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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Double-layer-based molecularly imprinted membranes for template-dependent recognition and separation: An imitated core-shell-based synergistic integration design

Yilin Wu,Jian Lu,Wendong Xing,Faguang Ma,Jia Gao,Xinyu Lin,Chao Yu,Ming Yan

Extensive efforts have been made for research on the development of selective separation membranes, however, the simultaneous promotion of stable selectivity and high permselectivity still faces its challenges. For the first time, a subversive synthesis strategy with hierarchical structure was proposed for the preparation of double-layer-based molecularly imprinted nanocomposite membranes (DLMIMs). Herein, the polydopamine (PDA) based imprinting process was initially performed on the surfaces of SiO 2 and activated carbon nanoparticles (ACNPs) to obtain the first PDA-based tetracycline (TC) imprinted layers. After a phase inversion process, a sol-gel polymerization procedure was then conducted for the preparation of second TC-imprinted layers. The TC-imprinted PDA-ACNPs/SiO 2 -based nanocomposite could be applied as the imprinting-initiated factors during the sol-gel TC-imprinted process, which led to the formation of imitated core-shell structure in the as-prepared blended membranes. Importantly, attributing to the as-synthesized double-layer-based TC-imprinted multilevel domains, abundant TC-recognition sites with high stability could be successfully synthesized in DLMIMs. Therefore, it was no surprise that large rebinding capacity (115.5 mg g −1 ), fast adsorption kinetics and high permselectivity coefficients (more than 6.5) were successfully achieved. The results of optimization experiments showed that the PDA-based TC-imprinted layer and sol-gel-based TC-imprinted layer would both cause for largely enhancing the rebinding capacity of DLMIMs. In addition, DLMIMs were synthesized without complicated procedures and the whole preparation process was feasible and pollution-free. Finally, we believed that the as-designed synthetic technique of DLMIMs would hold great potential in selective separation field.

研究领域: 材料科学 · 环境工程 · 生物技术
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DESALINATION · 2022 · IF 11.211

Hierarchically porous molecularly imprinted membranes with multiple transfer channels for micropollutants selective separation

Wendong Xing,Zhongfei Ma,Chong Wang,Jia Gao,Chao Yu,Yongsheng Yan,Li Yan,Chunxiang Li,Yilin Wu

Molecularly imprinted membranes (MIMs) have been considered as a promising material for the treatment of intractable micropollutants due to their predetermined selectivity and high stability. Herein, we proposed an exclusive design by incorporation of heterogeneous porous UiO-66-NH 2 and hierarchically porous structure nanofibrous membranes to fabricate a MOFs based hierarchically porous molecularly imprinted nanofiber membranes (HP-MINMs) with multiple mass transfer channels, achieving efficient selective removal of atrazine (ATZ). The heterogeneous pores UiO-66-NH 2 nanoparticles as matrix facilitated loaded with more densely and accessible imprinted recognition sites. Meanwhile, the multiple transfer channels formed in well-designed hierarchically porous nanofibrous membranes significantly enhancing of permeation flux and increase the contacting efficiency of target molecules with selective recognition sites. As a result, the obtained HP-MINMs possess synchronous enhanced permeation flux ( J  = 0.40 × 10 −3 , 1.01 × 10 −3 and 1.07 × 10 −3  mg min −1 cm −2 ) and permselectivity factors ( β  = 3.22 and 3.52), which much superior to those pure molecularly imprinted nanofiber membranes and other references. Importantly, the impressive selective separation performance (the separation efficiency for ATZ is 60.7 %) was achieved in continuous separation process. The presented work provides a fresh idea for addressing the trade-off effect in selective separation of MIMs.

研究领域: 环境科学 · 材料科学
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Journal of Environmental Chemical Engineering · 2021 · IF 5.909

Double-imprinted mixed matrix membranes with polydopamine-induced nanocomposite for selective recognition and separation applications

Faguang Ma,Yilin Wu,Qingyan Guo,Rongxin Lin,Kaicheng Zhang

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.

研究领域: 环境科学 · 材料科学 · 生物技术
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Hydrophilic imprinted MnO2 nanowires “coating” membrane with ultrahigh adsorption capacity for highly selective separation of Artemisinin/Artemether

Minjia Meng,Yi Li,Hui Peng,Binrong Li,Chuanxun Zhang,Jiajia Ren,Qingluola Ren,Yan Liu,Jianming Pan

The selective separation and purification of ART and ARE using molecularly imprinted membrane (MIM) has attracted considerable attention, but most of conventional blending MIM face low adsorption capacity and poor selectivity due to the blockage of imprinting sites. Herein, an alternative ART imprinted MnO 2 nanowires “coating” membrane (MINM) with   hydrophilicity was fabricated by vacuum filtration of imprinted MnO 2 nanowires and graphene oxide nanosheets on PVDF membrane surface for selective ART separation. For the MINM, the imprinted MnO 2 nanowires coating offers more available exposed imprinting sites on the MINM surface compared to that of the blending MIM, while the introduction of graphene oxide improves the hydrophilicity of MINM, significantly reducing the non-specific absorption. Consequently, the MINM exhibits ultrahigh ART adsorption capacity and selectivity, with the ART adsorption amount of 335 mg g −1 at 5 min using dynamic cross-flow separation system, about 12.18 times higher than that of ARE (27.5 mg g −1 ), and the separation factor ( a ) value of 12.39. Moreover, the ATR FT-IR dynamic spectrum discloses the in-situ formation of H-bond between ART and MINM, playing a key role in the selective adsorption process. This work provides an alternative strategy to prepare “coating” MIM for high-efficient and selective separation of complex analogue systems.

研究领域: 材料科学 · 药物化学 · 分离技术
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FOOD CHEMISTRY · 2020 · IF 6.306

Antifouling molecularly imprinted membranes for pretreatment of milk samples: Selective separation and detection of lincomycin

Zeqing Dong,Jian Lu,Yilin Wu,Minjia Meng,Chao Yu,Chang Sun,Muning Chen,Zulin Da,Yongsheng Yan

As a veterinary antibiotic, lincomycin (LIN) residues in milk are raising concerns of public on account of potential harm to human health. Efficient strategy is eagerly desired for detection of LIN from milk samples. Hence, lincomycin molecularly imprinted membranes (LINMIMs) were developed for selective separation of LIN as an efficient pretreatment of milk samples. The synergistic effect of polyethylenimine and dopamine provided effective antifouling performance by improving the hydrophilicity. Based on click chemistry, specific recognition sites were facilely formed on membranes using 4-vinylpyridine as functional monomers. The satisfactory rebinding capacity (151.62 mg g −1 ), permselectivity (4.43), together with the linear dependence ( R 2  = 0.9902) of concentrations in eluents and original samples. Moreover, the method was utilized to determine LIN from milk, with good recovery and relative standard deviation. Achievements in this work will actively promote the development of efficient detection technology.

研究领域: 食品科学 · 分析化学
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Solvent-driven controllable molecularly imprinted membrane with switched selectivity and fast regenerability enabled by customized bifunctional monomers

Jia Gao,Li Yan,Yan Yan,Li Chen,Jian Lu,Wendong Xing,Chao Yu,Muning Chen,Minjia Meng,Yongsheng Yan,Yilin Wu

Ensuring both selective separation and fast regenerability is still a challenge, especially for long-term operation in a harsh water system. Sustainable and effective development of molecularly imprinted membranes is highly desired. Herein, we propose a type of solvent-driven controllable molecularly imprinted membranes (CS-BMIMs) to realize the switched selectivity and fast regenerability by customized bifunctional monomers. The stable supramolecular envelope interaction and hydrogen bonds between the bifunctional monomers and the phenolic hydroxyl group is introduced to regulate the selectivity of BPA. The selectivity coefficients of CS-BMIMs can reach 7.52 ( α BPA/BP ) and 7.97 ( α BPA/HQ ). Poly (ethylene glycol) unit-containing chain of dynamic solvent-responsive cross-linker drives the swelling and deswelling polymer chains to accelerate the regenerability. Significantly, BPA can be readily adsorbed into the imprinted sites in a 25% methanol (MeOH) aqueous solution with an adsorption capacity of 41.88 mg g −1 while completely desorbed in 100% MeOH following the deswelling of BPA-imprinted sites. Compared with the ordinary elution methods ( V MeOH : V acetic acid , 9: 1), the solvent-driven controllable method displayed a fast adsorption/desorption process with desirable regenerability (15 min). Moreover, the proposal of “specially designed” stimulus–response material enriches the designability and options of membrane separation in water treatment, thereby laying a foundation for developing decontamination of the water.

研究领域: 环境科学 · 材料科学 · 水处理技术
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Catalysts · 2025 ·Vol. 15 ·期 2 ·192 · IF 4

Co/Mo2C-Embedded N-Doped Carbon Nanotubes Combined with Molecularly Imprinted Membranes for Selective Electrocatalytic Determination of Imidacloprid

Dongshi Feng,Jiangdong Dai,Yongsheng Yan,Chunxiang Li

Developing a catalyst with excellent electrical conductivity and catalytic performance for on-site testing of residual imidacloprid is significant and challenging. In situ growth of Mo2C nanodots on Co-induced N-doped carbon nanotubes (Co/Mo2C/N-CNT) was synthesized to construct a molecularly imprinted electrochemical sensor for the detection of imidacloprid. The results proved that the catalytic performance of Co/Mo2C/N-CNT for imidacloprid was over two times higher than those of Co/N-CNT and commercial CNT. This improvement was attributed to the formation of a heterostructure between Co species, Mo2C, and N-CNT, which facilitated highly exposed catalytic active sites. Additionally, the abundant Mo2C nano-dots promoted interfacial charge transfer to achieve optimal dynamics. The optimum preparation parameters of the catalysts were obtained by response surface methodology. By analyzing the relationship between different pH values and peak potential, as well as the influence of different scanning rates on peak potential, it was deduced that the possible electrocatalytic mechanism of imidacloprid involved the reduction of the nitro group to a hydroxylamine group and H2O. Under optimal conditions, the limit of detection (LOD) was 0.033 × 10−6mol·L−1(R2= 0.99698), and the linear range was 0.1 × 10−6~100 × 10−6mol·L−1. The application effect of the prepared sensor was evaluated by measuring the imidacloprid in two kinds of tea, indicating that the sensor possessed good sensitivity and selectivity, and was capable of meeting the requirements of on-site detection.

研究领域: 分析化学 · 环境科学 · 材料科学
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Journal of Inorganic and Organometallic Polymers and Materials · 2017 ·Vol. 27 ·期 2 ·586-597 · IF 1.577

Synthesis and Characterization of Hybrid Molecularly Imprinted Membrane with Blending SiO2 Nanoparticles for Ferulic Acid

Wei Mei-hua,Chen Hong-yan,Wang Shu,Jiang Wan-ying,Wang Yi,Wu Zhang-feng

A ferulic acid molecularly imprinted membrane (MIM) with blending SiO 2 nanoparticles was constructed using photoinitiated copolymerization. The MIMs were synthesized using ferulic acid as template, 2,2-azobisisobutyronitrile (AIBN) as functional monomer, Ethylene glycol dimethacrylate (EGDMA) as crosslinker. The synthetic conditions such as the mass content and size of the SiO 2 nanoparticles and the UV exposure times were optimized to obtain the membrane with superior performance. The scanning electron microscope (SEM) and FT-IR Spectrometer had been used to visualize the structure morphology of the molecularly imprinted membrane and to quantity pore size and the surface characteristics. The recognition properties of all prepared membranes were thoroughly investigated by using the cross flow membrane filtration equipment to calculate the selectivity factor and the water flux. Results indicated that the ferulic acid composite MIM which with 0.25 wt% SiO 2 nanoparticles and 130–140 min exposure time were founded be optimum parameters. It showed good recognition ability to ferulic acid as well as high hydrophilicity and outstanding mechanical strength.

CAS / MDL: 79-41-4
研究领域: 材料科学 · 化学工程
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TALANTA · 2015 · IF 3.545

Detection of 17β-estradiol in water samples by a novel double-layer molecularly imprinted film-based biosensor

Yuan Tan,Tianxin Wei

This study reports a novel double-layer molecularly imprinted film (MIF)-based biosensor for rapid, sensitive and highly selective detection of small molecule 17β-estradiol (E2) that is frequently detected in environmental water samples. In this system, the modification of gold surface of SPR chip was performed by 1-dodecanethiol. Then double-layer MIF was generated on the 1-dodecanethiol modified gold surface. The non-modified and imprinted surfaces were characterized by atomic force microscopy (AFM), scanning electron microscope (SEM) and contact angle measurements . Analysis of surface plasmon resonance (SPR) spectroscopy showed that the imprinted sensing film displayed good selectivity for E2 compared to other analog molecules and NIF. A good linear relationship was obtained between the SPR angle and E2 concentrations over a range of 2.50×10 −13 –2.50×10 − 9 mol/L ( R 2 =0.993) with the lowest measurable concentration of 2.50×10 −13   mol/L. The sensor can be regenerated with the mixture of acetic acid and PBS buffer (v/v=1:9) as a desorption agent over tens of times without significant deterioration of the sensor performance. Potential interference of real environmental sample matrix was assessed by spiked samples in several waste seawater effluents. This portable sensor system can be successfully applied for on-site real-time inexpensive and easy-to-use monitoring of E2 or other small molecule pollutants in environmental samples such as effluents or water bodies .

研究领域: 环境科学 · 生物传感技术
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RSC Advances · 2021 ·Vol. 11 ·期 58 ·36769-36776 · IF 3.361

4-Pentenoyl-isoleucyl-chitosan oligosaccharide and acrylamide functional monomer-dependent hybrid bilayer molecularly imprinted membrane for sensitive electrochemical sensing of bisphenol A

Qing Gao,Yang Zang,Ju Xie,Yongchuan Wu,Huaiguo Xue

In this work, an electrochemical sensor was designed for trace monitoring of bisphenol A (BPA) by decorating a hybrid bilayer molecularly imprinted membrane (MIM) on a multi-walled carbon nanotube-modified glassy carbon electrode. When BPA in the MIM was eluted, a composite molecularly imprinted electrochemical sensor was constructed. Under optimal conditions, the developed sensor showed two linear relationships between ΔIp and BPA concentration in the range of 0.04 μM to 8 μM, as well as good selectivity and stability, and was also applied to detect BPA in water samples with desirable recoveries ranging from 92.0% to 107.0%.

研究领域: 分析化学 · 环境科学 · 材料科学
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NANO · 2020 · IF 1.566

Biomass-Based Synthesis of Green and Biodegradable Molecularly Imprinted Membranes for Selective Recognition and Separation of Tetracycline

Wendong Xing,Yilin Wu,Jian Lu,Xinyu Lin,Chao Yu,Zeqing Dong,Yongsheng Yan,Chunxiang Li

Aggravating environmental problems have driven the unprecedented development of sustainable materials. Treatments of environmental pollutants with biomass-based sustainable materials are catching attention of more researchers. In the present work, a biomass-based strategy was developed to prepare sustainable molecularly imprinted nanocomposite membranes (S-MINMs). Based on this strategy, biomass-activated carbon nanoparticles (ACNPs) as the porous filler were integrated into the porous cellulose acetate (CA)/chitosan (CS) hybrid membranes to synthesize renewable and easy degradable basal membranes. The specific recognition sites were fabricated from simple free radical polymerization method, and using methacrylic acid (MAA) and acrylamide (Am) as functional monomers, we obtain improved adsorption capacity on tetracycline (TC, template molecule). Performance of S-MINMs was evaluated by adsorption isotherm, adsorption kinetics, perm-selectivity, reusability and biodegradability. Results indicated that the as-prepared S-MINMs not only exhibited desirable biodegradability, but also possess superior adsorption and separation performance toward TC (15.99 mg g − 1 for adsorption capacity and 4.91 for perms-selectivity factor). The method developed here shows great potential for development of sustainable membranes for selective separation of various pollutants.

研究领域: 环境科学 · 材料科学
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TALANTA · 2024 · IF 5.6

An electrochemical microbiosensor for serotonin based on surface imprinted layer coordinated bimetal functionalized acupuncture needle

Shanshan Zhan,Jiayi Zhang,Chunrong Gao,Zhengzhi Yin,Hongying Liu

Serotonin (5-hydroxytryptamine, 5-HT) is a pivotal monoamine neurotransmitter , which is widely distributed in human brain for biological, physical and psychopathological processes. The content of 5-HT can support diagnose of various diseases. To selectively detect 5-HT is very important in clinical medicine. Here, a novel microbiosensor for 5-HT is studied on acupuncture needle. Molecularly imprinted film enwrapped 5-HT was electropolymerized onto bimetallic gold/platinum (Au/Pt) nanoparticles on acupuncture needle microelectrode (ANME). Au/Pt nanostructure exhibited active sites to catalyze the oxidation of 5-HT and bind the generated polymer. 5-HT can be enwrapped by the functional monomer of pyrrole (Py) in the process of electropolymerization with suitably electroactive conformation. Comparing with interfaces of single metal or molecularly imprinted layer, synergistic microbiosensor exhibit better performance for 5-HT. 5-HT can be adsorbed and catalytically oxidized by the imprinted cavities. Under optimized conditions, the peak current linearly increases with the concentration of 5-HT from 0.03 to 500 μM, and a detection limit of 0.0106 μM is obtained. The performance of this microbiosensor is competitive with previous studies. Furthermore, the prepared microbiosensor showed effective application to analyze 5-HT in human serum and urine. Interestingly, the microbiosensor expressed the real-time monitoring ability to 5-HT from stimulated PC12 cells by K + . The microbiosensor also exhibited high selectivity, stability and reproducibility, which is promising in view of the low price, fast response and simple operation.

研究领域: 分析化学 · 神经生物学 · 临床医学
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