论文总字数：26371字

摘 要

随着时代和科技的日新月异，含氮化合物开始被应用于工业生产之中，而氮氧化物作为排放气体成为了现在的首要大气污染物之一，氮氧化物具有极大的毒害性，威胁着人类的健康和社会的有序发展，本文主要从吸附处理方面研究MOFs材料能够为社会带来怎样的贡献。

MOFs全称金属-有机骨架材料，是一类金属离子与有机配体之间通过配位键合的方式形成的新型有机-无机杂化材料，本文主要研究的是其中的Cu-MOF-199和Cu-MOF-74两种材料，分别测试了Cu-MOF-199和Cu-MOF-74的晶体结构、表面形貌、表面结构、热稳定性以及对氨气和一氧化氮的吸附性能。

本文首先对Cu-MOF-199进行了分析与测试，通过水热和溶剂热法进行合成，之后以乙酸为载体配位调节法对Cu-MOF-199进行改性，再次对比研究其性能和结构的变化。研究发现，乙酸可以起到封端剂和模板剂的作用，无论是否被改性，Cu-MOFs材料在低温SCR反应气氛下都具有完整的骨架结构。但是在改性后，MOFs结构中缺陷变多，具有复数级别孔道结构，对SCR催化的反应活性增强。

之后本文对Cu-MOF-94进行了分析与测试，同样通过水热和溶剂热法进行合成，结果表示改变共溶剂和合成温度之后，所制备出的材料晶体结构和性能也会同时改变。

关键词：Cu-MOFs；NH₃-SCR；催化

Abstract

With the rapid changes of the times and technology, nitrogen-containing compounds have been used in industrial production, and nitrogen oxides have become one of the most important atmospheric pollutants as exhaust gas. Nitrogen oxides are extremely toxic and threaten The health of human beings and the orderly development of society, this article mainly studies the contribution that MOFs materials can bring to society from the aspect of adsorption treatment.

The full name of MOFs is metal-organic framework material, which is a new type of organic-inorganic hybrid material formed by coordination bonding between metal ions and organic ligands. This article mainly studies Cu-MOF-199 and Cu-MOF-74 two kinds of materials, respectively tested the crystal structure, surface morphology, surface structure, thermal stability, and adsorption of ammonia and nitric oxide of Cu-MOF-199 and Cu-MOF-74.

This article firstly analyzed and tested Cu-MOF-199, synthesized by hydrothermal and solvothermal methods, then modified the Cu-MOF-199 with acetic acid as the carrier coordination adjustment method, and compared its performance and structure again. The change. The study found that acetic acid can play the role of end-capping agent and template agent, whether or not modified, Cu-MOFs material has a complete skeleton structure under low temperature SCR reaction atmosphere. However, after the modification, the defects in the MOFs structure become more, with a multi-level channel structure, and the reaction activity to the SCR catalysis is enhanced.

Afterwards, this article analyzed and tested Cu-MOF-94, and also synthesized by hydrothermal and solvothermal methods. The results show that after changing the co-solvent and the synthesis temperature, the crystal structure and properties of the prepared material will also change.

Key word:Cu-MOFs;NH₃-SCR;Catalysis

目 录

第一章 绪论.........................................................................................................1

1.1 MOFs的简介..............................................................................................1

1.2 MOFs的特点..............................................................................................1

1.3 MOFs的应用 ...........................................................................................2

1.4 MOFs的制备 ...........................................................................................3

1.5 氮氧化物的危害及其应对方法...............................................................4

第二章 实验原料及材料制备............................................................................5

2.1 实验原料...................................................................................................5

2.2 Cu-MOF-199的制备.................................................................................6

2.3 Cu-MOF-94的制备...................................................................................7

第三章 Cu-MOF-199的测试与分析.................................................................8

3.1 Cu-MOF-199的制备及其性能的研究.....................................................8

3.1.1晶体结构分析.....................................................................................8

3.1.2 形貌分析............................................................................................9

3.1.3 热稳定分析.......................................................................................10

3.1.4 比表面积和孔道结构分析..............................................................11

3.1.5 对NH₃和NO的吸附性能分析......................................................12

3.2 乙酸改性对Cu-MOF-199结构和性能的影响.....................................12

3.2.1 晶体结构分析..................................................................................13

3.2.2 形貌分析..........................................................................................14

3.2.3热稳定性分析..................................................................................15

3.2.4 比表面积和孔道结构分析.............................................................16

3.2.5 低温脱硝反应活性.........................................................................16

3.3 本章小结................................................................................................17

第四章 Cu-MOF-94的测试与分析................................................................15

4.1 Cu-MOF-94的制备及其性能的研究....................................................18

4.1.1 晶体结构分析.................................................................................18

4.1.2 形貌分析.........................................................................................18

4.1.3 热稳定性分析.................................................................................19

4.1.4 比表面积和孔道结构分析.............................................................20

4.1.5 对NH₃和NO的吸附性能分析....................................................21

4.2本章小结................................................................................................23

第五章 结论....................................................................................................23

参考文献..........................................................................................................24

致谢..................................................................................................................26

绪论

MOFs的简介

金属－有机骨架材料是一种以无机金属离子与有机配体通过自组装的方式形成的多孔材料^[1]。1995年科学界提出了MOFs材料的定义，同时也标志着MOFs的问世。作为多孔晶体材料的一种，其性能与Zeolites类似。随着时代发展也逐步进入人类社会的建设，应用于广阔的行业之中，比如气体吸附分离、储存能量、药物载体、渗透性和催化作用等领域^[2]。MOFs形成的过程如图1-1所示，这种结构赋予了MOFs材料稳定的结构和易于调节的孔道结构。

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