摘要本研究之目的以自製觸媒膜管應用於臭氧氧化高毒性含酚廢水，以多孔隙性陶瓷管作為支撐膜材並以水洗塗布法(wash-coat)覆蓋具高度臭氧催化活性之金屬氧化物為觸媒，以觸媒膜管反應器應用於處理含高毒性酚類廢水，並嘗試此系統與氧化處理後程序結合進行水資源回收並評估其效益。研究中陶瓷管上臭氧氧化活性金屬以硝酸鐵、硝酸銅作為原料，以氧化鋁無機陶瓷膜管為支撐材，研究中將鑑定陶瓷結構中金屬氧化物結晶構造對臭氧催化氧化活性之影響，及不同種類金屬鹽所製備陶瓷觸媒膜管催化氧化觸媒層活性及其對氫氧自由基生成量之影響。並進行氣-液接觸式(Gas-liquid Contactor) 觸媒反應器進行觸媒氧化反應，以觸媒反應器處理高毒性含酚廢水中污染物之轉化效率與TOC移除率之效能。研究結果也得知偏鹼性條件下有助系統氧化能力之提升，銅型觸媒催化活性高於鐵型觸媒，於鹼性條件下，120分鐘反應其酚轉化效率幾乎可達100%與TOC去除率銅型達 40%及鐵型20%以上，本研究結果亦發現酚臭氧氧化化過程中其自由基生成速率強烈受到pH之影響，臭氧分解反應與自由基生成處於競爭狀況共同影響酚污染物之轉化率及TOC降解率，另外亦針對觸媒反應器之氧化活性壽命作過詳細評估，由觸媒重複試驗也證明回收再利用的觸媒反應器經 5次重複試驗後在降解污染物的效率上仍然可達 99%以上，其催化氧化活性並無顯著降低。 AbstractThe purpose of this study is focus on the preparation of membrane contactor and applied for catalytic ozonation of phenolic effluents. The membrane contactor were prepared by coating iron and copper oxides on the ceramic support with wash-coat technology. The raw wash-coated membranes were activated by caicinating process in the suitable conditions. The activated membrane contactor were applied for the catalytic ozonation of phenol in aqueous soultion and valuated the comversion and TOC degredation of reaction. The oxidation process were attempted to connect with bio or chemical process in the wastewater treatment for the water resued considerartion. The iron nitrate and copper nitrate were used as the active metal sources in preparation of membrane contactor. The support materials were used the microporous alumina oxides tube. The composition of washcoat solution were preparaed with active metal salt and ethanol at 85C. After the washcoat material is well dissolved in the ethanol, the creamic tube was dipped in the solution and dry in the air for further activating the coated ceramic tube in the oven under the specfic conditions. The oxidation performance were valuated by the phenol conversion and TOC removal of oxidation. Based on the results of this study, the catalytic oxidation performance were promoted under the basic environment and the copper type membrane reactor was superior than the iron type in all tests. The completely conversion of phenol and over 40% TOC removal was achieved in 2 hours ozonation with 500 mg/L phenol at room temperature. All the tested samples showed that pH strong affect the free radical generation and oxidation performance of phenol in this study. The competition of ozone decomposition and catalytic ozonation dominated the performance of ozonation. The basic condition is bentifited to the catalytic ozonation mechanism in the investigation. After the life time test, it is indicated that membrane contactor presented the same ozonation performance after 5 times reused and over 99% phenol conversion can be also achieved in this study.
