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標題: 活性碳複合黃鐵礦材料製備及應用於處理四氯化碳污染物之探討
Synthesis of activated carbon/pyrite material for the remediation of carbon tetrachloride
作者: 簡維均
Chien, Wei-Chun
關鍵字: 氯化有機溶劑
Chlorinated solvents
reductive dechlorination
permeable reactive barrier
出版社: 環境工程學系所
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摘要: 本研究嘗試製備活性碳(Granular activated carbon, GAC)披覆黃鐵礦(Pyrite, FeS2)之反應性吸附材料,並探討其應用於處理四氯化碳(Carbon tetrachloride, CT)污染水體之可行性。實驗利用含浸法(Impregnation method)及鍛燒法(Calcination method)將FeS2披覆至GAC,形成GAC-FeS2複合材料,經由SEM分析發現GAC表面披覆許多角狀FeS2顆粒,其粒徑範圍約在80~100 nm;此外,XRD分析GAC-FeS2之圖譜顯示證實黃鐵礦之存在。批次實驗利用劑量為1 g/L之GAC-FeS2,於不同pH條件(pH 5.5~12),對100 mg/L CT之水溶液進行吸附及還原脫氯試驗,結果pH 12時,GAC-FeS2可有效對CT進行吸附並還原降解,反應28天觀測到脫氯百分率約為29%,並偵測到脫氯副產物氯仿(Chloroform, CF)生成,相較於其他pH條件,高pH環境下,FeS2本身氧化速率較快因而加速電子轉移,提升CT還原速率;此外,經XRD分析結果顯示,FeS2氧化生成赤鐵礦(Fe2O3)等鐵氧化物,並且在高pH環境下,鐵氧化物表面帶負電並吸引更多二價鐵鍵結,形成具有較高反應性之表面鍵結二價鐵,提高CT降解反應速率。當改變初始CT濃度,並觀察GAC-FeS2對CT還原速率影響,其結果得知CT之降解反應符合假一階反應動力模式,且在較低之初始CT濃度下CT還原速率較快。初始CT濃度為10 mg/L時,CT還原速率常數為0.057 day-1,隨著初始CT濃度增加至30及100 mg/L時,CT還原速率常數則分別降至0.039及0.023 day-1。
This study attempted to synthesize a reactive activated carbon by coating pyrite (FeS2) onto granular activated carbon (GAC) for the potential use of treating carbon tetrachloride (CT) contamination. The synthetic composites, i.e., GAC-FeS2 were successfully prepared by impregnation and calcination methods. SEM images showed that the particle size of FeS2 over GAC surface was about 80 to 100 nm. Furthermore, XRD patterns confirmed the existence of pyrite being coated on GAC. In batch experiments, the dosage of 1 g/L GAC-FeS2 under different pH conditions (pH 5.5~12) was employed for adsorbtion/dechlorination of 100 mg/L CT in aqueous phase. The results showed that GAC-FeS2 can effectively reduce CT within 28 days under pH 12 and 29% dechlorination and byproduct chloroform (CF) were observed. While comparing results among different pH conditions, dechlorination of CT was fast at high pH condition due to that FeS2 was promptly oxidized at alkaline pH and resulted in a fast electron transfer rate to accelerate dechlorination of CT. In addition, the result of XRD analysis showed that the FeS2 was mainly oxidized to form hematite (Fe2O3). The iron oxide species would attract more Fe2+ to form high reactive species, i.e., surface-bound Fe2+, and then increase CT reductive reaction rate. Then this study investigated effect of initial CT concentration on the CT reductive reaction rate. The results showed that CT degradation reaction fitted pseudo-first-order kinetic model. It was also found that the lower initial CT concentration results in the higher CT reductive reaction rate. When the initial CT concentration was 10 mg/L, CT reduction rate constant was 0.057 day-1; when the initial CT concentration increased to 30 and 100 mg/L, the CT reduction rate constants were reduced to 0.039 and 0.023 day-1, respectively.
其他識別: U0005-0108201210400700
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