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Dual-functional poly(2-methyl-2-oxazoline)/poly(2-(dimethylamine)ethyl methacrylate)mixed brushes with switchable protein adsorption and antibacterial properties

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Chinese Journal of Chemical Engineering 2024年第2期66卷 19-30页

作者： Kang He Liangyu Zhu Yanmei Wang CAS Key Laboratory of Soft Matter Chemistry Department of Polymer Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China

Herein,binary mixed brushes consisting of poly(2-methyl-2-oxazoline)(PMOXA)and poly(2-(dimethylamine)ethyl methacrylate)(PDMAEMA)with different chain lengths were fabricated by successive grafting of NH_(2)-terminated PMOXA and SH-terminated PDMAEMA onto polydopamine-anchored substrates.The mixed-brush coating was characterized by variable-angle spectroscopic ellipsometry,X-ray photoelectron spectroscopy,Fourier transform infrared spectroscopy,zeta potential measurements,water contact angle,and atomic force microscopy.The mixed brushes showed tunable surface charge,wettability,and surface roughness,depending on the degree of PDMAEMA swelling under varying pH and ionic strength(Ⅰ).Then the adsorption behaviors of pepsin,bovine serum albumin(BSA),γ-globulin,and lysozyme,four very different proteins with regard to isoelectric point,on the mixed brushes coating were studied by using fluorescence microscopy and surface plasmon resonance.When the chain length of PDMAEMA was about twice as long as PMOXA,the mixed brushes not only had high adsorption capacity for pepsin,BSA,and y-globulin but also had a desorption efficiency of 86.9%,87.1%,and 93.5%,respectively.It is explained that electrostatic attraction between the protonated PDMAEMA and positively charged acidic proteins(pepsin and BSA,whose isoelectric points were below the pK_(a) of PDMAEMA)would drive the intensive adsorption(at pH 3,I=10^(-3)mol·L^(-1)for pepsin,and pH 5,I=10^(-5)mol·L^(-1)for BSA),while desorption was dominated by the hydrophilic PMOXA when PDMAEMA was shrinking(at pH 7,I=10^(-1)mol·L^(-1)for pepsin,and pH 9,I=10^(-1)mol·L^(-1)for BSA).Furthermore,the isoelectric precipitation led to the adsorption of neutral protein(γ-globulin,whose isoelectric point was near the pK_a of PDMAEMA)at pH 7,I=10^(-5)mol·L^(-1),while electrostatic repulsion and antifouling PMOXA triggered the desorption of y-globulin at pH 3,I-10^(-1)mol·L^(-1).However,alkaline protein(lysozyme,whose isoelectric point was higher than the pK_(a) of PDMAEMA)exhibited slight adsorptio

关键词： Switchable conformation transition Controllable protein adsorption Mixed brushes Isoelectric point Antibacterial surface

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RANDOM COpolymer OF PROPYLENE OXIDE AND ETHYLENE OXIDE PREPARED BY DOUBLE METAL CYANIDE COMPLEX CATALYST

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Chinese Journal of polymer science 2002年第5期20卷 453-459页

作者： Yi-jun Huang Guo-rong Qi Guan-xi Chen department of polymer science and Engineering, Zhejiang University Hangzhou 310027,China department of polymer science and Engineering Zhejiang University Zhangzhou 310027 department of polymer science and Engineering Zhejiang University Hangzhou 310027

Copolymerization of propylene oxide (PO) and ethylene oxide (EO) using double metal cyanide (DMC) complex as the catalyst was carried out. The structure of random copolymers was confirmed by C-13-NMR and IR spectra. H-1-NMR analysis shows that the EO content in the copolymer is the same as that in the initial monomer feed. Moderate molecular weight copolymers with various EO content were obtained and their values of molecular weight distribution (MWD) fell in the range of 1.21-1.55. It was found that the molecular weight of copolymers is controlled by the mass ratio of EO+PO to initiator moles used, The reaction rate as well as polymer yield decrease with increasing EO content in the feed composition.

关键词： propylene oxide ethylene oxide double metal cyanide complex

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The Effect of Blending Ratio on the Structure and Properties of the PPR/PS In situ Fiber Reinforced System Prepared by Multi-Flow Vibration Injection Molding

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Chinese Journal of polymer science 2024年第6期42卷 851-863页

作者： Yan-Jiang Li Meng-Long Hu Jun-Wen Zhang Qiang Fu Jie Zhang College of polymer science and Engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu610065China

To enhance the mechanical properties of polypropylene random copolymer(PPR),polystyrene(PS)with four different contents were added to the PPR matrix through melt blending.Subsequently,using the Multi-Flow Vibration Injection Molding(MFVIM)technology,PPR/PS in situ microfiber composites(MFC)with different blending ratios were prepared.The results indicated that blending ratio had a great impact on the phase morphology and crystal structure of MFVIM samples,which was different from those of conventional injection molding(CIM)samples.PS ultrafine fibers could be formed under the shear field and could absorb the PPR molecular chains to form hybrid shish-kebab structures.Meanwhile,the PPR matrix could also form shish-kebab structures under the effect of strong shear.When the PS content reached 20%,under the combined action of PS in situ microfibers and highly oriented crystal structure,the tensile strength and Young’s modulus of the sample were obviously improved and the impact strength remained at a relatively high level.So a strong and tough balanced PPR based material was obtained.These results provide valuable insights for expanding the industrial and daily-life applications of PPR and show promising development prospects.

关键词： PPR MFVIM In situ microfibers Shearfield Hybrid shish-kebab structures

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Recent Advances in Asymmetric Structural Composites for Excellent Electromagnetic Interference Shielding: A Review

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Chinese Journal of polymer science 2024年第6期42卷 693-710页

作者： Ying Zhou Bai Xue Lan Xie Chang-Mei Wu Qiang Zheng department of polymer Materials and Engineering College of Materials and Metallurgy Guizhou University National Engineering Research Center for Compounding and Modification of polymer Materials National and Local Joint Engineering Research Center for Functional Polymer Membrane Materials and Membrane Processes State Key Laboratory of Public Big Data Guizhou University department of polymer science and Engineering Zhejiang University

Since electromagnetic pollution is detrimental to human health and the environment, numerous efforts have been successively made to achieve excellent electromagnetic interference shielding effectiveness(EMI SE) via designing the hierarchical structures for electromagnetic interference(EMI) shielding polymer composites. Among the plentiful structures, the asymmetric structures are currently a hot spot, principally categorizing into multi-layered, porous, fibrous, and segregated asymmetric structures, which endows the high EMI shielding performance for polymer composites incorporated with magnetic, conductive, and/or dielectric micro/nano-fillers, due to the “absorption-reflection-reabsorption” shielding mechanism. Therefore, this review provides the retrospection and summary of the efforts with respect to abundant asymmetric structures and multifunctional micro/nano-fillers for enhancing EMI shielding properties, which is conducive to the booming development of polymeric EMI shielding materials for the promising prospect in modern electronics and 5-generation(5G) technology.

关键词： Asymmetric structure Microano functional filler polymer composite Electromagnetic interference shielding

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Highly Hydrolysis-Resistant Polyimide Fibers Prepared by Thermal Crosslinking with Inherent Carboxyl Groups

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Chinese Journal of polymer science 2024年第2期42卷 247-255,I0010页

作者： Can-Can Zhang Jun-Long Yang Ya-Jiang Huang Guang-Xian Li College of polymer science and Engineering State Key Laboratory of Polymer Materials Engineering of ChinaSichuan UniversityChengdu610065China

Easy hydrolysis in alkaline environments limits the use of polyimide fibers in environmental protection. The hydrolysis resistance levels of polyimide fibers can be improved by crosslinking of the macromolecular chains. In this work, crosslinked polyimide fibers(CPI fibers) were produced by intrinsic carboxyl decarboxylation for the first time. The thermal stability of the polyimide fibers containing the intrinsic carboxyl groups(PIC fibers) was studied, and the temperature of the decarboxylation-crosslinking reaction was determined to be 450 ℃. The PIC fibers were hotdrawn to initiate thermal crosslinking of the carboxyl groups and molecular chain orientation at high temperature. The CPI fibers had high tensile strengths(0.72-1.46 GPa) and compressive strengths(401-604 MPa). The oriented macromolecules and chemically crosslinked structure improved the tightness of the molecular chains and endowed the CPI fibers with excellent hydrolytic resistance. The CPI-50 fiber did not dissolve in a 0.5 wt% NaOH solution during heating at 90 ℃ for 10 h, and the tensile strength retention reached 87% when treated in 0.5 wt% NaOH solutions at 90 ℃ for 1 h, providing a guarantee for its application in alkaline corrosive environments.

关键词： Polyimide Carboxyl group Crosslinking Hydrolysis-resistance

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Arbitrary skin metallization by pencil-writing inspired solid-ink rubbing for advanced energy storage and harvesting

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Journal of Energy Chemistry 2024年第1期88卷 592-602,I0013页

作者： Yonghan Zhou Zhongfeng Ji Wenrui Cai Xuewei He Ruiying Bao Xuewei Fu Wei Yang Yu Wang College of polymer science and Engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu 610065SichuanChina

The development of a durable metallic coating on diverse substrates is both intriguing and challenging,particularly in the research of metal-conductive materials for applications such as batteries,soft electronics,and beyond.Herein,by learning from the pencil-writing process,a facile solid-ink rubbing technology(SIR-tech)is invented to address the above challenge.The solid-ink is exampled by rational combination of liquid metal and graphite particles.By harnessing the synergistic effects between rubbing and adhesion,controllable metallic skin is successfully formed onto metals,woods,ceramics,and plastics without limitation in size and shape.Moreover,outperforming pure liquid-metal coating,the composite metallic skin by SIR-tech is very robust due to the self-lamination of graphite nanoplate exfoliated by liquid-metal rubbing.The critical factors controlling the structures-properties of the composite metallic skin have been systematically investigated as well.For applications,the SIR-tech is demonstrated to fabricate high-performance composite current collectors for next-generation batteries without traditional metal foils.Meanwhile,advanced skin-electrodes are further demonstrated for stable triboelectricity generation even under temperature fluctuation from-196 to 120℃.This facile and highly-flexible SIR-tech may work as a powerful platform for the studies on functional coatings by liquid metals and beyond.

关键词： Microadhesion guided technology Skin metallization by solid-ink rubbing Liquid metal composites Composite current collector Batteries and triboelectric nanogenerators

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Highly Improved Creep Resistance in Polypropylene Through Thermally Reduced Graphene Oxide and Its Creep Lifetime Prediction

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Chinese Journal of polymer science 2024年第2期42卷 256-266,I0010页

Polypropylene(PP) exhibits suboptimal creep resistance due to the presence of methyl groups on its main chain, leading to irregular chain segment distribution, diminished inter-chain interaction, and crystallinity. This structural feature causes chain slippage in PP under stress,significantly constraining its service lifetime. In this study, thermally reduced graphene oxide(TrGO) nanosheets were incorporated into the PP matrix, yielding a nanocomposite with exceptional creep resistance performance. Results demonstrated that at a stress of 25 MPa, a 2.0 wt% TrGO content could enhance the creep failure lifetime of PP by 21.5 times compared to neat PP. Rheology, transmission electron microscopy(TEM),and scanning electron microscopy(SEM) characterization techniques were employed to analyze the mechanism of TrGO's influence on PP's creep behavior. It was observed that when TrGO content exceeded 1.0 wt%, an effective particle network structure formed within the PP matrix. This homogeneously dispersed TrGO-formed particle network structure restricted the migration and rearrangement of PP molecular chains, enabling prolonged stress resistance without structural failure. By combining the time-strain superposition method with the critical failure strain as a criterion, generalized creep compliance curves for PP and its composites were established, facilitating the prediction of material creep failure lifetimes, with a strong agreement between experimental and predicted lifetime values. This research proposes a novel strategy aimed at developing polypropylene materials and products with enhanced long-term stability and durability, thus extending service life, reducing failure risk, and broadening their potential across various application domains.

关键词： Thermally reduced graphene oxide Polypropylene Creep failure and lifetime prediction

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CONTROLLED RADICAL COpolymerIZATION OF STYRENE AND MALEIC ANHYDRIDE UNDER GAMMA RADIATION IN THE PRESENCE OF BENZYL DITHIOBENZOATE

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Chinese Journal of polymer science 2002年第6期20卷 525-530页

作者： De-cheng Wu Ying-fang Zou Cai-yuan Pan department of polymer science and Engineering University of science and Technology of China, Hefei 230026, China department of polymer science and Engineering University of Science and Technology of China Hefei 230026

The copolymerization of styrene (St) with maleic anhydride (MAh) under gamma radiation at room temperature in the presence of benzyl dithiobenzoate (BDTB) was found to display 'living' nature evidenced by constant concentration of chain radicals during the copolymerization, linear evolution of molecular weights with conversion and narrow molecular weight distribution (M-w/M-n = 1.23-1.35). The compositional analysis and the sequence structural information of the copolymers obtained from DEPT (Distortionless Enhancement by Polarization Transfer) experiments demonstrate that the copolymers obtained also possess strictly alternating structure.

关键词： controlled radical polymerization alternating copolymer maleic anhydride styrene

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SYNTHESIS AND CHARACTERIZATION OF FOUR-ARMED BLOCK POLY(STYRENE-b-p-NITROPHENYL METHACRYLATE)PREPARED BY THE ATRP METHOD

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Chinese Journal of polymer science 2002年第4期20卷 353-360页

作者： Cai-yuan Pan Lei Tao Ye Liu department of polymer science and Engineering University of science and Technology of China, Hefei 230026 China department of polymer science and Engineering University of Science and Technology of China Hefei 230026

A novel tetrafunctional initiator, C [CH_2O (CH_2)_3 OOCCH(Br)CH_3]_4 (1), was synthesized through the reaction oftetraol with α-bromopropionyl chloride, and then was used as initiator of atom transfer radical polymerization (ATRP) in thepreparation of 4-armed polystyrene (PSt) with narrow polydispersity. The structure, molecular weight and molecular weightdistribution (MWD) of each arm were studied by ~1H-NMR and GPC data of hydrolyzed products of the 4-armed PSt. TheATRP of St using 1/CuBr/bpy as initiator system is of 'living' character based on the following evidence: narrow MWD,constant concentration of chain radical during the polymerization, control of molecular weight by the molar ratio of monomerconsumed to 1. The 4-armed poly(St-b-p-nitrophenyl methacrylate) [poly(St-b-NPMA)] was prepared by the ATRP ofNPMA using 4-armed PSt with terminal bromine as the initiator, and characterized by FT-IR, ~1H-NMR spectra and GPCcurves. The micelles with PSt as core, and PNPMA as shell were formed by dropping DMSO into a solution of 4-armedpoly(St-b-NPMA) in DMF, as proved by laser light scatter (LLS) method.

关键词： Tetrafunctional initiator Atom transfer radical polymerization 4-Armed polystyrene 4-Armed poly(styrene-b-pnitrophenyl methacrylate) Unimolecular micelles

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Preparation of Self-limiting Heating Cables with Excellent Processability, Mechanical Properties and PTC Effect via Thermal and Electrical Treatments

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Chinese Journal of polymer science 2024年第4期42卷 511-520页

作者： Tian-Hao Yang Tong Wu Qiang Fu State Key Laboratory of polymer Materials Engineering College of Polymer Science and EngineeringSichuan UniversityChengdu610065China State Key Laboratory of polymer Materials Engineering Polymer Research Institute of Sichuan UniversityChengdu610065China

polymer/conductive filler composites have been widely used for the preparation of self-limiting heating cables with the positive temperature coefficient (PTC) effect. The control of conductive filler distribution and network in polymer matrix is the most critical for performance of PTC materials. In order to compensate for the destruction of the filler network structure caused by strong shearing during processing, an excessive conductive filler content is usually added into the polymer matrix, which in turn sacrifices its processability and mechanical properties. In this work, a facile post-treatment of the as-extruded cable, including thermal and electrical treatment to produce high-density polyethylene (HDPE)/carbon black (CB) cable with excellent PTC effect, is developed. It is found for the as-extruded sample, the strong shearing makes the CB particles disperse uniformly in HDPE matrix, and 25 wt% CB is needed for the formation of conductive paths. For the thermal-treated sample, a gradually aggregated CB filler structure is observed, which leads to the improvement of PTC effect and the notable reduction of CB content to 20 wt%. It is very interesting to see that for the sample with combined thermal and electrical treatment, CB particles are agglomerated and oriented along the electric field direction to create substantial conductive paths, which leads to a further decrease of CB content down to 15 wt%. In this way, self-limiting heating cables with excellent processability, mechanical properties and PTC effect have simultaneously been achieved.

关键词： Self-limiting heating cables Positive temperature coefficient Thermal treatment Electrical treatment

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