Study on the Stability and Efficiency of Supported Catalysts
发布时间：2021-08-08 05:46
清洁安全的水资源是除空气以外的最重要的资源,然而由于人口的过度增长、城市化发展、工业以及其他行业对水资源的利用,导致水的持续利用成为一个很大的挑战。水污染问题很令人担忧,因为全球已经有11亿人面临饮用水不足的问题,而25亿人甚至使用污染水。为了解决这个问题,已经有很多传统的和先进的处理系统应用于水处理。然而,由于废水的复杂的化学性质,还没有一种处理技术能将难降解污染物高效地处理成法律可以接受的水平。双氧水是一种资源丰富、清洁、具有活性的氧化剂,这使它与具有缓冲能力的碳酸氢盐的联合使用处理废水具有很强的吸引力。本文中,我们应用碳酸氢盐活化过氧化氢的理念,主要集中于对已应用的处理方法在稳定和效率上的提高和改进。我们使用固定床降解氯酚和染料,评估这两项参数（效率和稳定性）。结果表明,碳酸氢盐不仅可以提高降解效率也可以使负载催化剂更加稳定,这对于绿色、高效和可持续的废水处理系统的发展有很大的帮助。本论文的第二部分,我们集中于使用碳酸氢盐活化双氧水体系在负载催化剂的条件下,降解了4一氯苯酚,2,4一二氯苯酚,2,4,6一三氯苯酚和苯酚这四个模型化合物。针对于对目标化合物的降解率、化学需氧量（CO...
【文章来源】：华中科技大学湖北省 211工程院校 985工程院校 教育部直属院校
【文章页数】：155 页
【学位级别】：博士
【文章目录】：
摘要
Abstract
1 Introduction
1.1 Water Pollution
1.2 Water Pollution with Organic Compounds
1.3 Conventional Technologies and Water Pollution
1.4 Advanced Oxidation Process (AOPs)
1.4.1 Catalytic Wet Hydrogen Peroxide Oxidation (CWPOs) Appeared to be the Best Solution
1.4.2 Application and Limitations of Fenton's Based Technology in Waste Water Treatment
1.4.3 Need for Searching an Alternative of Fenton's like Reagent in Waste Water Treatment
1.4.4 Application of Heterogeneous Catalyst in the Treatment of Wastewater
1.5 Hydrotalcite Based Supported Catalyst
1.5.1 Structure of Hydrotalcite
1.5.2 Layered Double Hydrotacites as Catalyst
1.5.3 Metals Exchanged Zeolites Based Supported Catalyst
1.6 Challenges in Catalytic Waste Water Treatments
1.7 Bicarbonate Activation of Hydrogen Peroxide system (BAP)
1.7.1 Role of Bicarbonate Activation of Hydrogen Peroxide (BAP) in Wastewater (M/HCO_3~-/H_2O_2 system)
1.7.2 Future of BAP System in the Development of Green Treatment System
1.8 Target Strategy and Content
1.9 Research Aim and Conclusion
References
2 Degradation of Chlorophenols by Supported Co-Mg-Al LDH BasedCatalyst in BAP System
2.1 Experimental Section
2.1.1 Chemicals and Reagents
2.1.2 Preparation of Powdered Catalyst for Bench Experiments (CoMgAl-HTs and MgAl-HTs)
2.1.3 Preparation of Supported Catalyst for Fixed Bed Experiments (CoMgAl-SHTs)
2.1.4 Pollutants Degradation in Bench Test Experiments
2.1.5 Pollutants Degradation in Fixed Bed Experiments
2.1.6 Analyses
2.2 Results and Discussion
2.2.1 Characterization of powdered catalysts
2.2.2 Activity of Catalyst/HCO_3~-/H_2O_2 System on Bench Level
2.3 Mechanistic Discussions
2.4 Application of Catalyst in Fixed Bed Reactor
2.5 Conclusions
References
3 Controlled Leaching with Prolonged Activity for Co-LDH SupportedCatalyst during Treatment of Organic Dyes Using BAP System
3.1 Experimental section
3.1.1 Chemical and Reagents
3.1.2 Preparation of Powdered Catalyst for Bench Expeirments (CoMgAl-HTs andMgAI-HTs)
3.1.3 Preparation of Catalyst for Fixed Bed
3.1.4 Degradation of Methylene Orange and Methylene Blue in Bench Experiment
3.1.5 Degradation of Methylene Blue in Fixed Bed Experiments
3.1.6 Procedure of Analysis
3.2 Result and Discussion
3.2.1 Catalyst Characterizations
3.3 Catalytic Performance of CoMgAl Catalysts in the Degradation of Methyl Orange
3.4 Effect of Operating Parameters
3.4.1 Effect of Hydrogen Peroxide
3.4.2 Effect of Sodium Bicarbonate
3.4.3 Effect of Catalyst Dose
3.4.4 Effect of Solution pH
3.4.5 Influence of Anions
3.4.6 Role of Bicarbonate in Controlling Catalyst Leaching
3.5 Stability and Life of CoMgAl-Na-Y Supported Catalyst in Fixed Bed Glass Reactor
3.6 Mechanistic Study for the Presence of Main Reactive Oxygen Species(ROS)
3.7 Conclusion
References
4 Effect of Cu on Promoting the Catalyst Activity of CoMgAl LDH BasedCatalyst Using Chlorophenols as Target Compounds
4.1 Experimental Section
4.1.1 Chemical and Reagents
4.1.2 Preparation of Powdered Catalyst for Bench Experiments
4.1.3 Catalyst Characterization Techniques
4.1.4 Degradation and Analysis of CPs (chlorophenols) During Bench Expeirment
4.1.5 Procedure for Monitoring the Stability of the Powdered Catalyst
4.2 Results and Discussion
4.2.1 Catalyst Characterization
4.3 Catalytic Performance
4.3.1 Influence of Different Metals on the Activity of MgAl Based Catalyst
4.3.2 Effect of Cu on Promotion CP Degradation with CuCoMgAl Catalyst Derived from CoMgAl Based LDH Catalyst
4.3.3 Redox Properties of CuCoMgAl Catalyst
4.3.4 Stability of CuCoMgAl Catalyst
4.3.5 Activity of CuCoMgAl Catalyst in Bicarbonate Activation of Hydrogen Peroxide System
4.3.6 Effect of CP Concentration on the Activity of the Catalyst...115
4.3.7 Effect of H_2O_2 on the Degradation of 4-Chlorophenol
4.3.8 Effect of Bicarbonate on the Degradation of 4-CP
4.3.9 Effect of Temperature on the Degradation of 4-CP
4.3.10 Effect of Solution pH on Degradation of CP
4.3.11 Activity of Catalyst for Other Organic Compounds
4.4 Mechanistic Study
4.4.1 Detection of Free Radicals
4.4.2 Possible Reaction Mechanism
4.5 Conclusion
References
5 Project Summary and Future Out Look
5.1 Project Summary
5.2 Future Out Look
Acknowledgement
List of Articles Published During PhD
【参考文献】：
期刊论文
[1]Novel Co-Mg-Al-Ti-O catalyst derived from hydrotalcite-like compound for NO storage/decomposition[J]. Jie Cheng, Xiaoping Wang, Chunyan Ma , Zhengping Hao Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China.. Journal of Environmental Sciences. 2012(03)
[2]Evaluation of media for simultaneous enumeration of total coliform and Escherichia coli in drinking water supplies by membrane filtration techniques[J]. FIESSEL Wanda. Journal of Environmental Sciences. 2008(03)
本文编号：3329353
【文章来源】：华中科技大学湖北省 211工程院校 985工程院校 教育部直属院校
【文章页数】：155 页
【学位级别】：博士
【文章目录】：
摘要
Abstract
1 Introduction
1.1 Water Pollution
1.2 Water Pollution with Organic Compounds
1.3 Conventional Technologies and Water Pollution
1.4 Advanced Oxidation Process (AOPs)
1.4.1 Catalytic Wet Hydrogen Peroxide Oxidation (CWPOs) Appeared to be the Best Solution
1.4.2 Application and Limitations of Fenton's Based Technology in Waste Water Treatment
1.4.3 Need for Searching an Alternative of Fenton's like Reagent in Waste Water Treatment
1.4.4 Application of Heterogeneous Catalyst in the Treatment of Wastewater
1.5 Hydrotalcite Based Supported Catalyst
1.5.1 Structure of Hydrotalcite
1.5.2 Layered Double Hydrotacites as Catalyst
1.5.3 Metals Exchanged Zeolites Based Supported Catalyst
1.6 Challenges in Catalytic Waste Water Treatments
1.7 Bicarbonate Activation of Hydrogen Peroxide system (BAP)
1.7.1 Role of Bicarbonate Activation of Hydrogen Peroxide (BAP) in Wastewater (M/HCO_3~-/H_2O_2 system)
1.7.2 Future of BAP System in the Development of Green Treatment System
1.8 Target Strategy and Content
1.9 Research Aim and Conclusion
References
2 Degradation of Chlorophenols by Supported Co-Mg-Al LDH BasedCatalyst in BAP System
2.1 Experimental Section
2.1.1 Chemicals and Reagents
2.1.2 Preparation of Powdered Catalyst for Bench Experiments (CoMgAl-HTs and MgAl-HTs)
2.1.3 Preparation of Supported Catalyst for Fixed Bed Experiments (CoMgAl-SHTs)
2.1.4 Pollutants Degradation in Bench Test Experiments
2.1.5 Pollutants Degradation in Fixed Bed Experiments
2.1.6 Analyses
2.2 Results and Discussion
2.2.1 Characterization of powdered catalysts
2.2.2 Activity of Catalyst/HCO_3~-/H_2O_2 System on Bench Level
2.3 Mechanistic Discussions
2.4 Application of Catalyst in Fixed Bed Reactor
2.5 Conclusions
References
3 Controlled Leaching with Prolonged Activity for Co-LDH SupportedCatalyst during Treatment of Organic Dyes Using BAP System
3.1 Experimental section
3.1.1 Chemical and Reagents
3.1.2 Preparation of Powdered Catalyst for Bench Expeirments (CoMgAl-HTs andMgAI-HTs)
3.1.3 Preparation of Catalyst for Fixed Bed
3.1.4 Degradation of Methylene Orange and Methylene Blue in Bench Experiment
3.1.5 Degradation of Methylene Blue in Fixed Bed Experiments
3.1.6 Procedure of Analysis
3.2 Result and Discussion
3.2.1 Catalyst Characterizations
3.3 Catalytic Performance of CoMgAl Catalysts in the Degradation of Methyl Orange
3.4 Effect of Operating Parameters
3.4.1 Effect of Hydrogen Peroxide
3.4.2 Effect of Sodium Bicarbonate
3.4.3 Effect of Catalyst Dose
3.4.4 Effect of Solution pH
3.4.5 Influence of Anions
3.4.6 Role of Bicarbonate in Controlling Catalyst Leaching
3.5 Stability and Life of CoMgAl-Na-Y Supported Catalyst in Fixed Bed Glass Reactor
3.6 Mechanistic Study for the Presence of Main Reactive Oxygen Species(ROS)
3.7 Conclusion
References
4 Effect of Cu on Promoting the Catalyst Activity of CoMgAl LDH BasedCatalyst Using Chlorophenols as Target Compounds
4.1 Experimental Section
4.1.1 Chemical and Reagents
4.1.2 Preparation of Powdered Catalyst for Bench Experiments
4.1.3 Catalyst Characterization Techniques
4.1.4 Degradation and Analysis of CPs (chlorophenols) During Bench Expeirment
4.1.5 Procedure for Monitoring the Stability of the Powdered Catalyst
4.2 Results and Discussion
4.2.1 Catalyst Characterization
4.3 Catalytic Performance
4.3.1 Influence of Different Metals on the Activity of MgAl Based Catalyst
4.3.2 Effect of Cu on Promotion CP Degradation with CuCoMgAl Catalyst Derived from CoMgAl Based LDH Catalyst
4.3.3 Redox Properties of CuCoMgAl Catalyst
4.3.4 Stability of CuCoMgAl Catalyst
4.3.5 Activity of CuCoMgAl Catalyst in Bicarbonate Activation of Hydrogen Peroxide System
4.3.6 Effect of CP Concentration on the Activity of the Catalyst...115
4.3.7 Effect of H_2O_2 on the Degradation of 4-Chlorophenol
4.3.8 Effect of Bicarbonate on the Degradation of 4-CP
4.3.9 Effect of Temperature on the Degradation of 4-CP
4.3.10 Effect of Solution pH on Degradation of CP
4.3.11 Activity of Catalyst for Other Organic Compounds
4.4 Mechanistic Study
4.4.1 Detection of Free Radicals
4.4.2 Possible Reaction Mechanism
4.5 Conclusion
References
5 Project Summary and Future Out Look
5.1 Project Summary
5.2 Future Out Look
Acknowledgement
List of Articles Published During PhD
【参考文献】：
期刊论文
[1]Novel Co-Mg-Al-Ti-O catalyst derived from hydrotalcite-like compound for NO storage/decomposition[J]. Jie Cheng, Xiaoping Wang, Chunyan Ma , Zhengping Hao Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China.. Journal of Environmental Sciences. 2012(03)
[2]Evaluation of media for simultaneous enumeration of total coliform and Escherichia coli in drinking water supplies by membrane filtration techniques[J]. FIESSEL Wanda. Journal of Environmental Sciences. 2008(03)
本文编号：3329353
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