Chemical design and chemical process for functional ceramics using ionomers

本工作的核心是在低温下制备均匀的多组分凝胶前体，用于合成各种先进的陶瓷材料。为了实现这一目标，从与各种溶剂中金属螯合络合物形成密切相关的溶液化学的基本方面到包括凝胶科学在内的聚合物科学领域的许多方面的研究都得到了系统的开展。特别重要的是如何制备具有所需化学计量的杂金属配合物作为陶瓷材料的合适的分子前驱体。包括拉曼、红外和核磁共振在内的各种光谱技术被用作工具，以深入了解在起始溶液或聚合物产品中形成的分子种类或键类型。另一个重要的工作是研究凝胶前驱体在热处理过程中的结构演变。这也是用上面列出的光谱技术…更多的技术以及x射线衍射技术来完成的。主要结果如下：1)在M- ti -柠檬酸（CA）体系中设计了不同的杂金属配合物，其中M=Ba, Sr， Pb和y.采用^<13>C-NMR谱建立了鉴定溶液中杂金属配合物的独特方法。在这些配合物的存在下，乙二醇和CA之间进行了聚合反应，得到了均匀的多组分凝胶。2)利用拉曼光谱和核磁共振光谱研究了多组分陶瓷的结构演变。最终产物的表征主要是通过拉曼散射和x射线衍射技术进行的。特别注意确定降低合成温度的条件。3)总体结果：建立了一种制备多组分凝胶前驱体的方案，该方案可用于低温高纯合成多组分陶瓷。少

Central in the present work is to prepare homogeneous multicomponent gel precursors for the synthesis of various advanced ceramic materials at reduced temperatures. To reach this goal, studies under the many aspects ranging from the basic aspects of the solution chemistry closely connected to metal-chelate complex formations in various solvents to the polymer science including the field of the gel science have been systematically carried out. Of particular importance is how to prepare hetero-metallic complexes with a desired stoichiometry as a suitable molecular precursor for ceramic materials. Various spectroscopic techniques involving Raman, infrared and NMR were used as tools to gain insight into molecular species or bonding type that are formed either in a starting solution or in a polymeric product. Another important part of the work is to study the evolution of structure during the heat treatment of the gel precursors. This also was done using the above listed spectroscopic techn … More iques as well as X-ray diffraction techniques. The main results obtained were summarized as below :1) Heterometallic complexes were designed in various M-Ti-citric acid (CA) systems, where M=Ba, Sr, Pb, and Y.A unique method for the identification of heterometallic complexes in solutions was established by employing ^<13>C-NMR spectroscopy. Polyesterification between ethyleneglycol and CA was carried out in the presence of these complexes in order to obtain homogeneous multi-component gels.2) Structural evolution of multi-component ceramics was studied by use of Raman and NMR spectroscopies. Characterization of the final product was developed mainly by Raman scattering and X-ray diffraction techniques. Particular attention was paid to determining conditions of reducing the synthesis temperatures.3) Overall outcome : A scheme to prepare homogeneous multicomponent gel precursors, that can be used for the high-pure synthesis of multi-component ceramics at reduced temperatures was built up. Less