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纳米介孔催化材料的组装构建及其应用研究
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摘要
随着人类现代化程度日益提高,环境和能源问题成为人类必须考虑的首要问题。发展新的催化技术和催化材料则是解决上述问题的关键所在,这是由于人类生产生活中几乎所有的产品均需借助于催化剂。大自然通过特有高效特异的反应体系创造了美丽奇妙的世界,其中重要的手段便是多层次多组分协同组装。受其启示,本论文旨在通过组装手段构筑新型高效非均相催化材料,研究工作涉及到几种典型的不同尺度大小的活性单元(有机金属小分子,纳米晶和酶纳米凝胶),进而将活性单元经组装后形成了一系列介孔催化剂。选取与能源环境相关的反应体系对获得的催化剂进行系统研究,以进一步检验与传统催化剂相比所具有的优越性。本论文对所开展的研究工作大致分为三个部分进行讨论:
     第三章主要介绍了利用表面活性剂诱导自组装方法,将结构导向剂,有机金属络合物硅烷和无机硅烷三者有机结合,制得一系列有序介孔有机金属催化材料,该方法能够有效地在分子水平保持催化官能团化学环境完整性和抑制反应过程中有机配体的离散,从而较传统负载型催化剂相比,组装催化剂具有较高的活性和重复使用能力;同时由于结构单元的可调,可以获得不同孔壁化学组分的催化剂,进而营造有利于水介质中催化反应的微环境;此外引入多个活性中心构筑单元,便可制得多功能催化材料,应用于水介质有机串联探针反应发现其具有协同催化效应,从而具有优异的催化活性和稳定性。
     第四章主要研究了将不同组分的纳米晶组装合成三维结构介孔催化剂的方法。采用喷雾协同自组装将两种不同半导体颗粒尺寸均一的纳米晶(CdS和TiO_2),一步制得具有三维纳米结构的偶合半导体介孔光催化材料,由于其纳米级构筑单元的优异性质,从而能在可见光激发下实现电子和空穴分离的同时有效减少电子和空穴的复合,从而具有良好可见光降解有机物的能力。同时,本节还将合金FePt纳米晶与表面活性剂形成微乳构筑介孔合金催化剂,其粒子大小均一(约100 nm)且具有直通型的介孔孔道,将其应用到甲酸电氧化反应中体现出良好的活性和抗毒性。
     第五章的主要内容是设计适宜生物催化剂(酶)所处的微环境的普适性方法。我们首先通过在酶表面原位聚合形成一层富含水分子的纳米级高分子水凝胶,之后以预合成的纳米酶凝胶作为构筑单元与无机硅烷组装形成生物活性介孔复合材料,由于该材料具有“软”和“硬”双重特质,一方面高分子的“软”有利于保持蛋白质的三维结构,也避免了常规固定化酶时与周围环境的直接接触;此外氧化硅的“硬”则有效地阻止酶在反应过程中的脱落和外界环境对酶中心的损害,同时其可调的表面化学性质,能够提高酶中心与底物接触几率,减少传质过程的阻碍。本节分别通过对单个脂肪酶体系和葡萄糖氧化酶和辣根过氧化酶复合体系进行了研究,结果表明该组装方法构筑的载体环境有利于保持酶高活性的同时还能提高酶的稳定性与重复利用能力。
Climate change is a growing concern around the world.Numerous research endeavors are being conducted in order to determine a variety of energy sources and technologies that can be implemented in order to mitigate the impacts of global warming.The design and application of new catalysts and catalytic systems is vital to achieving the dual goals of environmental protection and renewable energy generation. By examining activities in Nature,a beautiful world can be sustained depending on the ability to create specific and high efficiency system,and the ability to develop various mutual assemblies with different components in multi-level dimensions. Inspired by biological systems in Nature,the objective of this current research is to develop novel mesoporous catalytic systems based on the self-assembly of various functional building blocks composed of organometallic complexes,nanocrystals and enzymes.Several important catalytic reactions used in the environmental and energy fields have been adopted to characterize their superior catalytic efficiency over conventional supported catalyst.
     An effective method for the preparation of mesoporous organometallic catalyst (MOC) with pore structure and adjustable chemical compositions has been developed. A surfactant is used as the mesoporous-channel-building molecules,organosilanes are utilized as the scaffold-building molecules,and organornetallic silanesas provide the catalytic-functionality-building molecules.Hydrolysis and condensation reactions of the silanes generated silicate clusters that were subsequently assembled with the surfactant through hydrogen bonding.Hydrophobic interactions preferably locate the active sites(hydrophobic ligands) near the hydrophobic moieties of the surfactant assemblies.Silicate condensation reactions crosslink the building clusters,resulting in nanocomposites containing lytropic surfactant liquid crystalline phases.Subsequent surfactant removal creates mesoporous silica with surface-anchored active sites.This self-directing process spontaneously anchors the active sites on the scaffold while retaining the catalytic molecular configuration and activity.Judicious selection of the surfactant and the scaffold-building silanes allows for precise control of the pore structure(substrate diffusion pathways) and scaffold composition.Meanwhile,MOC materials with multiple catalytic active sites(MMOC) can easily be prepared by simply employing several functional organometallic silanes in the assembly process. The MMOC material has superior activity in water medium cascade reactions due to the synergic effect arisen from selective distribution in the mesopores.
     Mesoporous coupled semiconductor or noble metal alloy catalysts have been synthesized.The catalyst were formed via evaporate induced self-assmbly or microemulsion method by taking the use of CdS,TiO_2 or FePt nanocrystal as building blocks,The CdS/TiO_2 catalysts exhibit strong visible light absorption at about 550 nm. Meanwhile,it has high surface area and mesoporous character based on the average pore diameter.As expected,the CdS nanocrystal sensitized the TiO_2 nanocrystal materials resulting in enhanced activity in the oxidation of methylene blue in water. This is due to the effective transfer of photo-generated electrons from the conduction band of CdS to that of TiO_2.Also the as-synthesized mesoporous FePt alloy is approximately 100 nm in size and has a spherical shape.The results demonstrated that the assembled FePt catalyst exhibited similar catalytic activity and higher toxic tolerability in comparison to that of polycrystal Pt catalyst from the formic acid oxidation reaction.
     A novel approach towards the synthesis of bioactive inorganic composites with better-retained bioactivity has been developed.In comparison to current experimental approaches in which naked biomolecules are directly exposed to non-physiological environment,in this work we pre-wrapped each biomolecule with an enzyeme that functions as an artificial skin.The artificial skin is a thin layer of a soft hydrogel that helps to retain the structure and functionality of the biomolecules in the non-physiological environment.Using the above single enzyme nanogel as building blocks,bioactive mesoporous silica can be obtained by this assembly approach.This organic-inorganic hybrid nanomaterial has soft and hard properties.The soft polymer could retain the enzyme 3D structure;while the hard mesoporous silica can decrease enzyme leaching.Meanwhile,the mesopore channel allows effective transport of the substrates to contact the enzyme active sites.Single enzyme(liapse) or multiple enzymes(Glucose oxidase and Horseradish peroxidase) systems are also investigated. The results show that the assembled bioactive catalyst can retain the enzyme activity and increase stability.
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