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Nano-Micro Letters 2022年第2期14卷 190-205页

作者： Xuelin Xia Xiaoyuan yang Wei Huang Xiaoxia Xia deyue yan School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesShanghai Jiao Tong UniversityShanghai 200240People’s Republic of China State Key Laboratory of Microbial Metabolism School of Life Sciences and BiotechnologyShanghai Jiao Tong UniversityShanghai 200240People’s Republic of China

Affibody molecules are small nonimmunoglobulin affinity proteins,which can precisely target to some cancer cells with specific overexpressed molecular signatures.However,the relatively short in vivo half-life of them seriously limited their application in drug targeted delivery for cancer therapy.Here an amphiphilic affibody-drug conjugate is self-assembled into nanomicelles to prolong circulation time for targeted cancer therapy.As an example of the concept,the nanoagent was prepared through molecular self-assembly of the amphiphilic conjugate of Z_(HHR2:342)-Cys with auristatin E derivate,where the affibody used is capable of binding to the human epidermal growth factor receptor 2(HER2).Such a nanodrug not only increased the blood circulation time,but also enhanced the tumor targeting capacity(abundant affibody arms on the nanoagent surface) and the drug accumulation in tumor.As a result,this affibody-based nanoagent showed excellent antitumor activity in vivo to HER2-positive ovary and breast tumor models,which nearly eradicated both small solid tumors(about 100 mm^(3)) and large established tumors(exceed 500 mm^(3)).The relative tumor proliferation inhibition ratio reaches 99.8% for both models.

关键词： Molecular self-assembly Affibody-drug conjugate Nanoagent Targeted cancer therapy

Highly efficient tumor-targeted nanomedicine assembled from affibody-drug conjugate for colorectal cancer therapy

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Nano Research 2023年第4期16卷 5256-5264页

作者： Xiaoyuan yang Xuelin Xia Wei Huang Xiaoxia Xia deyue yan School of Chemistry and Chemical Engineering Shanghai Jiao Tong UniversityShanghai 200240China State Key Laboratory of Microbial Metabolism School of Life Sciences and BiotechnologyShanghai Jiao Tong UniversityShanghai 200240China

Affibody is a new class of small non-immunoglobulin affinity proteins that possesses high affinity at the picomole level to several tumor overexpressed receptors.Owing to the simple framework,affibody is flexible for modification with payload,but the relatively low molecular weight of this construction simultaneously results in short half-life time which hinders its application in cancer therapy.In this work,we prepared a nanomedicine self-assembled from the conjugate of affibody(ZPDGFRβ:09591,PDGFRβ:platelet-derived growth factor receptorβ)with monomethyl auristatin E(MMAE)through cathepsin B cleavable dipeptide linker for targeted colorectal cancer therapy.The nanoscale characteristics of ZPDGFRβ:09591-MMAE affibody-drug conjugate nanomedicine(ZPDGFRβ:09591-M ADCN)resulted in enhanced pharmacokinetics,improved drug accumulation,and promoted biosecurity performance than those of free drugs.As a result,ZPDGFRβ:09591-M ADCN exhibited excellent antitumor efficacy with tumor inhibition rates(TIR)over 99.0%in PDGFRβ-positive tumor models with small solid tumors(~150 mm^(3))or large established tumors(~500 mm^(3)),indicating that ZPDGFRβ:09591-MMAE ADCN is promising for the clinic application in colorectal cancer therapy.

关键词： olecular self-assembly ZPDGFRβ:09591 affibody monomethyl auristatin E(MMAE) nanodrug targeted delivery

ROS-responsive thioether-containing hyperbranchede polymer micelles for light-triggered drug releas

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SmartMat 2022年第3期3卷 522-531页

作者： Guanchun Wang Ping Huang Lei Wang Xinliang Chen Yongfeng Zhou Wei Huang deyue yan School of Chemistry and Chemical Engineering Shanghai Jiao Tong UniversityShanghaiChina The International Peace Maternity and Child Health Hospital School of MedicineShanghai Jiao Tong UniversityShanghaiChina

As a kind of promising drug carriers,smart polymers have attracted much attention due to the effective and controlled drug release in target cells.Herein,a reactive oxygen species(ROS)-responsive thioether-containing amphiphilic hyperbranched polymer prepared from MTPA and TMPTGE(HBPMT)is synthesized from 3-(methylthio)propylamine(MTPA)and trimethylolpropane triglycidyl ether(TMPTGE)by the amine-epoxy click reaction via A2+B3 onepot approach.Benefiting from its inherent amphiphilic nature,HBPMT can selfassemble into stable micelles in water.Triggered by H_(2)O_(2),these micelles can be dissociated rapidly because hydrophobic thioether segments in their cores are oxidized into hydrophilic sulfoxide or sulfone groups.Additionally,the ROS produced by photosensitizer under light irradiation can also play the same role of H_(2)O_(2).Such HBPMT micelles can be utilized to encapsulate anticancer drug paclitaxel(PTX)and photosensitizer chlorin e6(Ce6)simultaneously for drug delivery and control release.The methyl thiazolyl tetrazolium assay toward MCF-7 tumor cells(a human breast adenocarcinoma cell line)indicates that these micelles encapsulated with PTX and Ce6 exhibit a significant combinational efficacy of cell proliferation inhibition,which means the promising potential for synergistic chemo-photodynamic cancer therapy.Such a novel nanocarrier based on amphiphilic to hydrophilic transition would provide a candidate for controlled drug release and cancer combination therapy.

关键词： drug delivery hyperbranched polymer photosensitizer ROS-responsiveness triggered drug release

H_(2)O_(2)-responsive polymer prodrug nanoparticles with glutathione scavenger for enhanced chemo-photodynamic synergistic cancer therapy

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Bioactive Materials 2023年第7期25卷 189-200页

作者： Guanchun Wang Yue Su Xinliang Chen Yongfeng Zhou Ping Huang Wei Huang deyue yan School of Chemistry and Chemical Engineering Shanghai Jiao Tong UniversityShanghai200240China The International Peace Maternity and Child Health Hospital School of MedicineShanghai Jiao Tong UniversityShanghaiChina

The combination of chemotherapy and photodynamic therapy(PDT)based on nanoparticles(NPs)has been extensively developed to improve the therapeutic effect and decrease the systemic toxicity of current treatments.However,overexpressed glutathione(GSH)in tumor cells efficiently scavenges singlet oxygens(^(1)O_(2))generated from photosensitizers and results in the unsatisfactory efficacy of PDT.To address this obstacle,here we design H_(2)O_(2)-responsive polymer prodrug NPs with GSH-scavenger(Ce6@P(EG-a-CPBE)NPs)for chemo-photodynamic synergistic cancer therapy.They are constructed by the co-self-assembly of photosensitizer chlorin e6(Ce6)and amphiphilic polymer prodrug P(EG-a-CPBE),which is synthesized from a hydrophilic alternating copolymer P(EG-a-PD)by conjugating hydrophobic anticancer drug chlorambucil(CB)via an H_(2)O_(2)-cleavable linker 4-(hydroxymethyl)phenylboronic acid(PBA).Ce6@P(EG-a-CPBE)NPs can efficiently prevent premature drug leakage in blood circulation because of the high stability of the PBA linker under the physiological environment and facilitate the delivery of Ce6 and CB to the tumor site after intravenous injection.Upon internalization of Ce6@P(EG-a-CPBE)NPs by tumor cells,PBA is cleaved rapidly triggered by endogenous H_(2)O_(2)to release CB and Ce6.Ce6 can effectively generate abundant^(1)O_(2)under 660 nm light irradiation to synergistically kill cancer cells with CB.Concurrently,PBA can be transformed into a GSH-scavenger(quinine methide,QM)under intracellular H_(2)O_(2)and prevent the depletion of^(1)O_(2),which induces the cooperatively strong oxidative stress and enhanced cancer cell apoptosis.Collectively,such H_(2)O_(2)-responsive polymer prodrug NPs loaded with photosensitizer provide a feasible approach to enhance chemo-photodynamic synergistic cancer treatment.

关键词： H_(2)O_(2)-responsiveness Alternating copolymer prodrug GSH-scavenger Photosensitizer Chemo-photodynamic synergistic cancer therapy

Intrinsic viscosity of polymer solutions: fresh ideas to an old problem

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Science China Chemistry 2015年第5期58卷 835-838页

作者： deyue yan State Key Laboratory of Metal Matrix Composites School of Chemistry and Chemical Engineering Shanghai Jiao Tong University

Intrinsic viscosity is one of the most fundamental properties of dilute polymer solutions; its study forms an integral part of the cornerstone of the modern macromolecular theory. However, a general theory applicable to any chain architectures and solvent conditions has remained elusive, due to the formidable challenges in the theoretical treatment of the long-range, many-body and accumulative hydrodynamic effects. Recently, Lijia An and coworkers at the Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, has developed a new approach that largely overcomes these challenges. Their new theory provides a simple and unified theoretical framework for describing the intrinsic viscosity of polymers with arbitrary architectures under any solvent conditions and forms the theoretical basis for inferring the polymer chain structure from intrinsic viscosity measurements. Comparisons with existing experimental data yield extensive, quantitative agreement.

关键词：聚合物溶液特性粘度新鲜组成部分分子理论动力效应应用化学粘度测量

Supramolecular nanoscale drug-delivery system with ordered structure

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National Science Review 2019年第6期6卷 1128-1137页

作者： Xin Jin Lijuan Zhu Bai Xue Xinyuan Zhu deyue yan School of Chemistry and Chemical Engineering State Key Laboratory of Metal Matrix Composites Shanghai Jiao Tong University

Supramolecular chemistry provides a means to integrate multi-type molecules leading to a dynamic organization. The study of functional nanoscale drug-delivery systems based on supramolecular interactions is a recent trend. Much work has focused on the design of supramolecular building blocks and the engineering of supramolecular integration, with the goal of optimized delivery behavior and enhanced therapeutic effect. This review introduces recent advances in supramolecular designs of nanoscale drug delivery. Supramolecular affinity can act as a main driving force either in the self-assembly of carriers or in the loading of drugs. It is also possible to employ strong recognitions to achieve self-delivery of drugs. Due to dynamic controllable drug-release properties, the supramolecular nanoscale drug-delivery system provides a promising platform for precision medicine.

关键词： supramolecular chemistry drug-delivery system host–guest recognition self-delivery system precision medicine

Synthesis and characterization of amphiphilc block copolymer poly(methyl acrylic acid)-block-polytetrahydrofuran

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Chinese Science Bulletin 2000年第21期45卷 1948-1953页

作者： Guojian Wang deyue yan College of Chemistry and Chemical Technology Shanghai Jiao Tong University Shanghai China

Under the specially designated condition the polymerization of both tetrahydrofuran (THF) and tert-butyl methacrylate (tBMA) is a living one. The diblock copolymer, poly(tert-butyl methacrylate)-block-polytetrahydrofuran (PtBMA-b-PTHF), was successfully synthesized by meansof the coupling reaction of living cationic PTHF+, SbF6 with living anionic PtBMA-, Li+. LiCI, whichhas a beneficial effect on the molecular weight distribution (MWD) in the anionic polymerization of (meth)acrylates, hinders the coupling reaction of living chains and cannot be used in the preparation of tBMA precursor. The hydrolysis of the aforementioned diblock copolymer under acid condition results in the amphiphilic diblock copolymer, i.e. poly(methyl acrylic acid)-block-polytetra-hydrofuran (PMAA-b-PTHF). The diblock copolymers were characterized with GPC and IR.

关键词： amphiphilic diblock copolymer coupling reaction living polymerization tert-butyl methacrylate methyl acrylic acid tetrahydrofuran.

Preparation of fluorescent hyperbranched polymer materials by end-capping approach

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Chinese Science Bulletin 2000年第19期45卷 1760-1764页

作者： Chao Gao deyue yan Shanghai Jiao Tong Univ Coll Chem & Chem Technol Shanghai 200240 Peoples R China

Two kinds of novel fluorescent hyperbranched polymers were synthesized by the end-capping approach. The fluorescent hyperbranched polyether (FPEOTM) was obtained by end capping the hyperbranched poly(hydroxyl ether) (PEOTM) with guest molecules N,N-dimethylaminobenzaldehyde (DMABA). In addition, in the presence of triethylamine, the hyperbranched polysulfone-amine with terminal double bonds (HPSA) was synthesized by polyaddition of a new AB2 type monomer (SAP, sulfone amine piperazine) at 40℃ for 60 h in chloroform solution. Then the fluorescent hyperbranched polysulfone-amine (FHPSA) was prepared by addition of guest molecules N,N-dimethylaminoanilines (DMAA) with the terminal double bonds of HPSA. The two resulting polymers fluoresce yellow-green color in both solid and solution states. The maximum emission wavelength is (460 ±10) nm and (470±10) nm, respectively. A novel 'complex quenching effect' for hyperbranched polymer was observed. The fluorescence can be quenched by transition metal

关键词： end-capping approach fluorescence material hyperbranched polymer functionalization.

Computer simulation studies of the influence of side alkyl chain on glass transition behavior of carbazole trimer

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Science China Chemistry 2017年第3期60卷 377-384页

作者： Chunyang Yu Li Ma Wei Huang Yongfeng Zhou Jingui Qin deyue yan State Key Laboratory of Metal Matrix Composites School of Chemistry & Chemical EngineeringShanghai Jiao Tong University Department of Chemistry Wuhan University

In this work,all-atom molecular dynamics simulations were employed to study the influence of the side alkyl chain on glass transition behavior of several carbazole trimers(CT) in a temperature range from 423 to 183 K.The glass transition temperatures were obtained from the break in the slope of the volume-temperature curves and found to agree with the experimental values.The short time dynamics of four CT molecules were probed by usingvelocity autocorrelation functions and mean-square displacements.The current studies showed that the dynamics of CT systems can be easily interpreted through the cage effect.Furthermore,the investigation of the torsional autocorrelation function and P_(2-state)/P_(3-state) functions showed that the rotational barriers of side chains can slow down the conformational relaxation and lead to stronger temperature dependence of conformational relaxation.The relaxation time,characteristic time of P_(2-state)(t) and P_(3-state)(t) functions were all found to have Arrhenius-type temperature dependence.

关键词： carbazole trimer molecular dynamics simulation glass transition relaxation time

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橡胶混凝土与变形钢筋黏结性能试验研究

建筑科学与工程学报 2024年第1期41卷 171-180页

作者：颜岩章德越马从伟王迎斌白应华湖北工业大学土木建筑与环境学院湖北武汉430068 西藏交通勘察设计研究院有限公司西藏拉萨850000

共设计制作9组试件,对钢筋内贴应变片的试件进行拉拔试验,系统研究了橡胶体积取代率、钢筋直径、锚固长度对变形钢筋与橡胶混凝土黏结性能的影响。观察了试件破坏形态并通过计算得出试件极限黏结应力和滑移量,得到了不同因素下黏结应力... 详细信息

共设计制作9组试件,对钢筋内贴应变片的试件进行拉拔试验,系统研究了橡胶体积取代率、钢筋直径、锚固长度对变形钢筋与橡胶混凝土黏结性能的影响。观察了试件破坏形态并通过计算得出试件极限黏结应力和滑移量,得到了不同因素下黏结应力、相对滑移分布规律以及不同锚固位置处的黏结应力-滑移曲线。建立了考虑橡胶体积取代率下变形钢筋与橡胶混凝土黏结应力-滑移本构关系模型;通过对相同滑移值下不同位置(距自由端距离)处黏结应力的量纲一化处理,得到了不同橡胶体积取代率下的变形钢筋与橡胶混凝土的黏结位置函数。结果表明:橡胶体积取代率增加,极限黏结应力减小,对应加载端滑移量先增加后减少;钢筋直径、锚固长度增大均会导致极限黏结应力减小,对应加载端滑移量减少;对比各位置处黏结应力-滑移曲线发现,橡胶体积取代率增加、钢筋直径及锚固长度增大均会加剧黏结应力的不均匀分布;相对滑移量会随着橡胶体积取代率增加而增加,随着钢筋直径、锚固长度的增大而减少。

关键词：变形钢筋橡胶混凝土黏结性能黏结应力-滑移本构关系位置函数