 2 -loaded dual-imprinted membranes (GS-DIMs) were constructed based on the self-polymerization imprinting technique of dopamine, in which a twice polydopamine (PDA)-based imprinting strategy had been successfully developed to obtain the three-dimensional nanocomposite membrane-based separation system. Meanwhile, the pollution-intensive antibiotics of tetracycline (TC) was used as template molecule throughout the GS-DIMs synthesis, and the dopamine molecules were simultaneously used as functional monomer and cross-linking agent during the twice polydopamine (PDA)-based imprinting processes. Therefore, dual-TC-imprinted sites had been prepared based on the as-designed dual imprinting processes, the as-prepared GS-DIMs-based separation system with dual-TC-imprinted structures could not only allow for the largely enhanced rebinding result of 65.61 mg/g and faster adsorption equilibrium rate within 20 min, but also facilitate the permselectivity performance from TC-based complex separation system and mimetic water sample. Importantly, we demonstrated the applications and effects of the dual-imprinted membrane-based separation materials to selective rebinding and separation of TC from complex solution systems and mimetic water samples. The as-obtained permselectivity factors (β) around 4.0 strongly illustrated the efficiently selective separation ability and high-intensitive recognizability of TC than any other non-template molecules based on our GS-DIMs-based separation system. Overall, the as-designed GS-DIMs had great potential for selective separation applications and provided critical comparisons based on the as-achieved excellent rebinding and permselectivity performance, which encompassed innovative GO/SiO 2 -loaded nanocomposite and PDA-based dual-TC-imprinted system. [ABSTRACT FROM AUTHOR]

Molecularly imprinted nanocomposite membranes with C-MSNs-based imprinting structure, in which lysozyme was template molecule, was constructed based on our newly-developed synergetic synthesis strategy of the sol–gel imprinting-initiated system. [Display omitted] • LYZ-MINMs improved the problem embedding and aggregation of nanoparticles. • Uniform and dense C-MSNs layer was loaded on the doubles faces of membrane by self-assembly strategy. • Double-faced C-MSNs-based imprinting structure was constructed by the sol–gel imprinting-initiated system. • High rebinding capacity and selectivity of LYZ-MINMs were obtained simultaneously. • Well-designed bidirectional LYZ-imprinted membrane was applied as selective separation device. In recent years, the combination of membranes and nanomaterials has made remarkable progress in separation of proteins. Nevertheless, the current combination methods suffer from the drawbacks of aggregation and embedding of nanomaterials, leading to a loss of membrane performance. In present work, the lysozyme molecularly imprinted nanocomposite membranes (LYZ-MINMs) with uniform and dense carboxyl functionalized mesoporous silica nanoparticles (C-MSNs) layer were successfully prepared by a double-faced self-assembly strategy for selective separation of LYZ from chicken egg white. Notably, the resulted LYZ-MINMs exhibit both promoted hydrophilicity (36.2°) and enhanced rebinding capacity (509 mg g−1) by comparing with the MINMs designed with the blending method. The selectivity of LYZ-MINMs toward LYZ is improved by the sol–gel imprinting process, resulting in a satisfactory rebinding selectivity of 2.98, 3.22 and 3.45 for Cytochrome C , Bovine haemoglobin, and Ovalbumin, respectively. After ten cycles, the high regeneration rate (>90 %) demonstrates the potential of LYZ- MINMs for practical applications. In addition, the practicability of LYZ- MINMs further verified by utilizing diluted egg white. The work shows great promise for next-generation membranes for protein separation. [ABSTRACT FROM AUTHOR]