论文总字数：18540字

摘 要

含氯挥发性有机物(Chlorinated Volatile Organic Compounds，简称CVOCs)被认为是造成环境污染主要原因之一，对大气环境及人类健康造成了严重的危害。1,2-二氯乙烷(1,2-Dichloroethane，简称DCE)，是CVOCs中的典型代表，随着人类工业生产的扩大，越来越多的DCE被排放到空气中，严重污染了环境，威胁着人类的健康。对此，我们迫切需要一种高效，泛用的DCE处理方法。

本文采用自制的能显著提高DCE催化氧化反应降解率的圆柱形催化剂，用于研究DCE催化氧化反应动力学。固定床反应器从上至下被分为三个部分，底段和上段装填拉磁环，中间部分充满石英砂和催化剂的混合物，该填充方法用于确保反应物在反应器床层中具有相同的停留时间。在高气体流速(500 mL·min^-1)条件下消除了外扩散阻力对反应动力学的影响，同时忽略了内扩散阻力的影响。在此基础上，在温度320~420 ℃、0~1244.44 g·h·mol^-1进料质量空时、压力为大气压的条件下测定了动力学的实验数据。通过对催化氧化DCE的反应步骤(历程)分析并结合反应产物组成，提出将DCE及两种生成量相对较多的氯乙烯(VC)及四氯乙烯(PCE)作为关键组分、忽略产物中微量的其它含氯烯烃的复杂反应网络，并由此建立了反应动力学模型。通过MATLAB软件中非线性最小二乘法对实验数据进行了拟合计算，得到了各反应步骤的动力学参数。同时测定了模型的显著性，结果模型是高度适定的。最终得到DCE在该催化剂作用下的反应动力学模型，为今后工业设计、实际生产操作提供参考依据。

关键词：1,2-二氯乙烷 催化燃烧 动力学

ABSTRACT

Chlorinated Volatile Organic Compounds (CVOCs) are considered to be one of the main causes of environmental pollution. The environment and human health have caused serious harm. 1,2-Dichloroethane (DCE) is a typical representative of CVOCs. With the expansion of human industrial production, more and more DCE is discharged into the air, which seriously pollutes the environment. , threatening human health. In this regard, we urgently need an efficient and widely used DCE decomposition method.

In this paper, a self-made cylindrical catalyst which can significantly increase the degradation rate of 1,2-dichloroethane catalytic oxidation reaction was used to study the kinetics of catalytic oxidation of 1,2-dichloroethane. The fixed bed reactor has upper, middle and bottom sections. The bottom section and the upper section are filled with Raschig rings. The middle section is filled with a mixture of quartz sand and catalyst. This filling method is used to ensure that the reactants are the same in the reactor bed. The time of stay. At the high gas flow rate (500 mL/min), the influence of the external diffusion resistance on the reaction kinetics was eliminated, while the influence of the internal diffusion resistance was ignored. On this basis, experimental data of kinetics were measured under the condition of temperature of 320-420°C, raw material gas mass time of 0~1244.44 g·min·mol-1 and pressure of atmospheric pressure. By the analysis of the reaction steps of catalytic oxidation of DCE and the composition of reaction products, a complex reaction network was proposed, in which DCE and two kinds of vinyl chloride (VC) and tetrachloroethylene (PCE) were treated as the key components and trace amounts of other chloroolefins in the products were neglected. Afterwards, the kinetic model of the reaction was established. The experimental data were fitted by nonlinear least square method in MATLAB, and the kinetic parameters of each reaction were obtained. The results are very consistent; at the same time, the significance of the model is determined and the model is highly well-defined. Finally, the reaction kinetic model of 1,2-dichloroethane under the action of the catalyst was obtained, which provided a reference for future industrial design and actual production operations.

KEYWORDS：1,2-Dichloroethane，Catalytic combustion，Kinetic

目 录

摘 要 I

ABSTRACT I

目 录 i

第一章 文献综述 1

1.1 DCE的物化性质 1

1.2 DCE的应用和危害 1

1.2.1 DCE的应用 1

1.2.2 DCE的危害 2

1.3 DCE的处理方法 2

1.3.1 回收技术 2

1.3.2 降解技术 3

1.4 DCE催化氧化反应动力学研究 5

1.5 本论文的研究意义及研究内容 5

第二章 实验装置、流程及分析方法 6

2.1 实验试剂及仪器 6

2.1.1 原料和试剂 6

2.1.2 实验仪器 6

2.2 实验装置与流程 6

2.3 实验仪器标定 7

2.4 分析方法 9

2.5 计算方法 9

2.6本章小结 10

第三章 动力学模型的构建及参数的求解 11

3.1 内、外扩散阻力的消除 11

3.1.1 内扩散阻力的消除 11

3.1.2 外扩散阻力的消除 11

3.2 反应网络的构建 12

3.3 反应动力学模型的构建及参数的求解 13

3.4 模型的显著性检验 20

3.5 本章小结 20

第四章 结论 22

参考文献 23

致 谢 26

第一章 文献综述

挥发性有机化合物(volatitle organic compounds，简称 VOCs)^[1]通常指在标准大气压下沸点低于373.15 K的有机化合物。易于挥发至大气中造成污染，普遍存在于空气中并且成分较为复杂的特点使其被定义为有机污染物。

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