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    Please use this identifier to cite or link to this item: https://ir.csmu.edu.tw:8080/ir/handle/310902500/18743


    Title: 以微波輔助多元醇法製備鎳、鉑/二氧化鈦複合型光觸媒去除甲苯之研究
    Synthesizing Pt-Ni co-doped TNT photocatalyst with microwave-assisted polyol method for toluene removal
    Authors: 游子毅
    You, Zih-Yi
    Contributors: 盧啟元
    Keywords: 多元醇法;二氧化鈦奈米管;甲苯去除;田口方法;信號雜訊比
    Polyol method;TNT;Toluene degradation;Taguchi methods;S/N ratio
    Date: 2017
    Issue Date: 2018-03-07T07:50:17Z (UTC)
    Abstract: 本研究使用微波輔助多元醇法合成Pt-Ni-C/TNT光觸媒，並利用田口方法─L9直交表設計三個3水準之觸媒製備參數組合，選擇以甲苯作為Pt-Ni-C/TNT在可見光照射下光催化活性測試的目標汙染物，透過ANOVA、S/N信號比分析實驗數據，評估適合的觸媒製備參數組合，並以TEM、XRD、XPS及BET進行觸媒的物化特性分析。

    首先，以150?C水熱法合成的TNT-150展現出最佳的孔道結構因此被選為M/TNT光觸媒製備的基礎材料，在去除甲苯的測試中，Pt-Ni/TNT的表現結合了Ni/TNT、Pt/TNT兩種觸媒的優點，包含良好光催化活性以及穩定的光催化反應性，但從XPS分析結果中發現，金屬微波加熱還原過程中，Ni、Pt離子會競爭還原所需能量，使金屬還原效率減低，將鉑顆粒搭載於已製備之Ni/TNT觸媒上可改善此現象之發生，並提升觸媒對甲苯的去除效率，達到55%的去除效果；然而經長時間的測試，伴隨著觸媒失活情形的發生，為抑制觸媒的失活，本研究在觸媒Pt-Ni/TNT中添加了碳元素，結果顯示，隨著觸媒中碳重量百分比提升，觸媒的光催化活性也隨之增加，其中以Pt-Ni-10%C/TNT展現出較佳的甲苯去除率，從XRD的分析結果說明碳的搭載會抑制觸媒中金紅石(Rutile)晶相的生成，而Pt-Ni-C/TNT的光催化活性則隨著Anatase/Rutile增加而有所提升，此外，高比表面積以及大的孔隙體積也是增進觸媒光催化活性的重要因子。

    微波功率、加熱時間以及非金屬之添加選為3個觸媒製備的控制條件，並以ANOVA、S/N比分析實驗數據，探討Pt-Ni-C/TNT觸媒的最佳製備參數組合。ANOVA分析結果說明三項參數之間對於觸媒的光催化效率的影響力並無顯著差異；計算S/N比則發現微波功率對觸媒光催化活性影響最大，其次為非金屬的添加方式，最後為加熱時間，Pt-Ni-C/TNT的觸媒最佳製備參數組合為微波功率600w、加熱時間120s以及在觸媒製備過程中以氨水處理摻雜氮元素。Pt-Ni-C/TNT photocatalysts were prepared by the microwave assisted polyol method in this study. The Taguchi’s orthogonal array L9 was employed to study the parameters of preparation, including three factors and three levels. Toluene was chosen as a gaseous reactant for activity test on Pt-Ni-C/TNT under visible light irradiation. Then, the experimental results were analyzed by the ANOVA and S/N ratio to evaluate the suitable parameters for Pt-Ni-C/TNT preparation. The characterizations of photocatalysts were analyzed by TEM, XRD, XPS, and BET.
    First, TNT-150 was synthesized at 150?C by the hydrothermal method and chosen for M/TNT photocatalysts preparation with optimum mesoporous structure. The toluene removal efficiencies over M/TNT catalysts showed that Pt-Ni/TNT presented the two advantages of good photocatalytic activity and photocatalytic stabilization from Ni/TNT and Pt/TNT, respectively. During the microwave assisted heating process of the Pt-Ni/TNT preparation, the XPS analysis results indicated that the metals reduction efficiencies were decreased with the competition of energy between Ni and Pt ions. Then, the modified preparation of Pt-Ni/TNT was carried out by doping Pt particles on the synthesized Ni/TNT. Pt-Ni/TNT showed the improved toluene removal efficiency arrived at 55%; however, the decay of photocatalyst was observed after long time reaction. Finally, the carbon was doped on the Pt-Ni/TNT to inhibit the decay under visible light irradiation. One can see that the photocatalytic activity was increased with Carbon loading weight, and Pt-Ni-10%C/TNT presented the better toluene removal efficiency than others. XRD patterns showed that the amount of rutile phase was inhibited with Carbon doped. The photocatlaytic activity of Pt-Ni-C/TNT was improved with the increase of the Anatase/Rutile ratio. Moreover, the high specific surface area and large pore volume of Pt-Ni-C/TNT were also the factors for improvement of photocatalytic activity.
    For the analysis of ANOVA and S/N ratio, power of microwave, heating time, and the addition of nonmetal were chosen as three factors to study the optimum parameters of Pt-Ni-C/TNT preparation on toluene photocatalytic removal. The analysis results of ANOVA showed that there was no obviously different between those three factors on toluene removal. The S/N values presented that the level effects of the factors was in the order power of microwave > the addition of nonmetal > heating time. The optimum parameters for the power of microwave was 600w, that for the heating time was 120s, and that for the addition of nonmetal was N (from ammonia).
    URI: https://ir.csmu.edu.tw:8080/ir/handle/310902500/18743
    Appears in Collections:[公共衛生學系暨碩士班] 博碩士論文

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