MACROMOLECULES
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2025
·
IF 5.2
Mengjie Si,Yan-Jie Wang,Yueman Tang,Wei Jian,Ji Lin,Si Yu Zheng,Jintao Yang
Zwitterionic hydrogels have great potential as implant materials due to their excellent resistance to protein adsorption. However, it remains a great challenge to toughen these gels owing to the ultrastrong hydration capability of polyzwitterions, which leads to weak associations between hydrated chains. Herein, a zwitterionic hydrogel with integration of toughness and protein resistance was developed by programming the benzene–methylene–imidazolium motif into the zwitterionic moiety and regulating its association behavior. It was found that the benzene and imidazolium did not interfere with the hydration of the anionic group, yet they changed the water coordination shell around the cationic group to allow the formation of compact zwitterion pairs. Taking advantage of 1H NMR technology and MD simulation, all of the benzene, imidazolium, and methylene between them were revealed as key moieties that facilitate the associations, especially at high monomer concentrations. Among them, the imidazolium was proven to be the predominant factor. Then, the densely associated monomers were conducive to polymerizing into a highly entangled network, contributing to simultaneous improvements in Young’s modulus, toughness, and resilience. Meanwhile, the typical characteristics of a zwitterionic gel were not sacrificed, showing high resistance to protein adsorption. This work provides new insights into the chemical and mechanical design of the zwitterionic gels.
研究领域:
材料科学
·
生物医学工程
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2017
·
IF 3.387
Yufeng Lei,Yaling Lin,Anqiang Zhang
Zwitterionic polymers have been used to cope with nonspecific protein adsorption and bio-fouling problems for a wide range of materials, including biomedical devices, marine coatings and membrane separation. However, direct surface modification with highly water-soluble zwitterionic polymers is rather difficult due to their poor attachment to hydrophobic solid surfaces. In this work, we utilize the hydrophobic interaction to anchor zwitterionic polysiloxanes grafted with cysteine onto surfaces by adding an hydrophobic block of polydimethylsiloxanes, referred as PDMS- b -(PDMS- g -Cys)s. The synthesis involves only three steps of reactions, and the structures of each product were characterized using GPC, FT-IR and 1 H NMR. The adsorption and protein resistance of PDMS- b -(PDMS- g -Cys)s on a gold surface are investigated with QCM-D. The results show that the hydrophobic interaction moieties of the additional PDMS blocks help the hydrophilic cysteine-grafted blocks stably attach and then function on the sensor. These findings suggest that the addition of hydrophobic moieties provides an effective approach to construct anti-fouling interfaces with zwitterionic polymers in aqueous solution.
研究领域:
材料科学
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生物医学工程
·
表面化学
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DOI
高影响因子
LANGMUIR
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2015
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IF 4.457
Jielin Ma,Chunfeng Ma,Guangzhao Zhang
Protein resistance is the central issue in marine antibiofouling. We have prepared poly(ε-caprolactone) (PCL)-based polyurethane with 2-(dimethylamino) ethyl methacrylate (DEM) as pendant groups by a combination of the thiol–ene click reaction and the condensation reaction. By the use of quartz crystal microbalance with dissipation (QCM-D) and surface plasmon resonance (SPR), we have investigated the adsorption of fibrinogen, bovine serum albumin (BSA), and lysozyme on the polymer surface. The polymer exhibits protein resistance in seawater but not in fresh water because DEM pendant groups carry net neutral charges in the former. The evaluation of antibacterial adhesion of the polymer by using Micrococcus luteus demonstrates that the polymer can effectively inhibit the settlement of marine bacteria. Our studies also show that the polymer is degradable in marine environments.
研究领域:
材料科学
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生物医学工程
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海洋科学
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DOI
PubMed
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2014
·Vol. 131
·期 21
·
IF 1.64
Renchang Zeng,Jiang Cheng,Shouping Xu,Qin Liu,Xiufang Wen,Pihui Pi
Reversible addition–fragmentation chain-transfer polymerization was introduced to prepare a series of zwitterionic poly(hydroxyethyl methacrylate)- g -poly(sulfobetaine methacrylate) (PSBMA) hydrogels (HSGs) with different monomer feed ratios. Compared with PSBMA hydrogels, these hydrogels exhibited enhanced mechanical strengths. Then, the HSGs were characterized by Fourier transform infrared spectroscopy, scanning electron microscopy, and swelling measurements. We found that the equilibrium swelling ratios, mechanical strengths, and drug-release behaviors were significantly affected by the feed ratios of the gels. The hydrophilic tetracycline hydrochloride release results suggest that the hydrophilic drug release from the HSGs could be prolonged by the variation of the hydroxyethyl methacrylate amount in the gel networks. The bovine serum albumin adsorption data showed that the zwitterionic HSG with 18.2 wt % sulfobetaine methacrylate exhibited good protein-resistance properties. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014 , 131 , 41041.
研究领域:
材料科学
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生物医学工程
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高分子化学
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产品关联
DOI
高影响因子
LANGMUIR
·
2014
·
IF 4.384
Chunhua Wang,Chunfeng Ma,Changdao Mu,Wei Lin
We have developed a novel approach to introduce zwitterions into polyurethane for the preparation of antibiofouling coating. First, the thiol–ene click reaction between 2-(dimethylamino)ethyl methacrylate (DMAEMA) and 3-mercapto-1,2-propanediol (TPG) is used to synthesize dihydroxy-terminated DMAEMA (DMA(OH)2) under UV catalysis. The product has been proved by gel permeation chromatography (GPC), Fourier transform infrared spectrum (FT-IR), proton nuclear magnetic resonance (1H NMR), and high resolution mass spectrometry (HRMS). DMA(OH)2 is then incorporated into polyurethane as side groups by polyaddition with diisocyanate and further reacts with 1,3-propane sultone to obtain the zwitterionic polyurethanes. The presence of sulfobetaine zwitterions side groups has been demonstrated by FT-IR and X-ray photoelectron spectroscopy (XPS). Thermal analysis indicates that the thermal stability is decreased with the increasing content of zwitterionions. The antibiofouling property of polyurethanes has been investigated by the measurement of adsorption of fibrinogen, bovine serum albumin (BSA), and lysozyme on the polyurethanes surface using quartz crystal microbalance with dissipation (QCM-D). The results show that the polyurethane coatings exhibit effective nonspecific protein resistance at higher content of zwitterionic side groups.
研究领域:
材料科学
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生物医学工程
·
表面化学
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产品关联
DOI
PubMed
高影响因子
REACTIVE & FUNCTIONAL POLYMERS
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2015
·
IF 2.515
Chong Zhang,Lijuan Chen,Lin Tan,Xiajun Zheng,Yanmei Wang
In this study, a set of well-defined multiarm star copolymers , hyperbranched poly(ethylenimine)-graft-poly(ethylene glycol) (bPEI- g -PEG) with different PEG grafting ratios were synthesized. The star PEG-based coatings were then prepared by immobilizing the corresponding copolymers onto poly(dopamine) (PDA)-coated substrates. The chemical composition , hydrophilicity , surface topography , and thickness of the coatings were studied by X-ray photoelectron spectroscopy (XPS), water contact angle (WCA), atomic force microscopy (AFM), and variable angle spectroscopic ellipsometry (VASE), respectively. Furthermore, the surface PEG chain density of star PEG-based coating was evaluated quantitatively and compared with that of linear PEG-based coating. Our results showed that the amount of proteins (albumin from bovine serum, fibrinogen, and lysozyme) adsorbed on the star PEG-based coating as measured by surface plasmon resonance (SPR) was found to be dependent on the surface PEG chain density, which was controlled by the polymer incubation concentrations and PEG grafting ratios. Generally, the star-shaped PEG gave the surface with higher PEG chain density than linear ones and the amount of adsorbed proteins decreased with increasing surface PEG chain density. At last, the star PEG-based coating was successfully applied into the capillary inner surface for protein separation by capillary electrophoresis (CE).
研究领域:
材料科学
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生物医学工程
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分析化学
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DOI
高影响因子
MACROMOLECULAR RESEARCH
·
2017
·Vol. 25
·期 8
·817-825
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IF 1.405
Xu Yiting,Huang Jiamei,Li Yuntong,Wang Meijie,Cao Ying,Yuan Conghui,Zeng Birong,Dai Lizong
A novel zwitterionic hybrid amphiphilic copolymer containing polyhedral oligomericsilsesquioxane (POSS), and poly(methacrylate isobutyl POSS)- b -poly (3-dimethyl(methacryloyloxyethyl) ammonium propane sulfonaten- co -2-(diethylamino) ethyl methacrylate- co -styrene) (PMAiBuPOSS- b -P(DMAPS- co -DMAEMA- co -St)), was prepared by the ring open reaction of 1, 3-propane sultone with tertiary amine on the precursor polymer. This hybrid copolymer could self-assemble into spherical micelle with a relatively narrow size distribution. The micelle size exhibited a great dependence on pH, as the size of the micelles was of evidently decreases with the increase of the pH value. Controllable release of pyrene from the micelles was investigated by fluorescent emission spectra. Micelles with more zwitterionic units would lead to less pyrene release and longer equilibrium time. The protein adsorption resistance of the micelles was tested by mixing them with fetal bovine serum. The antifouling ability was improved by increasing the number of zwitterionic units as well as decreasing the number of DMAEMA units. This novel hybrid amphiphilic random copolymer with the pH-responsive and anti-protein-fouling ability, can be potentially used for drug carriers for controlled release.
研究领域:
材料科学
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生物医学工程
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DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
·
IF 4.9
Miaomiao Ma,Yuhong Qi,Chuanjun Gu,Zhanping Zhang
Revealing the adsorption behavior of proteins on amphiphilic polymers is an interesting study. For the first time, the adsorption behavior of bovine serum albumin (BSA) protein on the surface of polyethylene glycol polystyrene (PEG-PS) amphiphilic polymer membrane is developed by molecular dynamics (MD) simulations and experiments. We found that PEG-PS has the ability to resist BSA protein adsorption. The adsorption of BSA on its surface undergoes a process of "rotation-preadsorption-desorption-final adsorption". After adsorption, the helical structure of BSA underwent "tight-loose-unwinding" changes. The transition from PEG chain helical structure to free coil structure is a key factor leading to the adsorption and desorption of BSA. Furthermore, the hydrophobic force of PS is the main driving force for BSA adsorption. These studies can inspire the design of amphiphilic materials to realize protein antifouling or transportation materials.
研究领域:
生物物理学
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材料科学
·
蛋白质工程
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产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Lingmin Yi,Kai Xu,Guanying Xia,Jiawei Li,Weixiang Li,Ying Cai
Methacryloyl-terminated poly[methyl(3,3,3-trifluoropropyl)siloxane] (PMTFPS-MA) macro-monomers with controlled segment length were designed and synthesized by anionic ring-opening polymerization of 1,3,5-trimethyl-1,3,5-tri(3′,3′,3′-trifluoropropyl)cyclotrisiloxane (F 3 ). Then, a series of novel amphiphilic fluorosiloxane-containing graft copolymers were prepared using PMTFPS-MA, poly(ethylene glycol) methyl ether methacrylate (PEG-MA) and methyl methacrylate (MMA) as the co-monomers, and their surface properties and protein-resistant performance were investigated. It was found that the composition of amphiphilic graft copolymers would play an important role in the protein-resistant properties. When the copolymers contain 65.5 wt% PEO segments and 6.4 wt% PMTFPS segments, the coating surface exhibits strong protein-resistant property and shows almost no protein adsorption on it. Based on the surface analysis of amphiphilic graft copolymer films both in dry and wet conditions, the protein-resistant property of amphiphilic copolymers can be owing to the transition from a hydrophobic surface to hydrophilic surface with highly efficient water-driven PEO surface migration. The PEO segments are utilized to prevent protein adsorption whereas the low surface energy PMTFPS segments are utilized to drive away the adsorbed proteins.
研究领域:
材料科学
·
生物医学工程
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DOI
高影响因子
LANGMUIR
·
2014
·
IF 4.384
Qiongxia Shen,Lichao Liu,Weian Zhang
A novel surface-modification strategy has been developed for the construction of a photocontrolled silicon wafer surface with switchable wettability based on host–guest inclusion complexation. The silicon wafer was first modified by guest molecule azobenzene (Azo) via a silanization reaction. Subsequently, a series of polymers with different polarities were attached to host molecule β-cyclodextrin (β-CD) to prepare β-CD-containing hemitelechelic polymers via click chemistry. Finally, a photocontrolled silicon wafer surface modified with polymers was fabricated by inclusion complexation between β-CD and Azo, and the surface properties of the substrate are dependent on the polymers we used. The elemental composition, surface morphology, and hydrophilic/hydrophobic property of the modified surfaces were characterized by X-ray photoelectron spectroscopy (XPS), atomic force microscope, and contact angle measurements, respectively. The antifouling property of the PEG-functionalized surface was evaluated by a protein adsorption assay using bovine serum albumin, which was also characterized by XPS. The results demonstrate that the surface modified with PEG possesses good protein-resistant properties.
研究领域:
材料科学
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表面化学
·
生物材料
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产品关联
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2016
·
IF 2.567
Hao Yang,Leiming Guo,Zhaogen Wang,Nina Yan,Yong Wang
Poly(ethylene oxide) (PEO) is well-known for its excellent resistance to the nonspecific adsorption of proteins. However, it remains challenging to fabricate surfaces with uniform and robust coverage of PEO chains in a simple and efficient way. Simply by treating the block copolymer polystyrene-block-poly(ethylene oxide) (PS-b-PEO) in ethanol, we obtain nanoporous polymeric films with superior resistance to protein adsorption. The pores are nondestructively formed via the selective swelling-induced pore generation mechanism in which PEO microdomains embedded in PS matrix are selectively swollen in ethanol and collapsed in the subsequent air drying. Pore sizes and porosities can be typically tuned in the ranges ∼20–50 nm and ∼20–70%, respectively, by changing swelling durations and temperatures. Interestingly, the PEO chains are simultaneously migrated on the film surface and pore walls in the selective swelling-induced pore forming process. Atomic force microscopy examinations reveal that PEO chains are solvated when the film is wetted with water, closing the pores in the film. Thus, produced SEO films adsorb much less proteins than PS films without PEO on the surface, and also demonstrate a better fouling resistance than many reported PEO-covered surfaces prepared by other methods.
研究领域:
高分子材料学
·
生物界面学
·
表面科学
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生物医学工程
·
纳米技术
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DOI
高影响因子
Materials
·
2020
·Vol. 13
·期 16
·3478
·
IF 3.057
Hongpu Huang,Yefeng Feng,Jia Qu
A series of tem-responsive and protein-resistance property silica-di-block polymers SiO2-g-PMMA-b-P(PEGMA) hybrids are synthesized with methyl methacrylate (MMA) and poly (ethylene glycol) methyl ether methacrylate (PEGMA) by the surface-initiated atom transfer radical polymerization (SI-ATRP). The morphology in tetrahydrofuran (THF) solution, lower critical solution temperature (LCST), surface morphology, bovine serum albumin (BSA)-resistance property, and thermal stability of nanoparticles were analyzed. The results of1H-NMR, GPC, and TEM prove that the silica-di-block hybrids have been obtained. The silica-di-block hybrids shows the LCST (52–64 °C) in aqueous solution. The hybrid films casted by THF present distributed uniform granular bulges and the film surface is relatively smooth (Ra = 15.4 nm ~ 10.5 nm). The results of QCM-D showed that only a small amount of BSA protein(△f= 18.6 ~ 11.8 Hz) was adsorbed on the surface of the films. The result of XPS also demonstrated that only a small amount of BSA protein was absorbed onto the surface of the film (N% = 1.86). The TGA analyses indicate that the thermal decomposition temperature of hybrids is 288 °C. Thus, it is suggested that the hybrids are served as a suitable coating with BSA resistance property and thermal stability.Keywords:silica-di-block hybrids;LCST;surface properties;BSA resistance;coating
研究领域:
材料科学
·
生物医学工程
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产品关联
DOI
PubMed
高影响因子