孔雀石绿分子印迹聚合物的制备及性能研究

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摘要

分子印迹技术是一种新型的高效分离技术，因其具有优越的识别性和选择性，

目前已在众多领域展现了其广阔的应用前景。本课题以孔雀石绿（MG）为模板分

子、α-甲基丙烯酸（MAA）为功能单体、乙二醇二甲基丙烯酸酯（EGDMA）为交

联剂、偶氮二异丁腈（AIBN）为引发剂、乙腈为溶剂，采用沉淀聚合法制备了孔

雀石绿分子印迹聚合物。实验主要对模板和单体的结合原理进行了研究，优化了

孔雀石绿分子印迹聚合物的制备条件，并通过多种方式对聚合物的性能进行了表

征。

实验结果如下：

(1) 紫外光谱研究和分子模拟结果表明模板分子孔雀石绿和功能单体α-甲基丙烯

酸在聚合之前发生了相互作用，形成了模板-单体摩尔比为1:2的复合物，二者之间

主要通过氢键和离子键相结合。

(2) 以吸附量为指标，对孔雀石绿分子印迹聚合物制备中溶剂的添加量、引发剂

的添加量、模板与单体的比例以及单体与交联剂的比例进行优化。结果表明，当溶

剂的添加量为40 mL，引发剂为40 mg，模板、单体、交联剂三者的比例为1:8:16时，

所制备的分子印迹聚合物具有较好的印迹效果。

(3) 采用沉淀聚合法制备的分子印迹聚合物微球，粒径分布在0.5~1.5 µm之间。平

衡吸附实验表明：MIP、NIP的吸附量随着孔雀石绿浓度的增加而增大，单位质量

MIP的吸附量显著大于单位质量NIP的吸附量。Scatchard分析表明MIP对孔雀石绿

分子存在两类不同的结合位点，其中高亲和力结合位点的平衡离解常数Kd1=11.223

μg/mL，最大表观结合量Qmax1=4.45×102 μg/g；低亲和力结合位点的平衡离解常数

Kd2 =156.25 μg/mL，最大表观结合量Qmax2 = 5.033×103 μg/g。

(4) 特异性吸附实验表明MIP对孔雀石绿的结合量大于NIP的结合量；MIP与NIP

对孔雀石绿的吸附量均高于相同浓度的结晶紫，表现出良好的特异性吸附能力。

(5) 通过固相萃取对MIP的回收率进行了研究，研究表明，

MIP对不同浓度的孔雀

石绿的回收率能达到75%左右，具有较好的回收效果。

关键词：分子印迹聚合物孔雀石绿沉淀聚合特异吸附

ABSTRACT

Molecular imprinting technology (MIT) is a new and highly efficient separation

technique for preparing specialized recognition media that is called molecularly

imprinted polymer (MIP). It has been used in many fields due to its superior

recognizability and selectivity. Molecularly imprinted polymer was prepared via

precipitation polymerization with MG as template molecule, MAA as functional

monomer, EGDMA as cross-linker, AIBN as initiator and acetonitrile as solvent. In this

study, the combination principle of template molecule and monomer, the the condition

of preparing MIP, and the characters of MIP were studied.

The results were as follows:

(1) The mechanism between MG and MAA was determined by UV-Vis and molecular

simulation. The results indicated that the interactions should be cooperative hydrogen

bonds or ionic bond produced by self-assembly before polymerization. The

stoichiometric mole ratio of MG-MAA complex was 1:2.

(2) The effects of the addition amount of solvent, initiator, the ratio of template

molecule and functional monomer, the ratio of functional monomer and cross-linker on

adsorption of MG were studied. The results showed that the optimum

technical parameters for imprinting effect were solvent of 40mL, AIBN of 40 mg, the

ratio of MG-MAA-EGDMA of 1:8:16.

(3) The diameter of molecularly imprinted polymer microspheres was in the range of

0.5 to 1.5 μm. Binding isotherm showed that the adsorption capacity of MIP 、NIP

increased with the increase of the concentration of malachite green. However, the

adsorption capacity of MIP was significantly greater than the adsorption capacity of NIP.

Scatchard analysis showed that two classes of binding sites were formed in the

imprinted polymers. The calculated dissociation constant Kd1 and the apparent

maximum binding capacities Qmax1 for the high affinity sites were 11.223μg/mL and

4.45×102μg/g , while Kd2 and Qmax2 for the low affinity sites were 156.25μg/mL and

5.033×103μg/g , respectively.

(4) Specific adsorption showed that the adsorption capacity of MIP was greater than

NIP. MIP and NIP on malachite green adsorption were higher than the same

concentration of crystal violet, showing the specific adsorption capacity.

(5) The recovery of MIP on malachite green was studied by solid phase extraction. It

indicated the recoveries of different concentrations of malachite green could reach 75%,

showing a good recovery performance.

Key Words: molecularly imprinted polymer, malachite green,

precipitation polymerization, specific adsorption

摘要

ABSTRACT

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

§1.1 分子印迹技术的产生与发展 ...........................................................................1

§1.2 分子印迹技术的基本原理 ...............................................................................1

§1.2.1 预组装法 .................................................................................................2

§1.2.2 自组装法 .................................................................................................3

§1.3 分子印迹体系的构成 .......................................................................................4

§1.3.1 模板分子 .................................................................................................4

§1.3.2 功能单体 .................................................................................................4

§1.3.3 交联剂 .....................................................................................................5

§1.3.4 溶剂 .........................................................................................................6

§1.3.5 引发剂与引发方式 .................................................................................7

§1.4 分子印迹聚合物的制备方法 ...........................................................................7

§1.4.1 本体聚合法 .............................................................................................7

§1.4.2 悬浮聚合法 .............................................................................................7

§1.4.3 沉淀聚合法 .............................................................................................7

§1.4.4 原位聚合 .................................................................................................8

§1.4.5 表面印迹 .................................................................................................8

§1.4.6 乳液聚合 .................................................................................................8

§1.5 分子印迹技术的应用 .......................................................................................9

§1.5.1 固相萃取 .................................................................................................9

§1.5.2 传感器 .....................................................................................................9

§1.5.3 膜分离 ...................................................................................................10

§1.5.4 模拟酶 ...................................................................................................11

§1.6 本课题的背景及意义 .....................................................................................11

第二章孔雀石绿模板与单体结合机理研究 ...............................................................13

§2.1 前言 .................................................................................................................13

§2.2 材料与设备 .....................................................................................................13

§2.2.1 材料 .......................................................................................................13

§2.2.2 设备 .......................................................................................................13

§2.3 实验方法 .........................................................................................................13

§2.3.1 溶液的配制 ...........................................................................................13

§2.3.2 紫外光谱法研究模板分子与功能相单体间的相互作用 ...................14

§2.3.3 模板分子与功能单体分子结合机理研究 ...........................................14

§2.3.4 分子模拟模板分子与功能单体结合实验 ...........................................14

§2.4 结果与讨论 .....................................................................................................15

§2.4.1 模板分子与功能单体之间的相互作用研究 .......................................15

§2.4.2 模板分子与功能单体的结合机理研究 ................................................15

§2.4.3 分子模拟实验 ........................................................................................18

§2.5 本章小结 .........................................................................................................21

第三章孔雀石绿分子印迹聚合物制备条件的优化 ...................................................22

§3.1 前言 .................................................................................................................22

§3.2 材料与设备 .....................................................................................................22

§3.2.1 材料 .......................................................................................................22

§3.2.2 设备 .......................................................................................................22

§3.3 实验方法 .........................................................................................................23

§3.3.1 工作曲线的建立 ...................................................................................23

§3.3.2 分子印迹聚合物制备方法 ...................................................................23

§3.3.3 吸附量的测定 .......................................................................................23

§3.3.4 制备条件的优化 ...................................................................................24

§3.4 结果与讨论 .....................................................................................................25

§3.4.1 孔雀石绿工作曲线的制定 ...................................................................25

§3.4.2 溶剂添加量对孔雀石绿吸附性能的影响 ...........................................27

§3.4.3 模板与功能单体比例对孔雀石绿吸附性能的影响 ...........................28

§3.4.4 功能单体与交联剂比例对孔雀石绿吸附性能的影响 .......................29

§3.4.5 引发剂的添加量对孔雀石绿吸附性能的影响 ...................................30

§3.5 本章小结 .........................................................................................................31

第四章孔雀石绿分子印迹聚合物的性能表征 ...........................................................32

§4.1 前言 .................................................................................................................32

§4.2 材料与设备 .....................................................................................................32

§4.2.1 材料 .......................................................................................................32

§4.2.2 设备 .......................................................................................................32

§4.3 实验方法 .........................................................................................................33

§4.3.1 分子印迹聚合物对孔雀石绿的平衡吸附实验 ...................................33

§4.3.2 分子印迹聚合物对孔雀石绿的吸附动力学 .......................................33

§4.3.3 特异性吸附实验 ...................................................................................33

§4.3.4 分子印迹聚合物的 SEM 分析 ............................................................ 33

§4.3.5 分子印迹聚合物的红外分析 ...............................................................33

§4.3.6 分子印迹固相萃取的制备及研究 .......................................................33

§4.4 结果与讨论 .....................................................................................................34

§4.4.1 平衡吸附实验 .......................................................................................34

§4.4.2 吸附动力学实验 ...................................................................................35

§4.4.3 特异性结合实验 ...................................................................................36

§4.4.4 SEM 实验 .............................................................................................. 37

§4.4.5 印迹聚合物的红外分析 .......................................................................38

§4.4.6 分子印迹固相萃取 ...............................................................................39

§4.5 本章小结 .........................................................................................................41

第五章结论与展望 .......................................................................................................43

§5.1 结论 .................................................................................................................43

§5.2 展望 .................................................................................................................43

参考文献 .........................................................................................................................45

在读期间公开发表的论文和承担科研项目及取得成果 .............................................51

致谢 .................................................................................................................................52

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摘要：

摘要分子印迹技术是一种新型的高效分离技术，因其具有优越的识别性和选择性，目前已在众多领域展现了其广阔的应用前景。本课题以孔雀石绿（MG）为模板分子、α-甲基丙烯酸（MAA）为功能单体、乙二醇二甲基丙烯酸酯（EGDMA）为交联剂、偶氮二异丁腈（AIBN）为引发剂、乙腈为溶剂，采用沉淀聚合法制备了孔雀石绿分子印迹聚合物。实验主要对模板和单体的结合原理进行了研究，优化了孔雀石绿分子印迹聚合物的制备条件，并通过多种方式对聚合物的性能进行了表征。实验结果如下：(1)紫外光谱研究和分子模拟结果表明模板分子孔雀石绿和功能单体α-甲基丙烯酸在聚合之前发生了相互作用，形成了模板-单体摩尔比为1:2的复合物，二者...

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