本文關(guān)鍵詞： 微納米 無機(jī)功能材料 形貌控制 表面MOFs化　出處：《北京科技大學(xué)》2015年博士論文　論文類型：學(xué)位論文

【摘要】：微納米無機(jī)功能材料由于具有獨(dú)特的磁、光、電、催化等性能,受到了全世界科研工作者的廣泛關(guān)注。材料的形貌、結(jié)構(gòu)、尺寸對(duì)其性能有著重要影響,因此探索無機(jī)功能材料的可控合成方法對(duì)于提升其性能具有重要意義。本論文從無機(jī)功能材料的控制合成入手,基于絡(luò)合沉淀法制備了一系列具有特殊形貌、新穎結(jié)構(gòu)的無機(jī)功能材料,提出了其可能的生長機(jī)制并發(fā)展了新的可控合成方法,探索了其在催化領(lǐng)域的應(yīng)用并研究了材料微納米結(jié)構(gòu)與性能之間的構(gòu)效關(guān)系,為微納米無機(jī)功能材料的結(jié)構(gòu)設(shè)計(jì)、性能調(diào)控及其在相關(guān)領(lǐng)域的實(shí)際應(yīng)用提供了理論和實(shí)驗(yàn)依據(jù)。 基于絡(luò)合沉淀法,發(fā)展了一種制備多級(jí)結(jié)構(gòu)微納米無機(jī)功能材料的普適性方法,利用添加劑的絡(luò)合作用和結(jié)構(gòu)導(dǎo)向作用控制反應(yīng)速度及產(chǎn)物的形成過程,制備得到了多種具有新穎結(jié)構(gòu)的無機(jī)功能材料(雙輪狀組裝體結(jié)構(gòu)鎳鈷氫氧化物/氧化物,兩面刷結(jié)構(gòu)摻鎳氫氧化鈷/四氧化三鈷及yolk/shell堿式硫酸銅),并通過控制實(shí)驗(yàn)參數(shù)實(shí)現(xiàn)了產(chǎn)物形貌和尺寸的調(diào)控。 在制備多種結(jié)構(gòu)無機(jī)功能材料的基礎(chǔ)上,系統(tǒng)研究了添加劑加入量、反應(yīng)溫度、pH環(huán)境、前軀體種類、前軀體與絡(luò)合劑濃度比等因素對(duì)產(chǎn)物形貌的影響,提出了上述微納米多級(jí)結(jié)構(gòu)產(chǎn)物的生長機(jī)制,為微納米材料的可控合成提供了理論基礎(chǔ)。 利用自模板法實(shí)現(xiàn)了特定無機(jī)功能材料的表面原位轉(zhuǎn)化,制備得到了無機(jī)功能材料@MOFs,實(shí)現(xiàn)了MOFs優(yōu)異的結(jié)構(gòu)特性(超大的比表面積,均勻的孔徑分布,可控的拓?fù)浣Y(jié)構(gòu)及可調(diào)的孔徑)和微納米粒子催化特性的優(yōu)勢集成,克服了傳統(tǒng)的層層自組裝法制備微納米粒子@MOFs存在的反應(yīng)條件苛刻、周期長且后處理復(fù)雜等缺點(diǎn)。 圍繞所制備的多級(jí)結(jié)構(gòu)微納米無機(jī)功能材料,探索了其在催化領(lǐng)域的應(yīng)用研究,上述產(chǎn)物對(duì)烯烴環(huán)氧化反應(yīng)、縮醛反應(yīng)和醇的分子氧氧化反應(yīng)等反應(yīng)具有優(yōu)異的催化效果。
[Abstract]:Due to their unique magnetic, optical, electrical and catalytic properties, micro-nano inorganic functional materials have been widely concerned by researchers all over the world. The morphology, structure and size of the materials have an important impact on their properties. Therefore, it is very important to explore the controllable synthesis method of inorganic functional materials for improving their properties. In this paper, a series of special morphologies were prepared based on complex precipitation method, starting with the controlled synthesis of inorganic functional materials. The possible growth mechanism of inorganic functional materials with novel structure was proposed and a new controllable synthesis method was developed. Their applications in the field of catalysis were explored and the structure-activity relationship between microstructures and properties of the materials was studied. It provides theoretical and experimental basis for the structure design, performance control and practical application in the related fields of micro and nano inorganic functional materials. Based on the complexation precipitation method, a universal method for the preparation of multilevel structure microinorganic functional materials was developed. The reaction rate and the formation process of the product were controlled by the complexation and structure-oriented action of additives. A variety of inorganic functional materials (nickel cobalt hydroxide / oxide) with novel structure were prepared. The structure of two-sided brush was doped with nickel hydroxide cobalt oxide / cobalt trioxide and yolk/shell basic copper sulfate. The morphology and size of the product were controlled by controlling the experimental parameters. On the basis of the preparation of various inorganic functional materials, the effects of additives, reaction temperature and pH environment, the species of precursor and the concentration ratio of precursor to complexing agent on the morphology of the product were studied systematically. The growth mechanism of the products is proposed, which provides a theoretical basis for the controllable synthesis of micro- and nanocrystalline materials. Self-template method was used to realize the surface in-situ conversion of specific inorganic functional materials, and the inorganic functional material @ @ @ MOFs was prepared, which realized the excellent structural properties of MOFs (large specific surface area). Uniform pore size distribution, controllable topology and adjustable pore size) are integrated with the catalytic properties of microparticles. It overcomes the disadvantages of the traditional layer-by-layer self-assembly method in preparing micro-and nano-particles, such as harsh reaction conditions, long period and complex post-processing. Based on the multilevel structure microinorganic functional materials, the application of these materials in the field of catalysis was explored, and the epoxidation of olefin by the above products was studied. The acetal reaction and the molecular oxygen oxidation of alcohol have excellent catalytic effect.
【學(xué)位授予單位】：北京科技大學(xué)
【學(xué)位級(jí)別】：博士
【學(xué)位授予年份】：2015
【分類號(hào)】：TB383

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