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甲基苯駢三唑雜環化合物環境友善型氧化反應催化研究 = Study on ...

國立高雄大學應用化學系碩士班

甲基苯駢三唑雜環化合物環境友善型氧化反應催化研究 = Study on enviromental benign catalytic oxidation of tolyl triazole heterocyclic compounds

紀錄類型:	書目-語言資料,印刷品 : 單行本
並列題名:	Study on enviromental benign catalytic oxidation of tolyl triazole heterocyclic compounds
作者:	梁鼎煒,
其他團體作者:	國立高雄大學
出版地:	[高雄市]
出版者:	撰者;
出版年:	2009[民98]
面頁冊數:	118面圖、表 : 30公分;
標題:	四氧化三鈷
標題:	carboxy-benzotriazole
電子資源:	http://handle.ncl.edu.tw/11296/ndltd/62388961672044266163
附註:	參考書目：面106-109
附註:	指導教授：蔡振章
摘要註:	本文研究新型環境友善型氧化技術，甲基苯駢三唑(tolyl triazole, TTA)氧化生成羧基苯駢三氮唑(carboxy-benzotriazole, CBT)，期能取代傳統劑量高錳酸鉀與硝酸等強氧化劑的方法，避免氧化劑毒性與生產過程之廢棄物排放問題，提高反應選擇性及產率。以金屬氧化物觸媒催化氧化反應，TBHP氧化劑，探討不同參數以期達到最高效能。結果發現，溶劑種類對於氧化反應性能會有顯著影響，以水 – 異丁醇混合溶劑之反應結果最佳。Mn3O4催化可達約15% CBT產率，性能優於其他錳金屬氧化物。擔載於二氧化矽所製備之氧化錳擔載觸媒，氯化錳為前驅物之擔載觸媒呈現Mn3O4晶相，催化TTA轉化率18%，CBT選擇率91%，催化結果優於其他錳化合物擔載觸媒呈現Mn2O3晶相之擔載觸媒。同時發現，鹼性添加劑可大幅增加金屬氧化物之轉化率和酸選擇率，其中使用四氧化三鈷為觸媒，於異丁醇–水混和溶劑中添加氫氧化鈉，可以大幅提升轉化率近4倍和酸選擇性2倍，並抑制副產物醛生成，CBT最高產率可達約43%。醋酸鈷、醋酸鎳、醋酸銅等金屬鹽類化合物之甲基苯駢三唑氧化反應催化結果以醋酸鈷較佳，不過發現產生不為UV光譜所吸收之副產物，造成反應物損失，然而醋酸鹽類並不會造成甲基吡啶產生回收問題，原因仍需進一步研究探討。 Traditionally, oxidation tolyl triazole (TTA) to carboxy-benzotriazole (CBT) is catalyzed by potassium permanganate and the nitric acid. This process is corrosive, toxic and pollutant with excessive MnO2 waste formation. This study is devoted to the study of new environment friendly oxidation catalyses in the presence of peroxide oxidants.Several factors were studied. It was found that Mn3O4 has better catalysis performance than other transition metal oxide catalysts. In addition, solvent affected catalysis performance significantly. The best solvent system was found to be water – tert-butanol solvent mixture. Oxidation over Mn3O4 reaching 15% CBT yield was superior to other manganese oxides. Crystal phase of SiO2 supported manganese oxide differed with various manganese precursors among which manganese chloride precursor producing Mn3O4 crystalling phase showed the highest TTA conversion of 18% and CBT selectivity of 91%.Furthermore, it was found that alkaline solution can greatly accelerate oxidation rate and promote carboxylic acid product selectivity in the compensation of aldehyde product selectivity. Particularly, Co3O4 catalyst showed higher conversion by nearly four folds at two times higher selectivity, producing CBT yield of 43%. Althogh the conversion over cobalt acetate was higher than other metallic salt compounds/metal oxides, its produces selecitivy was rather low with formation of UV insensitive by-products. On the other hand, methyl-picoline behaved differently.Several transition metal oxide on mesoporous silica (metal oxide@mesoporous silica) prepared by direct synthesis method were tested. It was found that with t-butyl hydroperoxide oxidant, the catalytic activity ranks in the order of Cr >> Cu > Co > Mn >> Fe > V > Ti > W, which is attributed to the influence of reaction mechanism. The catalytic activity over early transition metal oxides (V, Ti, W) by means of perxometal mechanism was lower than that over other metal oxides through oxometal mechanism. Over the various Cr2O3 samples, Cr2O3@mesoporous silica prepared by direct synthesis showed better catalytic performance than Cr2O3/SiO2 prepared by impregnation, which had TTA conversion of 31.1% and 17.6%, respectively with similar CBT selectivity about 87%.

甲基苯駢三唑雜環化合物環境友善型氧化反應催化研究 = Study on enviromental benign catalytic oxidation of tolyl triazole heterocyclic compounds
梁, 鼎煒

甲基苯駢三唑雜環化合物環境友善型氧化反應催化研究 = Study on enviromental benign catalytic oxidation of tolyl triazole heterocyclic compounds / 梁鼎煒撰 - [高雄市] : 撰者, 2009[民98]. - 118面 ; 圖、表 ; 30公分.
參考書目：面106-109指導教授：蔡振章.
四氧化三鈷carboxy-benzotriazole

甲基苯駢三唑雜環化合物環境友善型氧化反應催化研究 = Study on enviromental benign catalytic oxidation of tolyl triazole heterocyclic compounds
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330 $a 本文研究新型環境友善型氧化技術，甲基苯駢三唑(tolyl triazole, TTA)氧化生成羧基苯駢三氮唑(carboxy-benzotriazole, CBT)，期能取代傳統劑量高錳酸鉀與硝酸等強氧化劑的方法，避免氧化劑毒性與生產過程之廢棄物排放問題，提高反應選擇性及產率。以金屬氧化物觸媒催化氧化反應，TBHP氧化劑，探討不同參數以期達到最高效能。結果發現，溶劑種類對於氧化反應性能會有顯著影響，以水 – 異丁醇混合溶劑之反應結果最佳。Mn3O4催化可達約15% CBT產率，性能優於其他錳金屬氧化物。擔載於二氧化矽所製備之氧化錳擔載觸媒，氯化錳為前驅物之擔載觸媒呈現Mn3O4晶相，催化TTA轉化率18%，CBT選擇率91%，催化結果優於其他錳化合物擔載觸媒呈現Mn2O3晶相之擔載觸媒。同時發現，鹼性添加劑可大幅增加金屬氧化物之轉化率和酸選擇率，其中使用四氧化三鈷為觸媒，於異丁醇–水混和溶劑中添加氫氧化鈉，可以大幅提升轉化率近4倍和酸選擇性2倍，並抑制副產物醛生成，CBT最高產率可達約43%。醋酸鈷、醋酸鎳、醋酸銅等金屬鹽類化合物之甲基苯駢三唑氧化反應催化結果以醋酸鈷較佳，不過發現產生不為UV光譜所吸收之副產物，造成反應物損失，然而醋酸鹽類並不會造成甲基吡啶產生回收問題，原因仍需進一步研究探討。 Traditionally, oxidation tolyl triazole (TTA) to carboxy-benzotriazole (CBT) is catalyzed by potassium permanganate and the nitric acid. This process is corrosive, toxic and pollutant with excessive MnO2 waste formation. This study is devoted to the study of new environment friendly oxidation catalyses in the presence of peroxide oxidants.Several factors were studied. It was found that Mn3O4 has better catalysis performance than other transition metal oxide catalysts. In addition, solvent affected catalysis performance significantly. The best solvent system was found to be water – tert-butanol solvent mixture. Oxidation over Mn3O4 reaching 15% CBT yield was superior to other manganese oxides. Crystal phase of SiO2 supported manganese oxide differed with various manganese precursors among which manganese chloride precursor producing Mn3O4 crystalling phase showed the highest TTA conversion of 18% and CBT selectivity of 91%.Furthermore, it was found that alkaline solution can greatly accelerate oxidation rate and promote carboxylic acid product selectivity in the compensation of aldehyde product selectivity. Particularly, Co3O4 catalyst showed higher conversion by nearly four folds at two times higher selectivity, producing CBT yield of 43%. Althogh the conversion over cobalt acetate was higher than other metallic salt compounds/metal oxides, its produces selecitivy was rather low with formation of UV insensitive by-products. On the other hand, methyl-picoline behaved differently.Several transition metal oxide on mesoporous silica (metal oxide@mesoporous silica) prepared by direct synthesis method were tested. It was found that with t-butyl hydroperoxide oxidant, the catalytic activity ranks in the order of Cr >> Cu > Co > Mn >> Fe > V > Ti > W, which is attributed to the influence of reaction mechanism. The catalytic activity over early transition metal oxides (V, Ti, W) by means of perxometal mechanism was lower than that over other metal oxides through oxometal mechanism. Over the various Cr2O3 samples, Cr2O3@mesoporous silica prepared by direct synthesis showed better catalytic performance than Cr2O3/SiO2 prepared by impregnation, which had TTA conversion of 31.1% and 17.6%, respectively with similar CBT selectivity about 87%.
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