臺灣博碩士論文加值系統

本實驗採以商用型Degussa P-25 TiO2觸媒，並使用高壓汞燈(400 W)做為光降解納乃得(Methomyl)與巴拉松(Parathion)農藥試驗溶液中之光源，並藉由改變TiO2觸媒添加量 (0 g~1.5 g)、納乃得與巴拉松濃度(10 mg/L~30 mg/L)、pH值 (4~10) 改變等條件進行實驗，以探討納乃得(Methomyl)與巴拉松(Parathion)在TiO2光觸媒降解過程中的降解變化、pH對降解的影響及礦化程度等差異性與效果。
由實驗結果發現在TiO2/UV 系統中，納乃得與巴拉松之濃度會在0.5 h ( t )內會快速降解，其降解趨勢可以擬一階反應描述，而其反應速率常數會隨著納乃得與巴拉松濃度增加而減少、隨著TiO2濃度增加而增加。若添加過多觸媒則會因遮蔽效應，而延長光催化效率的時間與降低降解效率，且由實驗觀察出(0 g~1.5 g)、初始納乃得與巴拉松農藥水溶液，兩者在降解的趨勢非常的相似，其濃度會在30 min (t)內快速降低，而30 min (t)後的降解速率則逐漸趨向線性呈現，並由降解實驗結果可得知，本實驗之TiO2 / 納乃得的最佳濃度0.75 g/L，巴拉松的最佳濃度1 g/L，pH值在pH4(弱酸)、pH10(弱鹼)時，由於有溶液中的電子加入反應機制中、及呈現水解效果，故皆有較高的降解效率。
利用紫外線/可見光分光光譜儀 (UV / Vis)分析，納乃得與巴拉松在TiO2/UV系統中，溶液反應所得之氨氮( NH4十 )及硝酸鹽氮( NO2-)與亞硝酸鹽氮( NO3- )與磷酸鹽 ( PO4- )等分析結果，由於強氧化環境的作用，光催化氧化處理能使它們完全無機化，並且定量生成亞硝酸鹽氮( NO3- )、磷酸鹽 ( PO4- )、二氧化碳(CO2)等無機產物。
雖然到目前為止，運用此方法來降解廢水中之有機污染物質並非普及，而本文將TiO2光降解技術應用到含納乃得與巴拉松廢水的降解，用以解決自然水體中的農藥廢水的淨化處理及有關的環境問題，克服了傳統廢水處理技術淨化不徹底等缺點及可節省高成本的土地、時間與能源消耗，是一種處理效率高且可以避免二次污染的淨化技術。

The experimental mining Commercial Degussa P-25 TiO2 catalyst and as photodegradation Methomyl (Methomyl), and Ba Lasong (Parathion) pesticide test solution, the light source, the use of high-pressure mercury lamp (400 W) by change the TiO2 catalyst loading (0 g to 1.5 g), Methomyl Bala Song concentration (10 mg / L to 30 mg / L), pH values (4 to 10) and changes in condition to conduct experiments to explore satisfied trusted (Methomyl), and Ba Lasong (Parathion) Degradation of TiO2 photocatalytic degradation process of pH on the degradation and mineralization of the differences and effect.
Experimental results found in TiO2/UV system, Methomyl concentration and Bala Song of 0.5 h (t) will rapidly degrade, degradation trends can be a first-order reaction is described, and its reaction rate constant with The Methomyl Bala Song concentration is reduced, increasing with the increase in TiO2 concentration. If you add too much catalyst will be due to the shadowing effect, time and extend the photocatalytic efficiency reduce degradation of efficiency, and the experimental observation (0 g to 1.5 g), the initial Methomyl, and Bala Song pesticide aqueous solution, both very similar to the trend of degradation of its concentration at 30 min (t) quickly reduced, while the rate of degradation after 30 min (t) is gradually moving towards linear presented by degradation results show that under the experiment TiO2 / Methomyl optimum concentration of 0.75 g / L, Bala Song the optimal concentration of 1 g / L, and the pH value pH4 (weak acid), pH10 (weak), since the electrons in the solution was added to the reaction mechanism , presented Hydrolysis Both contain a higher degradation efficiency.
The use of UV / visible spectrophotometer (UV / Vis) analysis, Methomyl Bala Song TiO2/UV system, the solution obtained by the reaction of ammonia (NH4 +) and nitrate nitrogen (NO2-) and nitrite nitrogen (NO3-) and phosphate (PO4-)analytical results, due to the strong oxidizing environment, photocatalytic oxidation treatment to make them completely inorganic, and quantitative formation of nitrite nitrogen (NO3-), phosphate (PO4-), carbon dioxide (CO2) and other inorganic product.
Although so far, the use of this method of degrading organic pollutants in the wastewater is not popular, and the article will TiO2 photodegradation technology applied to a containing methomyl Bala Song wastewater degradation, pesticide wastewater to solve the natural water bodies purification and environmental issues related to overcome the conventional wastewater treatment technologies purification not completely disadvantages and can save the high cost of land, time and energy consumption, a high treatment efficiency and secondary contamination can be avoided purification technology.

摘要………………………………………………………………………………………… I
Abstract ……………………………………………………………………………………..II
誌謝…………………………………………………………………………………………Ⅳ
目錄…………………………………………………………………………………………Ⅴ
圖目錄………………………………………………………………………………………IX
表目錄…………………………………………………………………………………… ⅩII
第一章 緒論…………………………………………………………………………………...1
1.1研究緣起…………………………………………………………………………….1
1.2研究目的…………………………………………………………………………….2
1.3研究流程…………………………………………………………………………….3
第二章 文獻回顧……………………………………………………………………………...4
2.1臺灣農藥使用與現況……………………………………………………………….4
2.1.1臺灣的農藥管理…………………………………………………………………..5
2.1.2農藥的影響及傳輸途徑…………………………………………………………..6
2.1.3農藥銷售現況……………………………………………………………………..7
2.1.4中國農藥使用與現況……………………………………………………………10
2.1.5農藥類別與區分…………………………………………………………………11
2.1.6農藥之毒性與安全………………………………………………………………12
2.1.7農藥對生態環境的影響…………………………………………………………14
2.2氨基甲酸(酯)鹽類農藥與有機磷農藥…………………………………………….15
2.2.1氨基甲酸鹽(酯)類農藥…………………………………………………………..15
2.2.2納乃得農藥結構及物理化學性質………………………………………………17
2.2.3有機磷類農藥……………………………………………………………………19
2.2.4巴拉松農藥結構及物理化學性質………………………………………………22
2.2.5水體優養化………………………………………………………………………24
2.3常用農藥廢水的處理方式…………………………………………………………25
2.3.1溶劑萃取回收法…………………………………………………………………26
2.3.2生物處理法………………………………………………………………………26
2.3.3活性碳吸附法……………………………………………………………………27
2.3.4化學氧化法………………………………………………………………………27
2.3.5濕式空氣氧化技術………………………………………………………………28
2.3.6電解法…………………………………………………………………………….28
2.3.7光催化法…………………………………………………………………………28
2.4高級氧化處理程序(Advanced Oxidation Processes，AOPs)…………………….31
2.4.1光觸媒降解技術…………………………………………………………………31
2.4.2二氧化鈦(TiO2)特性………………………………………………………….....32
2.4.3 TiO2光觸媒催化原理…………………………………………………………..34
2.4.4二氧化鈦(TiO2)的超親水(油)特性……………………………………………38
2.4.5二氧化鈦反應機制…………………………………………………………… 39
2.4.6二氧化鈦的用量……………………………………………………………… 41
2.4.7添加劑的種類………………………………………………………………… 41
2.4.8觸媒的毒化…………………………………………………………………… 42
2.4.9二氧化鈦的來源……………………………………………………………… 42
2.4.10晶相分析………………………………………………………………………44
2.4.11表面結構分析…………………………………………………………………47
2.5反應條件與影響…………………………………………………………………49
2.5.1光強度及光波長……………………………………………………………… 49
2.5.2光解半衰期……………………………………………………………………49
2.5.3光催化之動力學………………………………………………………………51
2.5.4降解反應動力模式……………………………………………………………53
2.6氧氣的催化反應…………………………………………………………………55
2.7礦化作用…………………………………………………………………………55
第三章 研究內容、材料與方法…………………………………………………………….57
3.1研究內容…………………………………………………………………………57
3.2試劑製備方法及步驟……………………………………………………………57
3.2.1檢量線溶液之配製……………………………………………………………57
3.2.2市售巴拉松及納乃得溶液之配製……………………………………………57
3.2.3 pH調整試劑……………………………………………………………………57
3.2.4檢量線配製方法……………………………………………………………… 58
3.3常見光源與選擇…………………………………………………………………59
3.3.1氙燈(xenon lamp)………………………………………………………………59
3.3.2高壓汞燈………………………………………………………………………60
3.3.3反應器光源選擇………………………………………………………………61
3.3.4反應器裝置……………………………………………………………………63
3.4背景與光解試驗分析方法………………………………………………………65
3.4.1吸附反應試練…………………………………………………………………65
3.4.2暗箱自然降解試驗……………………………………………………………65
3.4.3自然日光光解試驗……………………………………………………………66
3.4.4單一農藥UV光解試驗………………………………………………………66
3.4.5不同pH值對納乃得與巴拉松溶液降解之影響……………………………66
3.4.6轉速對於納乃得、巴拉松溶液試驗之影響…………………………………67
3.4.7含氮化合物中間產物的分析方法……………………………………………67
3.4.8含磷化合物中間產物的分析方法……………………………………………67
3.4.9總有機碳測定分析……………………………………………………………68
第四章 結果與討論………………………………………………………………………….69
4.1背景實驗…………………………………………………………………………69
4.1.1吸附反應試驗結果……………………………………………………………69
4.1.2納乃得、巴拉松在暗箱自然降解試驗結果…………………………………72
4.1.3自然日光光解試驗結果………………………………………………………74
4.1.4自然日光+TiO2觸媒光解試驗結果………………………………………… 77
4.2單獨UV光解及TiO2/UV之不同參數試驗結果………………………………79
4.2.1 UV光解實驗之分析結果…………………………………………………… 79
4.2.2 TiO2/UV之試驗結果………………………………………………………… 81
4.2.3不同pH值對納乃得、巴拉松溶液降解之試驗結果……………………… 89
4.2.4轉速對納乃得、巴拉松溶液降解之影響結果………………………………92
4.2.5納乃得、巴拉松溶液TOC濃度變化與TOC去除率………………………92
4.3反應速率方程式…………………………………………………………………93
4.4結構關係對降解效果的影響……………………………………………………99
4.5降解產物之鑑定…………………………………………………………………100
4.5.1納乃得經二氧化鈦光觸媒反應程序中之降解產物鑑定……………………100
4.5.2巴拉松經二氧化鈦光觸媒反應程序中之降解產物鑑定……………………102
第五章 結論………………………………………………………………………………...104
第六章 參考文獻…………………………………………………………………………...106

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