石墨烯纳米钛管复合材料的研制及其对活性黑和扑热息痛降解的研究

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摘要

近年来，染料废水因其色度高，毒性大、可生化性差、COD 高等特点，染料

废水的处理一直是水处理的一大焦点，而扑热息痛(Paracetamol)作为一种广泛应用

的药品与个人护理药品，属于解热镇痛药，与人类生活密切相关同时又危害环境

和人类健康，广泛存在于空气，水体和土壤中。越来越多的研究集中去除扑热息

痛。本文分别以二氧化钛纳米管(Titanium Nanotube, TNT)为钛前驱体和氧化石墨为

碳前驱体合成石墨烯钛纳米管复合材料，以提高复合材料的光催化效果。使用

UV-vis、XRD、FT-IR、BET、TGA 等方法对复合材料表征，并在紫外光照射条件

下采用 TNT 及GR-TNT 复合材料对染料 RBk5 和扑热息痛及二者混合体系的光催

化降解效果进行分析，确定了最佳的反应条件，同时通过 GC-MS 检测光催化过程

中的中间产物，并对反应过程的反应机理做进一步研究。经过多次实验研究，初

步得到以下结论：

1. 本实验分别通过改进的 Hummers 法制备氧化石墨和水热法制备二氧化钛

纳米管，以二者分别作为碳和钛前驱体，通过水热法成功合成石墨烯钛纳米管复

合材料(GR-TNT)。

2. 在光催化降解染料 RBk5 和扑热息痛及二者混合体系过程中，GR-TNT 具

有很高的光催化降解性能。

3. 染料浓度、石墨烯添加量、催化剂投加量、pH、反应温度等实验条件都会

对于光催化效果有明显影响。初始浓度低时，光催化效果更好；随着石墨烯添加

量增多，光催化效果增强，石墨烯添加量为 10%时，GR-TNT 复合光催化剂紫外

光解 RBK5 的实验具有最高降解效率，然而添加过多石墨烯会导致光催化效率降

低；投加量有最佳值，本实验中为 0.1 g L-1；最佳反应温度为 35℃；酸性条件有利

于光催化降解染料 RBk5，最佳 pH 为3。

4. GR-TNT 复合材料光催化降解扑热息痛最佳实验条件为石墨烯添加量为

5%，催化剂投加量为 0.1 g L-1，pH 为9。实验中通过加入不同捕获剂得知，光催

化降解染料 RBk5 和扑热息痛过程中空穴为主要活性物质。通过循环实验得知，复

合催化剂具有很高的稳定性，可多次被循环使用，仍具有较高的光催化效率。

5. GR-TNT 复合光催化剂对染料和扑热息痛的混合体系仍具有较高的光催化

效率。染料 RBK5 优先扑热息痛降解，且染料在混合体系中的降解率高于相同条

件下的单一体系。

6. 通过 GC-MS 对光催化过程中产生的中间产物进行检测，并推测出反应路

径，同时对 GR-TNT 复合材料光催化降解污染物的反应机理进行了探究。

关键词：石墨烯二氧化钛纳米管染料扑热息痛光催化

ABSTRACT

In recent years, due to its high chromaticity, high toxicity and high biological

difference, COD, dye wastewater is always the focus of water treatment. While

Paracetamol (acetaminophen) as a kind of widely used antipyretic analgesics drug, is

belonged to pharmaceutical and personal care, it is closely related to human life and is

bad for the environment and human health, but widely exists in the air, water and soil.

More and more studies focus on removing paracetamol. In order to improve the

photocatalytic effect of the composites, titanium dioxide nanotubes (TNT) and graphite

as titanium and carbon precursor respectively, The composites were characterized by

UV-vis, XRD, FT-IR, BET and TGA. Under the condition of UV irradiation, TNT and

GR-TNT compounds were used for dye RBk5 and paracetamol photocatalytic

degradation, and the best reaction conditions were determined. At the same time, the

intermediate products were detected by GC-MS. The process of photocatalytic reaction

mechanism were also further researched. After many experiments, the preliminary

conclusions were as following :

1. Graphene titanium nanotube composites (GR-TNT) were successfulsynthesized

by he hydrothermal method, using graphite oxide and titania nanotubes as the carbon

and titanium precursor, respectively.

2. In the photocatalytic degradation of dye RBk5 and paracetamol and two hybrid

system, GR-TNT composites have very high photocatalytic degradation performance.

3. The concentration of dye, graphene addition amount, catalyst dosing, pH,

temperature had significant effect on the catalytic effect. The lower the initial

concentration, the better photocatalytic effect; As graphene content increased,

photocatalytic effect is enhanced, graphene addition amount was 10%, the RBK5

degradation by GR-TNT has the highest efficiency, however, adding too much graphene

can reduce photocatalytic efficiency; The best dosage was 0.1 gL-1; The best reaction

temperature of 35 ℃; The best pH is 3.

4. The optimum experiment conditions for photocatalytic degradation of

paracetamol by GR-TNT composites is 5% graphene adding amount, the catalyst dosing

is 0.1 g L-1, pH 9. EDTA (hole scavengers) and t-BuOH (radical scavengers) were used

to detect the main active oxidative species in the system. The results showed that the

holes are the main oxidation species in the photocatalytic process. Composite catalysts

have high stability in cycle experiment.

5. In the mixture system of RBk5 and paracetamol, GR-TNT composites have

higher photocatalytic efficiency. Dye RBK5 priority to paracetamol degradation, and

degradation of dye in the mixed system is higher than the same conditions of a single

system.

6. The intermediate products of the photocatalyctic degradation were tested by

GC-MS and the reaction path was infered, at the same time mechanism of

photocatalytic degradation were also studied.

Key words: Graphene, Titanium Nanotubes, RBk5, Paracetamol,

Photocatalytic degradation

中文摘要

ABSTRCAT

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

1.1 研究缘起 .......................................................................................................... 1

1.1.1 染料性质、分类、危害及处理方法 ................................................. 1

1.1.2 扑热息痛性质、危害及处理方法 ..................................................... 5

1.2 研究目的及内容 .............................................................................................. 6

1.2.1 研究目的 ............................................................................................. 6

1.2.2 研究内容 ............................................................................................. 6

1.3 技术路线 ........................................................................................................... 7

第二章光催化技术及材料表征 ..................................................................................... 9

2.1 光催化的定义及发展 ...................................................................................... 9

2.1.1 光催化剂定义 ...................................................................................... 9

2.1.2 光催化发展 ......................................................................................... 9

2.2 光催化的作用原理 .......................................................................................... 9

2.3 TiO2的基本特性 ............................................................................................. 11

2.3.1 二氧化钛纳米管生成原理及特征 ................................................... 12

2.3.2 二氧化钛纳米管制备方法 ............................................................... 12

2.4 纳米管的改性 ................................................................................................ 13

2.4.1 离子掺杂 ........................................................................................... 13

2.4.2 贵金属沉积 ....................................................................................... 14

2.4.3 半导体复合 ....................................................................................... 14

2.4.4 染料光敏化 ....................................................................................... 15

2.4.5 聚合物改性 ....................................................................................... 15

2.4.6 碳族材料掺杂 ................................................................................... 15

2.5 石墨烯概述 ..................................................................................................... 16

2.5.1 石墨烯的制备方法 ........................................................................... 16

2.5.2 石墨烯复合材料 ............................................................................... 17

2.6 光催化剂的应用 ............................................................................................ 18

2.6.1 光催化剂在污染防治方面的的应用 ............................................... 18

2.6.2 光催化剂在日常生活中的应用 ....................................................... 18

2.6.3 光催化剂在产业上的应用 ............................................................... 18

2.7 光催化剂的特性分析 .................................................................................... 18

2.7.1 紫外可见光光谱仪 ............................................................................ 18

2.7.2 粉末 X光射线衍射 ........................................................................... 19

2.7.3 傅立叶红外线光谱仪 ....................................................................... 19

2.7.4 穿透式电子显微镜 ............................................................................ 19

2.7.5 氮气吸附/脱附仪 ............................................................................... 20

2.7.6 热重分析 ........................................................................................... 20

第三章材料及研究方法 ............................................................................................... 21

3.1 实验药品及所需仪器 .................................................................................... 21

3.1.1 实验主要试剂 .................................................................................... 21

3.1.2 实验仪器 ........................................................................................... 21

3.2 实验方法及步骤 ............................................................................................ 22

3.2.1 材料制备 ........................................................................................... 22

3.2.2 实验步骤 ........................................................................................... 23

3.3 实验部分 ........................................................................................................ 24

3.3.1 吸附实验 ............................................................................................ 24

3.3.2 光催化实验 ........................................................................................ 24

3.4 污染物检测方法 ............................................................................................. 25

3.4.1 染料 RBk5 的测定原理及方法 ........................................................ 25

3.4.2 水中扑热息痛的测定原理及方法 ................................................... 25

第四章光催化剂的表面特性分析 ............................................................................... 27

4.1 紫外-可见分光光度计 .................................................................................... 27

4.2 X 射线衍射仪 ................................................................................................. 28

4.3 傅里叶红外光谱 ............................................................................................ 29

4.4 高解析度电子显微镜 ..................................................................................... 30

4.5 N2等温吸附脱附 ............................................................................................ 31

4.6 热重分析和差热分析 .................................................................................... 31

第五章光催化降解染料 RBk5 ..................................................................................... 33

5.1 反应条件对实验的影响研究 ........................................................................ 33

5.1.1 直接光解作用 ................................................................................... 33

5.1.2 不同石墨烯添加量对光催化反应的影响 ........................................ 33

5.1.3 初始浓度对反应的影响 ................................................................... 34

5.1.4 投加量对光催化反应的影响 ........................................................... 35

5.1.5 pH 对光催化的影响实验 .................................................................. 37

5.1.6 温度对光催化效果的影响 ............................................................... 39

5.1.7 不同合成方法对光催化效果的影响 ............................................... 40

5.1.8 捕获剂(EDTA-2Na/t-BuOH)在光催化反应中的作用 .................... 40

5.1.9 光催化剂循环使用效率 ................................................................... 41

5.2 反应动力学拟合 ............................................................................................ 42

5.3 小结 ................................................................................................................ 44

第六章光催化降解扑热息痛 ....................................................................................... 45

6.1 不同反应条件的影响 .................................................................................... 45

6.1.1 背景实验 ............................................................................................ 45

6.1.2 扑热息痛初始浓度的影响 ............................................................... 45

6.1.3 石墨烯添加量对扑热息痛降解效率的影响 ................................... 46

6.1.4 光催化剂投加量的影响 ................................................................... 47

6.1.5 pH 影响实验研究 .............................................................................. 48

6.1.6 反应温度的影响 ............................................................................... 49

6.1.7 不同捕获剂的影响 ........................................................................... 50

6.2 反应动力学研究 ............................................................................................ 50

6.3 小结 ................................................................................................................. 52

第七章光催化降解混合物 ........................................................................................... 53

7.1 不同石墨烯含量催化剂对光催化效果的影响 ............................................ 53

7.2 混合物浓度比例对光催化实验的影响 ........................................................ 54

7.3 投加量对光催化效率的影响 ......................................................................... 55

7.4 光催化降解染料 RBk5 的反应路径 .............................................................. 56

7.5 光催化降解扑热息痛的反应路径 ................................................................. 58

7.6 光催化反应机理 ............................................................................................ 58

第八章结论与展望 ....................................................................................................... 60

8.1 结论 ................................................................................................................ 60

8.2 研究不足与展望 ............................................................................................. 61

参考文献 ......................................................................................................................... 62

在读期间公开发表的论文和承担科研项目及取得成果论文 ................................... 71

致谢 ................................................................................................................................. 72

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摘要：

摘要近年来，染料废水因其色度高，毒性大、可生化性差、COD高等特点，染料废水的处理一直是水处理的一大焦点，而扑热息痛(Paracetamol)作为一种广泛应用的药品与个人护理药品，属于解热镇痛药，与人类生活密切相关同时又危害环境和人类健康，广泛存在于空气，水体和土壤中。越来越多的研究集中去除扑热息痛。本文分别以二氧化钛纳米管(TitaniumNanotube,TNT)为钛前驱体和氧化石墨为碳前驱体合成石墨烯钛纳米管复合材料，以提高复合材料的光催化效果。使用UV-vis、XRD、FT-IR、BET、TGA等方法对复合材料表征，并在紫外光照射条件下采用TNT及GR-TNT复合材料对染料RBk5和扑...

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