本文關鍵詞： 金屬氧化物 納米復合材料 吸附 光催化 高級氧化技術 污水處理 有機染料　出處：《吉林大學》2015年博士論文　論文類型：學位論文

【摘要】：隨著全球經濟和現(xiàn)代化工業(yè)的迅速發(fā)展，水體污染問題日益突出，已經成為當今世界的一大難題。水體污染物尤其是染料廢水的排放對人類和生態(tài)環(huán)境的危害是及其巨大的。因此，有效地處理染料廢水對于保護人類和生態(tài)環(huán)境，以實現(xiàn)可持續(xù)發(fā)展的意義重大。 為了去除廢水中的染料污染物，一些物理，化學，生物方法,例如，吸附，離子交換，化學催化氧化，生物降解，光催化氧化，納米過濾等方法已被廣泛研究。本文所采用的吸附法，光催化氧化法和化學催化氧化法是處理染料廢水行之有效的方法。然而這三種污水處理方法也存在著一些問題，例如：吸附量小、不易回收、光利用率低、穩(wěn)定性差等。 因此，本文在大量現(xiàn)有文獻的基礎上，，制備了幾種新型納米金屬氧化物材料做為高效、環(huán)保的污水處理劑，在一定程度上可以有效的解決之前吸附劑和催化劑的一些弊端。并對制備材料的結構、形貌、生長機理、性能等方面進行系統(tǒng)的研究。本論文以實驗研究為主，結合機理討論，主要研究工作如下: （1）通過簡單的水熱法合成了CoFe2-xMxO4(M=Al3+,In3+和Cu2+)鐵氧體納米晶體，并對它們吸附剛果紅（CR）的能力進行了比較。摻雜后的鐵氧體仍為尖晶石結構，其矯頑力以及吸附能力得到顯著增強。與純鈷鐵氧體的磁學性質相比，我們推測Al3+占據(jù)了四面體空隙A位，In3+和Cu2+占據(jù)了八面體空隙B位。物理吸附是其主要的吸附性質。首次提出磁性材料的矯頑場比其表面積對其吸附能力有更重要的影響。為了解釋矯頑場與吸附能力之間的關系，我們提出了水磁化機理。所制備的CoFe2-xMxO4鐵氧體具有較強的磁性，可通過外加磁場進行磁分離，把污染物從水體中快速分離出來。在所有對比樣品中，矯頑力最大（達2014.2Oe）的In3對CR具有最高的吸附能力（605.4mg g1）。 （2）結合簡便的水熱法和適度的超聲制備了一系列的磁性可回收MnO2薄片包覆Fe3O4納米復合材料。光催化研究表明這種MnO2/Fe3O4納米復合材料在紫外-可見光的照射條件下對降解亞甲基藍溶液表現(xiàn)出優(yōu)秀的光催化效率和穩(wěn)定性。磁性測試證明MnO2/Fe3O4納米復合材料擁有鐵磁性質，這就使得它在光催化反應后可以通過一個簡單的外加磁場來實現(xiàn)回收再利用。它良好的耐酸性和可回收性使其成為潛在的具有重要應用前景的光催化劑。 （3）采用簡單的一步水熱法制備了Mn3O4/石墨烯納米復合材料。這種復合材料具有尺寸分布窄、分散性好的特點。我們仔細研究了它在異質催化過硫酸氫鹽（PMS）去降解一種偶氮染料（橙黃II）方面的應用。相對于單獨的Mn3O4納米顆粒或者石墨烯納米片而言，Mn3O4/石墨烯納米復合材料由于之間存在協(xié)同效應使之具有更高的催化活性。在250ml濃度為30mg L1的橙黃II溶液中，加入Mn3O4/石墨烯納米復合材料（0.05g L1）和PMS（15g L1），90min可100%降解橙黃II染料。另外，我們分析了Mn3O4/石墨烯納米復合材料/PMS體系降解橙黃II染料的機理。同時，利用電感耦合等離子體質譜分析得出錳離子的析出量是很低的。通過穩(wěn)定性試驗，在四次連續(xù)循環(huán)后，這種復合材料仍然表現(xiàn)出良好的穩(wěn)定性。
[Abstract]:With the rapid development of the global economy and modern industry, water pollution problems have become increasingly prominent, has become a big problem in the world today. Water pollutants especially dye wastewater emissions harmful to human and ecological environment is huge. Therefore, effective treatment of dye wastewater for the protection of human and ecological environment, to achieve sustainable development of great significance.
In order to dye pollutants, the removal of some physical, chemical and biological methods, such as adsorption, ion exchange, chemical oxidation, biological degradation, photocatalytic oxidation, nano filtering methods have been widely studied. The adsorption method used in this paper, photocatalytic oxidation and chemical oxidation method is effective in treating dye however, these three kinds of wastewater. Wastewater treatment methods also exist some problems, such as adsorption capacity, easy recovery, low light utilization rate, poor stability and so on.
Therefore, based on a large number of existing literature on the preparation of several new nano metal oxide materials as efficient, environment-friendly sewage treatment agent, can effectively solve the drawbacks of adsorbent and catalyst in a certain extent. And the structure of the material on the morphology, growth mechanism, performance and other aspects system research. In this paper, experimental research, the binding mechanism is discussed, the main research work is as follows:
(1) CoFe2-xMxO4 was synthesized by a simple hydrothermal method (M=Al3+, In3+ and Cu2+) ferrites nanocrystals, and the adsorption of Congo red (CR) ability were compared. The doped ferrite is spinel structure, the coercivity and the adsorption capacity was significantly enhanced. Compared with the the magnetic properties of cobalt ferrite, we speculate that Al3+ occupy the tetrahedral A, In3+ and Cu2+ accounted for eight of the surface of body clearance B. Physical adsorption is the main adsorption properties of magnetic materials. First proposed the coercive field than the surface area of the adsorption capacity of the more important influence to the relationship. Interpretation of the coercive field and adsorption capacity, we put forward the mechanism of water magnetization. CoFe2-xMxO4 ferrite prepared with strong magnetic, magnetic separation can be carried out by the external magnetic field, the contaminant separated quickly from the water. In all contrast sample, the coercivity of the The In3 of large (up to 2014.2Oe) has the highest adsorption capacity for CR (605.4mg G1).
(2) a series of magnetic Recyclable sheet MnO2 coated Fe3O4 nano composite materials were prepared by ultrasonic hydrothermal method is simple and modest. The research of photocatalytic show that the radiation condition of this MnO2/Fe3O4 nano composite material in ultraviolet visible light degradation of methylene blue solution showed excellent photocatalytic efficiency and stability. The test has proved the ferromagnetic magnetic properties of MnO2/Fe3O4 nano composite material, which makes it through a simple magnetic field to achieve the recycling in the photocatalytic reaction. Its good acid resistance and Recyclable of the photocatalyst has important potential application prospect.
(3)閲囩敤綆

本文編號：1456307