光化學(xué)降解是環(huán)境中污染物轉(zhuǎn)化的重要途徑,并且其降解效率較高。眾所周知,Fe（Ⅲ）-多羧酸鹽配合物具有很高的光催化活性,在陽(yáng)光的作用下可經(jīng)歷快速光化學(xué)反應(yīng),生成強(qiáng)氧化性自由基,催化降解有機(jī)污染物。其中,Fe（III）-oxalate、Fe（III）-citrate的光化學(xué)性質(zhì)得到了非常廣泛和透徹的研究。目前,由于氨基多羧酸類配合物（APCAs）的廣泛使用,并且在環(huán)境水體及土壤中均檢出高濃度的APCAs, APCAs的研究引起了科學(xué)家們強(qiáng)烈的興趣。氨基多羧酸類配合物具有多羧酸類配合物相似的化學(xué)行為。已有Fe（III）-EDTA、Fe（III）-NTA光化學(xué)反應(yīng)的報(bào)道。乙二胺二琥珀酸（EDDS）是一種天然的氨基多羧酸,具有非常強(qiáng)的金屬絡(luò)合能力。由于EDDS具有安全和環(huán)境友好性,被提議作為EDTA的替代品用于土壤修復(fù)。EDDS能與鐵形成穩(wěn)定的配合物,有關(guān)Fe（III）-EDDS的物理化學(xué)性質(zhì)已經(jīng)有報(bào)道。但是,對(duì)于Fe（III）-EDDS的光化學(xué)性質(zhì)還未見(jiàn)深入研究。黏土和鐵礦物廣泛存在于各種地質(zhì)體中,它們具有特殊的晶體結(jié)構(gòu)和表面帶電性質(zhì)。作為土壤、大氣、水體漂浮顆粒和沉積物的主要成分之一,這些固... 

【文章來(lái)源】：武漢大學(xué)湖北省 211工程院校 985工程院校 教育部直屬院校

【文章頁(yè)數(shù)】：221 頁(yè)

【學(xué)位級(jí)別】：博士

【文章目錄】：
摘要
ABSTRACT
Acnkowledgements
CATALOGUE
Ⅰ-Introduction
Ⅱ-Bibliography study
    A-Clay and iron oxide minerals in the environment
        A-1 Properties of clay and iron oxides
            A-1-1 The structure and properties of clay
            A-1-2 Iron in clay minerals
            A-1-3 The structure and properties of iron-oxides
        A-2 Photochemical behavior of clay and iron oxide minerals
            A-2-1 Raw clay and iron oxides photocatalysis
            A-2-2 Heterogeneous Photo-Fenton-like catalysis
            A-2-3 Other modified clay/iron oxides photocatalysis
    B-Iron-carboxylate complex
        B-1 EDDS:one of naturally occurring aminopolycarboxylic acids （APCAs）
        B-2 Fe（Ⅲ）-EDDS
        B-3 The photochemistry of iron-carboxyate complex
    C-Endocrine disrupting compounds
        C-1 E2 in the environment
        C-2 E2 degradation
Ⅲ-Materials and methods
    A-Reagents
    B-Preparation of materials and solutions
        B-1-Synthesis of goethite
        B-2-Preparation of stock solutions
        B-3-Preparation of reaction solutions
    C-Irradiation
        C-1-Ferrioxalate actinometry
        C-2-Irradiation with monochromator
        C-3-Irradiation centered at 365 nm
        C-4-Irradiation with Metal halid lamp
    D-Analysis method
        D-1 Minerals
        D-2 Chemicals
            D-2-1 Spectroscopy methods
            D-2-2 Chromatographic methods
            D-2-3 Dosage methods
Ⅳ-Results and discussion
    Ⅳ-A Physicochemical property of E2, Fe（Ⅲ）-EDDS, and Minerals
        A-1 Property of 17β-estradiol
        A-2 Properties of Fe（Ⅲ）-EDDS
            A-2-1 Properties of EDDS
            A-2-2 Properties of Fe（Ⅲ）-EDDS
        A-3 Characterization of the minerals
    Ⅳ-B Photodegradation of E2 in the Fe（Ⅲ）-EDDS complexes solution
        B-1 Quantum yields of·OH formation in Fe（Ⅲ）-EDDS complex
            B-1-1 Effect of Fe（Ⅲ）-EDDS complex concentration
            B-1-2 Effect of pH
            B-1-3 Effect of wavelength
            B-1-4 Effect of oxygen
2+">            B-1-5 Comparison with the aquacomplex Fe（OH）2+

        B-2 The rate constants for the reaction of·OH with E2 and EDDS
        B-3 Photodegradation of E2 in the Fe（Ⅲ）-EDDS complex solutions
            B-3-1 Effect of Fe（Ⅲ）-EDDS concentration
            B-3-2 Effect of pH
            B-3-3 Effect of oxygen
            B-3-4 Effect of iron concentration
        B-4 Photoproducts
        Conclusions
    Ⅳ-C-Photochemical formation of hydroxyl radicals catalyzed by montmorillonite
        C-1 Oxidation of benzene to phenol
        C-2 Effect of clay concentration
        C-3 Effect of initial pH
        C-4 Effect of citrate ions
        C-5 Mechanism of hydroxyl radicals formation
            C-5-1 Charged surface of nano clay
            C-5-2 Free iron ions in clays
            C-5-3 Structural iron in the clays
        Conclusions
    IV-D Degradation of E2 photoinduced by KSF and KSF-EDDS
        D-1 Adsorption of E2 on KSF
        D-2 Photodegradation of E2 in KSF solutions
            D-2-1 Effect of KSF concentration on the degradation of E2
            D-2-2 Effect of pH on the degradation of E2
        D-3 Photodegradation of E2 in KSF solutions in the presence of EDDS
            D-3-1 Effect of KSF concentration on the degradation of E2
            D-3-2 Effect of pH on the photodegradation of E2
            D-3-3 Effect of EDDS concentration on the degradation of E2
            D-3-4 Effect of oxygen on the degradation of E2
            D-3-5 Effect of 2-propanol on the degradation of E2
            D-3-6 Effect of initial concentration of E2
        Conclusions
    IV-E Degradation of E2 photoinduced by NM and NM-EDDS
        E-1 Adsorption of E2 on NM
        E-2 Photodegradation of E2 in the NM suspensions
            E-2-1 Effect of the clay concentration on the photodegradation of E2
            E-2-2 Effect of pH on the photodegradation of E2
        E-3 Photodegradation of E2 in NM-EDDS suspensions
            E-3-1 Effect of NM concentration on the photodegradation of E2
            E-3-2 Effect of EDDS concentration on the degradation of E2
            E-3-3 Effect of pH on the degradation of E2
            E-3-4 Effect of oxygen on the degradation of E2
            E-3-5 Effect of 2-propanol on the photodegradation of E2
            E-3-6 Effect of the initial E2 concentration
        Conclusions
    Ⅳ-F Degradation of E2 photoinduced by Goethite and Goethite-EDDS
        F-1 Adsorption of E2 on Goethite
        F-2 Photodegradation of E2 in the Goethite suspensions
            F-2-1 Effect of Goethite concentration on the photodegradation of E2
            F-2-2 Effect of pH on the photodegradation of E2
        F-3 Photodegradation of E2 in the Goethite-EDDS complex solutions
            F-3-1 Effect of Goethite concentration on the photodegradation of E2
            F-3-2 Effect of EDDS concentration on the photodegradation of E2
            F-3-3 Effect of pH on the photodegradation of E2
            F-3-4 Effect of oxygen on the photodegradation of E2
            F-3-5 Effect of 2-propanol on the photodegradation of E2
            F-3-6 Comparison of the homogenous and heterogeneous reaction
            F-3-7 Effect of initial concentration of E2
        Conclusions
Ⅴ-General conclusions
Ⅵ-APPENDIX
    Ⅵ-1 List of tables
    Ⅵ-2 List of figures
    Ⅵ-3 List of scheme
Ⅶ-REFERENCES
Paper published


【參考文獻(xiàn)】：
期刊論文
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