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研究生:趙鵬文
論文名稱:以UV/TiO2程序處理氣相中三氯乙烷之研究
指導教授:謝永旭謝永旭引用關係
學位類別:碩士
校院名稱:國立中興大學
系所名稱:環境工程學系
學門:工程學門
學類:環境工程學類
論文種類:學術論文
論文出版年:1999
畢業學年度:87
語文別:中文
論文頁數:148
中文關鍵詞:異相光催化二氧化鈦三氯乙烷化學氣相沈積法
相關次數:
  • 被引用被引用:13
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本研究係以化學氣相沈積法披覆二氧化鈦光觸媒於環管狀反應器上,並採用365 nm波長之UV燈管置於反應器中央為激發光源,實驗採用連續流方式,進行三氯乙烷之異相光催化分解反應的探討。控制因子包括初始濃度、氣體流量、光強度、溼度、氧含量等。最後對反應後的最終產物作分析,以瞭解最終產物的影響因子及礦化情形。
ˉˉ實驗結果顯示,在各種操作參數下,三氯乙烷最高的分解速率為2.554 m mole/s-m2,最高的量子產量為 0.37,而轉換率平均在45 %以上最高可達99.93 %。其中,流量的增加使得反應速率呈現上升的趨勢,但在流量364 ml/min以上時,反應速率的增加則趨於平緩。就溼度的影響效應而言,在溼度小於154 mM時,反應速率隨著濕度的增加而增加,而在溼度大於154 mM時,反應速率則隨之下降。氧氣在反應中扮演著電子捕捉者的角色,而降低了電子-電洞對重組的速率,因此反應速率隨著氧氣的增加而上升,但當氧含量達12 %後,反應速率即達到穩定而不再上升。而濃度的增加使得反應速率增加,但轉換率卻隨之下降。光照強度的增加則增加了光子數目,使得反應速率上升,但同時也提高了電子-電洞對重組的速率,所以量子產量並沒有隨著增加。
ˉˉ本研究之反應動力可運用Langmuir-Hinshelwood之雙分子模式來描述,由模式模擬的結果可以得知反應速率與光照強度的0.58次方成正比,且水分子會與三氯乙烷競爭吸附TiO2表面的活化位置,但與氧分子卻無競爭吸附的現象。
在最終產物方面,當氧分子增加時,HCl、Cl2和CO2的產量均會隨著增加,但當濕度增加時,除了HCl的產量下降外,Cl2和CO2的產量卻會隨之上升。而由質量平衡可知,三氯乙烷之異相光催化的礦化程度不佳,推估三氯乙烷反應後並無完全地轉換為無機產物,而是以其他的中間產物型態存在。
摘要I
表目錄VII
圖目錄IX
第一章ˉ緒論1
1-1 前言1
1-2 研究目的5
第二章ˉ基礎理論與文獻回顧6
2-1ˉ揮發性有機物之特性及影響6
2-2ˉ紫外光∕半導體之光催化反應14
2-2-1 光化學反應14
2-2-2 半導體之基本性質與光催化特性20
2-2-3 光催化半導體之種類26
2-2-4 異相光催化反應之原理和機制28
2-3ˉ觸媒的催化理論33
2-4 光觸媒製備方法36
2-4-1 含浸法36
2-4-2 溶液凝膠法36
2-4-3 化學氣相沈積法37
2-5 光催化反應器41
2-6 影響光催化反應之因素46
2-6-1 停留時間46
2-6-2 溼度46
2-6-3 氧氣含量49
2-6-4 起始濃度50
2-6-5 光照強度51
2-6-6 溫度51
2-7 異相光催化反應之動力模式52
2-7-1 表面吸附現象53
2-7-2 等溫吸附方程式54
2-7-3 異相光催化之速率式55
第三章ˉ實驗設備與方法62
3-1ˉ實驗材料62
3-1-1ˉ實驗藥品62
3-1-2ˉ實驗氣體64
3-2ˉ實驗裝置及設備64
3-3ˉ實驗流程70
3-3-1 光觸媒之製備70
3-3-2ˉ背景實驗73
3-3-3ˉ異相光催化反應74
3-4 分析方法75
3-4-1ˉ光觸媒之定性分析75
3-4-2ˉ量子產量分析76
3-4-3ˉ反應動力分析78
3-4-4ˉ最終產物分析78
第四章ˉ結果與討論81
4-1 光觸媒製備81
4-1-1 披覆成果81
4-1-2 觸媒定性分析82
4-2 背景實驗86
4-2-1ˉ直接光解實驗86
4-2-2ˉ不照光實驗90
4-2-3ˉ異相光催化測試實驗90
4-2-4 觸媒活性持續性試驗93
4-3ˉ異相光催化反應93
4-3-1ˉ氣體流量對光催化反應的影響93
4-3-2ˉ溼度對光催化反應的影響98
4-3-3ˉ氧氣含量對光催化反應的影響100
4-3-4ˉ初始濃度對光催化反應的影響104
4-3-5ˉ光照強度對光催化反應的影響104
4-4ˉ量子產量107
4-5ˉ反應動力分析108
4-6 最終產物監測117
4-6-1 溼度對最終產物的影響117
4-6-2 氧氣對最終產物的影響119
4-6-3 質量平衡119
第五章ˉ結論與建議124
5-1 結論124
5-2 建議125
參考文獻127
附錄A 二氧化鈦及1,1,1-三氯乙烷的特性141
附錄B 相對溼度與絕對濕度之換算144
附錄C 流量與反應速率及轉換率之關係圖145
附錄D 三氯乙烷檢量線147
附錄E 最終產物檢量線148
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