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Self-assembled nanochaperones enable the disaggregation of amyloid insulin fibrils

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Science China Chemistry 2022年第2期65卷 353-362页

作者： Hui Wang Ang Li Menglin Yang Yu Zhao Linqi Shi rujiang ma Key Laboratory of Functional Polymer materials of Ministry of Education Institute of Polymer ChemistryCollege of ChemistryNankai UniversityTianjin 300071China State Key Laboratory of Medicinal Chemical Biology Nankai UniversityTianjin 300071China

The deposition of highly ordered amyloid fibrils is recognized as a hallmark of amyloidosis diseases such as Alzheimer’s disease and Parkinson’s *** the amyloid fibrils is considered as one of the effective strategies for the control and treatment of amyloidosis *** this article,by simulating the function of natural molecular chaperones,co-assembled block copolymer micelles with coordination groups of nitrilotriacetic acid(NTA)and hydrophobic microdomains of poly(Nisopropylacrylamide)(PNIPAM)on the surface were used as nanochaperones(n Chaps)to disaggregate amyloid insulin *** ions chelated by NTA can bind the histidine imidazole residues while the PNIPAM microdomains can interact with the exposed hydrophobic sites on the amyloid insulin fibrils,which synergistically perturb the stability of amyloid insulin fibrils,loosen their structure,and finally promote their disaggregation.A combination of characterizations with fluorescence spectroscopy,transmission electron microscopy(TEM),dynamic hight scattering(DLS),and quartz crystal microbalance(QCM)demonstrated that mature amyloid insulin fibrils were completely disaggregated after incubating with n Chaps for 90 *** study may provide a promising strategy for the development of n Chaps for the treatment of amyloidosis diseases.

关键词： amyloid fibrils insulin nanochaperones disaggregation

Optic and catalytic properties of gold nanoparticles tuned by homopolymers

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Science China Chemistry 2009年第9期52卷 1372-1381页

作者： CHEN Xi ZHAO DongYun ZHAO LiZhi AN YingLi ma rujiang SHI LinQi HE QiJun CHEN Li Tianjin Key Laboratory of Fiber Modification and Functional Fiber School of Materials Science and Chemical EngineeringTianjin Polytech UniversityTianjin 300160China Key Laboratory of Functional Polymer materials Ministry of EducationInstitute of Polymer ChemistryNankai UniversityTianjin 300071China

Gold nanoparticles (GNs) are prepared through in situ reduction using NaBH4 in the presence of homopolymer PDmaEma. The sizes of the GNs can be adjusted by alternating the molar ratio of gold to DmaEma. Pure PDmaEma aqueous solution shows a phase-transition at 50°C at pH 10 and 25°C at pH 14, while PDmaEma-supported GNs aqueous solution shows a phase-transition at 47°C at pH 10 because of the increasing hydrophobic property resulting from GNs. Due to the pH and temperature-responsible characteristics of PDmaEma, the resulting PDmaEma-supported GNs exhibit pH adjustable temperature-responsive characteristics in optic and catalytic aspects. Under an acidic condition (pH 2), the GNs show unchanged surface Plasmon absorbance with a peak of 518 nm in a temperature range from 20 to 65°C. Under a basic condition (pH 10), the GNs first show the same absorbance with a peak at 518 nm in a temperature range from 20 to 40°C, and then the absorbance red shifts from 518 to 545 nm as temperature increases from 40 to 65°C. When the GNs are used as catalysts to catalyze the reduction of p-nitrophenol, the catalytic activity can be adjusted by changing the permeation of reactants in the PDmaEma layer at low and high temperatures, respectively.

关键词： gold nanoparticles catalyst homopolymer

Micellization of copolymers via noncovalent interaction with TPPS and aggregation of TPPS

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Science China Chemistry 2011年第2期54卷 343-350页

作者： ZHAO LiZhi XIANG Rui ZHANG LiYan WU ChengLin ma rujiang AN YingLi SHI LinQi Key Laboratory of Functional Polymer materials Ministry of EducationInstitute of Polymer ChemistryNankai UniversityTianjin 300071China

Aggregation of 5,10,15,20-tetrakis-(4-sulfonatophenyl)-porphyrin (TPPS) was investigated in complex micelles composed of poly(ethylene glycol)-block-poly(4-vinylpyridine) (PEG-b-P4VP) and poly(2-(dimethylamino)ethyl methylacrylate)-b-poly(Nisopropylacrylamide) (PDmaEma-b-PNIPAM) in aqueous *** resultant complex micelles had a complex P4VP/ PDmaEma/TPPS core and a mixed PEG/PNIPAM *** noncovalent interaction modes between the porphyrin and each copolymer accomplished a co-effect on the aggregation of *** formation of aggregates was *** pH 3.2–6.5,TPPS existed as a mixture of H-aggregates and monomers because of the aromatic-aromatic interaction with P4VP and electrostatic interaction with *** monomers translated into J-aggregates,stabilized by electrostatic interaction with the both polyelectrolyte blocks,upon decreasing the pH to *** free-base monomer was the one and only form for the dye at pH 11.0 due to aromatic stacking with the pyridyl rings.

关键词： block copolymer TPPS H-aggregates J-aggregates

Protein@PP-Zn nanocomplex assembled by coordination of zinc ions used for intracellular protein delivery

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Science China Chemistry 2023年第8期66卷 2354-2362页

作者： Liyun Cui Sainan Liu Fan Wu Hua Chen Yuanfeng Li Linqi Shi Yong Liu rujiang ma Key Laboratory of Functional Polymer materials of Ministry of Education Institute of Polymer ChemistryCollege of ChemistryNankai UniversityTianjin300071China Wenzhou Institute University of Chinese Academy of SciencesWenzhou Key Laboratory of Interdiscipline and Translational MedicineWenzhou325001China Translational Medicine Laboratory the First Affiliated Hospital of Wenzhou Medical UniversityWenzhou325035China

In recent years,intracellular delivery of protein drugs has attracted great attention,and polymer-based systems have been extensively exploited to develop efficient and safe ***,efficient intracellular delivery of protein drugs remains a challenge because of the cell membrane barrier and endosome ***,we report a protein@PP-Zn nanocomplex,which consists of an imidazole-containing block polymer poly(ethylene glycol)-block-poly(β-amino ester)(PEG-b-PAE(Im),PP),zinc ions,and protein drugs,for efficient intracellular protein ***-b-PAE(Im)could conjugate proteins via the bridging effect of zinc ions which simultaneously coordinate with imidazole groups on polymer and electron donor groups,such as imidazole and primary amine groups,on protein to improve the loading stability of *** a slightly acidic environment near cancer cells,the protonation of PAE(Im)backbone increases the positive charge density of the nanocomplex and promotes *** under a more acidic environment in endosomes,further protonation of imidazole groups leads to the disintegration of the nanocomplex and the breakdown of endosomes because of the proton sponge ***,protein is released into the *** the assistance of the nanocomplex,proteins with different sizes and isoelectric points are effectively delivered into *** work provides a stable,efficient and universal strategy for intracellular protein delivery.

关键词： protein zinc ions intracellular delivery coordination polymer

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Dynamic covalent nano-networks comprising antibiotics and polyphenols orchestrate bacterial drug resistance reversal and inflammation alleviation

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Bioactive materials 2023年第9期27卷 288-302页

作者： Yuanfeng Li Yin-Zi Piao Hua Chen Keqing Shi Juqin Dai Siran Wang Tieli Zhou Anh-Tuan Le Yaran Wang Fan Wu rujiang ma Linqi Shi Yong Liu Translational Medicine Laboratory The First Affiliated Hospital of Wenzhou Medical UniversityWenzhouZhejiang325035China Wenzhou Institute University of Chinese Academy of SciencesOujiang LaboratoryZhejiang Lab for Regenerative MedicineVision and Brain HealthWenzhouZhejiang325001China Key Laboratory of Functional Polymer materials of Ministry of Education Institute of Polymer ChemistryCollege of ChemistryNankai UniversityTianjin300071China Department of Clinical Laboratory The First Affiliated Hospital of Wenzhou Medical UniversityWenzhouZhejiang325035China Nano Institute Phenikaa UniversityYen NghiaHa DongHa NoiViet Nam

New antimicrobial strategies are urgently needed to meet the challenges posed by the emergence of drug-resistant bacteria and bacterial *** work reports the facile synthesis of antimicrobial dynamic covalent nano-networks(aDCNs)composing antibiotics bearing multiple primary amines,polyphenols,and a cross-linker acylphenylboronic ***,the iminoboronate bond drives the formation of aDCNs,facilitates their stability,and renders them highly responsive to stimuli,such as low pH and high H2O2 ***,the representative A1B1C1 networks,composed of polymyxin B1(A1),2-formylphenylboronic acid(B1),and quercetin(C1),inhibit biofilm formation of drug-resistant Escherichia coli,eliminate the mature biofilms,alleviate macrophage inflammation,and minimize the side effects of free *** bacterial eradication and inflammation amelioration efficiency of A1B1C1 networks are also observed in a peritoneal infection *** facile synthesis,excellent antimicrobial performance,and biocompatibility of these aDCNs potentiate them as a much-needed alternative in current antimicrobial pipelines.

关键词： Biofilms Dynamic covalent bonds On-demand drug release Resistance reversal Biosafety

Synthesis of Fe_3O_4@SiO_2@polymer nanoparticles for controlled drug release

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Science China Chemistry 2010年第3期53卷 514-518页

作者： WU ChengLin,HE Huan,GAO HongJun,LIU Gan,ma rujiang,AN YingLi & SHI LinQi Key Laboratory of Functional Polymer materials,Ministry of Education Institute of Polymer Chemistry,Nankai University,Tianjin 300071,China Key Laboratory of Functional Polymer materials Ministry of Education Institute of Polymer Chemistry Nankai University Tianjin China

Novel multifunctional nanoparticles containing a magnetic Fe3O4@SiO2 sphere and a biocompatible block copolymer poly(ethylene glycol)-b-poly(aspartate)(PEG-b-PAsp) were *** silica coated on the superparamagnetic core was able to achieve a magnetic dispersivity,as well as to protect Fe3O4 against oxidation and acid *** PAsp block was grafted to the surface of Fe3O4@SiO2 nanoparticles by amido bonds,and the PEG block formed the outermost *** anticancer agent doxorubicin(DOX) was loaded into the hybrid nanoparticles via an electrostatic interaction between DOX and *** release rate of DOX could be adjusted by the pH value.

关键词： magnetic nanoparticle Fe3O4@SiO2 multifunctional controlled drug release

苯硼酸酯化驱动的自组装胶束用于蛋白质药物的负载与胞内递送

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离子交换与吸附 2022年第3期38卷 217-230页

作者：陈臻睿张艳丽邓飞马如江高分子化学研究所功能高分子材料教育部重点实验室化学学院南开大学

本文利用2-甲酰基苯硼酸(2-FPBA)修饰蛋白质药物,通过苯硼酸与邻二醇的作用使蛋白质药物与糖基功能化聚合物聚N-异丙基丙烯酰胺-b-聚(天冬氨酸-co-天冬酰胺基葡萄糖)[PNIPAM-b-P(Asp-co-AspAGA)]键合,进一步通过与含苯硼酸聚合物聚乙二... 详细信息

本文利用2-甲酰基苯硼酸(2-FPBA)修饰蛋白质药物,通过苯硼酸与邻二醇的作用使蛋白质药物与糖基功能化聚合物聚N-异丙基丙烯酰胺-b-聚(天冬氨酸-co-天冬酰胺基葡萄糖)[PNIPAM-b-P(Asp-co-AspAGA)]键合,进一步通过与含苯硼酸聚合物聚乙二醇-b-聚(天冬氨酸-co-天冬酰胺基苯硼酸)[PEG-b-P(Asp-co-AspPBA)]的反应,自组装形成了一种具有pH和谷胱甘肽(GSH)响应性的蛋白质药物纳米载体。采用~1H-NMR对嵌段共聚物进行了表征;通过动态光散射(DLS)和透射电子显微镜(TEM)对载药复合胶束的形态结构进行了表征;利用荧光分光光度计研究了载药复合胶束的载药量以及在pH=5和GSH=5g/L条件下的体外释放行为;使用细胞流式术和激光共聚焦显微镜(CLMS)观察了载药复合胶束的胞内递送行为。结果表明,该载药复合胶束呈球形且粒径均一,能够高效负载多种蛋白类药物并在响应性条件下完成对药物的缓慢释放,同时拥有良好的胞内递送能力。

关键词：苯硼酸复合胶束蛋白质药物胞内递送

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强夯加固在湿陷性黄土地基中的效果探讨

资源环境与工程 2008年第6期22卷 588-590页

作者：时红莲马如江中国地质大学(武汉)工程学院湖北武汉430074 新疆电力设计院新能岩土工程中询有限责任公司新疆乌鲁木齐830011

结合大量的试验、勘察数据资料,分析地基土的基本工程性质、存在的工程地质问题,提出采用强夯法对地基土进行处理。根据检测结果,分析比较了处理前、处理后湿陷性黄土的物理力学、湿陷性等特性,证明了强夯处理湿陷性黄土效果显著。

关键词：强夯湿陷性黄土地基承载力

含pH敏感聚(4-乙烯基吡啶)的嵌段共聚物成核胶束化过程的NMR研究

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高分子学报 2008年第7期18卷 691-696页

作者：何振平孙平川熊德安马如江林海史林启功能高分子材料教育部重点实验室南开大学高分子化学研究所天津300071

利用NMR技术研究了聚乙二醇-b-聚(4-乙烯基吡啶)(PEG114-b-P4VP107)和聚(N-异丙烯基丙烯酰胺)-b-聚(4-乙烯基吡啶)(PNIPAM53-b-P4VP260)在逐步降低聚(4-乙烯基吡啶)链段质子化程度时嵌段共聚物的胶束化过程.在开始形成胶束时,吡啶环上... 详细信息

利用NMR技术研究了聚乙二醇-b-聚(4-乙烯基吡啶)(PEG114-b-P4VP107)和聚(N-异丙烯基丙烯酰胺)-b-聚(4-乙烯基吡啶)(PNIPAM53-b-P4VP260)在逐步降低聚(4-乙烯基吡啶)链段质子化程度时嵌段共聚物的胶束化过程.在开始形成胶束时,吡啶环上氢原子的自旋-晶格弛豫时间(T1)急剧减小.结果表明,PEG114-b-P4VP107在质子化程度降为0.54时已有胶束生成;PNIPAM53-b-P4VP260在质子化程度降为0.58时也能观测到胶束生成的信号.将两个嵌段共聚物各自制得胶束的溶液相混合,观测到了发生在高分子链间的2DNOE信号,这表明所制得溶液中胶束与高分子链间有链交换的动态平衡.

关键词：聚(禾乙烯基吡啶) NMR 胶束