星状共轭聚合物的单分子胶束化发光策略及其应用
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摘要
共轭聚合物是主链上含有大离域π键的一类聚合物，其主链是由碳-碳单键、双键或三键连接而成。共轭聚合物通常具有荧光或磷光性质和导电性，是当前化学、材料学等学科交叉的研究前沿。在共轭聚合物里，超支化共轭聚合物是一类具有三维拓扑结构的共轭聚合物。相比于线性共轭聚合物，超支化共轭聚合物在聚集态下具有优越的光学性能。以超支化共轭聚合物为主体引入其他聚合物构建单分子胶束体系，并赋予其两亲性和智能响应性等性能，有助于拓宽其应用，开发新型功能材料。本文在综述前人关于自组装对共轭聚合物光学性质影响的基础上，将聚乙二醇、聚甲基丙烯酸N,N-二甲氨基乙酯引入到超支化共轭聚合物表面，制备了星状共轭共聚物单分子胶束。采用单分子胶束化策略，通过自组装、温度调控和有机/无机杂化等方式构建了不同功能化的共轭纳米粒子，并应用于纳米科学和生物成像等领域。主要研究内容和结论概括如下：
1．自组装控制星状共轭共聚物的光学性质
利用自组装方法成功控制了星状共轭共聚物的光学性质。首先，通过Wittig交叉偶联法，以N-(正己基)-3,6-二醛基咔唑和1,3,5-(三苯基膦基)溴代均三甲苯为单体，合成了超支化共轭聚合物，并进一步通用酰腙键将聚乙二醇接枝到超支化共轭聚合物上，得到了星状共轭聚合物。通过核磁共振(NMR)、红外光谱(FTIR)、凝胶渗透色谱(GPC)等测试手段对超支化共轭聚合物和星状共轭共聚物的结构进行了分析表征。由于具有两亲性，星状共轭聚合物在共溶剂中发生自组装。借助动态光散射(DLS)、透射电镜(TEM)、核磁共振(NMR)和紫外-可见光谱(UV-vis)等测试手段，对组装体的形貌和光学性质进行了观察分析。在酸性环境下，酰腙键的存在改变了聚合物链的共轭长度，从而改变了星状共轭聚合物的光学性能。自组装破坏了酰腙键的质子化能力，从而影响了星状共轭聚合物的光学性质。
2．多胶束聚集自组装增强星状共轭共聚物的荧光性能
研究共溶剂自组装方法对星状共轭共聚物组装体荧光性能的影响。星状共轭共聚物具有三维核-壳结构，在自组装过程中形成单分子胶束的多胶束聚集体。在这种聚集体中，超支化共轭聚合物核被外围聚合物臂所保护，有效防止了浓度自淬灭效应的发生，限制了共轭聚合物核的分子间相互聚集，从而提高了聚合物组装体的荧光性能。动态光散射(DLS)、透射电镜(TEM)和荧光分光光度计(PL)等实验结果表明，星状共轭共聚物的单分子胶束形成了多胶束聚集体。通过调节星状共轭共聚物的结构，可以控制星状共轭共聚物组装体的荧光性能。具有优良荧光性能的星状共轭共聚物组装体可用于细胞成像。
3．星状共轭共聚物荧光监测药物的细胞内释放
以星状共轭共聚物为药物载体，利用其荧光性能监测了药物在肿瘤细胞中的释放过程。首先，采用核磁共振(NMR)、红外光谱(FTIR)、凝胶渗透色谱(GPC)等对星状共轭共聚物进行了结构表征。动态光散射(DLS)和透射电镜(TEM)实验结果表明，星状共轭共聚物在水溶液中自组装成单分子胶束的多胶束聚集体。以MTT方法测定了星状共轭共聚物胶束的细胞毒性，在1mg/mL聚合物浓度下，NIH-3T3细胞在48小时后存活率为80%，表明星状共轭共聚物具有较低的细胞毒性。以阿霉素为模型药物，利用星状共轭共聚物胶束对药物进行负载。体外释放研究表明，药物在酸性环境下的释放要明显快于中性环境，具有pH响应性的星状共轭共聚物更有利于药物的释放。由于π-π堆积和能量共振转移，阿霉素淬灭超支化共轭聚合物的荧光。随着药物的释放，π-π堆积和能量转移减弱，星状共轭共聚物的荧光强度逐渐恢复。利用这种荧光变化，可以实时监测药物阿霉素在细胞内的释放。
4．温度诱导增强星状共轭共聚物的荧光性能及细菌检测
通过温度诱导增强了星状共轭共聚物的荧光性能。首先以超支化共轭聚合物为大分子引发剂，采用原子转移自由基聚合方法在共轭聚合物的表面接枝不同臂长的温度响应性聚甲基丙烯酸-2-(N,N-二甲氨基)乙酯(PDMAEMA)，制备了星状共轭共聚物(HCP-star-PDMAEMA)，并通过核磁共振(NMR)、红外光谱(FTIR)、凝胶渗透色谱(GPC)等测试手段对星状共轭共聚物的结构进行了分析表征。变温紫外-可见光谱(UV-vis)实验结果表明，接枝了PDMAEMA的星状共轭共聚物具有典型的温敏相转变行为。当溶液温度高于PDMAEMA的最低临界共溶温度(LCST)时，星状共轭共聚物中的超支化共轭聚合物核被坍缩的PDMAEMA分子链所包覆，限制了其浓度自淬灭效应，因而增强了星状共轭聚合物的荧光性能。利用温度诱导星状共轭共聚物的荧光增强，成功实现了大肠杆菌的检测。
5．荧光性单分子核壳有机/无机纳米杂化材料的制备和应用
以单分子胶束为模板制备具有优异荧光性能的单分子核壳有机/无机纳米杂化材料，实现其在生物成像中的应用。以超支化共轭聚合物为核、聚甲基丙烯酸-2-(N,N-二甲氨基)乙酯为臂的星状共轭共聚物(HCP-star-PDMAEMA)为模板，合成了单分子核壳有机/无机纳米杂化材料(HCP@SiO_2)，并借助红外光谱(FTIR)、热重分析(TGA)、动态光散射(DLS)、透射电镜(TEM)和能量色散谱(EDS)进行了结构和性能表征。二氧化硅外壳的存在有效限制了共轭聚合物核与核之间的π-π相互作用，使得单分子核壳有机/无机纳米杂化颗粒不仅具有很强的荧光性能，而且还保持着共轭聚合物原有的光学性质。通过MTT方法测定了单分子核壳有机/无机纳米杂化颗粒对NIH-3T3细胞的毒性，当细胞在最大浓度为500μg/mL的纳米粒子溶液中孵育24小时后，细胞的存活率大于90%，说明纳米粒子具有较低的细胞毒性。流式细胞分析和荧光显微镜实验结果表明，具有优良荧光性能的单分子核壳有机/无机纳米杂化颗粒可用作生物成像探针，其表面电荷对纳米粒子的细胞内摄具有很大影响。
Conjugated polymers are the long π-delocalized polymers with carbon-carbon single bond,double bond or triple bond backbone. Conjugated polymers have become a promising fieldin interdisciplinary subject of chemistry and material science, due to their uniqueflorescence/phosphorescence or conductive properties. Among various conjugated polymers,the hyperbranched conjugated polymers have highly branched three-dimensional architecture.Compared with those of linear conjugated polymers, hyperbranched conjugated polymersshow good optical properties under the aggregated state. To construct the unimolecularmicelle system, other functional polymers, such as amphiphility, stimuli-responsibility andso on, have been introduced onto the surface of hyperbranched conjugated polymers toextend the application of conjugate polymers and develop newly functional materials. In thisdissertation, based on the summarization of previous research works about the influence ofself-assembly on the optical properties of conjugated polymers, poly(ethylene glycol) andpoly(2-(dimethylamino) ethyl methacrylate) chain were introduced into hyperbranchedconjugated polymer to form the star conjugated copolymer. With the helpf of unimolecularmicellization strategy, the conjugated nanoparticles with different functionalization wereprepared through self-assembly, temperature variation and organic/inorganic hybridapproaches, which could be used in various applications, like nano-science and bioimaing.The main research contents and results are shown as follows:
1. Self-assembly control of the optical properties of star conjugated copolymer
Self-assembly approach to tune the optical properties of the star conjugated copolymer hasbeen developed. The hyperbranched conjugated polymer (HCP) was synthesized via Wittigcoupling reaction of N-(n-hexyl)-3,6-diformylcarbazole and1,3,5-bis[(p-triphenyl phosphonio) methyl] benzene tribromide. Subsequently, the linear poly(ethylene glycol)arms were grafted onto the HCP by acylhydrazone connection to form the star conjugatedcopolymer (HCP-star-PEG). The structures of HCP and HCP-star-PEG were characterizedby NMR, FTIR and GPC techniques. Due to its amphiphilic structure, HCP-star-PEG couldself-assemble in the co-solvent of chloroform and acetonitrile. The morphologies and opticalproperties of HCP-star-PEG had been characterized by DLS, TEM, NMR and UV-visspectra. Owing to the protonation of imine group (C=N) in acyldydrazone bond in the acidcondition, the conjugation of HCP-star-PEG increased and the optical properties changedfrom pale green to red. Co-solvent self-assembly would affect the protonation of imine groupgreatly, resulting in the control of optical properties of HCP-star-PEG.
2. Emission enhancement of conjugated polymer through self-assembly ofunimolecular micelles to multi-micelle aggregates
The emission of star conjugated copolymer (HCP-star-PEG) was enhanced greatly byco-solvent self-assembly approach. Owing to the three-dimensional architecture ofhyperbranched conjugated polymer, the HCP-star-PEG could form multi-micelle aggregatesfrom unimolecular micelles, which was characterized by DLS and TEM. For themulti-micelle aggregates, the HCP core was well wrapped in the interior of the unimolecularmicelles by PEG arms, resulting in emission enhancement of HCP-star-PEG in the aggregatestate through restriction of concentration self-quenching and intermolecular aggregation ofconjugated polymer core. The length of PEG arm showed great influence on the size andoptical properties of self-assembled HCP-star-PEG. The high emission of HCP-star-PEGmicelles exhibits excellent cellular imaging application.
3. Real-time monitoring of drug release from star conjugated copolymer in tumor cell
Star conjugated copolymer was used as drug carrier to monitor the drug release in tumorcell by fluorescent change. The star conjugated copolymer combined hyperbranchedconjugated polymer core and poly(ethylene glycol) arms with acylhydrazone or ether linkagewas synthesized successfully, named as HCP-star-PEG and HCP-O-PEG, respectively. Thestructures of HCP-star-PEG and HCP-O-PEG were characterized by NMR, FTIR, GPC,TGA, etc. The DLS and TEM results confirmed that star conjugated polymers self-assemblyinto multi-micelle aggregates from unimolecular micelles. The in vitro cytotoxicity ofHCP-star-PEG and HCP-O-PEG micelles was evaluated by MTT assay against NIH-3T3normal cells. The cell viabilities after48h incubation with star conjugated copolymers at concentration of1mg/mL remained above80%, compared to the untreated cells. The resultssuggested that HCP-star-PEG and HCP-O-PEG showed the low cytotoxicity. Doxorubicin(DOX), used as model drug, was encapsulated into star conjugated copolymer micelles. Invitro release studies demonstrated that the release of DOX from micelles was significantlyfaster at mildly acid pH of5.0compared to physiological pH of7.4. Owing to the existenceof acylhydrazone bond, the release of drug from HCP-star-PEG micelles was much fasterthan that from HCP-O-PEG micelles at acid environment. The emission of star conjugatedcopolymer was quenched efficiently by DOX through π-π stacking and fluorescenceresonance energy transfer. After DOX release from polymeric micelles, the fluorescentintensity of HCP-star-PEG or HCP-O-PEG was recovered gradually. The fluorescencechange of star conjugated copolymer demonstrates the drug release in tumor cell.
4. Temperature-induced emission enhancement of star conjugated copolymer withthermo-responsive poly(2-(dimethylamino) ethyl methacrylate) coronas for bacteriadetection
A facile strategy for temperature-induced emission enhancement of star copolymer hasbeen developed. The star polymers (HCP-star-PDMAEMA) with different PDMAEMAchain length were synthesized successfully from the hyperbranched conjugated polymermacroinitiator by atom transfer radical polymerization (ATRP). The structures ofHCP-star-PDMAEMAs were characterized by NMR, FTIR, GPC and TGA. Thevariable-temperature UV-vis measurements confirmed that star conjugated copolymersexhibited classical thermo-responsive phase transitions with adjustable lower critical solutiontemperature (LCST), depending on the pH of copolymer solution. Above the LCST, theemission of HCP-star-PDMAEMA was enhanced greatly through restriction ofintermolecular aggregation of conjugated polymer core. The emission performance ofHCP-star-PDMAEMA could be readily adjusted by changing PDMAEMA length. Thistemperature-dependent emission enhancement of HCP-star-PDMAEMA is a good candidatefor detection of E. coil.
5. Highly fluorescent core-shell hybrid nanoparticles from unimolecular starconjugated polymer for biological tool
Highly fluorescent unimolecular core-shell hybrid nanoparticles (HCP@SiO_2) wereprepared for their application in biological imaging. The nanoparticles were readilyfabricated from the soft template of unimolecular star conjugated polymer (HCP-star-PDMAEMA) under mild condition, which were confirmed by FTIR, TGA, DLSand EDS. With the isolation of hyperbranched conjugated polymer (HCP) core from SiO_2shell, the fluorescent performance of HCP@SiO_2were retained in the aqueous solution. Thecytotoxicity of HCP@SiO_2was evaluated by MTT assay against NIH-3T3normal cells.After24h incubation with HCP@SiO_2at concentration of500μg/mL, the cell viabilitiesremained above90%compared with the untreated cells, suggesting the low cytotoxicity ofHCP@SiO_2. This highly fluorescent HCP@SiO_2could be used as biological imaging. Theflow cytometry and fluorescence microscope measurements demonstrated that the surfacecharge of HCP@SiO_2had profound effect on the cellular uptake of nanoparticles by HeLacells.
1．自组装控制星状共轭共聚物的光学性质
利用自组装方法成功控制了星状共轭共聚物的光学性质。首先，通过Wittig交叉偶联法，以N-(正己基)-3,6-二醛基咔唑和1,3,5-(三苯基膦基)溴代均三甲苯为单体，合成了超支化共轭聚合物，并进一步通用酰腙键将聚乙二醇接枝到超支化共轭聚合物上，得到了星状共轭聚合物。通过核磁共振(NMR)、红外光谱(FTIR)、凝胶渗透色谱(GPC)等测试手段对超支化共轭聚合物和星状共轭共聚物的结构进行了分析表征。由于具有两亲性，星状共轭聚合物在共溶剂中发生自组装。借助动态光散射(DLS)、透射电镜(TEM)、核磁共振(NMR)和紫外-可见光谱(UV-vis)等测试手段，对组装体的形貌和光学性质进行了观察分析。在酸性环境下，酰腙键的存在改变了聚合物链的共轭长度，从而改变了星状共轭聚合物的光学性能。自组装破坏了酰腙键的质子化能力，从而影响了星状共轭聚合物的光学性质。
2．多胶束聚集自组装增强星状共轭共聚物的荧光性能
研究共溶剂自组装方法对星状共轭共聚物组装体荧光性能的影响。星状共轭共聚物具有三维核-壳结构，在自组装过程中形成单分子胶束的多胶束聚集体。在这种聚集体中，超支化共轭聚合物核被外围聚合物臂所保护，有效防止了浓度自淬灭效应的发生，限制了共轭聚合物核的分子间相互聚集，从而提高了聚合物组装体的荧光性能。动态光散射(DLS)、透射电镜(TEM)和荧光分光光度计(PL)等实验结果表明，星状共轭共聚物的单分子胶束形成了多胶束聚集体。通过调节星状共轭共聚物的结构，可以控制星状共轭共聚物组装体的荧光性能。具有优良荧光性能的星状共轭共聚物组装体可用于细胞成像。
3．星状共轭共聚物荧光监测药物的细胞内释放
以星状共轭共聚物为药物载体，利用其荧光性能监测了药物在肿瘤细胞中的释放过程。首先，采用核磁共振(NMR)、红外光谱(FTIR)、凝胶渗透色谱(GPC)等对星状共轭共聚物进行了结构表征。动态光散射(DLS)和透射电镜(TEM)实验结果表明，星状共轭共聚物在水溶液中自组装成单分子胶束的多胶束聚集体。以MTT方法测定了星状共轭共聚物胶束的细胞毒性，在1mg/mL聚合物浓度下，NIH-3T3细胞在48小时后存活率为80%，表明星状共轭共聚物具有较低的细胞毒性。以阿霉素为模型药物，利用星状共轭共聚物胶束对药物进行负载。体外释放研究表明，药物在酸性环境下的释放要明显快于中性环境，具有pH响应性的星状共轭共聚物更有利于药物的释放。由于π-π堆积和能量共振转移，阿霉素淬灭超支化共轭聚合物的荧光。随着药物的释放，π-π堆积和能量转移减弱，星状共轭共聚物的荧光强度逐渐恢复。利用这种荧光变化，可以实时监测药物阿霉素在细胞内的释放。
4．温度诱导增强星状共轭共聚物的荧光性能及细菌检测
通过温度诱导增强了星状共轭共聚物的荧光性能。首先以超支化共轭聚合物为大分子引发剂，采用原子转移自由基聚合方法在共轭聚合物的表面接枝不同臂长的温度响应性聚甲基丙烯酸-2-(N,N-二甲氨基)乙酯(PDMAEMA)，制备了星状共轭共聚物(HCP-star-PDMAEMA)，并通过核磁共振(NMR)、红外光谱(FTIR)、凝胶渗透色谱(GPC)等测试手段对星状共轭共聚物的结构进行了分析表征。变温紫外-可见光谱(UV-vis)实验结果表明，接枝了PDMAEMA的星状共轭共聚物具有典型的温敏相转变行为。当溶液温度高于PDMAEMA的最低临界共溶温度(LCST)时，星状共轭共聚物中的超支化共轭聚合物核被坍缩的PDMAEMA分子链所包覆，限制了其浓度自淬灭效应，因而增强了星状共轭聚合物的荧光性能。利用温度诱导星状共轭共聚物的荧光增强，成功实现了大肠杆菌的检测。
5．荧光性单分子核壳有机/无机纳米杂化材料的制备和应用
以单分子胶束为模板制备具有优异荧光性能的单分子核壳有机/无机纳米杂化材料，实现其在生物成像中的应用。以超支化共轭聚合物为核、聚甲基丙烯酸-2-(N,N-二甲氨基)乙酯为臂的星状共轭共聚物(HCP-star-PDMAEMA)为模板，合成了单分子核壳有机/无机纳米杂化材料(HCP@SiO_2)，并借助红外光谱(FTIR)、热重分析(TGA)、动态光散射(DLS)、透射电镜(TEM)和能量色散谱(EDS)进行了结构和性能表征。二氧化硅外壳的存在有效限制了共轭聚合物核与核之间的π-π相互作用，使得单分子核壳有机/无机纳米杂化颗粒不仅具有很强的荧光性能，而且还保持着共轭聚合物原有的光学性质。通过MTT方法测定了单分子核壳有机/无机纳米杂化颗粒对NIH-3T3细胞的毒性，当细胞在最大浓度为500μg/mL的纳米粒子溶液中孵育24小时后，细胞的存活率大于90%，说明纳米粒子具有较低的细胞毒性。流式细胞分析和荧光显微镜实验结果表明，具有优良荧光性能的单分子核壳有机/无机纳米杂化颗粒可用作生物成像探针，其表面电荷对纳米粒子的细胞内摄具有很大影响。
Conjugated polymers are the long π-delocalized polymers with carbon-carbon single bond,double bond or triple bond backbone. Conjugated polymers have become a promising fieldin interdisciplinary subject of chemistry and material science, due to their uniqueflorescence/phosphorescence or conductive properties. Among various conjugated polymers,the hyperbranched conjugated polymers have highly branched three-dimensional architecture.Compared with those of linear conjugated polymers, hyperbranched conjugated polymersshow good optical properties under the aggregated state. To construct the unimolecularmicelle system, other functional polymers, such as amphiphility, stimuli-responsibility andso on, have been introduced onto the surface of hyperbranched conjugated polymers toextend the application of conjugate polymers and develop newly functional materials. In thisdissertation, based on the summarization of previous research works about the influence ofself-assembly on the optical properties of conjugated polymers, poly(ethylene glycol) andpoly(2-(dimethylamino) ethyl methacrylate) chain were introduced into hyperbranchedconjugated polymer to form the star conjugated copolymer. With the helpf of unimolecularmicellization strategy, the conjugated nanoparticles with different functionalization wereprepared through self-assembly, temperature variation and organic/inorganic hybridapproaches, which could be used in various applications, like nano-science and bioimaing.The main research contents and results are shown as follows:
1. Self-assembly control of the optical properties of star conjugated copolymer
Self-assembly approach to tune the optical properties of the star conjugated copolymer hasbeen developed. The hyperbranched conjugated polymer (HCP) was synthesized via Wittigcoupling reaction of N-(n-hexyl)-3,6-diformylcarbazole and1,3,5-bis[(p-triphenyl phosphonio) methyl] benzene tribromide. Subsequently, the linear poly(ethylene glycol)arms were grafted onto the HCP by acylhydrazone connection to form the star conjugatedcopolymer (HCP-star-PEG). The structures of HCP and HCP-star-PEG were characterizedby NMR, FTIR and GPC techniques. Due to its amphiphilic structure, HCP-star-PEG couldself-assemble in the co-solvent of chloroform and acetonitrile. The morphologies and opticalproperties of HCP-star-PEG had been characterized by DLS, TEM, NMR and UV-visspectra. Owing to the protonation of imine group (C=N) in acyldydrazone bond in the acidcondition, the conjugation of HCP-star-PEG increased and the optical properties changedfrom pale green to red. Co-solvent self-assembly would affect the protonation of imine groupgreatly, resulting in the control of optical properties of HCP-star-PEG.
2. Emission enhancement of conjugated polymer through self-assembly ofunimolecular micelles to multi-micelle aggregates
The emission of star conjugated copolymer (HCP-star-PEG) was enhanced greatly byco-solvent self-assembly approach. Owing to the three-dimensional architecture ofhyperbranched conjugated polymer, the HCP-star-PEG could form multi-micelle aggregatesfrom unimolecular micelles, which was characterized by DLS and TEM. For themulti-micelle aggregates, the HCP core was well wrapped in the interior of the unimolecularmicelles by PEG arms, resulting in emission enhancement of HCP-star-PEG in the aggregatestate through restriction of concentration self-quenching and intermolecular aggregation ofconjugated polymer core. The length of PEG arm showed great influence on the size andoptical properties of self-assembled HCP-star-PEG. The high emission of HCP-star-PEGmicelles exhibits excellent cellular imaging application.
3. Real-time monitoring of drug release from star conjugated copolymer in tumor cell
Star conjugated copolymer was used as drug carrier to monitor the drug release in tumorcell by fluorescent change. The star conjugated copolymer combined hyperbranchedconjugated polymer core and poly(ethylene glycol) arms with acylhydrazone or ether linkagewas synthesized successfully, named as HCP-star-PEG and HCP-O-PEG, respectively. Thestructures of HCP-star-PEG and HCP-O-PEG were characterized by NMR, FTIR, GPC,TGA, etc. The DLS and TEM results confirmed that star conjugated polymers self-assemblyinto multi-micelle aggregates from unimolecular micelles. The in vitro cytotoxicity ofHCP-star-PEG and HCP-O-PEG micelles was evaluated by MTT assay against NIH-3T3normal cells. The cell viabilities after48h incubation with star conjugated copolymers at concentration of1mg/mL remained above80%, compared to the untreated cells. The resultssuggested that HCP-star-PEG and HCP-O-PEG showed the low cytotoxicity. Doxorubicin(DOX), used as model drug, was encapsulated into star conjugated copolymer micelles. Invitro release studies demonstrated that the release of DOX from micelles was significantlyfaster at mildly acid pH of5.0compared to physiological pH of7.4. Owing to the existenceof acylhydrazone bond, the release of drug from HCP-star-PEG micelles was much fasterthan that from HCP-O-PEG micelles at acid environment. The emission of star conjugatedcopolymer was quenched efficiently by DOX through π-π stacking and fluorescenceresonance energy transfer. After DOX release from polymeric micelles, the fluorescentintensity of HCP-star-PEG or HCP-O-PEG was recovered gradually. The fluorescencechange of star conjugated copolymer demonstrates the drug release in tumor cell.
4. Temperature-induced emission enhancement of star conjugated copolymer withthermo-responsive poly(2-(dimethylamino) ethyl methacrylate) coronas for bacteriadetection
A facile strategy for temperature-induced emission enhancement of star copolymer hasbeen developed. The star polymers (HCP-star-PDMAEMA) with different PDMAEMAchain length were synthesized successfully from the hyperbranched conjugated polymermacroinitiator by atom transfer radical polymerization (ATRP). The structures ofHCP-star-PDMAEMAs were characterized by NMR, FTIR, GPC and TGA. Thevariable-temperature UV-vis measurements confirmed that star conjugated copolymersexhibited classical thermo-responsive phase transitions with adjustable lower critical solutiontemperature (LCST), depending on the pH of copolymer solution. Above the LCST, theemission of HCP-star-PDMAEMA was enhanced greatly through restriction ofintermolecular aggregation of conjugated polymer core. The emission performance ofHCP-star-PDMAEMA could be readily adjusted by changing PDMAEMA length. Thistemperature-dependent emission enhancement of HCP-star-PDMAEMA is a good candidatefor detection of E. coil.
5. Highly fluorescent core-shell hybrid nanoparticles from unimolecular starconjugated polymer for biological tool
Highly fluorescent unimolecular core-shell hybrid nanoparticles (HCP@SiO_2) wereprepared for their application in biological imaging. The nanoparticles were readilyfabricated from the soft template of unimolecular star conjugated polymer (HCP-star-PDMAEMA) under mild condition, which were confirmed by FTIR, TGA, DLSand EDS. With the isolation of hyperbranched conjugated polymer (HCP) core from SiO_2shell, the fluorescent performance of HCP@SiO_2were retained in the aqueous solution. Thecytotoxicity of HCP@SiO_2was evaluated by MTT assay against NIH-3T3normal cells.After24h incubation with HCP@SiO_2at concentration of500μg/mL, the cell viabilitiesremained above90%compared with the untreated cells, suggesting the low cytotoxicity ofHCP@SiO_2. This highly fluorescent HCP@SiO_2could be used as biological imaging. Theflow cytometry and fluorescence microscope measurements demonstrated that the surfacecharge of HCP@SiO_2had profound effect on the cellular uptake of nanoparticles by HeLacells.
引文
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