多种拓扑结构聚合物的合成及性能研究
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摘要
作为聚合物结构特征的重要方面,分子链的拓扑结构对聚合物的性能如组装性能、热性能、机械性能等产生重要影响。然而由于一些特殊拓扑结构的聚合物如环型聚合物、多嵌段聚合物等在制备上存在较大困难,因此目前这方面的研究尚存在较多空白。基如此,本论文结合近年来倍受关注的可控自由基聚合、点击化学(Click Chemistry)、超分子自组装等,制备了多种拓扑结构的聚合物,其分子链的结构包括二嵌段线型和环型聚合物,多嵌段聚合物,以及特殊星型聚合物等,并研究了其在超分子自组装和热性能等方面的独特性质。具体来说,本论文的工作包括以下几个方面:
1.在二嵌段聚合物的合成与性质研究方面,我们先通过黄酸盐交换的大分子设计(macromolecular design via the interchange of xanthates,MADIX)制备了温度敏感的全亲水性聚合物聚(N,N-二甲基丙烯酰胺)-b-聚(N-乙烯基己内酰胺)(PDMA-b-PVCL),这种聚合物的温度敏感性与常见的含聚(N-异丙基丙烯酰胺)(PNIPAM)链的全亲水性聚合物类似,但由于PVCL的生物相容性比PNIPAM好,因此其拥有更广阔的应用前景。进一步地,我们利用ATRP制备了水溶液具有多重温度响应性的聚(4-乙烯基吡啶)-6-聚(N-异丙基丙烯酰胺)(P4VP-b-PNIPAM),在其酸性水溶液中加入8-氨基萘基-1,3,6-三磺酸二钠盐(ANTS),发现体系在低温下由于质子化的P4VP嵌段与磺酸根络合组装成囊泡,高温下则组装成PNIPAM为核的胶束,而在中间温度下高分子处于分子溶解状态,即通过简单升温就可使体系发生从囊泡到胶束的转变。最后,我们结合ATRP、超分子自组装及Click反应,成功实现了在较高浓度下进行线型前体聚合物的分子内关环反应,同时抑制前体分子间的偶合反应,从而达到了高效高产率制备环型嵌段聚合物的目的,所得pH敏感的环型嵌段聚合物聚(甲基丙烯酸-2-二甲胺基乙酯)-6-(甲基丙烯酸-2-二乙胺基乙酯)(cyclic-PDMAEMA-b-PDEAEMA)与其线型前体相比表现出不一样的自组装性质。
2.在多嵌段聚合物的制备与性质研究方面,我们合成了一种新的线型聚三硫酯,以其为链转移剂通过RAFT聚合制备了一系列不同聚合度的温度敏感的全亲水性多嵌段聚合物m-PDMA-PNIPAM,分别研究了其在低浓度下的胶束化行为与较高浓度下的凝胶化行为。发现这种特殊结构的聚合物在两个浓度范围内的相转变行为都与其PDMA和PNIPAM嵌段长度密切相关。在低浓度下,如果PNIPAM链较长而PDMA链较短,则其水溶液升温产生多分子胶束聚集体;当PDMA嵌段较长而PNIPAM嵌段较短时,升温体系则产生独特的单分子胶束。相应地,前者在高浓度下升温发生相分离不能形成物理凝胶,而后者则形成稳定的物理凝胶。与PNIPAM-b-PDMA-PNIPAM三嵌段聚合物得到的凝胶相比,由多嵌段得到的凝胶强度更好,临界凝胶化浓度(COC)更低,而加入小分子无机盐则可以有效提升凝胶的强度,同时加盐能大大降低ABA型聚合物的CGC但是对多嵌度聚合物影响不大。在此工作基础之上,我们制备了多嵌段聚合物m-P(NIPAM-co-DMA)-b-P4VP,其酸性水溶液在加入小分子盐2,6-萘二磺酸钠(NDSNa)后会表现出多重温度响应性相转变行为:低温和高温下体系都为凝胶状态,而在中间温度(人体温度范围内)体系却为能自由流动的高分子溶液状态,即升温可使体系发生Gel-Sol-Gel的特殊相转变,这在以前的文献中还未见报道。
3在前两部分工作的基础之上,我们进一步致力于高分子纳米自组装体的结构固定。在第一部分工作中,我们通过Click反应制备了一种新的含有氨基的单体1-3'-氨丙基-4丙烯酰胺基-1,2,3-三氮唑环(APAT),利用RAFT聚合制备了其与NIPAM的嵌段聚合物PNIPAM-b-PAPAT。借助于PAPAT嵌段上含有的氨基及PNIPAM嵌段的LCST效应,我们在其20℃和50℃的水溶液中分别制备了CCL胶束和SCL胶束,进一步地,我们利用由Click反应产生的1,2,3-三氮唑环对金属的强络合和稳定作用,分别对CCL胶束的内核与SCL胶束的外壳用金纳米粒子进行选择性修饰。在第二部分工作中,我们利用RAFT聚合制备了不同嵌段比的聚(三甲氧基硅丙基甲基丙烯酸酯)-b-聚环氧乙烷-b-聚(三甲氧基硅丙基甲基丙烯酸酯)(PMPS-b-PEO_(104)-b-PMPS),这种ABA型的两亲性聚合物在水溶液中的自组装体的形貌可以通过调节PMPS嵌段的长度以及初始有机聚合物的极性来改变。更为重要的是,由于PMPS嵌段上含有极易水解交联的-Si-(OCH_3)_3功能团,这些组装体的形貌可以在组装的同时得到结构固定,这为我们方便快捷制备结构稳定的纳米组装体提供了有益的借鉴。
4在最后一章中,我们致力于新型星状聚合物的合成及其热性能的研究。在第一个课题的工作中,我们先通过“先臂法”制备了含多个聚苯乙烯(PS)链的星状聚合物前驱体,其特别之处在于,在此星状聚合物的表面上,每根臂都带有两个炔基功能团。接着,我们合成了一种结构规整的含八个叠氮功能团的无机分子—多面低聚倍半硅氧烷(POSS),以其为交联剂,我们通过Click反应在即稀浓度下实现了前驱体星型聚合物的分子内表面交联,得到了外层为无机分子交联,内层为有机高分子的星状高分子,这种新型的星状聚合物表现出了优良的热稳定性能。在第二个课题的工作中,我们采用“先核法”通过ATRP制备了以POSS分子为内核的含有八根线性臂的星状PS,接着,我们通过Click反应在极稀条件下使得此星状聚合物的臂分子内两两偶联,得到了以POSS为内核,非线性的环形PS为臂的星状高分子,DSC测试表明此星状聚合物表现出比前体星状高分子略高的玻璃化转变温度。
As one of the basic parameters of polymer structures,chains' topologies play an important role in the properties of block copolymers such as self-assembly, thermo-properties,and mechanical properties.However,it is still less studied concerning the detailed relationship between the polymer topologies and properties, since it is difficult for the preparation of polymers with some special topologies such as ring polymers and multiblock copolymers.In this dissertation,a series of block copolymers with particular topologies involving linear and cyclic diblock copolymers, multiblock copolymers,and novel star polymers,were prepared in the combination of widely-noted controlling radical polymerizations(CRP),supramolecular self-assembly,and click chemistry.The properties of the obtained polymers including the self-assembly and thermo-properties were also researched.The dissertation includes the following four parts:
1.As for the synthesis and aggregation behavior of linear and cyclic diblock copolymers,three works are concerned.First,we prepared thermo-responsive double hydrophilic block copolymers(DHBCs)of N,N-dimethylacrylamide (DMA)and N-Vinyl Caprolactam(VCL)by the use of MADIX(Macromolecular Design via Interchange of Xanthanes).The aqueous solution of the obtained polymer,PDMA-b-PVCL,showed similar phase transition behavior with those more common DHBCs containing PNIPAM block,while it is more expectable for this new polymer to be used in biomedical fields since PVCL is more biocompatible than the PNIPAM.Second,double thermo-responsive block copolymer of 4-vinylpyridine(4VP)and NIPAM,P4VP-b-PNIPAM,was prepared via the consecutive atom transfer radical polymerization(ATRP).When the temperature of the aqueous solution of P4VP-b-PNIPAM with 8-aminonaphthalene-1,3,6-trisulfonic acid disodium salt(ANTS)(pH 1.5)was low,the polymers self-assembled into vesicles due the complex between the protonated P4VP block and SO_3~-;with the temperature increasing,the complex was destroyed and the block copolymer dissolved molecularly;while when the temperature was even higher,micelles was formed due to the lower critical solution temperature(LCST)behavior of PNIPAM block.Namely,the nano-aggregates of P4VP-b-PNIPAM can be easily transformed from vesicles to micelles upon heating.Thirdly,we prepared cyclic poly[2-(dimethylamino)ethyl methacrylate]- b-poly-[2-(diethylamino)ethyl methacrylate] (cyclic-PDMAEMA-b-PDEAEMA)via the intramolecular ring-closure reaction of linear-PDMAEMA- b-PDEAEMA,in selective solvents at relatively high concentrations.Owning to self-assembly of the linear precursor,the reactive end functionalities were spatial organized and interchain coupling was effectively prevented.On the other hand,intrachain ring-closure reactions can proceed unhindered for unimers at a concentration of critical micellar concentration(CMC) which was often very low.Thus,cyclic block copolymers can be prepared with high efficiency at relatively high concentrations.The obtained cyclic pH-responsive DHBC showed different aggregation behavior compared with its linear precursor.
2.Using a synthesized polytrithiocarbonate,we prepared multiblock DHBCs via RAFT polymerizations.First,a series of multiblock copolymers of DMA and NIPAM with different sequence length were prepared,and the micellation behavior at low concentration and gelation behavior at relative high concentration were further researched compared with corresponding diblock and ABA triblock copolymers,respectively.It was found that when the PNIPAM block was short and PDMA block was long,unimolecular micelle and gelation behavior occured at low and high concentrations,respectively.While multimolecular micelles and phase separation occurred for the polymers with long PNIPAM sequence and short PDMA sequence.The gel from multiblock copolymers showed higher strength and lower critical gelation concentrations(CGCs)compared with that from ABA triblock copolymers.Furthermore,it was found that addition of inorganic salts can effectively facilitate the gelation behavior,such as elevating the gel strength and decreasing the CGC valuses.On the basis of the work concerning gelation behavior of multiblock copolymers,multiblock copolymer of 4-vinylpyridine and NIPAM,m-P(NIPAM-co-DMA)-b-P4VP,was further synthesized to prepare multi thermo-responsive physical gel.When sodium 2,6-naphthalene disulfonate was added into the aqueous solutions of m-P(NIPAM- co-DMA)-b-P4VP(pH 1.5),physical gels can be obtained both at tow and high temperatures while free-flowing solution was obtained at the middle temperatures in the range of body temperature,i.e.,Gel-Sol-Gel transition was achieved for the first time upon heating the aqueous solution.
3.On the basis of the works concerning the aggregation behavior of block copolymers in selective solvents mentioned above,we are further devoted to fixation of the nano-structures from the self-assembly of block copolymers.First, we synthesized a new monomer,1-(3'-aminopropyl)-4-acrylamido-1,2,3-triazole hydrochloride(APAT),via click chemistry and its block copolymer with NIPAM, PNIPAM-b-PAPAT,via RAFT polymerization.On the basis of the reaction between amine groups of the PAPAT block and glutaric dialdehyde,core cross-linked and shell cross-linked micelles with inverted structures were prepared at 25℃and 50℃,respectively.Furthermore,the shell or core of the crosslinked micelles can be modified with gold nanoparticles due to the metal coordination and stabilization properties of the triazole groups along the PAPAT block.In the second work,we prepared ABA block copolymer ofγ-methacryloxypropyl- trimethoxysilane(MPS)and ethylene oxide (PMPS-b-PEOob-PMPS)with different PMPS block lengths via RAFT polymerizations.In aqueous medium,this block copolymer self-assembled into nano-aggregaetes whose morphologies were largely influenced by the block length and the initial organic common solvent,furthermore,the structure of the aggregated can be self-fixed at the same time due to hydrolysis and cross-linking of the PMPS block in water.
4.In the last section,we prepared two novel structured star polymers in the combination of ATRP and click chemistry.First,core crosslinked star polystyrene (PS)with dialkynyl groups on the surface per arm,was pre-synthesized by polymerizing divinylbenzene(DVB)employing a dialkynyl-containing ATRP macroinitiator.Then the surface of the star polymer was intramolecularly crosslinked using octa(3-azidopropyl)polyhedral oligomeric silsesquioxane, POSS-(N_3)_8,as the inorganic multifunctional crosslinker at high dilution concentration via click chemistry,forming a novel POSS/polymer hybrid nanostructure.Thermogravimetric analysis shows that after surface crosslinking, the thermostability of the core crosslinked PS can be remarkably improved.In the second work,we synthesized of a novel polymer with quatrefoil-shaped topology. Star-linear-polystyrene(starolinear-PS)with～8 linear arms was pre-synthesized from atom transfer radical polymerization(ATRP)employing an eight-functional initiator.Then the objective polymer,star-cyclic-PS,was prepared via intramolecular arm-arm coupling of the star-linear-PS precursor via click reaction at high dilution concentration.Differential scanning calorimetry thermograms (DSC)characterization showed that star-cyclic-PS possessed a little higher glass transition temperature(T_g)than that of the star linear precursor.
1.在二嵌段聚合物的合成与性质研究方面,我们先通过黄酸盐交换的大分子设计(macromolecular design via the interchange of xanthates,MADIX)制备了温度敏感的全亲水性聚合物聚(N,N-二甲基丙烯酰胺)-b-聚(N-乙烯基己内酰胺)(PDMA-b-PVCL),这种聚合物的温度敏感性与常见的含聚(N-异丙基丙烯酰胺)(PNIPAM)链的全亲水性聚合物类似,但由于PVCL的生物相容性比PNIPAM好,因此其拥有更广阔的应用前景。进一步地,我们利用ATRP制备了水溶液具有多重温度响应性的聚(4-乙烯基吡啶)-6-聚(N-异丙基丙烯酰胺)(P4VP-b-PNIPAM),在其酸性水溶液中加入8-氨基萘基-1,3,6-三磺酸二钠盐(ANTS),发现体系在低温下由于质子化的P4VP嵌段与磺酸根络合组装成囊泡,高温下则组装成PNIPAM为核的胶束,而在中间温度下高分子处于分子溶解状态,即通过简单升温就可使体系发生从囊泡到胶束的转变。最后,我们结合ATRP、超分子自组装及Click反应,成功实现了在较高浓度下进行线型前体聚合物的分子内关环反应,同时抑制前体分子间的偶合反应,从而达到了高效高产率制备环型嵌段聚合物的目的,所得pH敏感的环型嵌段聚合物聚(甲基丙烯酸-2-二甲胺基乙酯)-6-(甲基丙烯酸-2-二乙胺基乙酯)(cyclic-PDMAEMA-b-PDEAEMA)与其线型前体相比表现出不一样的自组装性质。
2.在多嵌段聚合物的制备与性质研究方面,我们合成了一种新的线型聚三硫酯,以其为链转移剂通过RAFT聚合制备了一系列不同聚合度的温度敏感的全亲水性多嵌段聚合物m-PDMA-PNIPAM,分别研究了其在低浓度下的胶束化行为与较高浓度下的凝胶化行为。发现这种特殊结构的聚合物在两个浓度范围内的相转变行为都与其PDMA和PNIPAM嵌段长度密切相关。在低浓度下,如果PNIPAM链较长而PDMA链较短,则其水溶液升温产生多分子胶束聚集体;当PDMA嵌段较长而PNIPAM嵌段较短时,升温体系则产生独特的单分子胶束。相应地,前者在高浓度下升温发生相分离不能形成物理凝胶,而后者则形成稳定的物理凝胶。与PNIPAM-b-PDMA-PNIPAM三嵌段聚合物得到的凝胶相比,由多嵌段得到的凝胶强度更好,临界凝胶化浓度(COC)更低,而加入小分子无机盐则可以有效提升凝胶的强度,同时加盐能大大降低ABA型聚合物的CGC但是对多嵌度聚合物影响不大。在此工作基础之上,我们制备了多嵌段聚合物m-P(NIPAM-co-DMA)-b-P4VP,其酸性水溶液在加入小分子盐2,6-萘二磺酸钠(NDSNa)后会表现出多重温度响应性相转变行为:低温和高温下体系都为凝胶状态,而在中间温度(人体温度范围内)体系却为能自由流动的高分子溶液状态,即升温可使体系发生Gel-Sol-Gel的特殊相转变,这在以前的文献中还未见报道。
3在前两部分工作的基础之上,我们进一步致力于高分子纳米自组装体的结构固定。在第一部分工作中,我们通过Click反应制备了一种新的含有氨基的单体1-3'-氨丙基-4丙烯酰胺基-1,2,3-三氮唑环(APAT),利用RAFT聚合制备了其与NIPAM的嵌段聚合物PNIPAM-b-PAPAT。借助于PAPAT嵌段上含有的氨基及PNIPAM嵌段的LCST效应,我们在其20℃和50℃的水溶液中分别制备了CCL胶束和SCL胶束,进一步地,我们利用由Click反应产生的1,2,3-三氮唑环对金属的强络合和稳定作用,分别对CCL胶束的内核与SCL胶束的外壳用金纳米粒子进行选择性修饰。在第二部分工作中,我们利用RAFT聚合制备了不同嵌段比的聚(三甲氧基硅丙基甲基丙烯酸酯)-b-聚环氧乙烷-b-聚(三甲氧基硅丙基甲基丙烯酸酯)(PMPS-b-PEO_(104)-b-PMPS),这种ABA型的两亲性聚合物在水溶液中的自组装体的形貌可以通过调节PMPS嵌段的长度以及初始有机聚合物的极性来改变。更为重要的是,由于PMPS嵌段上含有极易水解交联的-Si-(OCH_3)_3功能团,这些组装体的形貌可以在组装的同时得到结构固定,这为我们方便快捷制备结构稳定的纳米组装体提供了有益的借鉴。
4在最后一章中,我们致力于新型星状聚合物的合成及其热性能的研究。在第一个课题的工作中,我们先通过“先臂法”制备了含多个聚苯乙烯(PS)链的星状聚合物前驱体,其特别之处在于,在此星状聚合物的表面上,每根臂都带有两个炔基功能团。接着,我们合成了一种结构规整的含八个叠氮功能团的无机分子—多面低聚倍半硅氧烷(POSS),以其为交联剂,我们通过Click反应在即稀浓度下实现了前驱体星型聚合物的分子内表面交联,得到了外层为无机分子交联,内层为有机高分子的星状高分子,这种新型的星状聚合物表现出了优良的热稳定性能。在第二个课题的工作中,我们采用“先核法”通过ATRP制备了以POSS分子为内核的含有八根线性臂的星状PS,接着,我们通过Click反应在极稀条件下使得此星状聚合物的臂分子内两两偶联,得到了以POSS为内核,非线性的环形PS为臂的星状高分子,DSC测试表明此星状聚合物表现出比前体星状高分子略高的玻璃化转变温度。
As one of the basic parameters of polymer structures,chains' topologies play an important role in the properties of block copolymers such as self-assembly, thermo-properties,and mechanical properties.However,it is still less studied concerning the detailed relationship between the polymer topologies and properties, since it is difficult for the preparation of polymers with some special topologies such as ring polymers and multiblock copolymers.In this dissertation,a series of block copolymers with particular topologies involving linear and cyclic diblock copolymers, multiblock copolymers,and novel star polymers,were prepared in the combination of widely-noted controlling radical polymerizations(CRP),supramolecular self-assembly,and click chemistry.The properties of the obtained polymers including the self-assembly and thermo-properties were also researched.The dissertation includes the following four parts:
1.As for the synthesis and aggregation behavior of linear and cyclic diblock copolymers,three works are concerned.First,we prepared thermo-responsive double hydrophilic block copolymers(DHBCs)of N,N-dimethylacrylamide (DMA)and N-Vinyl Caprolactam(VCL)by the use of MADIX(Macromolecular Design via Interchange of Xanthanes).The aqueous solution of the obtained polymer,PDMA-b-PVCL,showed similar phase transition behavior with those more common DHBCs containing PNIPAM block,while it is more expectable for this new polymer to be used in biomedical fields since PVCL is more biocompatible than the PNIPAM.Second,double thermo-responsive block copolymer of 4-vinylpyridine(4VP)and NIPAM,P4VP-b-PNIPAM,was prepared via the consecutive atom transfer radical polymerization(ATRP).When the temperature of the aqueous solution of P4VP-b-PNIPAM with 8-aminonaphthalene-1,3,6-trisulfonic acid disodium salt(ANTS)(pH 1.5)was low,the polymers self-assembled into vesicles due the complex between the protonated P4VP block and SO_3~-;with the temperature increasing,the complex was destroyed and the block copolymer dissolved molecularly;while when the temperature was even higher,micelles was formed due to the lower critical solution temperature(LCST)behavior of PNIPAM block.Namely,the nano-aggregates of P4VP-b-PNIPAM can be easily transformed from vesicles to micelles upon heating.Thirdly,we prepared cyclic poly[2-(dimethylamino)ethyl methacrylate]- b-poly-[2-(diethylamino)ethyl methacrylate] (cyclic-PDMAEMA-b-PDEAEMA)via the intramolecular ring-closure reaction of linear-PDMAEMA- b-PDEAEMA,in selective solvents at relatively high concentrations.Owning to self-assembly of the linear precursor,the reactive end functionalities were spatial organized and interchain coupling was effectively prevented.On the other hand,intrachain ring-closure reactions can proceed unhindered for unimers at a concentration of critical micellar concentration(CMC) which was often very low.Thus,cyclic block copolymers can be prepared with high efficiency at relatively high concentrations.The obtained cyclic pH-responsive DHBC showed different aggregation behavior compared with its linear precursor.
2.Using a synthesized polytrithiocarbonate,we prepared multiblock DHBCs via RAFT polymerizations.First,a series of multiblock copolymers of DMA and NIPAM with different sequence length were prepared,and the micellation behavior at low concentration and gelation behavior at relative high concentration were further researched compared with corresponding diblock and ABA triblock copolymers,respectively.It was found that when the PNIPAM block was short and PDMA block was long,unimolecular micelle and gelation behavior occured at low and high concentrations,respectively.While multimolecular micelles and phase separation occurred for the polymers with long PNIPAM sequence and short PDMA sequence.The gel from multiblock copolymers showed higher strength and lower critical gelation concentrations(CGCs)compared with that from ABA triblock copolymers.Furthermore,it was found that addition of inorganic salts can effectively facilitate the gelation behavior,such as elevating the gel strength and decreasing the CGC valuses.On the basis of the work concerning gelation behavior of multiblock copolymers,multiblock copolymer of 4-vinylpyridine and NIPAM,m-P(NIPAM-co-DMA)-b-P4VP,was further synthesized to prepare multi thermo-responsive physical gel.When sodium 2,6-naphthalene disulfonate was added into the aqueous solutions of m-P(NIPAM- co-DMA)-b-P4VP(pH 1.5),physical gels can be obtained both at tow and high temperatures while free-flowing solution was obtained at the middle temperatures in the range of body temperature,i.e.,Gel-Sol-Gel transition was achieved for the first time upon heating the aqueous solution.
3.On the basis of the works concerning the aggregation behavior of block copolymers in selective solvents mentioned above,we are further devoted to fixation of the nano-structures from the self-assembly of block copolymers.First, we synthesized a new monomer,1-(3'-aminopropyl)-4-acrylamido-1,2,3-triazole hydrochloride(APAT),via click chemistry and its block copolymer with NIPAM, PNIPAM-b-PAPAT,via RAFT polymerization.On the basis of the reaction between amine groups of the PAPAT block and glutaric dialdehyde,core cross-linked and shell cross-linked micelles with inverted structures were prepared at 25℃and 50℃,respectively.Furthermore,the shell or core of the crosslinked micelles can be modified with gold nanoparticles due to the metal coordination and stabilization properties of the triazole groups along the PAPAT block.In the second work,we prepared ABA block copolymer ofγ-methacryloxypropyl- trimethoxysilane(MPS)and ethylene oxide (PMPS-b-PEOob-PMPS)with different PMPS block lengths via RAFT polymerizations.In aqueous medium,this block copolymer self-assembled into nano-aggregaetes whose morphologies were largely influenced by the block length and the initial organic common solvent,furthermore,the structure of the aggregated can be self-fixed at the same time due to hydrolysis and cross-linking of the PMPS block in water.
4.In the last section,we prepared two novel structured star polymers in the combination of ATRP and click chemistry.First,core crosslinked star polystyrene (PS)with dialkynyl groups on the surface per arm,was pre-synthesized by polymerizing divinylbenzene(DVB)employing a dialkynyl-containing ATRP macroinitiator.Then the surface of the star polymer was intramolecularly crosslinked using octa(3-azidopropyl)polyhedral oligomeric silsesquioxane, POSS-(N_3)_8,as the inorganic multifunctional crosslinker at high dilution concentration via click chemistry,forming a novel POSS/polymer hybrid nanostructure.Thermogravimetric analysis shows that after surface crosslinking, the thermostability of the core crosslinked PS can be remarkably improved.In the second work,we synthesized of a novel polymer with quatrefoil-shaped topology. Star-linear-polystyrene(starolinear-PS)with～8 linear arms was pre-synthesized from atom transfer radical polymerization(ATRP)employing an eight-functional initiator.Then the objective polymer,star-cyclic-PS,was prepared via intramolecular arm-arm coupling of the star-linear-PS precursor via click reaction at high dilution concentration.Differential scanning calorimetry thermograms (DSC)characterization showed that star-cyclic-PS possessed a little higher glass transition temperature(T_g)than that of the star linear precursor.
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