摘要
分别作为典型的一维和二维的碳纳米材料,碳纳米管(CNTs)和石墨烯(graphene)因其特殊的结构和优异的力学、电学、热学和光学性能,受到广泛的关注。CNTs和graphene基纳米杂化材料尤其是与聚合物形成的纳米杂化材料不仅实现了CNTs和graphene的功能化和分散性,还拓宽了其在纳米复合材料、传感器、电子器件和生物医药等领域的应用。因此,本论文旨在探索-种方便有效的方法制备功能化CNTs和graphene基纳米杂化材料,并研究实验条件对CNTs和graphene功能化程度的影响,探讨形成不同形貌的原因。本工作为功能化CNTs和graphene基纳米杂化材料的应用开辟新的机会。
本论文主要工作包括：
(1)采用超临界CO2辅助制备聚乙烯(PE)和聚环氧乙烷(PEO)/CNTs纳米杂化材料,并研究了PE和PEO在CNTs表面形成不同形貌的原因。
PE在CNTs上形成“纳米杂化串晶”结构,而PEO则在CNTs表面形成很薄的无定形聚合物涂层。PE/CNTs和PEO/CNTs纳米杂化材料的不同形貌取决于聚合物分子链的构象和聚合物链与CNTs之间的相互作用。实验结果表明CNTs为PE提供异相成核点,形成的纳米杂化串晶结构阻止了聚合物链的扩散和晶体的生长。而CNTs对PEO分子链起抗成核效应。本工作为制备多功能性CNTs基纳米杂化材料提供理论支持。
(2)利用超临界CO2辅助制备芘基聚乙二醇(pyrene-PEG)/CNTs纳米杂化材料及其稳定性研究
实验结果发现pyrene-PEG与CNTs形成强的非共价键π-π相互作用,而PEG分子链赋予CNTs良好的水溶液分散性。由于pyrene-和CNTs之间的π-π相互作用引起了强的光诱导电荷转移/或能量转移,从而导致pyrene-PEG/CNTs纳米杂化材料水溶液的荧光强度显著降低。pyrene-PEG/CNTs纳米杂化材料在O.1M HCl和强离子溶液中稳定分散,为CNTs在生物领域的应用提供可能。
(3)超临界CO2辅助制备聚乙烯-b-聚环氧乙烷(PE-b-PEO)/氧化石墨烯(GO)纳米杂化材料及进一步功能化
成功制备了两亲性双结晶性嵌段共聚物PE-b-PEO/GO纳米杂化材料,实验结果发现溶剂体系和超临界CO2对PE-b-PEO分子链在GO表面的结晶、聚集和组装具有显著的影响。同时以PE-b-PEO/GO纳米杂化材料为模板将金纳米粒子(Au NPs)和碲化镉纳米晶(CdTe NPs)固定在GO表面,成功地制备了GO基多功能性纳米杂化结构。
(4)基于超临界CO2和芘基聚合物直接剥离石墨制备石墨烯(graphene)
基于芘基聚合物(pyrene-PEG和pyrene-PCL)和超临界CO2直接剥离石墨制备了高质量的、在不同溶液中稳定分散的graphene溶液。剥离过程包括石墨、溶剂、芘基聚合物和超临界CO2之间的多重相互作用,其中超临界CO2作为渗透剂、膨胀剂和抗溶剂,芘基聚合物作为分子楔和改性剂获得高产量的稳定分散的graphene溶液。此方法结合高产量制备和功能化graphene为一体,为进-步制备多功能的graphene基材料提供了可能,从而拓宽了graphene的应用领域。
As typical one-dimensional and two-dimensional carbon nanomaterials, carbon nanotubes (CNTs) and graphene, have attracted considerable interest due to their specific structure, and extraordinary mechanical, electrical, thermal and optic properties. CNTs and graphene based nanohybrids especially polymer nanohybrids not only endow good functionalization and dispersion of CNTs and graphene, but broaden their application in nanocomposite, sensor, electronic device and biomedical fields. Therefore, this work is aim at exploring a facile and efficient method to fabricate functional CNTs and graphene based nanohybrids, and studying the effect of experimental conditions on the functionalization degree of CNTs and graphene. Meanwhile the varing morphologies of the nanohybrids will also be discussed. This work will open up new opportunities for nanoscience and nano techno logy and accelerate their application
The main work in this paper contains:
(1) Fabrication of polyethylene (PE) and poly(ethylene oxide)(PEO)/CNTs nanohybrids via supercritical CO2, and comparison study of varing morphologies of PE and PEO on CNTs.
CNTs were decorated by PE lamellar crystals, forming "nanohybrid shish-kebab" structure, whereas PEO only wrapped on CNTs and formed thin amorphous polymer coating on the surface of CNTs. The results showed that the varing morphologies of PE/CNTs and PEO/CNTs nanohybrids depend on the molecular conformantin and the interaction between polymer chains and CNTs. CNTs provided heterogeneous nucleation sites for PE and the fromed shish-kebab structure hindered PE chains diffusion and crystal growth, whereas CNTs played antinucleation effect on PEO chains. This work provided theoretical understanding of fabricating multifunctional CNTs based nanohybrids.
(2) Fabrication of pyrene-PEG/CNTs nanohybrids based on supercritical CO2and study of their stability in different solvents.
The results showed that pyrene-PEG can form strong noncovalent π-π interaction with CNTs, and PEG chains endow good dispersion of CNTs in aqueous solution. There exists fluorescence quenching of pyrene-PEG/CNTs solution as a result of strong photoinduced electron/energy transfer between pyrene-and CNTs. In addition, pyrene-PEG/CNTs nanohybrids showed good stability in0.1M HCl and strong ionic solution, which paved way for CNTs in the field of biological application.
(3) Fabrication of PE-b-PEO/graphite oxide (GO) nanohybrids via supercritical CO2and its further functionalization
In this section, we succefully fabricated amphiphilic double-crystalline block copolymer PE-b-PEO/GO nanohybrids via supercritical CO2-The results showed that the solvent system and supercritical CO2play remarkable influence on the crystallization,aggregation and assembly of PE-b-PEO chains on the surface of GO. Furthermore, the PE-b-PEO/GO nanohybrid was used as template to immobilize Au nanoparticles (Au NPs) and CdTe nanoparticles (CdTe NPs), which succefully produced multifunctional GO based nanohybrids.
(4) Direct exfoliation of graphite to graphene based on supercritical CO2and pyrene-polymer
In this section, we used pyrene-polymers and supercrital CO2, that the large-scale direct exfoliation of graphite into defect-free graphene sheets has been achieved, leading to stable graphene dispersions in solutions. This novel exfoliation process involves with multiple interactions among graphite, solvent, pyrene-derivatives and SC CO2, where SC CO2acts as penetrant, expanding agent and antisolvent, and pyrene-derivatives act as molecular wedges and modifier to obtain high-yield and stable graphene solutions. The method of combining high-throughput production and functionalization of graphene in one step, which might pave the way for developing multifunctional high-performance applications of graphene and graphene-based materials in various fields.
引文
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