两亲性超支化超分子嵌段共聚物的制备及自组装行为研究
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摘要
超分子化学（Supramolecular Chemistry）是二十世纪八九十年代逐渐形成的一门新兴学科，主要研究不同化学物种间通过分子间的相互作用力（即非共价键相互作用）而形成的具有特定结构和功能的超分子聚集体系，属多学科交叉形成的新兴研究领域，主要涵盖化学、材料及生命科学等热点研究领域。超分子聚合物（Supramolecular Polymer）是超分子化学在高分子领域中的一个分支。超支化聚合物（Hyperbranched Polymer）隶属于树形聚合物，是一类具有三维准球形立体构造的高度支化聚合物，从分子构型上看，在分子外围和内部存在大量末端官能团易于功能化，同时准球形分子内部还存在很多空穴，易于包覆尺寸和极性匹配的客体分子形成复合物。这些独特的分子结构特点使得它逐渐成为高分子科学研究中的一个热点方向。本文在综述前人有关超分子聚合物和超支化多臂共聚物自组装等工作的基础上，将超分子作用引入到基于超支化嵌段共聚物的构筑上，设计合成了多种具有不同初始单元（Focal Point）的单反应性超支化聚合物，利用初始单元之间的主客体包结络合作用将疏水的超支化聚合物与亲水的超支化聚合物或线形聚合物进行主客体复合组装，得到了具有超支化-超支化和线形-超支化结构的两亲性超支化超分子嵌段共聚物，并且研究了所合成超分子聚合物的自组装及解组装行为。此外，还设计合成了共价键合的两亲性超支化-超支化和线形-超支化嵌段共聚物，研究了其在选择性溶剂中的自组装行为。主要研究内容和结论概括如下：
1．光响应性Janus型两亲性超支化-超支化超分子嵌段共聚物的制备与自组装行为研究；
采用阳离子开环和氧阴离子开环聚合的方法，合成了具有偶氮苯Focal Point的疏水超支化聚醚（AZO-g-HBPO）和具有环糊精Focal Point的亲水性的超支化聚醚（β-CD-g-HPG）。通过在共溶剂中缓慢滴加选择性溶剂的方法诱导环糊精-偶氮苯主客体识别，实现了AZO-g-HBPO和β-CD-g-HPG的超分子复合，制备了Janus型两亲性超支化-超支化超分子嵌段共聚物。最后将共溶剂透析除去得到超分子嵌段共聚物的组装体。采用DLS、2D NOESY谱跟踪Janus超分子共聚物的形成过程，证明通过偶氮苯-环糊精的包结络合作用形成超分子聚合物。通过SEM、TEM、AFM以及Cryo-TEM等表征手段证明所得组装体均为囊泡结构，囊泡的壁厚约为9.6±0.6nm，恰好与两个Janus超支化超分子聚合物的尺寸之和一致，由此可以推断囊泡膜结构为双分子层。最后，通过加入竞争主客体分子、加热以及紫外光照射的方法对超分子囊泡的稳定性和解组装行为进行探讨。结果表明所制备的聚合物囊泡对竞争主客体分子和温度稳定，但在紫外光照射下可以发生解组装。此外，还采用耗散粒子动力学（Dissipative Particle Dynamics，PDP）方法对超分子聚合物的自组装行为进行理论模拟，模拟结果与实验结果吻合。
2.电化学响应的两亲性超支化超分子嵌段共聚物的制备与自组装行为研究；
采用阳离子开环聚合的方法，合成了具有二茂铁Focal Point的疏水超支化聚醚（Fc-g-HBPO）。通过β-环糊精6-位单取代的化学修饰的方法合成了以β-环糊精为末端官能团的甲氧基聚氧乙烯（β-CD-g-PEO）。结合前面合成的以环糊精为Focal Point的超支化聚醚（β-CD-g-HPG），通过Fc-g-HBPO和β-CD-g-HPG，及Fc-g-HBPO和β-CD-g-PEO之间的环糊精-二茂铁的主客体识别，得到两亲性超支化-超支化和线性-超支化两种超分子嵌段共聚物。采用DLS、2D NOESY谱跟踪了超分子共聚物的形成过程。通过SEM、TEM等直观的形貌表征手段证明所得组装体为囊泡结构。最后，通过加入竞争主客体分子以及化学和电化学氧化还原方法对超分子囊泡的稳定性和解组装行为进行探讨。结果表明所得的聚合物囊泡对竞争主客体分子稳定，在电化学氧化后也能保持稳定，但在电化学氧化后加入电解质超分子组装瞬间发生解组装。
3.光响应性两亲性线性-超支化超分子嵌段共聚物的制备与光控的自组装形貌转变研究；
采用阳离子开环聚合结合click反应，以丙炔醇和6-位单取代β-CD-N_3为原料合成了具有β-环糊精Focal Point的疏水超支化聚醚（β-CD-g-HBPO）。以4-偶氮苯甲酸和甲氧基聚乙二醇为原料，制备了偶氮苯为末端官能团的甲氧基聚氧乙烯（AZO-g-PEO）。TEM和SEM表征表明β-CD-g-HBPO和AZO-g-PEO可以分别在水中自组装形成片层和纤维结构。通过β-CD-g-HBPO和AZO-g-PEO在共溶剂中缓慢滴加选择性溶剂的方法实现环糊精-偶氮苯主客体识别，得到两亲性线性-超支化超分子嵌段共聚物，最后将共溶剂透析除去得到超分子嵌段共聚物的组装体。采用DLS跟踪了超分子共聚物的形成过程。通过SEM、TEM等表征手段证明所得组装体为囊泡结构。最后，对超分子聚合物的组装和解组装行为进行了研究，结果表明在紫外光和可见光的作用下，超分子聚合物可以发生可逆的形貌转变。
4.共价键合的两亲性超支化嵌段共聚物的合成及自组装行为研究；
采用阳离子开环和氧阴离子开环聚合的方法，分别以丙炔醇和3-叠氮基丙醇为引发剂，采用缓慢滴加的方法合成了具有炔基和叠氮Focal Point的超支化聚醚（YNE-g-HBPO和N_3-g-HPG）。通过YNE-g-HBPO和N_3-g-HPG的点击化学反应得到共价键合的Janus型超支化-超支化嵌段共聚物（HBPO-b-HPG）。采用DLS，TEM、SEM等表征方法，详细研究了HBPO-b-HPG在不同的选择性溶剂中的自组装行为。结果表明，HBPO-b-HPG在水和四氢呋喃中均组装成囊泡结构。此外，采用阳离子开环聚合的方法，以甲氧基聚乙二醇和聚乙二醇为引发剂制备了线性-超支化两亲性分子（HBPO-b-PEO和HBPO-b-PEO-b-HBPO）。以同样的方法研究了HBPO-b-PEO和HBPO-b-PEO-b-HBPO这两种共聚物在水中的自组装行为。
Supramolecular chemistry is the chemistry of the intermolecular bond, covering thestructures and functions of the entities formed by association of two or more chemicalspecies. The intermolecular bond includes hydrogen bonding, metal coordination,hydrophobic forces, van der Waals forces, π-π interactions and electrostatic effects.Supramolecular chemistry has become a exciting and promising research field ininterdisciplinary subject of physics, chemistry, biology, materials science, as well as lifescience. Supramolecular polymer is an important branch of supramolecular chemistry inthe field of polymer chemistry. Hyperbranched polymer is also an important branch ofdendritic polymers which has a large amount of terminal functional groups and manyinner cavities. In this dissertation, based on the review and summarization of previousoutstanding research works of supramolecular polymer and self-assembly ofhyperbranched multiarm copolymers, supramolecular host-guest interaction was used toconstruct hyperbranched block polymer. Hyperbranched polymers with multiple kinds ofmono-reactive focal point were synthesized, the host-guest complexation between focalpoints was utilized to couple the hydrophobic hyperbranched polymer with hydrophilichyperbranched or linear polymer, and then the amphiphilic hyperbranched supramolecularpseudo block copolymers were obtained. Subsequently, the self-assembly and disassemblybehaviors of them were investigated. In addition, the hyperbranched-hyperbranched andlinear-hyperbranched copolymers based on covalent bond were synthesized, theself-assembly behaviors in selected solvent of them were investigated. The main resultsare shown as follows.
1. Synthesis and its photo-responsive self-assembly behavior of Janus amphiphilichyperbranched-hyperbranched supramolecular pseudo block copolymer.
Hydrophobic hyperbranched poly3-ethyl-3-oxetanemethanol with azobenzene asfocal point (AZO-g-HBPO) and hydrophilic hyperbranched polyglycidol withcyclodextrin as core (β-CD-g-HPG) were synthesized according to the cationicring-opening polymerization and oxyanionic ring-opening multibranching polymerization,respectively. The recognization of cyclodextrin and azobenzene was achieved by addingselected solvent to common solvent, and then, Janus amphiphilic hyperbranched-hyperbranched supramolecular pseudo block copolymer was obtained. After dialysisagainst water, the self-assembly of supramolecular polymer completed. DLS and2DNOESY were used to track the formation and self-assembly process of Janussupramolecular copolymer, the results demonstrated the complexation of cyclodextrin andazobenzene. TEM, SEM, Cryo-TEM and AFM were used to directly detect themorphology of the self-assembly objects. The results indicated that the supramolecularcopolymer self-assembled into vesicle with narrow size distribution in water, the thicknessof the vesicle wall was about9.6±0.6nm which is equal with double length of Janussupramolecular copolymer. The vesicles may possess a bilayer structure with twohydrophilic HPG shell layers and one hydrophobic HBPO core layer. Adding competitivehost or guest moleculars with a stronger complexation capacity and irradiation with UVlight with365nm were used to investigate the stability and the disassembly behaviour ofsupramolecular vesicle. The results show that the supramolecular viescle was stable withcompetitive host or guest moleculars and heating, disassembled with irradiation of UVlight with365nm. In addition, the details of the self-assembly process as well as thevesicle structure have been disclosed by a dissipative particle dynamics (DPD) simulation.
2. Synthesis and its electrochemical-responsive self-assembly behavior of Janusamphiphilic hyperbranched supramolecular pseudo block copolymers
Hydrophobic hyperbranched poly3-ethyl-3-oxetanemethanol with ferrocene as focalpoint (Fc-g-HBPO) was synthesized according to the cationic ring-opening polymerization.Hydrophilic end-capped polyethylene oxide with β-cyclodextrin (β-CD-g-PEO) wassynthesized according to the mono-6-deoxy substitution of β-cyclodextrin. Combined withβ-CD-g-HPG in the first part, Janus amphiphilic hyperbranched-hyperbranched andlinear-hyperbranched supramolecular pseudo block copolymers were obtained by recognization between cyclodextrin and ferrocene. After dialysis against water, theself-assembly of supramolecular polymers completed. DLS and2D NOESY were used totrack the formation and self-assembly process of supramolecular copolymers, the resultsdemonstrated the complexation of cyclodextrin and ferrocene. TEM and SEM were usedto directly detect the morphology of the self-assembly objects. The results indicated thatthe supramolecular copolymers self-assembled into vesicle in water. Adding competitivehost or guest moleculars with a stronger complexation capacity, chemical andelectrochemical oxidation were used to investigate the stability and the disassemblybehaviour of supramolecular vesicles. The results show that the supramolecular vesicleswere stable with competitive host or guest moleculars, chemical and electrochemicaloxidation. The supramolecular vesicles disassembled after adding electrolyte to thesupramolecular system after electrochemical oxidation.
3. Synthesis of Janus amphiphilic linear-hyperbranched supramolecular pseudo blockcopolymer and its photo controlled self-assembly and morphology transformation fromvesicles to lamellar structure and fibers.
Hydrophobic hyperbranched poly3-ethyl-3-oxetanemethanol with yne group as focalpoint (YNE-g-HBPO) was synthesized according to the cationic ring-openingpolymerization. Janus type amphiphilic hyperbranched polymer (β-CD-g-HBPO) wasobtained after click reaction between YNE-g-HBPO and mono-6-deoxy-6-azide-β-cyclodextrin. Polyethylene oxide end-capped with azobenzene (AZO-g-PEO) wassynthesized using4-(Phenylazo)benzoic acid and methoxypolyethylene glycol as rawmaterials. Interestingly, the amphiphilic β-CD-g-HBPO and AZO-g-PEO self-assembledto lamellar structure and fiber respectively. The amphiphilic linear-hyperbranchedsupramolecular pseudo block copolymer was obtained by recognization of cyclodextrinand azobenzene. After dialysis against water, the self-assembly of supramolecularpolymers completed. DLS and2D NOESY were used to track the formation andself-assembly process of Janus supramolecular copolymer, the results demonstrated thecomplexation of cyclodextrin and azobenzene. TEM, SEM were used to directly detect themorphology of the self-assembly objects. The results indicated that the supramolecularcopolymer self-assembled into vesicle in water. UV light with365nm was used toinvestigate the stability and the disassembly behaviour of supramolecular vesicles. Theresults show that the supramolecular vesicles disassembled into lamellar structure and fibers. They could reversibly assemble into vesicle under the irriadiation of visible light.
4. Synthesis and self-assembly of amphiphilic hyperbranched-hyperbranched andlinear-hyperbranched copolymers based on covalent bond;
Hydrophilic hyperbranched polyglycidol with azide group as focal point (N_3-g-HPG)was synthesized according to the oxyaionic ring-opening polymerization using3-azidopropan-1-ol as initiator. Janus amphiphilic hyperbranched-hyperbranched blockcopolymer (HBPO-b-HPG) was obtained after click reaction between N_3-g-HPG andYNE-g-HBPO mentioned in the former part. DLS, SEM and TEM were used toinvestigate the self-assembly of HBPO-g-HPG in selected solvent. The resultsdemonstrated that Janus amphiphilic block copolymer self-assembled into vesicles ingboth water and THF. In addition, Janus amphiphilic linear-hyperbranched blockcopolymer (HBPO-b-PEO and HBPO-b-PEO-b-HBPO) were synthesized usingmethoxypolyethylene glycol and polyethylene glycol as initiator through cationicring-opening polymerization. The self-assembly behaviours of them were also discussed atthe same time.
1．光响应性Janus型两亲性超支化-超支化超分子嵌段共聚物的制备与自组装行为研究；
采用阳离子开环和氧阴离子开环聚合的方法，合成了具有偶氮苯Focal Point的疏水超支化聚醚（AZO-g-HBPO）和具有环糊精Focal Point的亲水性的超支化聚醚（β-CD-g-HPG）。通过在共溶剂中缓慢滴加选择性溶剂的方法诱导环糊精-偶氮苯主客体识别，实现了AZO-g-HBPO和β-CD-g-HPG的超分子复合，制备了Janus型两亲性超支化-超支化超分子嵌段共聚物。最后将共溶剂透析除去得到超分子嵌段共聚物的组装体。采用DLS、2D NOESY谱跟踪Janus超分子共聚物的形成过程，证明通过偶氮苯-环糊精的包结络合作用形成超分子聚合物。通过SEM、TEM、AFM以及Cryo-TEM等表征手段证明所得组装体均为囊泡结构，囊泡的壁厚约为9.6±0.6nm，恰好与两个Janus超支化超分子聚合物的尺寸之和一致，由此可以推断囊泡膜结构为双分子层。最后，通过加入竞争主客体分子、加热以及紫外光照射的方法对超分子囊泡的稳定性和解组装行为进行探讨。结果表明所制备的聚合物囊泡对竞争主客体分子和温度稳定，但在紫外光照射下可以发生解组装。此外，还采用耗散粒子动力学（Dissipative Particle Dynamics，PDP）方法对超分子聚合物的自组装行为进行理论模拟，模拟结果与实验结果吻合。
2.电化学响应的两亲性超支化超分子嵌段共聚物的制备与自组装行为研究；
采用阳离子开环聚合的方法，合成了具有二茂铁Focal Point的疏水超支化聚醚（Fc-g-HBPO）。通过β-环糊精6-位单取代的化学修饰的方法合成了以β-环糊精为末端官能团的甲氧基聚氧乙烯（β-CD-g-PEO）。结合前面合成的以环糊精为Focal Point的超支化聚醚（β-CD-g-HPG），通过Fc-g-HBPO和β-CD-g-HPG，及Fc-g-HBPO和β-CD-g-PEO之间的环糊精-二茂铁的主客体识别，得到两亲性超支化-超支化和线性-超支化两种超分子嵌段共聚物。采用DLS、2D NOESY谱跟踪了超分子共聚物的形成过程。通过SEM、TEM等直观的形貌表征手段证明所得组装体为囊泡结构。最后，通过加入竞争主客体分子以及化学和电化学氧化还原方法对超分子囊泡的稳定性和解组装行为进行探讨。结果表明所得的聚合物囊泡对竞争主客体分子稳定，在电化学氧化后也能保持稳定，但在电化学氧化后加入电解质超分子组装瞬间发生解组装。
3.光响应性两亲性线性-超支化超分子嵌段共聚物的制备与光控的自组装形貌转变研究；
采用阳离子开环聚合结合click反应，以丙炔醇和6-位单取代β-CD-N_3为原料合成了具有β-环糊精Focal Point的疏水超支化聚醚（β-CD-g-HBPO）。以4-偶氮苯甲酸和甲氧基聚乙二醇为原料，制备了偶氮苯为末端官能团的甲氧基聚氧乙烯（AZO-g-PEO）。TEM和SEM表征表明β-CD-g-HBPO和AZO-g-PEO可以分别在水中自组装形成片层和纤维结构。通过β-CD-g-HBPO和AZO-g-PEO在共溶剂中缓慢滴加选择性溶剂的方法实现环糊精-偶氮苯主客体识别，得到两亲性线性-超支化超分子嵌段共聚物，最后将共溶剂透析除去得到超分子嵌段共聚物的组装体。采用DLS跟踪了超分子共聚物的形成过程。通过SEM、TEM等表征手段证明所得组装体为囊泡结构。最后，对超分子聚合物的组装和解组装行为进行了研究，结果表明在紫外光和可见光的作用下，超分子聚合物可以发生可逆的形貌转变。
4.共价键合的两亲性超支化嵌段共聚物的合成及自组装行为研究；
采用阳离子开环和氧阴离子开环聚合的方法，分别以丙炔醇和3-叠氮基丙醇为引发剂，采用缓慢滴加的方法合成了具有炔基和叠氮Focal Point的超支化聚醚（YNE-g-HBPO和N_3-g-HPG）。通过YNE-g-HBPO和N_3-g-HPG的点击化学反应得到共价键合的Janus型超支化-超支化嵌段共聚物（HBPO-b-HPG）。采用DLS，TEM、SEM等表征方法，详细研究了HBPO-b-HPG在不同的选择性溶剂中的自组装行为。结果表明，HBPO-b-HPG在水和四氢呋喃中均组装成囊泡结构。此外，采用阳离子开环聚合的方法，以甲氧基聚乙二醇和聚乙二醇为引发剂制备了线性-超支化两亲性分子（HBPO-b-PEO和HBPO-b-PEO-b-HBPO）。以同样的方法研究了HBPO-b-PEO和HBPO-b-PEO-b-HBPO这两种共聚物在水中的自组装行为。
Supramolecular chemistry is the chemistry of the intermolecular bond, covering thestructures and functions of the entities formed by association of two or more chemicalspecies. The intermolecular bond includes hydrogen bonding, metal coordination,hydrophobic forces, van der Waals forces, π-π interactions and electrostatic effects.Supramolecular chemistry has become a exciting and promising research field ininterdisciplinary subject of physics, chemistry, biology, materials science, as well as lifescience. Supramolecular polymer is an important branch of supramolecular chemistry inthe field of polymer chemistry. Hyperbranched polymer is also an important branch ofdendritic polymers which has a large amount of terminal functional groups and manyinner cavities. In this dissertation, based on the review and summarization of previousoutstanding research works of supramolecular polymer and self-assembly ofhyperbranched multiarm copolymers, supramolecular host-guest interaction was used toconstruct hyperbranched block polymer. Hyperbranched polymers with multiple kinds ofmono-reactive focal point were synthesized, the host-guest complexation between focalpoints was utilized to couple the hydrophobic hyperbranched polymer with hydrophilichyperbranched or linear polymer, and then the amphiphilic hyperbranched supramolecularpseudo block copolymers were obtained. Subsequently, the self-assembly and disassemblybehaviors of them were investigated. In addition, the hyperbranched-hyperbranched andlinear-hyperbranched copolymers based on covalent bond were synthesized, theself-assembly behaviors in selected solvent of them were investigated. The main resultsare shown as follows.
1. Synthesis and its photo-responsive self-assembly behavior of Janus amphiphilichyperbranched-hyperbranched supramolecular pseudo block copolymer.
Hydrophobic hyperbranched poly3-ethyl-3-oxetanemethanol with azobenzene asfocal point (AZO-g-HBPO) and hydrophilic hyperbranched polyglycidol withcyclodextrin as core (β-CD-g-HPG) were synthesized according to the cationicring-opening polymerization and oxyanionic ring-opening multibranching polymerization,respectively. The recognization of cyclodextrin and azobenzene was achieved by addingselected solvent to common solvent, and then, Janus amphiphilic hyperbranched-hyperbranched supramolecular pseudo block copolymer was obtained. After dialysisagainst water, the self-assembly of supramolecular polymer completed. DLS and2DNOESY were used to track the formation and self-assembly process of Janussupramolecular copolymer, the results demonstrated the complexation of cyclodextrin andazobenzene. TEM, SEM, Cryo-TEM and AFM were used to directly detect themorphology of the self-assembly objects. The results indicated that the supramolecularcopolymer self-assembled into vesicle with narrow size distribution in water, the thicknessof the vesicle wall was about9.6±0.6nm which is equal with double length of Janussupramolecular copolymer. The vesicles may possess a bilayer structure with twohydrophilic HPG shell layers and one hydrophobic HBPO core layer. Adding competitivehost or guest moleculars with a stronger complexation capacity and irradiation with UVlight with365nm were used to investigate the stability and the disassembly behaviour ofsupramolecular vesicle. The results show that the supramolecular viescle was stable withcompetitive host or guest moleculars and heating, disassembled with irradiation of UVlight with365nm. In addition, the details of the self-assembly process as well as thevesicle structure have been disclosed by a dissipative particle dynamics (DPD) simulation.
2. Synthesis and its electrochemical-responsive self-assembly behavior of Janusamphiphilic hyperbranched supramolecular pseudo block copolymers
Hydrophobic hyperbranched poly3-ethyl-3-oxetanemethanol with ferrocene as focalpoint (Fc-g-HBPO) was synthesized according to the cationic ring-opening polymerization.Hydrophilic end-capped polyethylene oxide with β-cyclodextrin (β-CD-g-PEO) wassynthesized according to the mono-6-deoxy substitution of β-cyclodextrin. Combined withβ-CD-g-HPG in the first part, Janus amphiphilic hyperbranched-hyperbranched andlinear-hyperbranched supramolecular pseudo block copolymers were obtained by recognization between cyclodextrin and ferrocene. After dialysis against water, theself-assembly of supramolecular polymers completed. DLS and2D NOESY were used totrack the formation and self-assembly process of supramolecular copolymers, the resultsdemonstrated the complexation of cyclodextrin and ferrocene. TEM and SEM were usedto directly detect the morphology of the self-assembly objects. The results indicated thatthe supramolecular copolymers self-assembled into vesicle in water. Adding competitivehost or guest moleculars with a stronger complexation capacity, chemical andelectrochemical oxidation were used to investigate the stability and the disassemblybehaviour of supramolecular vesicles. The results show that the supramolecular vesicleswere stable with competitive host or guest moleculars, chemical and electrochemicaloxidation. The supramolecular vesicles disassembled after adding electrolyte to thesupramolecular system after electrochemical oxidation.
3. Synthesis of Janus amphiphilic linear-hyperbranched supramolecular pseudo blockcopolymer and its photo controlled self-assembly and morphology transformation fromvesicles to lamellar structure and fibers.
Hydrophobic hyperbranched poly3-ethyl-3-oxetanemethanol with yne group as focalpoint (YNE-g-HBPO) was synthesized according to the cationic ring-openingpolymerization. Janus type amphiphilic hyperbranched polymer (β-CD-g-HBPO) wasobtained after click reaction between YNE-g-HBPO and mono-6-deoxy-6-azide-β-cyclodextrin. Polyethylene oxide end-capped with azobenzene (AZO-g-PEO) wassynthesized using4-(Phenylazo)benzoic acid and methoxypolyethylene glycol as rawmaterials. Interestingly, the amphiphilic β-CD-g-HBPO and AZO-g-PEO self-assembledto lamellar structure and fiber respectively. The amphiphilic linear-hyperbranchedsupramolecular pseudo block copolymer was obtained by recognization of cyclodextrinand azobenzene. After dialysis against water, the self-assembly of supramolecularpolymers completed. DLS and2D NOESY were used to track the formation andself-assembly process of Janus supramolecular copolymer, the results demonstrated thecomplexation of cyclodextrin and azobenzene. TEM, SEM were used to directly detect themorphology of the self-assembly objects. The results indicated that the supramolecularcopolymer self-assembled into vesicle in water. UV light with365nm was used toinvestigate the stability and the disassembly behaviour of supramolecular vesicles. Theresults show that the supramolecular vesicles disassembled into lamellar structure and fibers. They could reversibly assemble into vesicle under the irriadiation of visible light.
4. Synthesis and self-assembly of amphiphilic hyperbranched-hyperbranched andlinear-hyperbranched copolymers based on covalent bond;
Hydrophilic hyperbranched polyglycidol with azide group as focal point (N_3-g-HPG)was synthesized according to the oxyaionic ring-opening polymerization using3-azidopropan-1-ol as initiator. Janus amphiphilic hyperbranched-hyperbranched blockcopolymer (HBPO-b-HPG) was obtained after click reaction between N_3-g-HPG andYNE-g-HBPO mentioned in the former part. DLS, SEM and TEM were used toinvestigate the self-assembly of HBPO-g-HPG in selected solvent. The resultsdemonstrated that Janus amphiphilic block copolymer self-assembled into vesicles ingboth water and THF. In addition, Janus amphiphilic linear-hyperbranched blockcopolymer (HBPO-b-PEO and HBPO-b-PEO-b-HBPO) were synthesized usingmethoxypolyethylene glycol and polyethylene glycol as initiator through cationicring-opening polymerization. The self-assembly behaviours of them were also discussed atthe same time.
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