论文总字数：20503字

摘 要

本文首先简要讲述了高硫原油以及空气中过量CO的对环境和人体的危害，并给出了常用的解决办法——HDS和CO催化氧化，而上述方法都离不开催化剂的作用。载体材料作为催化剂的重要构成部分，对催化效果影响甚大。

由于粘土材料具有层状结构，阳离子交换容量高，可作为一种理想的载体材料。但粘土的比表面积较其他传统材料低的多，这也是限制粘土类载体材料发展的主要原因。实验中采用膨胀土为粘土原料，尝试了多种改性手段对其进行处理，并通过浸渍法分别负载了NiMoW、CuO等活性组分。

利用XRD、热分析及电镜等手段对粘土材料进行表征，并对其催化活性进行了测试。结果表明：①CuO负载量过低无法完全催化CO氧化，过高则会导致Cu物种聚集，会降低Cu物种的分散度，以负载量15%最为合适；②多种改性方法中以磷酸改性的膨胀土负载NiMoW的脱硫效果最好，反应4h后脱硫率可达到97%，且当酸浓度低于5mol/kg时，脱硫率与磷酸浓度呈正比；③以磷酸改性白色膨胀土为载体的催化剂活性优于黄色膨胀土。

关键词：加氢脱硫 CO氧化 载体材料 粘土改性

Preparation and Its Catalytic Performance of Novel Composite Clay Material

Abstract

This article first briefly describes the hazards to the environment and human body of high-sulfur crude oil and excess CO in the air, and gives the commonly used solution - HDS and CO catalytic oxidation, and the above methods are inseparable from the role of the catalyst.As an important part of the catalyst, the carrier material has a great influence on the catalytic effect.

Due to its’ layered structure and high cation exchange capacity,the clay can be used as an ideal carrier material.However, the specific surface area of clay is much lower than other traditional materials, which is also the main reason for limiting the development of clay-based carrier materials.In the experiment, expansive soil was used as clay raw material, and various modification methods were tried to handle it.Then,NiMoW,CuO and other active components were loaded by impregnation method.

The clay material was characterized by XRD, thermal analysis and electron microscopy etc, and its catalytic activity was tested.The results show:①When the CuO loading is too low, CO oxidation cannot be fully catalyzed. If the CuO loading is too low, the Cu species will aggregate, which will reduce the dispersion of the Cu species. The loading of 15% is most suitable.②The desulfurization effect of NiMoW loaded with phosphoric acid modified expansive soil is best among 3 kinds of modification methods, its’ desulfurization rate can reach 97% after 4h reaction, and when the acid concentration is lower than 5mol/kg, the desulfurization rate is proportional to the concentration of phosphoric acid.③The activity of the catalyst with the phosphoric acid modified white expansive soil as the carrier is superior to the yellow expansive soil.

Key Words:Hydrodesulfurization;CO oxidation;Carrier material;Clay modification

目 录

摘 要 I

ABSTRACT II

第一章 绪论 1

1.1引言 1

1.2加氢脱硫(HDS)研究进展 1

1.2.1 HDS反应机理 1

1.2.2 HDS催化剂 2

1.3 CO催化氧化研究进展 6

1.3.1 CO氧化反应机理 6

1.3.2 CO氧化催化剂 6

1.4粘土复合材料 8

1.4.1粘土改性 8

1.4.2制备方法 10

1.5课题的提出及目的 11

第二章 实验方法 12

2.1试剂和仪器 12

2.2实验过程 12

2.2.1催化剂的制备 12

2.2.2表征测试 14

2.2.3催化测试 14

第三章 实验结果及分析 17

3.1表征分析 17

3.1.1 XRD分析 17

3.1.2热分析 22

3.1.3透射电镜(TEM)分析 23

3.2催化活性分析 24

3.2.1加氢脱硫（HDS） 24

3.2.2 CO催化氧化 27

第四章 结论与展望 28

4.1结论 28

4.2展望 28

参考文献 29

致 谢 32

绪论

1.1引言

请支付后下载全文，论文总字数：20503字