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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Design of ion-imprinted amino-modified chitosan for selective chromium (Ⅲ) ion removal

Dongxue Fu,Guifang Wang,Li Zhao,Yuwen Hong,Baoming Yang,Huiling Cheng

Green ion-imprinting technique was applied to construct a Cr(III) ion-imprinted absorbent material from an amino functionalized chitosan derivative. First, nitrogenous organic compounds (GACS) as functional monomer is synthesized by a Schiff base reaction followed by a grafting reaction. In the end, imprinting was completed by cross-linking with epichlorohydrin (ECH) in aqueous media and eluting the coordinated ions with hydrochloric acid to obtain chromium-imprinted polymers (Cr(III)-IIP) with pores. The relevant parameters of the imprinting system were explored, and the superior polymer (Cr(III)-IIP 9 ) has an excellent adsorption capacity 385.89 mg/g, wide pH range adsorption, good adsorption rates and equilibrium times (≤120 min) for Cr(III) ion. Additionally, the kinetic study is best defined in terms of pseudo-second order, while the Freundlich isotherm model fits the data well. Competitive adsorption of the quaternary system of Cr(III)/ Cd(II)/ Ni(II)/ Cu(II) were also investigated, it demonstrated a greater affinity for the Cr(III) ion than other ions. Hence, the imprinting materials prepared by amino functionalized chitosan enhances the adsorption of Cr(III) ions in the simulation of actual water sample. The adsorption mechanism accords with the hard and soft acid and base theory (HSAB), which is expected to be is utilized for the separation of Cr(III) ions in the environment.

研究领域: 环境科学 · 材料科学
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NANOTECHNOLOGY · 2021 ·Vol. 32 ·期 15 ·155503 · IF 3.874

Improving TiO2 gas sensing selectivity to acetone and other gases via a molecular imprinting method

Wangyang Yang,Honglie Shen,Jiawei Ge,Binbin Xu

Various gas sensors have made considerable improvements to the quality of people's lives. However, in most cases, changing of materials is necessary to adapt to the changing of the target gas, which limits the further application of gas sensors. To meet this challenge, in this work, molecular imprinting (MI) technology is introduced. Acrylic acid is used as a functional monomer, while gas molecules, including acetone, are used as templates. The MI process with an acetone template helps improve the acetone selectivity of TiO2 by up to 1.74–2.80 times. Moreover, it proved that other templates can increase the corresponding selectivity by at least 1.5 times by using the same matrix material. These results demonstrate the potential importance of the MI process in constructing a highly compatible gas sensor industry. Beyond this, the MI process has proved to achieve an ultrahigh specific surface area of 384.36 m2 · g−1. The optimal acetone sensor exhibits desirable comprehensive performance compared with other reports. An excellent TiO2 based prototype acetone sensor working at 300 °C with a low detection limit of 18 ppb is obtained.

研究领域: 材料科学 · 化学工程 · 传感技术
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MOLECULES · 2022 ·Vol. 27 ·期 20 ·6987 · IF 4.927

A Capillary Electrophoresis Method Based on Molecularly Imprinted Solid-Phase Extraction for Selective and Sensitive Detection of Histamine in Foods

Yixuan Fan,Runze Yu,Yongfeng Chen,Yufeng Sun,Geoffrey I. N. Waterhouse,Zhixiang Xu

In this study, a sensitive capillary electrophoresis (CE) method based on molecularly imprinted solid-phase extraction (MISPE) was proposed to determine histamine in foods. A molecularly imprinted polymer (MIP) synthesized by bulk polymerization was used as the MISPE adsorbent for the selective extraction of histamine. Under the optimal conditions, the MISPE-CE method possessed good linearity for histamine detection in the concentration range of 0.1–100.0 μg/L. The limit of detection and limit of quantification of the method were calculated to be 0.087 μg/L and 0.29 μg/L, respectively. The histamine in spiked rice vinegar and liquor samples were detected by the developed method with recoveries of 92.63–111.00%. The histamine contents in fish, prawn, pork, chicken breast and soy sauce samples were determined using the developed method and a high-performance liquid chromatography method, with no significant difference found between the two methods.Keywords:histamine;molecular imprinting technology;solid-phase extraction;capillary electrophoresis

研究领域: 分析化学 · 食品科学
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RSC Advances · 2015 ·Vol. 5 ·期 17 ·12517-12529 · IF 3.84

Synthesis of novel ion-imprinted polymers by two different RAFT polymerization strategies for the removal of Cs(I) from aqueous solutions

Xiangguo Meng,Yan Liu,Minjia Meng,Zheyu Gu,Liang Ni,Guoxing Zhong,Fangfang Liu,Zhaoyong Hu,Rui Chen,Yongsheng Yan

In this work, two novel Cs(I) ion-imprinted polymers (Cs(I)-IIP1 and Cs(I)-IIP2) have been prepared by surface imprinting technique based on support matrix of SBA-15. The strategy was carried out by introducing two different reversible addition–fragmentation chain transfer (RAFT) polymerization including using the free RAFT agent in solution and surface-anchored RAFT agent with appropriate initiation method, which is expected to generate a well-defined surface ion-imprinted polymer with excellent adsorption capacity. The materials were verified by FT-IR, SEM, TEM, nitrogen adsorption–desorption and TGA. Owing to the intrinsic advantages of surface-anchored RAFT polymerization, the resultant surface ion-imprinted polymer (Cs(I)-IIP2) exhibited more homogeneous and thinner polymer layer (15 nm) with excellent macrostructure in comparison to Cs(I)-IIP1 (75 nm) prepared by using the free RAFT agent in solution. Furthermore, the adsorption capacity of both polymers are compared, indicating that Cs(I)-IIP2 displays higher adsorption property and excellent selectivity for Cs(I).

研究领域: 材料科学 · 环境科学
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Journal of Cleaner Production · 2017 · IF 5.715

A facile strategy toward ion-imprinted hierarchical mesoporous material via dual-template method for simultaneous selective extraction of lithium and rubidium

Xuechao Xu,Yang Li,Dongya Yang,Xudong Zheng,Yuanyuan Wang,Jianming Pan,Tao Zhang,Jicheng Xu,Fengxian Qiu,Yongsheng Yan,Chunxiang Li

With the increasing market demands of lithium (Li) and rubidium (Rb) around the world, the shortage of Li and Rb seriously restrict the further development of relevant industries. In this work, we report a superior lithium/rubidium imprinted hierarchical porous silica (Li/Rb-IHPS) for the simultaneous selective extraction of lithium and rubidium from aqueous solution. Li/Rb-IHPS was prepared by ion imprinting technology (IIT) by using 12-crown-4 (12-C-4) and N-[(3-Trimethoxysilyl) propyl] ethylendiamine triacetic acid trisodium salt (TMS-EDTA) as functional monomers . The structure, thermal property and surface functional groups of as-prepared Li/Rb-IHPS material were characterized by Fourier infrared spectroscopy (FT-IR), elemental analysis, thermogravimetric analyzer (TGA), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), and nitrogen adsorption-desorption. The results indicate that the as-prepared material has a hierarchical mesoporous structure (peak pore at ca. 3–4 nm and 12–15 nm) with high specific surface area (BET) (242.47 m 2  g −1 ). The adsorption experiments show that Li/Rb-IHPS has a high adsorption capacity for Li + (166 μg g −1 ) and Rb + (141 μg g −1 ). The adsorption process can be described by pseudo-second-order kinetic model , suggesting that the adsorption for Li + and Rb + is controlled by chemical adsorption . And the Langmuir isotherm model can well fit the experimental data, illustrating that the adsorption process are all monolayer adsorption reactions. Additionally, the adsorption selectivity and reusability measurements were also investigated. Compared with some ions such as Na + , K + , Mg 2+ and Cs + , Li/Rb-IHPS material shows excellent adsorption selectivity for Li + and Rb + . After five cycles, the Li/Rb-IHPS material remains high adsorption capacity for Li + (94%) and Rb + (93%). The obtained results indicate that Li/Rb-IHPS can be used to extract the lithium and rubidium from oceans and lakes selectively, rapidly, and environmentally.

研究领域: 材料科学 · 环境科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2021 · IF 7.312

Site-imprinted hollow composites with integrated functions for ultra-efficient capture of hexavalent chromium from water

Hua-Rong Yang,Chen Yang,Shan-Shan Li,Xiang-Cheng Shan,Gui-Lin Song,Qing-Da An,Shang-Ru Zhai,Zuo-Yi Xiao

The design of high-efficiency adsorptive composites for selective removal of Cr(VI) ions with high capacity from aqueous solution remains great challenging owing to the complicated numerous co-existing ions. Herein, a novel type of Cr(VI) site-imprinted hollow composites (Cr(VI)-IIHS) with integrated sorption affinity, fast adsorption kinetics, capturing performance and high adsorption capacity was designed with aluminum-gelled carboxymethyl cellulose microspheres as starting substrate, Cr(VI) as the templated sites and polymeric PEI as modifying agent via a controllable glutaraldehyde cross-linking process. The adsorption of Cr(VI) over-designed Cr(VI)-IIHS could reach equilibrium within a relatively short time and the maximum adsorption capacity was 679.13 mg/g, which is the record-high adsorption results for Cr(VI) from water. Most importantly, the Cr(VI) adsorption over the Cr(VI)-IIHS remained a high level of recycling performance, for which beyond 530.91 mg/g can maintain even with six cycles of regeneration. The adsorption kinetics and equilibrium isotherms are in full agreement with the pseudo-second-order kinetic and Langmuir isotherm model, reflecting the monolayer chemisorption mechanism. By virtue of integrated features and controllable preparative process, this study might shed light on guidance for the construction of fascinating hollow adsorptive composites for remediation of emerging pollutants contaminated water-body.

CAS / MDL: 9004-32-4 9002-98-6
研究领域: 环境科学 · 材料科学
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JOURNAL OF HAZARDOUS MATERIALS · 2022 · IF 14.224

A rotary multi-positioned cloth/paper hybrid microfluidic device for simultaneous fluorescence sensing of mercury and lead ions by using ion imprinted technologies

Liyan Wang,Bowei Li,Jianan Wang,Ji Qi,Jinhua Li,Jiping Ma,Lingxin Chen

A novel rotary cloth/paper hybrid microfluidic analytical device (μCPAD) was proposed via the synergy of the fluorescence sensing cloth-based component and rotary paper-based microfluidic analytical device (μPAD) for simultaneous detection of mercury (Hg 2+ ) and lead (Pb 2+ ) ions. Fluorescence sensing cloth-based component was prepared by grafting quantum dots onto cotton cloth and then modifying with ion imprinted polymers (IIP). Because the cloth has good ductility and durability, it can bear strong oscillation during the fabrication of grafting quantum dots and IIP, and brings a lot of convenience to the production process. At the same time, because rotary μCPAD was stacked by three-layer papers with designed hydrophilic channels and hydrophobic barriers, it could realize simultaneous detection of Hg 2+ and Pb 2+ ions by rotating top layer counterclockwise or clockwise. The fluorescence signals were obtained through quantum dots’ electron transfer fluorescence quenching effect with the limits of detection were 0.18 and 0.07 μg/L, respectively. This method successfully realized the transference of specific and sensitive fluorescence sensing materials (quantum dots) onto the microfluidic device to improve the portability and expanded applications. Moreover, the novel microfluidic device may have great potential in point-of-care testing of heavy metal ions in environmental monitoring fields.

研究领域: 分析化学 · 环境科学 · 生物医学工程
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Analytical Methods · 2022 ·Vol. 14 ·期 41 ·4077-4084 · IF 3.532

Dy(III)-coordination imprinted self-assembly microspheres based on a silica core for highly sensitive and selective detection of two carbamate pesticides

Zerong Long,Shilin Shen,Hui Yuan

Carbamate (CB) pesticides possess potential carcinogenic and mutagenic activities towards humans even at very low dosages. Thus, broad-specificity probes with high sensitivity and speed are needed for multiple CB determination. This study is the first to focus on Dy3+ ions-coordinated self-assembly on a silica core using a surface imprinting procedure, for the simultaneous fluorometric detection of residues of metolcarb (MC) and pirimicarb (PC) insecticides. A simple and mild solvothermal method was applied for the preparation of fluorescent imprinted microspheres starting from 1,10-phenanthroline (Phen)-ligated Dy3+ ions to guide imprinted self-assembly of chitosan (CTS), glutaraldehyde (GA), and two carbamate pesticides (MC and PC) on the silica surface by means of coordinate bonds and hydrogen bonds. The as-prepared microspheres displayed strong fluorescence emissions via the antenna effect derived from the Phen ligand and the Schiff base oligomers for sensitizing the Dy3+ ions. An expanded in-depth mechanism study was performed on the fluorescence enhancement involving Förster resonance energy transfer (FRET) from the pesticides (donor) to the acceptor. A linear increase in fluorescence at 483 nm for MC and 574 nm for PC upon the imprinted microspheres was observed under the same 350 nm excitation wavelength. Moreover, the quantitative recognition process could be carried out simultaneously and tolerate strong distractions both from five other similar carbamate insecticides and from complicated matrices (e.g., an extract of Chrysanthemum morifolium Ramat). The detection limit was 4 ng mL−1 with a range of 10–60 ng mL−1 for MC and 0.4 ng mL−1 with a range of 1–30 ng mL−1 for PC. Further characterization of the material, including TEM, SEM, XPS, and FTIR, Raman, and fluorescence spectra, verified that the Dy3+ ions play a decisive role in promoting imprinted self-assembly around the silica core. Hence, a novel polynuclear Ln–organic imprinted probe having high selectivity, stability, and sensitivity for the detection of two carbamate insecticides is presented in this study.

研究领域: 分析化学 · 环境科学 · 食品科学
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Chemosensors · 2023 ·Vol. 11 ·期 6 ·339 · IF 4.2

An Electrochemical Sensor for Trimethoprim Based on a Magnetic Molecularly Imprinted Carbon Paste Electrode

Peng Liu,Ruiying Zhang,Liyan Zheng,Qiue Cao

In order to achieve simple, rapid, and highly sensitive detection of trimethoprim (TMP), a magnetic molecularly imprinted carbon paste electrode (MCPE) was prepared by drop-coating magnetic molecularly imprinted polymer (MIP@Fe3O4@MWNTs) on the surface of reduction graphene oxide (rGO)/MCPE doped with Fe3O4@MWNTs. The introduction of multi-walled carbon nanotubes (MWNTs) and rGO served as dual signal-amplification materials, which can improve the response sensitivity of the sensor. In addition, the magnetic interaction between the substrate electrode and the molecularly imprinted material was beneficial to increasing the stability of the sensor. As expected, the electrochemical sensor not only showed sensitivity and selectivity for the detection of TMP, but it also possessed good stability. The detection range for TMP was 4.0 × 10−9~5.0 × 10−4mol/L, and the detection limit was 1.2 × 10−9mol/L. The response performance varied within 10% when the sensor was placed for more than 2 months and used more than 60 times. The spiked recoveries of TMP in environmental water samples, urine samples, and pharmaceuticals (drugs) were between 91% and 110%, and the relative standard deviation (RSD) was within 5%.Keywords:trimethoprim;molecular imprinting technique;electrochemical sensor

研究领域: 分析化学 · 生物医学工程
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JOURNAL OF SEPARATION SCIENCE · 2015 ·Vol. 38 ·期 18 ·3279-3287 · IF 2.737

Preparation of “dummy” l-phenylalanine molecularly imprinted microspheres by using ionic liquid as a template and functional monomer

Ji Li,Xiaoling Hu,Ping Guan,Dongmen Song,Liwei Qian,Chunbao Du,Renyuan Song,Chaoli Wang

In this study, dummy imprinting technology was employed for the preparation of l- phenylalanine-imprinted microspheres. Ionic liquids were utilized as both a “dummy” template and functional monomer, and 4-vinylpyridine and ethylene glycol dimethacrylate were used as the assistant monomer and cross-linker, respectively, for preparing a surface-imprinted polymer on poly(divinylbenzene) microspheres. By the results obtained by theoretical investigation, the interaction between the template and monomer complex was improved as compared with that between the template and the traditional l- phenylalanine-imprinted polymer. The batch experiments indicated that the imprinting factor reached 2.5. Scatchard analysis demonstrated that the obtained “dummy” molecularly imprinted microspheres exhibited an affinity of 77.4 M·10 −4 , significantly higher that of a traditional polymer directly prepared by l- phenylalanine, which is in agreement with theoretical results. Competitive adsorption experiments also showed that the molecularly imprinted polymer with the dummy template effectively isolated l- phenylalanine from l- histidine and l- tryptophan with separation factors of 5.68 and 2.68, respectively. All these results demonstrated that the polymerizable ionic liquid as the dummy template could enhance the affinity and selectivity of molecularly imprinted polymer, thereby promoting the development of imprinting technology for biomolecules.

研究领域: 化学 · 生物化学
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JOURNAL OF SEPARATION SCIENCE · 2013 · IF 2.591

Preparation and evaluation of a novel molecularly imprinted SPE monolithic capillary column for the determination of auramine O in shrimp

Jiangmei Li,Haiyun Zhai,Zuanguang Chen,Qing Zhou,Zhenping Liu,Zihao Su

A novel method combining molecular imprinting and SPE was developed in a capillary column for the determination of auramine O in shrimp. The capillary monolithic column was prepared by UV-initiated in situ polymerization, using auramine O as template and methacrylic acid and ethylene dimethacrylate as functional monomer and cross-linker, respectively. The properties of the prepared capillary monolithic column were investigated under the optimized conditions coupled with HPLC, and then the morphologies of the inner polymers were characterized by SEM. The calibration curve was expressed as A = 103 C + 19.8 ( r = 0.9992) with a linear range of 0.25–25.0 μg/mL, and the recoveries of auramine O at different concentrations in shrimp ranged from 90.5 to 92.4% with RSDs ranging from 2.1 to 4.4%. The capacities of the molecularly imprinted polymer and nonimprinted polymer columns were 0.722 and 0.147 μg/mg, respectively, and the LOD (S/N = 3) of auramine O in shrimp was 17.85 μg/kg. Under the selected conditions, the enrichment factors obtained were higher than 70-fold. The results indicate that the prepared molecularly imprinted capillary monolithic column was reliable and applicable to the analysis of auramine O in shrimp.

研究领域: 分析化学 · 食品安全
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

Continuous-imprinted-layer nanofiber membrane with MXene-based precise-designed nanocages for high-accuracy recognition and separation of shikimic acid

Rongxin Lin,Jian Lu,Faguang Ma,Ming Yan,Yilin Wu,Jianming Pan

Ti 3 C 2 T x (MXene) has attracted extensive attention from scholars at home and abroad due to its rich surface termination functional groups and two-dimensional multilayer structure. In this work, MXene was introduced to the membrane by vacuum-assisted filtration processes, and the formed interlayer channel facilitated the construction of recognition sites and molecular transmission. In this paper, PDA@MXene@PDA@SiO 2 -PVDF dual-imprinted mixed matrix membrane (PMS-DIMs) were developed by the cooperative dual-imprinting strategy, which was used for the adsorption of shikimic acid (SA). Firstly, SiO 2 -PVDF nanofiber basement membrane were prepared by electrospinning method and the first Polydopamine (PDA)-based imprinted layer was constructed on the membrane. PDA not only realized the imprinting process, PDA modification was used to give MXene nanosheets better antioxidant properties and to confer the SiO 2 -PVDF nanofiber membrane the interface stability. After that, the second-imprinted sites were constructed on the stacked MXene nanosheets surface as well as between the layers. The SA dual-imprinted sites significantly increased the efficiency of the selective adsorption efficiency, when the template molecule passed through the membrane, the cooperative dual-imprinting strategy enabled multiplex recognition and adsorption of template molecules. As a consequence, which greatly improving the rebinding ability(262.17 g m −2 ), and mselectivity factors ( β Catechol/SA , β P-HB/SA , β P-NP/SA were 2.34, 4.50 and 5.68). High stability proved the potentials of the PMS-DIMs for practical application. Precise SA-recognition sites were constructed on the PMS-DIMs, PMS-DIMs not only exhibit excellent selective rebinding properties but also have high permeability.

研究领域: 材料科学 · 生物化学 · 环境工程
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