模拟飞灰中二噁英的从头合成
发布时间：2021-08-27 09:51
多氯代二苯并二恶英和多氯代二苯并呋喃（PCDD/F）,统称为“二恶英”,是持久性有机污染物（POPs）,几乎出现在所有热力系统中。其中,城市固体废物焚烧炉（MSWIs）是其主要源头之一。在焚烧炉后燃烧区,不完全燃烧产物（PICs）、氯源、催化金属和有机前体可以通过一系列的化学反应生成PCDD/F。异相催化生成的两种机制,即从头合成和前驱物合成,已被广泛研究并被认为是PCDD/F生成的主要途径,但是两者的相关重要性仍然存在争议。本文围绕研磨和非研磨模拟飞灰样品中PCDD/F的生成特性,进行了一系列实验。主要结果概括如下:（1）模拟飞灰（Modelflyash,MFA）样品由二氧化硅、氯化钠和活性炭组成,掺杂金属氯化物（0.2wt%Cu,Cr,Fe,ZnandCa）,以300rpm转速进行高强度球磨（球磨时间分别为1h和8h）。采用热重分析（TGA）和差示扫描量热法（DSC）（温度:25℃～600℃）研究氧气气氛中研磨对MFA的影响。研磨1h和8h后,TG曲线显示样品重量略有增加,而测量样品经研磨处理后的物理增重也可以支持这一结果。MFA样品在404.4℃显示有放热峰。拉曼光谱分析表明,研...
【文章来源】：浙江大学浙江省 211工程院校 985工程院校 教育部直属院校
【文章页数】：148 页
【学位级别】：博士
【文章目录】：
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
【参考文献】：
期刊论文
[1]两种典型生活垃圾焚烧炉烟气中二噁相态分布特征[J]. 李艳静,张素坤,冯桂贤,任明忠,张漫雯,许振成,张入元,完颜华. 中国环境科学. 2011(10)
[2]Characterization of mechanochemical treated fly ash from a medical waste incinerator[J]. Zheng Peng1,2,Qiong Ding1,Yangzhao Sun1,Chen Jiang1,Xinhua Gao1,Jianhua Yan2,1.Foreign Economic Cooperation Offce,Ministry of Environmental Protection,Beijing 100035,China2.State Key Laboratory of Clean Energy Utilization,Institute for Thermal Power Engineering,Zhejiang University,Hangzhou 310027,China. Journal of Environmental Sciences. 2010(10)
[3]Mechanochemical decomposition of pentachlorophenol by ball milling[J]. WEI Yinglei, YAN Jianhua, LU Shengyong, LI XiaodongState Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310027, China.. Journal of Environmental Sciences. 2009(12)
本文编号：3366129
【文章来源】：浙江大学浙江省 211工程院校 985工程院校 教育部直属院校
【文章页数】：148 页
【学位级别】：博士
【文章目录】：
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
【参考文献】：
期刊论文
[1]两种典型生活垃圾焚烧炉烟气中二噁相态分布特征[J]. 李艳静,张素坤,冯桂贤,任明忠,张漫雯,许振成,张入元,完颜华. 中国环境科学. 2011(10)
[2]Characterization of mechanochemical treated fly ash from a medical waste incinerator[J]. Zheng Peng1,2,Qiong Ding1,Yangzhao Sun1,Chen Jiang1,Xinhua Gao1,Jianhua Yan2,1.Foreign Economic Cooperation Offce,Ministry of Environmental Protection,Beijing 100035,China2.State Key Laboratory of Clean Energy Utilization,Institute for Thermal Power Engineering,Zhejiang University,Hangzhou 310027,China. Journal of Environmental Sciences. 2010(10)
[3]Mechanochemical decomposition of pentachlorophenol by ball milling[J]. WEI Yinglei, YAN Jianhua, LU Shengyong, LI XiaodongState Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310027, China.. Journal of Environmental Sciences. 2009(12)
本文编号：3366129
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