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N 2 O在分子筛和氧化物上的直接分解研究

发布时间:2024-02-15 03:42
  笑气催化分解成氮气和氧气是减少化学工程过程中氮氧化物排放有效的技术。同时,近些年来这种技术越来越受关注。为了控制化工过程笑气排放,本论文研究了离子交换分子筛、负载体系和单一的或者复合的氧化物这几种类型的催化剂。第一部分:制备一系列用于笑气直接分解的浸渍在蜂窝状堇青石上M(Fe,Co)-BEA催化剂。离子交换方法制备M(Fe,Co)-BEA(M=1wt%)分子筛,之后用5 wt%和10 wt%硅溶胶或者是铝溶胶作为粘合剂将分子筛浸渍在堇青石载体上。制备的整体式样品的形貌通过扫描电子显微镜分析,结果显示相对低的含量(5 wt%)M(Fe,Co)-BEA分子筛粉末在用硅溶胶或铝溶胶做粘合剂比较好地浸渍在堇青石上。笑气分解活性评价实验结果有(I)铝溶胶能明显促进Fe-BEA整体式样品催化分解笑气,然而硅溶胶能提高Co-BEA整体式样品催化分解笑气的活性;(Ⅱ)低含量的粘合剂(5 wt%)比高含量的粘合剂(10 wt%)更有利于制备整体式催化剂。利用计算流体动力学(CFD)模拟笑气在M(Fe,Co)-BEA整体式催化剂分解,研究了流体动力学的质量分布和压力降。第二部分:研究了一系列混合金属氧化物...

【文章页数】:134 页

【学位级别】:博士

【文章目录】:
摘要
Abstract
Abbreviations
Nomenclature
Chapter Ⅰ Literature
    1.1 Introduction and Motivation
    1.2 The main sources of nitrous oxide emissions
        1.2.1 Human sources of nitrous oxide emission
        1.2.2 Natural sources of nitrous oxide emissions
    1.3 Present status of CDM projects to reduce N2O emissions
    1.4 Mechanism of catalytic N2O decomposition
    1.5 Remediation technologies for N2O abatement
    1.6 Diffrent types of catalysts for N2O decomposition
        1.6.1 Metal oxides
        1.6.2 Supported metals
        1.6.3 Transition metal ions exchanged zeolites for direct N2O decomposition
Chapter Ⅱ M(Fe, Co)-BEA washcoated honeycomb cordierite for N2O directdecomposition
    2.1 Introduction
    2.2 Experimental and computational methods
        2.2.1 Experimental method
        2.2.2 Computational method
    2.3 Results and discussion
        2.3.1 Characterization of the M(Fe, Co)-BEA powder catalyst
        2.3.2 Characterization of the M(Fe, Co)-BEA monolith catalyst
        2.3.3 Activity measurement
        2.3.4 CFD simulations of M(Fe, Co)-BEA monolith for N20 direct decomposition
    2.4 Conclusion
Chapter Ⅲ Preparation of NiCe mixed oxidesfordirectN2O decomposition in theabsence of oxygen
    3.1 Introduction
    3.2 Experimental section
        3.2.1 Catalysts preparation
        3.2.2 Catalysts Characterization
        3.2.3 Activity tests
    3.3 Results and discussion
        3.3.1 Characterization of the mixed oxide catalyst
        3.3.2 Activity measurement
    3.4 Conclusion
Chapter Ⅳ NiM(Rh, Ce) mixed oxides for direct N20 decomposition in the absenceof oxygen
    4.1 Introduction
    4.2 Experimental section
        4.2.1 Catalysts preparation
        4.2.2 Catalysts Characterization
        4.2.3 Activity tests
    4.3 Results and discussion
        4.3.1 Characterization of the mixed oxide catalyst
        4.3.2 Activity measurement
    4.4 Conclusion
Chapter Ⅴ Summary
References
Liste of publications
Acknowledgements
作者和导师简介
附件



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