多氯代二苯并二惡英和多氯代二苯并呋喃（PCDD/F）,統(tǒng)稱為“二惡英”,是持久性有機(jī)污染物（POPs）,幾乎出現(xiàn)在所有熱力系統(tǒng)中。其中,城市固體廢物焚燒爐（MSWIs）是其主要源頭之一。在焚燒爐后燃燒區(qū),不完全燃燒產(chǎn)物（PICs）、氯源、催化金屬和有機(jī)前體可以通過一系列的化學(xué)反應(yīng)生成PCDD/F。異相催化生成的兩種機(jī)制,即從頭合成和前驅(qū)物合成,已被廣泛研究并被認(rèn)為是PCDD/F生成的主要途徑,但是兩者的相關(guān)重要性仍然存在爭議。本文圍繞研磨和非研磨模擬飛灰樣品中PCDD/F的生成特性,進(jìn)行了一系列實(shí)驗(yàn)。主要結(jié)果概括如下:（1）模擬飛灰（Modelflyash,MFA）樣品由二氧化硅、氯化鈉和活性炭組成,摻雜金屬氯化物（0.2wt%Cu,Cr,Fe,ZnandCa）,以300rpm轉(zhuǎn)速進(jìn)行高強(qiáng)度球磨（球磨時(shí)間分別為1h和8h）。采用熱重分析（TGA）和差示掃描量熱法（DSC）（溫度:25℃～600℃）研究氧氣氣氛中研磨對(duì)MFA的影響。研磨1h和8h后,TG曲線顯示樣品重量略有增加,而測量樣品經(jīng)研磨處理后的物理增重也可以支持這一結(jié)果。MFA樣品在404.4℃顯示有放熱峰。拉曼光譜分析表明,研... 

【文章來源】：浙江大學(xué)浙江省 211工程院校 985工程院校 教育部直屬院校

【文章頁數(shù)】：148 頁

【學(xué)位級(jí)別】：博士

【文章目錄】：
Acknowledgements
摘要
Abstract
Chapter 1. Literature Review
    1.1 Introduction
    1.2 Properties, sources and formation of PCDD/F
        1.2.1 Properties of PCDD/F
        1.2.2 Sources of PCDD/F
        1.2.3 Formation of PCDD/F
    1.3 Potential Precursors for PCDD/F Formation
    1.4 Research Objectives
Chapter 2. High intensity ball milling of metal doped model fly ash
    2.1 Introduction
    2.2 Materials and methods
        2.2.1 Chemicals
        2.2.2 Preparation of MFA
        2.2.3 Characteristics of original materials
        2.2.4 Milling of MFA
        2.2.5 Analytical methods
        2.2.6 Clean up and analysis of PCDD/F
    2.3 Results and Discussion
        2.3.1 Physical weight gain
        2.3.2 Composition of MFA samples
        2.3.3 Specific surface and size
        2.3.4 SEM/EDX mapping
        2.3.5 Crystallinity
        2.3.6 TGA/DSC
        2.3.7 Raman Spectroscopy
        2.3.8 PCDD and PCDF (PCDD/F) output
    2.4 Conclusion
Chapter 3. De novo formation of selected compounds from milled model fly ash
    3.1 Introduction
    3.2 Materials and methods
        3.2.1 Chemicals
        3.2.2 MFA sample preparation and milling treatment and analytical methods
        3.2.3 Experimental Procedure
        3.2.4 Sampling and analysis of PCDD/F, PCB, CP, CBz and PAH
    3.3 Results and discussion
        3.3.1 Characteristics of fly ash after 0, 1,and 8 h of milling
        3.3.2 De novo synthesis of organic pollutants
        3.3.3 Relationship between I-TEQ reduction of all organics with milling time
        3.3.4 Degrees of chlorination
        3.3.5 Resulting isomer patterns of PCDD/F in samples with 0, 1 and 8 hmilling
    3.4 Conclusion
Chapter 4. PCDD/F-formation in milled fly ash: metal chloride catalysis
    4.1 Introduction
    4.2 Materials and Methods
        4.2.1 MFA Preparation and Experimental Procedure
    4.3 Results and Discussion
        4.3.1 PCDD/F formation during de novo tests
        4.3.2 The PCDF/PCDD-ratio
        4.3.3 Homologue Profiles
        4.3.4 2,3,7,8-PCDD/F profiles
        4.3.5 Isomer distribution
        4.3.6 Discussion
    4.4 Conclusion
Chapter 5. Effect of milling time on PCDD/F and PCB yield from fly ash
    5.1 Introduction
    5.2 Materials and Methods
        5.2.1 MFA Preparation and Experimental Procedure
        5.2.2 TGA/DSC of MFA
    5.3 Results and Discussion
        5.3.1 TGA/DSC
        5.3.2 PCDD/F output in milled (0, 1,2, 4 and 8 h) MFA
        5.3.3 PCB output in milled (0, 1,2,4 and 8h)MFA
    5.4 Conclusion
Chapter 6. PCDD/F formation from 2,4,6-trichlorophenol added model fly ash
    6.1 Introduction
    6.2 Materials and methods
        6.2.1 Model fly ash preparation
        6.2.2 Experimental procedure
    6.3 Results and Discussion
        6.3.1 Formation of PCDD/F (P=4-8)
        6.3.2 The ratio PCDF/PCDD
        6.3.3 Average chlorination degree
        6.3.4 Homologues and HAEGENMIER profile
        6.3.5 Monitoring individual isomers
    6.4 Conclusion
Chapter 7. Conclusion
References
List of Abbreviations
Curriculum Vitae


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