臺灣博碩士論文加值系統

本研究藉電弧離子鍍(Arc ion plating, AIP)特有之高離子密度、設備簡單、製程溫度低及潔淨無公害等優勢，於工業用高分子聚對苯二甲酸二丁酯(Poly-Butylene Terephthalate, PBT)表面低溫合成具有光觸媒特性之二氧化鈦鍍膜的被覆技術，探討不同施鍍參數對鍍膜微觀組織、晶體結構以及保固性能的影響。更進一步分析所建置之光觸媒風扇元件進行以甲醇為例之空氣清淨效能及其分解效率的動力學行為，為評估實現「無濾網」式的空氣淨化風扇之可行性，從而擴大光觸媒二氧化鈦鍍膜的應用範疇。
研究結果顯示：以電弧離子鍍被覆技術可以成功地藉由調整沉積總壓、弧電流及沉積時間等變數製備出具有銳鈦礦相結構之TiO2鍍膜。其中鍍膜沉積速率高達6.0 um/h，明顯高於許多PVD製程。在保固特性方面；對應於不同沉積總壓、弧電流及沉積時間所得之TiO2鍍膜其鉛筆硬度落於4H到5H之間，且附著性可達到規範最高等級5B。這表示在AIP沉積技術之下的確可提供TiO2鍍膜與基材之間高度附著性的保證。
於分解甲醇氣體之空氣清淨實驗結果中得知：以波長382.2 nm之UV-LED照射未施鍍的PBT風扇或是未施予UV-LED照射之TiO2光觸媒風扇需花費超過12小時來分解甲醇氣體，而且其數據線藉由取樣微分後呈現兩段斜率。發現之所以產生兩段斜率是因為甲醇氣體吸附於腔體內的器壁表面而提高分解甲醇氣體的難度造成兩段不同的斜率(活化能)在影響反應進行。沉積總壓0.25 Pa、弧電流80 A及沉積25 min所得之光觸媒風扇組受到 UV-LED照射可獲得最佳分解時間約為3小時。後續為了確認出最佳甲醇分解效率光觸媒風扇之動力學行為，將腔體溫度設定為298K、303K、313K及323K分別進行甲醇氣體分解效率試驗。藉由亞瑞尼士方程式所求出之光觸媒風扇於初期及後期之甲醇分解活化能為5.6 KJ/mole及16.0 KJ/mole，明顯低於其他種類觸媒催化甲醇所需之活化能值。分析兩段動力學行為發現：分解甲醇的過程中中間物會降低二氧化鈦之光催化活性，導致後期活化能提升阻礙反應的進行。在評估不同製程參數及所得鍍膜之晶體結構可知：當鍍膜沉積至一定厚度時其結晶性與甲醇分解效率不僅都能獲得相當顯著的提升，更能降低反應活化能促進甲醇分解效率的提升。故若有機會實際商品化本研究所研發之光觸媒風扇時，應當以提升鍍膜厚度為優先考量藉此獲得足夠的銳鈦礦相鍍膜結晶性，以取得最佳的光催化能力分解甲醇或是同質性的有機氣體。

Arc ion plating (AIP) beneficial from high cathode ionization rate, simple procedure, low process temperature, high film deposition rate, strong film adhesion and environmental friendly, are employed in this study to establish the coating technique for depositing photocatalytic titanium dioxide layer on poly-butylene terephthalate (PBT) surface. The correlation among deposition parameter, microstructure, crystalline structure and mechanical performance of TiO2 coating were discussed as well. Furthermore, the photodecomposition efficiency of methanol for TiO2-coated fan device and its kinetic behavior to the decomposition of methanol were also measured for evaluating the feasibility of this filter-free air purification fan device.
The experimental results indicated that by adjusting the coating parameters including total pressure, cathode current and deposition time, the TiO2 coating with major anatase phase and minor rutile phase strucutre could be successfully fabricated. The deposition rate with single cathodic source could reach 6.0 �慆/h. For mechanical performance, pencil hardness values of TiO2 coated specimens are between 4H to 5H. The coating adhesion by tape test grades 5B, the highest rank of specification. These all indicate that the AIP depositing technique could provide satisfactory mechanical performance of the TiO2 coating.
The photodecomposition efficiency of fan blade (without and with TiO2-coating) to methanol was revealed without and with 382.2 nm UV-LED illuminating over 12 hr. Moreover, two separated slopes were found for the curve of methanol concentration as a function of decomposition time, indicating two different activation energies during decomposing methanol. It is believed that methanol gas absorbed on the fan blade and the inner wall of chamber surface rise the difficult in decomposing methanol gas. However, the TiO2-coated fan blade deposited under 0.25 Pa oxygen pressure, 80 A cathode current and 25 min deposition time with UV-LED illuminating show that the optima decomposition time is 3.05 h. Based on the calculation of this particular case, it is found that activation energy of photodecomposition give two individual value, 5.6 KJ/mole and 16.0 KJ/mole, respectively, far lower than the value for other reported catalytic materials could provide (100~500 KJ/mole). The reduced reaction activation energy and ease of chemical reaction is obtained. It is believed that the CO intermediate absorbed on the TiO2 surface retards photocatalytic reaction and consequently two separated activation energies. Taking all coating parameters into consideration, not only the crystallinity degree of the deposits and methanol decomposition efficiency could both be promoted when deposited film came to a certain thickness. It is therefore recommended that a satisfactory film thickness for acquiring the sufficient film crystallinity would be first priority to provide the optima photodecomposition efficiency for methanol gas or other volatile organic compounds when commercializing the photocatalytic fan blade developed in this study.

誌謝.................................................. I
中文摘要.............................................. II
Abstract ............................................. IV
總目錄 ............................................. VI
圖目錄 ............................................. VIII
表目錄 ............................................. X
第一章 前言 .........................................1
第二章 文獻回顧......................................3
2-1 空氣污染..................................... 3
2-1-1 一氧化碳......................................4
2-1-2 二氧化氮......................................5
2-1-3 二氧化硫......................................6
2-1-4 微粒..........................................6
2-1-5 有機揮發性氣體化合物..........................7
2-2 有機甲醇物質分解模式..........................9
2-2-1 甲醇分解......................................9
2-2-2 蒸氣重組......................................9
2-2-3 甲醇部分氧化..................................9
2-3 空氣清淨方法..................................10
2-3-1 物理吸附......................................10
2-3-2 負離子........................................11
2-3-3 光化學分解....................................12
2-4 光觸媒........................................12
2-4-1 光觸媒材料....................................13
2-4-2 光觸媒活性控制因素............................19
2-4-3 二氧化鈦晶結構................................23
2-4-4 二氧化鈦晶面..................................27
2-4-5 二氧化鈦光觸媒反應機制........................27
2-5 二氧化鈦光觸媒應用............................36
2-5-1 抗菌..........................................36
2-5-2 自潔..........................................39
2-5-3 污水處理......................................43
2-5-4 空氣淨化......................................44
2-6 二氧化鈦被覆技術..............................46
2-6-1 薄膜成長過程..................................46
2-6-2 二氧化鈦鍍膜沉積技術..........................47
2-7 研究動機......................................57
第三章 研究方法......................................58
3-1 電弧離子鍍二氧化鈦鍍膜........................58
3-1-1 基材準備......................................58
3-1-2 製備二氧化鈦鍍膜..............................60
3-2 二氧化鈦鍍膜之顯微與晶體結構分析..............64
3-2-1 SEM形貌觀察...................................64
3-2-2 XRD結構分析...................................64
3-3 二氧化鈦鍍膜之保固性..........................64
3-3-1 鉛筆硬度試驗..................................64
3-3-2 附著力試驗....................................65
3-4 二氧化鈦鍍膜之空氣清淨........................67
第四章 結果與討論....................................72
4-1 電弧離子鍍二氧化鈦的成長行為..................72
4-1-1 不同沉積參數所得二氧化鈦鍍膜XRD結構分析.......74
4-1-2 不同沉積參數所得二氧化鈦鍍膜SEM形貌觀察.......79
4-2 電弧離子鍍二氧化鈦的保固性....................81
4-2-1 二氧化鈦鍍膜的鉛筆硬度........................81
4-2-2 二氧化鈦鍍膜的附著性..........................81
4-3 電弧離子鍍二氧化鈦之空氣清淨效能..............83
4-3-1 二氧化鈦光觸媒風扇針對甲醇氣體之分解效率......83
4-3-2 最佳甲醇分解效率光觸媒風扇之動力學行為........88
第五章 結論..........................................94
參考文獻...............................................95
研究成果...............................................113
壹. 參與計畫......................................113
貳. 發表論文......................................113
參. 獲獎記錄......................................116

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