铁配合物、黏土矿与铁氧化物引发的雌二醇光降解：乙二胺二琥珀酸的影响
发布时间：2021-04-25 06:32
光化学降解是环境中污染物转化的重要途径,并且其降解效率较高。众所周知,Fe（Ⅲ）-多羧酸盐配合物具有很高的光催化活性,在阳光的作用下可经历快速光化学反应,生成强氧化性自由基,催化降解有机污染物。其中,Fe（III）-oxalate、Fe（III）-citrate的光化学性质得到了非常广泛和透彻的研究。目前,由于氨基多羧酸类配合物（APCAs）的广泛使用,并且在环境水体及土壤中均检出高浓度的APCAs, APCAs的研究引起了科学家们强烈的兴趣。氨基多羧酸类配合物具有多羧酸类配合物相似的化学行为。已有Fe（III）-EDTA、Fe（III）-NTA光化学反应的报道。乙二胺二琥珀酸（EDDS）是一种天然的氨基多羧酸,具有非常强的金属络合能力。由于EDDS具有安全和环境友好性,被提议作为EDTA的替代品用于土壤修复。EDDS能与铁形成稳定的配合物,有关Fe（III）-EDDS的物理化学性质已经有报道。但是,对于Fe（III）-EDDS的光化学性质还未见深入研究。黏土和铁矿物广泛存在于各种地质体中,它们具有特殊的晶体结构和表面带电性质。作为土壤、大气、水体漂浮颗粒和沉积物的主要成分之一,这些固...
【文章来源】：武汉大学湖北省 211工程院校 985工程院校 教育部直属院校
【文章页数】：221 页
【学位级别】：博士
【文章目录】：
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
【参考文献】：
期刊论文
[1]Extraction of copper from sewage sludge using biodegradable chelant EDDS[J]. ZHANG Lihua~(1,2) ZHU Zhiliang~(1,*) ZHANG Ronghua~1 ZHENG Chengsong~3 ZHANG Hua~1 QIU Yanling~1 ZHAO Jianfu~1 1.State Key Laboratory of PoUution Control and Resource Reuse,Tongji University,Shanghai 200092,China.2.Department of Chemistry and Biology Engineering,Sanming College,Sanming,Fufian 365004,China 3.Sanming Environment Protection Bureau,Sanming,Fujian 365004,China. Journal of Environmental Sciences. 2008(08)
[2]Chemical composition and surface charge properties of montmorillonite[J]. 刘晓文,胡敏,胡岳华. Journal of Central South University of Technology. 2008(02)
[3]二氧化钛/蒙脱土复合光催化剂制备及对亚甲基蓝的催化降解[J]. 陈小泉,李芳柏,李新军,柳松,古国榜. 土壤与环境. 2001(01)
本文编号：3158891
【文章来源】：武汉大学湖北省 211工程院校 985工程院校 教育部直属院校
【文章页数】：221 页
【学位级别】：博士
【文章目录】：
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-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
【参考文献】：
期刊论文
[1]Extraction of copper from sewage sludge using biodegradable chelant EDDS[J]. ZHANG Lihua~(1,2) ZHU Zhiliang~(1,*) ZHANG Ronghua~1 ZHENG Chengsong~3 ZHANG Hua~1 QIU Yanling~1 ZHAO Jianfu~1 1.State Key Laboratory of PoUution Control and Resource Reuse,Tongji University,Shanghai 200092,China.2.Department of Chemistry and Biology Engineering,Sanming College,Sanming,Fufian 365004,China 3.Sanming Environment Protection Bureau,Sanming,Fujian 365004,China. Journal of Environmental Sciences. 2008(08)
[2]Chemical composition and surface charge properties of montmorillonite[J]. 刘晓文,胡敏,胡岳华. Journal of Central South University of Technology. 2008(02)
[3]二氧化钛/蒙脱土复合光催化剂制备及对亚甲基蓝的催化降解[J]. 陈小泉,李芳柏,李新军,柳松,古国榜. 土壤与环境. 2001(01)
本文编号：3158891
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