USST_Arts_112451341城市污水中优先控制微量有机污染物的筛选及其高级氧化研究

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摘要

基于建立的城市污水中优先控制微量有机污染物筛选体系，选取得分在前四

名的氯贝酸(CFA)、壬基酚(NP)、17α-乙炔基雌二醇(EE2)和卡马西平(CBZ)作为目

标物，运用固相萃取(SPE)分离提取浓缩技术和GC/MS检测方法，研究目标物在臭

氧、臭氧/超声、臭氧/光催化三种工艺下的去除特性，重点考察了臭氧浓度、pH值

和腐植酸(HA)浓度等影响因素对目标物去除效果的影响。主要结论如下：

(1) 臭氧单独氧化去除四种目标物(CFA、NP、EE2 和CBZ)，四种目标物的去

除率随着臭氧浓度的增大而提高，反应进行 12 min 后，去除率曲线趋于平缓。臭

氧投加浓度为 30 µg/L时，CFA、NP、EE2和CBZ四种目标物的去除率分别为 65.1%、

71.8%、61.8%和69.2%，继续增大臭氧投加量，目标物的去除率并没有很大的提

升。

(2) 臭氧-超声联合氧化处理四种目标物(CFA、NP、EE2 和CBZ)，超声功率

低于 240 W 时，目标物的去除率随着超声功率的增大而提高，超声功率由 0 W 增

加到 240 W，CFA、NP、EE2 和CBZ 的去除率分别提高了 17.8%、16.5%、19.8%

和14.9%，提高的效率要高于单独超声时对目标物的去除效果，可见超声强化了臭

氧的氧化作用，二者有协同作用。

(3) 臭氧-光催化联合氧化处理四种目标物(CFA、NP、EE2 和CBZ)，四种目

标物的去除效果随着光催化试剂投加量的增大而增加，光催化试剂由 5 mg/L 增加

到100 mg/L，CFA、NP、EE2 和CBZ 四种目标物的去除率分别增加了 11.4%、13.0%、

15.5%和9.1%。臭氧-光催化联合氧化时目标物的去除率要高于单独光催化氧化和

单独臭氧氧化目标物去除率之和，说明光催化剂强化了臭氧的氧化作用，光催化

氧化和臭氧氧化有协同作用。光催化试剂的吸附量要远小于光催化反应降解目标

物的量，说明研制的光催化试剂降解目标物主要依靠光催化反应，而不是吸附。

(4) 臭氧、臭氧-超声联合和臭氧-光催化联合对四种目标物(CFA、NP、EE2和

CBZ)进行氧化，随着pH的增大，四种目标物的去除率逐渐提高。随着水样中腐植

酸(HA)浓度的增加，四种目标物的去除率逐渐降低。

(5) 比较臭氧、臭氧-超声联合和臭氧-光催化联合对四种目标物氧化效果，当

臭氧单独氧化时，四种目标物的去除率仅在65.1%~71.8%之间。采用臭氧与超声联

合氧化时，目标物降解效果明显改善，四种目标物的降解效率分别提升了11.1%、

23.2%、19.8%和14.9%。当采用臭氧与自主烧制的光催化材料联合氧化时，目标物

去除效果也有所提高，目标物的去除效率提高范围在7.2%~19.3%之间。

关键词：臭氧臭氧-超声联合臭氧-光催化联合氯贝酸壬基酚

17α-乙炔基雌二醇卡马西平

ABSTRACT

With the screening system, the top four organic pollutants, ie clofibric acid (CFA),

nonylphenol (NP), 17α-ethinylestradiol (EE2) and carbamazepine (CBZ), were selected

as target compounds. The target compounds were separated and concentrated by solid

phase extraction (SPE) technique, and the degradation characteristics were dectected by

gas chromatography/mass spectrometry (GC/MS). The paper investigated with the

processes of ozone (O3), ozone-ultrasound (O3/US), ozone-photocatalysis through batch

experiment. The main conclusions are as follows：

(1) Ozonation alone was conducted with four target compounds (CFA、NP、EE2

and CBZ), and the removal rates of four target compounds were enhanced with the

ozone dose increasing. When the ozone dose was 30 µg/L, the removal rates of four

target compounds were 65.1%、71.8%、61.8% and 69.2% respectively. More ozone dose,

but the removal rates were not too much of a improvement.

(2) Ozone-ultrasonic combined process was conducted with four target compounds.

Compared with ozone oxidation only, the removal rates of CFA、NP、EE2 and CBZ

added 17.8%、16.5%、19.8% and 14.9% respectively when ultrasound power was 240 W.

Meanwhile, the removal rates added was more than the removal rates with ultrasound

oxidation only. This proved that ultrasound enhanced ozone oxidation and the two

processes had synergetic effect.

(3) Ozone-photocatalysis combined process was conducted with four target

compounds. the removal rates of four target compounds were enhanced with the

photocatalyst dose increasing. When photocatalyst concentration was increased to 100

mg/L from 5 mg/L, the removal rates of CFA、NP、EE2 and CBZ added 11.4%、13.0%、

15.5% and 9.1% respectively. The removal rates of four target compounds by

ozone-photocatalysis combined process were more than superposition of ozone and

ultrasonic alone respectively. This proved that photocatalysis enhanced ozone oxidation

and the two processes had synergetic effect. And the targets adsorption amount was far

less than degradation amount of photocatalytic reagents, so the removal of the target

was mainly relied on the photocatalytic reaction.

(4) When three oxidation processes were conducted with four target compounds,

removal rates of four target compounds were enhanced with pH increasing. However,

the removal rates were declined with humic acid (HA) concentration increased.

(5) The paper compared the effect of different process (O3, O3-US,

O3-photocatalysis) for degrading four targets. It showed that the removal rates of four

targets only ranged from 65.1%~71.8%. When ozone- ultrasonic combined process was

used, the removal rates of the targets added 11.1%、23.2%、19.8% and 14.9%

respectively. And removal rates added ranged from 7.2%~19.3% for

ozone-photocatalysis combined process.

Key Word: O3, Ozone-ultrasonic, Ozone-photocatalysis, CFA, NP, EE2,

CBZ

中文摘要

ABSTRACT

第一章绪论 ······················································································· 1

1.1 城市污水中的微量有机物概述 ······················································· 1

1.1.1 城市污水中环境内分泌干扰物的来源 ······································ 1

1.1.2 城市污水中药物的来源 ························································· 2

1.1.3 城市污水中内分泌干扰物的危害 ············································ 3

1.1.4 城市污水中药物的危害 ························································· 4

1.2 臭氧氧化技术 ············································································ 4

1.2.1 臭氧氧化机理 ····································································· 5

1.2.2 臭氧氧化技术在去除微量有机污染物方面的应用 ······················· 8

1.3 臭氧-超声联合氧化技术 ······························································· 9

1.3.1 臭氧-超声联合氧化机理 ························································ 9

1.3.2 臭氧-超声联合氧化技术在去除微量有机污染物方面的应用 ········ 11

1.4 臭氧-光催化联合氧化技术 ·························································· 11

1.4.1 臭氧-光催化联合氧化机理··················································· 11

1.4.2 臭氧-光催化联合氧化技术在去除微量有机污染物方面的应用 ····· 12

1.5 论文研究意义与主要内容 ··························································· 12

1.5.1 研究意义 ········································································· 12

1.5.2 主要研究内容 ··································································· 13

第二章优先控制微量有机污染物的筛选及分析方法 ··································· 14

2.1 优先控制微量有机污染物的筛选 ·················································· 14

2.1.1 筛选体系建立 ··································································· 14

2.1.2 筛选结果 ········································································· 15

2.2 优先控制微量有机污染物的分析方法 ············································ 19

2.2.1 采样及预处理 ··································································· 19

2.2.2 固相萃取 ········································································· 19

2.2.3 氮吹 ··············································································· 20

2.2.4 衍生化反应 ······································································ 20

2.2.5 GC-MS 分析 ····································································· 21

2.3 本章小结 ················································································ 21

第三章臭氧氧化微量有机污染物的特性 ·················································· 22

3.1 材料与方法 ············································································· 22

3.1.1 试剂及仪器 ······································································ 22

3.1.2 实验装置与流程 ································································ 23

3.1.3 分析方法 ········································································· 24

3.2 城市污水取样 ·········································································· 25

3.3 结果与讨论 ············································································· 25

3.3.1 臭氧投加量对单独臭氧氧化氧化效果的影响 ··························· 25

3.3.2 pH 值对单独臭氧氧化氧化效果的影响 ···································· 28

3.3.3 腐植酸浓度对单独臭氧氧化效果的影响 ································· 29

3.4 本章小结 ················································································ 30

第四章臭氧-超声联合氧化微量有机污染物的特性 ····································· 31

4.1 材料与方法 ············································································· 31

4.1.1 试剂及仪器 ······································································ 31

4.1.2 实验装置与流程 ································································ 31

4.1.3 分析方法 ········································································· 31

4.2 城市污水取样 ·········································································· 31

4.3 结果与讨论 ············································································· 32

4.3.1 超声功率对臭氧-超声联合氧化氧化效果的影响 ······················· 32

4.3.2 pH 值对臭氧-超声联合氧化氧化效果的影响 ····························· 33

4.3.3 腐植酸浓度对臭氧-超声联合氧化氧化效果的影响 ···················· 33

4.4 本章小结 ················································································ 34

第五章臭氧-光催化联合氧化微量有机污染物的特性 ·································· 36

5.1 材料与方法 ············································································· 36

5.1.1 试剂及仪器 ······································································ 36

5.1.2 实验装置与流程 ································································ 36

5.1.3 分析方法 ········································································· 36

5.2 城市污水取样 ·········································································· 36

5.3 结果与讨论 ············································································· 37

5.3.1 催化剂投加量对臭氧-光催化联合氧化氧化效果的影响 ·············· 37

5.3.2 pH 值对臭氧-光催化联合氧化氧化效果的影响 ·························· 38

5.3.3 腐植酸浓度对臭氧-光催化联合氧化氧化效果的影响 ················· 39

5.3.4 降解微量有机污染物效果比较 ············································· 40

5.4 本章小结 ················································································ 41

第六章结论与建议 ············································································· 42

6.1 结论 ······················································································ 42

6.2 建议 ······················································································ 43

参考文献 ··························································································· 44

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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