【摘要】：硅酸鹽是固體地球的主要組成成分,大自然中的硅酸鹽主要以島狀、鏈狀、網(wǎng)狀和層狀的形式存在,其中層狀硅酸鹽以其獨(dú)有的層狀孔道結(jié)構(gòu)而吸引了廣泛的研究。硅酸鹽材料由于其制備簡(jiǎn)單、來(lái)源豐富、價(jià)格便宜、及獨(dú)特的多孔結(jié)構(gòu)在吸附、催化、藥物等領(lǐng)域得到了廣泛應(yīng)用。但其固有的一些性能缺陷如導(dǎo)電性較差等又限制了實(shí)際的應(yīng)用。納米顆粒合成技術(shù)的發(fā)展使得各種形貌的硅酸鹽制備得以實(shí)現(xiàn),也便于將硅酸鹽和其他材料進(jìn)行復(fù)合以克服其缺點(diǎn),進(jìn)而發(fā)揮協(xié)同效應(yīng)。因此,本論文設(shè)計(jì)合成了一系列具有多層次結(jié)構(gòu)的層狀硅酸鹽納米復(fù)合材料,從組分和結(jié)構(gòu)上對(duì)硅酸鹽進(jìn)行優(yōu)化,提高其在水處理和鋰離子電池中的性能。例如,一維的碳納米管／層狀硅酸鎳的同軸結(jié)構(gòu),二維的硅酸鎂／氧化石墨烯三明治結(jié)構(gòu),三維的氧化鎂／介孔二氧化硅納米球核殼結(jié)構(gòu)。本課題的創(chuàng)新點(diǎn)主要在于：1)首次研究了同軸結(jié)構(gòu)的硅酸鎳／碳納米管在鋰離子電池負(fù)極當(dāng)中的應(yīng)用。通過(guò)引入碳納米管,克服了硅酸鎳導(dǎo)電性能差的缺點(diǎn),提高了復(fù)合材料的電化學(xué)性能。2)首次合成了三明治結(jié)構(gòu)的硅酸鎂／石墨烯,并對(duì)其重金屬離子和染料的吸附能力進(jìn)行了研究。3)首次合成了硅酸銀／氧化石墨烯和硅酸銀／碳納米管,并對(duì)其光催化性能進(jìn)行了比較和研究。1、使用碳納米管為物理模板和導(dǎo)電劑,合成了一維同軸結(jié)構(gòu)的硅酸鎳@碳納米管復(fù)合材料。層狀硅酸鎳納米片的層間距約為0.74納米,不僅有利于鋰離子的嵌入脫嵌,而且可以實(shí)現(xiàn)鈉離子嵌入脫嵌。碳納米管使復(fù)合材料的導(dǎo)電性能得以提升,有助于電子和鋰離子的傳輸；其空心管狀結(jié)構(gòu)也為循環(huán)充放電過(guò)程中鋰離子嵌入和脫嵌提供了緩沖空間,有利于循環(huán)穩(wěn)定性能的提高。作為鋰離子電池負(fù)極,硅酸鎳@碳納米管在電流密度為50 mA/g的條件下,50圈的循環(huán)充放電之后,仍能維持489 mA h/g的可逆容量,遠(yuǎn)高于純硅酸鎳納米管的107mAh/g,亦高于文獻(xiàn)報(bào)道的其他純硅酸鹽材料的可逆容量。2、通過(guò)水熱法制備二維三明治結(jié)構(gòu)的硅酸鎂/石墨烯復(fù)合材料,研究其對(duì)有機(jī)染料和重金屬離子的吸附性能。BET比表面積達(dá)到450m2/g。復(fù)合材料對(duì)亞甲基藍(lán)染料和鉛離子的吸附符合Langmuir吸附模型,對(duì)亞甲基藍(lán)和鉛離子的最大吸附量分別為424 mg/g和416mg/g,是純硅酸鎂材料的271%和126%。石墨烯不僅作為負(fù)載基體有效地分散硅酸鎂納米片結(jié)構(gòu),提高了復(fù)合材料的比表面積；其自身具有的大量含氧官能團(tuán)也為復(fù)合材料提供了更多的吸附位點(diǎn),微米尺寸片層結(jié)構(gòu)也使吸附劑可以在重力作用下進(jìn)行有效分離。除了保留各組分優(yōu)異物理化學(xué)特性,復(fù)合材料還表現(xiàn)出良好的協(xié)同作用,使機(jī)械穩(wěn)定性和吸附性能得以提高。該復(fù)合材料在水污染處理領(lǐng)域有較好的應(yīng)用潛力。3、合成了三維核殼結(jié)構(gòu)的氧化鎂@介孔二氧化硅復(fù)合材料。在由氧化鎂納米顆粒組裝形成的多孔微球外包覆一層介孔二氧化硅的外殼,不僅提高了氧化鎂的機(jī)械穩(wěn)定性,以防止在機(jī)械攪拌過(guò)程中結(jié)構(gòu)被破壞；同時(shí)還為溶液中污染物質(zhì)的擴(kuò)散提供了濃度梯度和更好的傳質(zhì)效果。合成的核殼結(jié)構(gòu)復(fù)合材料對(duì)鉛離子和亞甲基藍(lán)分別達(dá)到了3155毫克/克和420毫克/克的吸附容量,遠(yuǎn)高于純氧化鎂對(duì)鉛離子和亞甲基藍(lán)的2454毫克/克和61毫克/克的吸附容量。4、首次制備硅酸銀/碳納米管以及硅酸銀/氧化石墨烯復(fù)合材料,并對(duì)這兩種材料對(duì)有機(jī)染料的可見(jiàn)光催化降解性能進(jìn)行了比較。不同碳材料添加含量使復(fù)合材料的形貌和性能發(fā)生較大變化。對(duì)碳納米管而言,少量加入碳納米管即可明顯提高光催化效率,但進(jìn)一步增加碳納米管添加量反而會(huì)使光催化效率有所降低;對(duì)氧化石墨烯而言,亞甲基藍(lán)去除率隨著氧化石墨烯含量的增加而增加。
[Abstract]:Silicate is the main component of solid earth. The silicates in nature are mainly in the form of island, chain, reticulate, and stratified forms, in which the layered silicate attracts extensive research with its unique layered pore structure. Silicate materials are simple, rich, cheap, and unique porous structure. It has been widely used in the fields such as catalysis and medicine, but some of its inherent performance defects, such as poor conductivity, have restricted practical applications. The development of nano particle synthesis technology makes the preparation of various forms of silicate can be realized, and the silicate and other materials are compounded to overcome their shortcomings and thus play synergy. Therefore, a series of layered silicate nanocomposites have been designed and synthesized in this paper. The composition and structure of silicates are optimized to improve their performance in water treatment and lithium ion batteries. For example, the coaxial structure of one dimensional carbon nanotubes / layered nickel silicate, two dimensional magnesium silicate / graphite oxide The structure of the sandwich, three dimensional Magnesium Oxide / mesoporous silica nanospheres structure. The main innovation of this topic lies in: 1) the application of the coaxial structure of nickel silicate / carbon nanotubes in the anode of lithium ion battery for the first time. By introducing the carbon nanotube, the defects of poor conductivity of nickel silicate were overcome and the composite material was improved. The electrochemical properties of the material.2) the sandwich structure of magnesium silicate / graphene was synthesized for the first time. The adsorption capacity of heavy metal ions and dyes was studied for the first time..3) silver / graphene oxide and silver / carbon nanotubes were synthesized for the first time. The photocatalytic properties of them were compared and studied by.1, and the carbon nanotubes were used as the physical template. The interlayer spacing of the layered nickel silicate nanoplates is about 0.74 nanometers, which is not only conducive to the insertion of lithium ions, but also to embed and embed with sodium ions. The conductivity of the nanotube can be enhanced and the transmission of the electrons and lithium ions is helpful. The hollow tubular structure also provides a buffer space for the insertion and removal of lithium ion in the cycle charge and discharge process, which is beneficial to the improvement of the cyclic stability. As a negative electrode of lithium ion battery, under the condition of the current density of 50 mA/g, the nickel dioxide @ carbon nanotube can still maintain the reversible capacity of 489 mA h/g after the cycle of charging and discharging. 107mAh/g, which is higher than pure nickel silicate nanotube, is also higher than the reversible capacity.2 of other pure silicate materials reported in the literature. The two-dimension sandwich structure of magnesium silicate / graphene composite was prepared by hydrothermal method. The adsorption properties of the organic dyes and heavy metal ions were studied by the.BET specific surface area of the composite material for methylene blue dyeing. The adsorption of material and lead ions conforms to the Langmuir adsorption model. The maximum adsorption capacity for methylene blue and lead ions is 424 mg/g and 416mg/g respectively. It is 271% and 126%. graphene, which is a pure magnesium silicate material, not only effectively disperses magnesium silicate nanostructure as the load matrix, but also improves the specific surface area of the composite. The oxygen functional groups also provide more adsorption sites for the composites, and the micrometer layer structure also enables the adsorbents to be effectively separated under the action of gravity. In addition to retaining the excellent physical and chemical properties of each component, the composite also exhibits good synergy, which makes the mechanical stability and adsorption properties improved. The field of water pollution treatment has a good application potential.3, which has synthesized a three dimensional nuclear shell structure of Magnesium Oxide @ mesoporous silica composite. The outer shell of a porous silica coated with a porous microsphere assembled by Magnesium Oxide nanoparticles not only improves the mechanical stability of Magnesium Oxide, so as to prevent the structure of the mechanical agitation in the process of mechanical agitation. It also provides a concentration gradient and a better mass transfer effect for the diffusion of contaminants in the solution. The synthetic nuclear shell structure composite has a capacity of 3155 mg / g and 420 mg / g respectively for lead and methylene blue, which is far higher than that of pure Magnesium Oxide for 2454 mg / g and 61 mg of the lead and methylene blue. The adsorption capacity of.4, silver / carbon nanotubes and silver / graphene silicate composites were prepared for the first time. The visible photocatalytic degradation performance of these two materials for organic dyes was compared. The morphology and properties of the composites changed greatly with the addition of different carbon materials. Nanotube can obviously improve the photocatalytic efficiency, but the addition of carbon nanotubes will reduce the photocatalytic efficiency. For graphene oxide, the removal rate of methylene blue increases with the increase of the content of graphene oxide.
【學(xué)位授予單位】：北京化工大學(xué)
【學(xué)位級(jí)別】：博士
【學(xué)位授予年份】：2016
【分類號(hào)】：TB332;TQ170.1

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