JOURNAL OF MOLECULAR RECOGNITION
·
2023
·Vol. 36
·期 7
·e3024
·
IF 2.7
Ting Hu,Qianghong Zhao,Ming Wang,Kai Zhou,Zhining Xia,Yike Huang
Based on the synergistic action of hydrogen bond and electrostatic interaction, provided by methacrylic acid and 2-aminoethyl ester hydrochloride (FM2), respectively, novel molecularly imprinted polymers (SA-MIPs) were designed to improve its selective recognition ability. Diclofenac sodium (DFC) was chosen as the template molecule of this study. The interaction and their recognition sites between two functional monomers and templates were confirmed by nuclear magnetic resonance hydrogen spectroscopy. Because of the synergistic action of hydrogen bond and electrostatic interaction, the imprinting factor (IF) of SA-MIPs (IF = 2.26) is superior to the corresponding monofunctional monomer imprinting materials (IF = 1.52, 1.20) and the materials using two functional monomers with an only single type of interaction (IF = 1.54, 1.75). The results of selective adsorption experiments indicate that the selective recognition ability of SA-MIPs is significantly better than that of the other four MIPs, and the difference in selectivity coefficient for methyl orange is the largest between SA-MIPs and the MIPs only using FM2, which is about 70 times. In addition, x-ray photoelectron spectroscopy was used to verify the interaction between SA-MIPs and the template. This work and its explanation of the interaction mechanism at the molecular level will be helpful for the rational design of novel MIPs with higher selectivity. Besides, SA-MIPs have good adsorption performance (37.75 mg/g) for DFC in aqueous solutions, which could be used as potential adsorption materials for the effective removal of DFC in the aquatic environment.
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POLYMERS FOR ADVANCED TECHNOLOGIES
·
2022
·Vol. 34
·期 2
·549-558
·
IF 3.348
Wang Xie,Yuan Liu,Mingming Yu,Qi Wang
The synthesis of intrinsic flame retardant copolymer by copolymerization with reactive flame retardants is the most potential method to prepare transparent and flame retardant poly (methyl methacrylate) (PMMA) at present，but the main challenge of this method is that the copolymer usually has poor mechanical properties and heat resistance. In this work, the hydrogen bond enhancement strategy is adopted, and the flame retardant PMMA with excellent comprehensive properties is obtained by ternary copolymerization with methyl methacrylate (MMA) as matrix unit, diethyl (methacryloyloxymethyl) phosphonate (DEP) as flame retardant unit and methacrylamide (MAA) as hydrogen bond unit. Due to the formation of intermolecular hydrogen bond via MAA unit, the storage modulus, flexural strength and impact strength of the terpolymer containing 15 mol% MAA are 48%, 19%, and 24% higher than those of the copolymer of MMA and DEP, and its hardness, glass transition temperature and load thermal deformation temperature (increased by 7°C) are also superior. Moreover, owing to the gas-phase dilution and charring flame retardancy of MAA unit, the terpolymer shows increased limiting oxygen index (24.3%) and UL94 rating (V-1). This work not only provides a promising flame retardant PMMA for practical application, but also offers a new strategy to design flame retardant polymers with good mechanical properties.
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ACS Applied Polymer Materials
·
2023
·
IF 5
Yi Zhang,Donghao Liu,Weidong Guo,Yigang Ding
Selective recognition and separation of rare-earth elements (REEs) is considered a real challenge for the RE industry. In this work, two dual-site ion-imprinted polymers (IIP-AM and IIP-MAA) were synthesized via a radical copolymerization method for the removal of La(III) from aqueous solutions. The structures of samples were characterized and confirmed with various kinds of techniques, including IR, X-ray diffraction, field emission scanning electron microscopy, Brunauer–Emmett–Teller, thermogravimetry analysis, and X-ray photoelectron spectroscopy (XPS). Adsorption studies reveal that the pseudo-second-order kinetic model and the Langmuir isotherm model were well-fitted with the adsorption of La(III), showing high adsorption capacities of 45.65 and 50.05 mg/g for IIP-AM and IIP-MAA, respectively, after 120 min at pH = 5.5 and 25 °C. Impressively, the fabricated IIPs possess remarkable selectivity between La(III) and other REEs, as well as excellent reusability after five successive adsorption–regeneration cycles with less than 9% reduction of capacities. The adsorption mechanism indicates that the surface complexation and electrostatic attraction contribute to the adsorption of La(III) based on the characterization analysis of XPS, elemental mapping, and energy-dispersive spectrometry, as well as density functional theory calculations. Accordingly, these samples with tailored ion-imprinted cavities and abundant active O sites entirely exhibit the potentials for the selective recovery of REEs from aqueous solutions.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Yunye Hu,Chenxia Zhang,Zhengjie Jian,Dong Chen,Yuhong Ma,Wantai Yang
Surface molecularly imprinted polymers (SMIPs) are effective adsorbents for the separation and removal of antibiotics owing to their specific selectivity and high efficiency. Herein, a novel kind of glycidyl methacrylate (GMA)-functionalized poly(maleic anhydride- alt -styrene) (PMS) particles (PMS-GMA) are facilely prepared via self-stabilized precipitation polymerization, which can serve as an ideal support matrix for the scalable preparation of SMIPs. Methacrylic acid and ethylene glycol dimethacrylate were copolymerized in the presence of norfloxacin (NOR) template and PMS-GMA carrier to obtain NOR-imprinted SMIPs (PMS@MIPs). Due to the presence of NOR-imprinted layer, the resultant PMS@MIPs can effectively and selectively adsorb NOR, featured with high sorption capacity in short equilibrium time (149.3 mg/g in 60 min). The adsorption behavior of NOR by PMS@MIPs fitted better to pseudo-second-order and Freundlich model. More importantly, PMS@MIPs showed high selectivity for NOR over enrofloxacin and levofloxacin with similar chemical structure, and another commonly used antibiotics sulfonamides. Furthermore, PMS@MIPs exhibited excellent reusability, the NOR molecules can be facilely desorbed under acidic condition and the adsorption capacity of the recycled PMS@MIPs only reduced by 6.9% after four adsorption-desorption process, indicating great potential for selective adsorption of NOR.
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Arabian Journal of Chemistry
·
2023
·
IF 6
Zehu Wang,Zongqi Li,Ruiye Yan,Guangshuo Wang,Yanming Wang,Xiaoliang Zhang,Zhixiao Zhang
The polymer microspheres with hollow structure are of technological importance in the removal of pollutants because of the large specific surface area and low mass transfer resistance. In this work, we employ the Pickering emulsion polymerization stabilized with TiO 2 nanoparticles to build the molecularly imprinted polymers microspheres with hollow structure (H-MIPs) for the precise recognition of dibutyl phthalate (DBP), which would influence the biological reproductive system and endocrine system as a typical endocrine disrupting compound. The polymerization induced phase separation occurring within Pickering emulsion droplets plays a significant role in the formation of hollow structure. The morphology and structure of H-MIPs were observed via optical microscope and field emission scanning electron microscope, respectively. The results indicate that H-MIPs microspheres are of irregular spherical form with sunken surface and perfect hollow structure. The forming process of the hollow structure was analyzed in detail. Besides, the chemical structure and thermal stability of H-MIPs and H-NIPs were characterized by fourier transform infrared spectroscopy and thermal gravimetric analysis, respectively. The binding performance of H-MIPs and H-NIPs was investigated through a series of binding experiments, which consist of the binding kinetics, binding isotherm, selective test and reusability experiment. The results show that H-MIPs microspheres exhibit remarkable binding kinetics towards DBP, and the saturated adsorption time is not more than 30 min. Apart from the fast binding rate, H-MIPs also show considerable binding amount, accurate binding selectivity and good regenerability. The imprinting factor could reach to 2.56, and the binding amount towards DBP remains at a relatively high level within 3 cycles. The prepared H-MIPs microspheres have broad application prospects in environmental and analytical field involved DBP, and the study also offers an alternative method for the facile building of H-MIPs microspheres.
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JOURNAL OF CHEMICAL SCIENCES
·
2021
·Vol. 133
·期 2
·1-8
·
IF 1.573
Fu Guiyu,Weng Huanyuan,Lai Zhuzhi,Lin Zhengzhong,Huang Zhiyong
A rare earth complex Eu(MAA) 3 Phen was prepared with methacrylic acid and o -phenanthroline as ligands under mild conditions. The complex has a fluorescence emission centered at 618 nm with a half-peak width of 15 nm. Since the emission peak of the complex matches the absorption peak of malachite green (MG), the fluorescence of the complex will be quenched by MG through the fluorescence resonance energy transfer effect. The fluorescence testing conditions for MG were optimized based on fluorescence intensity and fluorescence quenching efficiency. The FRET efficiency was calculated to be 0.21. Under the optimal conditions, the response time was only 5 min. Compared with sulfonamides, chloramphenicol and other banned fishery drugs, the complex exhibited the highest quenching efficiency to MG. The linear range was 0.5–20 μmol L −1 , and the detection limit was 117.29 nmol L −1 (3σ/S, n = 9). This complex was used to detect MG residue in aquaculture water, and the recoveries were between 96.10% and 98.76%, indicating that the prepared fluorescent probe could be used for the rapid detection of MG in aquaculture water. Graphical abstract
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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Zeyu Geng,Qin Xie,Zhongjiao Fan,Weining Sun,Wei Zhao,Junhao Zhang,Jianqiu Chen,Yun Xu
Four tertiary amine-based protic ionic liquids (PILs) have been carefully designed to investigate the performance of SO 2 uptake. Their physical properties of densities and viscosities were determined. In the four PILs, the highest capacity for SO 2 of the four PILs reached up to 5.64 mol/kg ILs (P = 1.0 bar, T = 313.2 K). The ideal selectivity of SO 2 /CO 2 was up to 250 in the separation application of SO 2 from CO 2 . The kinetic study demonstrated that the PILs could efficiently capture SO 2 quickly under the ambient pressure. Based on the SO 2 absorption capacity and selectivity, excellent recyclability , and fast absorption process, the PILs in this work are considered as a potential alternative to traditional absorbents in the flue gas desulfurization (FGD).
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REACTIVE & FUNCTIONAL POLYMERS
·
2021
·
IF 3.975
Zehu Wang,Zeyang Zhang,Ruiye Yan,Xiying Fu,Guangshuo Wang,Yanming Wang,Zongqi Li,Xiaoliang Zhang,Junxian Hou
In this paper, the magnetic molecularly imprinted polymers (M-MIPs) for bisphenol A were synthesized via facile one-step Pickering emulsion polymerization using Fe 3 O 4 nanoparticles as the only stabilizer . The synthesis was based on non-covalent molecular imprinting strategy and performed by thermally initiated radical polymerization . The morphology of M-MIPs microspheres was examined by the field emission scanning electron microscope. The result indicated that most of prepared M-MIPs microspheres appeared snowman-like shape instead of the regular spherical form. The binding performance of M-MIPs microspheres was researched through a batch of binding tests including binding kinetics and binding isotherm. M-MIPs could reach binding equilibrium within 60 min. The binding capacity of M-MIPs (16.20 μmol g −1 ) was higher than that of magnetic non-imprinted polymers (M-NIPs), whose binding capacity was 9.44 μmol g −1 . The specific binding was also carried out with BPA and its structurally similar compounds. The result showed that the M-MIPs possessed high selectivity towards BPA with the imprinting factor of 1.69. The M-MIPs may be useful in the environmental and analytic fields.
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ACS Omega
·
2021
·
IF 3.512
Libin Wan,Huoliang Gao,Ge Yan,Haidong Gao,Mantang Chen
Molecularly imprinted polymers (MIPs) with high specific recognition capability are promising in environmental remediation. However, traditional MIPs usually show poor specific binding affinity toward templates in pure aqueous medium, thus greatly limiting their practical applications in wastewater treatment. Herein, we proposed a facile and versatile method to synthesize a water-compatible hierarchically porous MIP (HP-MIP), in which a metal–organic gel (MOG) was formed by in situ assembly and acted as a removable structural modulator. Remarkably, the integration of the MOG modulator and template imprinting defects significantly improved the specific template binding affinity of HP-MIP in water. The adsorption behavior of HP-MIP fitted well with the heterogeneous Freundlich isotherm, suggesting that HP-MIP possessed greater site heterogeneity to sildenafil than HP-NIP, which confirmed the efficiency of HP-MIP for the removal of sildenafil from water. This approach provides an important pathway to prepare water-compatible porous MIP for efficient removal of highly toxic organic pollutants from wastewater.
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Materials Today Chemistry
·
2021
·
IF 8.301
Y. Dong,W. Chen,X. Zhou
In this study, a novel flame retardant , that is, amino-terminated phosphorous polyborosiloxane (N-PBSi), was synthesized via a two-step polymerization reaction. The product's chemical structure was characterized firstly by Fourier transform infrared (FTIR) spectroscopy, nuclear magnetic resonance, and X-ray photoelectron spectroscopy. It was proved that the prepared N-PBSi was indeed amino terminated and contained multiple flame-retardant elements including P, B, and Si. Besides, based on the variation of its FTIR spectra from room temperature to 700 °C and the subsequent thermogravimetric results, there also showed that the resultant N-PBSi had desirable thermal stability. This is a prerequisite for preparing flame-retardant polymethacrylimide (PMI) as PMI synthesis requires a high temperature treatment process up to 160 °C. On this basis, the condition for N-PBSi synthesis was then optimized to obtain flame retardants with better quality and higher yield. According to the experiments, the reactant ratio and reaction time were recommended to be 1:1.33:3 and 6 h, respectively. To evaluate the effectiveness of N-PBSi further, the flame retardancy of PMI with N-PBSi grafted was then investigated. The UL-94 rating and limiting oxygen index value of the PMI with 15 wt.% of N-PBSi incorporated were tested to be V-0 and 27%, respectively, indicative of greatly enhanced flame-retardant properties. In addition, the flame-retardant mechanism of N-PBSi on PMI was also discussed. Given all of these, the prepared N-PBSi as a reactive and effective flame retardant was promising for PMI.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2021
·Vol. 414
·期 18
·5255-5262
·
IF 4.157
Qian Hai-Long,Liu Fang,Liu Xue,Yang Cheng,Yan Xiu-Ping
The separation of amino acid (AA) enantiomers shows significance for chemistry, food, and biology, but remains challenging due to their similar properties. A promising nanoporous chiral covalent organic framework (COF) as a stationary phase for high-performance liquid chromatography (HPLC) suffers from the irregularity and widely distributed particle size of the chiral COF. Herein, we show the facile preparation of a chiral COF-monolith as a stationary phase for HPLC enantiomeric separation of AAs via orthogonal experiments. The CTzDa-monolith is prepared by the incorporation of the model chiral COF named CTzDa into the porous poly(ethylene dimethacrylate-co-methacrylate) monolith and reveals great permeability and mechanical stability. The corresponding CTzDa-monolithic column gives better chiral HPLC separation of AAs than the commercial Poroshell 120 chiral-T column. Thermal dynamic analysis and molecular docking calculations imply the involvement of stereoscopic hydrogen, π-π, and van der Waals interactions between the CTzDa and AAs during HPLC enantioseparation. The facile incorporation of the chiral COF into the porous monolith will promote the potential of a chiral COF as a stationary phase for HPLC. Graphical abstract
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ADVANCED MATERIALS
·
2020
·Vol. 32
·期 33
·2001222
·
IF 27.398
Dewen Li,Xiaochen Bu,Zongpu Xu,Yingwu Luo,Hao Bai
Cellular plastics have been widely used in transportation, aerospace, and personal safety applications owing to their excellent mechanical, thermal, and acoustic properties. It is highly desirable to impart them with a complex porous structure and composition distribution to obtain specific functionality for various engineering applications, which is challenging with conventional foaming technologies. Herein, it is demonstrated that this can be achieved through the controlled freezing process of a monomer/water emulsion, followed by cryopolymerization and room temperature thawing. As ice is used as a template, this method is environmentally friendly and capable of producing cellular plastics with various microstructures by harnessing the numerous morphologies of ice crystals. In particular, a cellular plastic with a radially aligned structure shows a negative Poisson’s ratio under compression. The rigid plastic shows a much higher energy dissipation capability compared to other materials with similar negative Poisson’s ratios. Additionally, the simplicity and scalability of this approach provides new possibilities for fabricating high-performance cellular plastics with well-defined porous structures and composition distributions.
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