纳米聚苯胺、二氧化钛及其复合材料的制备和应用
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摘要
聚苯胺具有优良的环境稳定性，独特的酸／碱掺杂／脱掺杂性质，合成简易，原料价廉易得，使其成为“合成金属”家族的重要成员，已经成为导电高分子的研究热点。而具有纳米结构的聚苯胺具有更加独特的性能，不仅在聚苯胺传统的应用领域中具有更好的性能，而且能够在更新的应用领域中发挥重要作用。本文在综述聚苯胺的性质和制备的基础上，结合当前制备聚苯胺纳米材料的方法，特别是非模板法制备聚苯胺纳米纤维的方法，提出了紫外光辅助化学氧化法，在不同的聚合条件下制备聚苯胺纳米纤维，特别是聚苯胺纳米线。本文研究了氧化剂种类、浓度、搅拌以及反应温度等各种实验参数在紫外光照和避光条件下对合成产物形貌、酸掺杂和脱掺杂能力的影响。结果表明光辅助制备聚苯胺纳米纤维的方法不仅适用于具有不同氧化能力的氧化剂，而且适合在常规方法无法合成纳米纤维的条件下进行。有趣的是，光辅助法低温聚合可以在没有任何模板的存在下合成出聚苯胺纳米线。
基于苯胺及其聚合物被质子化能力与其它导电高分子体系相比较，第三章提出了一个新的理论模型来解释聚苯胺纳米纤维的形成机理，即“双电层”理论模型。该理论模型可以更加合理地解释为什么纳米纤维是聚苯胺的本质形貌。在手性樟脑磺酸的诱导下，本文同时探讨了各种实验参数对合成聚苯胺的形貌及其光学活性的影响，进一步证明“双电层”理论模型的合理性，并建立聚苯胺一维螺旋生长与其光学活性的关联性。
二氧化钛半导体光催化氧化技术因其自身突出的优点而成为科研工作者的研究热点。本文通过研究二氧化钛一维纳米化来提高二氧化钛紫外光催化活性；其次，利用聚苯胺可见光敏化来拓展二氧化钛可见光催化。第四章改进碱水热法，通过盐效应裁剪钛酸盐和二氧化钛的纳米结构，并重新审查了氢氧化钠在碱水热法中所扮演的重要角色。基于对产物形貌的演变规律，提出了一种合理的生长机理来解释各种钛酸盐和二氧化钛纳米结构的形成原因。
第五章通过自组装和嫁接聚合的方法制备二氧化钛与聚苯胺的纳米复合材料，并通过各种手段对该纳米复合材料进行表征。研究结果证实了二氧化钛表面自组装层和聚苯胺的形成，以及表明该复合材料具有更好的热稳定性和更高的可见光催化活性。我们进一步研究了不同浓度的苯胺在二氧化钛光催化表面的氧化行为，推荐了一种去除废水中苯胺的方法。此方法建议采用二氧化钛光催化技术降解并矿化低浓度苯胺；采用光催化法促进高浓度苯胺氧化聚合，制备二氧化钛与聚苯胺的纳米复合材料。
Polyaniline is unique among the family of conducting polymers due to its ease ofsynthesis,environmental stability and simple doping/dedoping chemistry,which hasreceived growing interest in recent years.Nanostructures of polyaniline can lead to betterperformance in the already established areas and create new opportunities.In thisdissertation,on the basis of the review on the properties and preparation of polyaniline andin combination with current ways of synthesizing polyaniline nanomaterials,especiallyfree-template methods to prepare polyaniline nanofibers,a new approach for the synthesisof polyaniline nanostructures (nanofibers and nanowires) under UV light illumination hasbeen developed.This dissertation investigated the effect of various experimentalparameters,such as the kind of oxidants,their concentration,stirring and reactiontemperature et al.on the morphology and the ability of acid doping/dedoping of theproducts from UV illumination and in dark,respectively.The results indicate that thisphoto-assisted method not only is fitted for various oxidants with different oxidationability,but also prepares polyaniline nanofibers on the rigorous conditions,in which thenanofibers can not be obtained by conventional routes in dark.It is interesting thatphoto-assisted method at lower temperature can produce polyaniline nanowires withoutany template.
In the consideration on the comparison of the protonation ability of aniline and itspolymer with other conductive polymers,a theoretical model was proposed to explain theformation of polyaniline nanofibers,namely“electric double layers”model.Thistheoretical model can better explain why the nanofibers are intrinsic morphology ofpolyaniline.In the presence of chiral CSA,this dissertation studied the effect of variousexperimental parameters on the polyaniline morphology and its optical activity,whichfurther confirms that it is rational for“electric double layers”model,and found the correlation between polyaniline one-dimensional growth and its optical activity.
TiO_2 photocatalytic technology attracts increasingly intesest due to its various merits.Inthe present work,in allusion to the existing problems,we tried to prepare one-dimensionalTiO_2 nanomaterials to enhance the UV photocatalytic activity;on the other hand,wedeveloped TiO_2 visible photocatalysts via the visible light sensitization of polyaniline.Infourth chapter,this dissertation modified alkaline hydrothermal method,salt effecttailoring TiO_2 and titanate nanostructures.We repeated investigating the important role ofNaOH in this alkaline hydrothermal method,and proposed a rational mechanism toexplain the formation of TiO_2 and titanate nanostructures on the basis of the evolutiveregulation of products morphology.
In fifth chapter,we successfully synthesized TiO_2/polyaniline nanocomposites viaself-assembling and graft polymerization.The resulted nanocomposites were characterizedby using various measuremental technologies.The results indicated the formation ofself-assembling layer and outside polyaniline,and the better thermal stability of thesenanocomposites.Moreover,these composites showed better photocatalytic activity undersunlight due to the sensitizing effect of polyaniline.We further studied the oxidationcharacteristics of aniline at different concentration on TiO_2 photocatalysts,and proposed away of removing aniline in aqueous systems.Our strategy is to degrade and mineralizelow-level aniline by using a photocatalytic degradation process,and to convert high-levelaniline to TiO_2/polyaniline nanocomposites via a photocatalytic polymerization approach.
基于苯胺及其聚合物被质子化能力与其它导电高分子体系相比较，第三章提出了一个新的理论模型来解释聚苯胺纳米纤维的形成机理，即“双电层”理论模型。该理论模型可以更加合理地解释为什么纳米纤维是聚苯胺的本质形貌。在手性樟脑磺酸的诱导下，本文同时探讨了各种实验参数对合成聚苯胺的形貌及其光学活性的影响，进一步证明“双电层”理论模型的合理性，并建立聚苯胺一维螺旋生长与其光学活性的关联性。
二氧化钛半导体光催化氧化技术因其自身突出的优点而成为科研工作者的研究热点。本文通过研究二氧化钛一维纳米化来提高二氧化钛紫外光催化活性；其次，利用聚苯胺可见光敏化来拓展二氧化钛可见光催化。第四章改进碱水热法，通过盐效应裁剪钛酸盐和二氧化钛的纳米结构，并重新审查了氢氧化钠在碱水热法中所扮演的重要角色。基于对产物形貌的演变规律，提出了一种合理的生长机理来解释各种钛酸盐和二氧化钛纳米结构的形成原因。
第五章通过自组装和嫁接聚合的方法制备二氧化钛与聚苯胺的纳米复合材料，并通过各种手段对该纳米复合材料进行表征。研究结果证实了二氧化钛表面自组装层和聚苯胺的形成，以及表明该复合材料具有更好的热稳定性和更高的可见光催化活性。我们进一步研究了不同浓度的苯胺在二氧化钛光催化表面的氧化行为，推荐了一种去除废水中苯胺的方法。此方法建议采用二氧化钛光催化技术降解并矿化低浓度苯胺；采用光催化法促进高浓度苯胺氧化聚合，制备二氧化钛与聚苯胺的纳米复合材料。
Polyaniline is unique among the family of conducting polymers due to its ease ofsynthesis,environmental stability and simple doping/dedoping chemistry,which hasreceived growing interest in recent years.Nanostructures of polyaniline can lead to betterperformance in the already established areas and create new opportunities.In thisdissertation,on the basis of the review on the properties and preparation of polyaniline andin combination with current ways of synthesizing polyaniline nanomaterials,especiallyfree-template methods to prepare polyaniline nanofibers,a new approach for the synthesisof polyaniline nanostructures (nanofibers and nanowires) under UV light illumination hasbeen developed.This dissertation investigated the effect of various experimentalparameters,such as the kind of oxidants,their concentration,stirring and reactiontemperature et al.on the morphology and the ability of acid doping/dedoping of theproducts from UV illumination and in dark,respectively.The results indicate that thisphoto-assisted method not only is fitted for various oxidants with different oxidationability,but also prepares polyaniline nanofibers on the rigorous conditions,in which thenanofibers can not be obtained by conventional routes in dark.It is interesting thatphoto-assisted method at lower temperature can produce polyaniline nanowires withoutany template.
In the consideration on the comparison of the protonation ability of aniline and itspolymer with other conductive polymers,a theoretical model was proposed to explain theformation of polyaniline nanofibers,namely“electric double layers”model.Thistheoretical model can better explain why the nanofibers are intrinsic morphology ofpolyaniline.In the presence of chiral CSA,this dissertation studied the effect of variousexperimental parameters on the polyaniline morphology and its optical activity,whichfurther confirms that it is rational for“electric double layers”model,and found the correlation between polyaniline one-dimensional growth and its optical activity.
TiO_2 photocatalytic technology attracts increasingly intesest due to its various merits.Inthe present work,in allusion to the existing problems,we tried to prepare one-dimensionalTiO_2 nanomaterials to enhance the UV photocatalytic activity;on the other hand,wedeveloped TiO_2 visible photocatalysts via the visible light sensitization of polyaniline.Infourth chapter,this dissertation modified alkaline hydrothermal method,salt effecttailoring TiO_2 and titanate nanostructures.We repeated investigating the important role ofNaOH in this alkaline hydrothermal method,and proposed a rational mechanism toexplain the formation of TiO_2 and titanate nanostructures on the basis of the evolutiveregulation of products morphology.
In fifth chapter,we successfully synthesized TiO_2/polyaniline nanocomposites viaself-assembling and graft polymerization.The resulted nanocomposites were characterizedby using various measuremental technologies.The results indicated the formation ofself-assembling layer and outside polyaniline,and the better thermal stability of thesenanocomposites.Moreover,these composites showed better photocatalytic activity undersunlight due to the sensitizing effect of polyaniline.We further studied the oxidationcharacteristics of aniline at different concentration on TiO_2 photocatalysts,and proposed away of removing aniline in aqueous systems.Our strategy is to degrade and mineralizelow-level aniline by using a photocatalytic degradation process,and to convert high-levelaniline to TiO_2/polyaniline nanocomposites via a photocatalytic polymerization approach.
引文
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