Please use this identifier to cite or link to this item: http://hdl.handle.net/11455/90140
標題: Effects of iron ions and pH on the oxidative removal of arsenite in an aerated zero-valent aluminum system
鐵離子及pH影響通氣的零價鋁系統氧化移除水溶液中之三價砷
作者: Che-En Hwang
黃&#x5586恩
關鍵字: Arsenite;ZVAl;Fenton-like reaction;砷;零價鋁;氧化
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Chromate reduction by zero-valent Al metals as catalyzed by polyoxometalate. Water Res. 43: 5015-5022 Matheson, L. J., and P.G. Tratnyek. 1994. Reductive Dehalogenation of Chlorinated Methanes by Iron Metal. Environ. Sci. Technol. 28 (12): 2045-2053. Ng, J.C., J. Wang and A. Shraim. 2003. A global health problem caused by arsenic from natural sources. Chemosphere 52: 1353-1359. O'Neill, P. 1995. Arsenic. In 'Heavy Metals in Soil' (B. J. Alloway, Ed.). Blackie Academic & Professional, Glasgow. Raven, K.P., A. Jain, and R.H. Loeppert. 1998. Arsenite and arsenate adsorption on ferrihydrite: Kinetics, equilibrium, and adsorption envelopes. Environ. Sci. Technol. 32: 344-349. Sadiq, M. 1997. Arsenic chemistry in siols: An overview of thermodynamic predictions and field observations. Water Air Soil Pollut. 93: 117-136. Scherer, M. M., S. Richter, R. L. Valentine, and P. J. J. Alvarez. 2000. Chemistry and microbiology of permeable reactive barriers for in situ groundwater clean up. Environ. 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摘要: 
Arsenic, a commonly found pollutant in the environment, has received much scientific concern because it, particularly in the inorganic form, is very toxic and carcinogenic to human. Arsenic consists of two major forms of As(III) and As(V). Since As(III) is more toxic than As(V), the oxidation of As(III) and subsequent removal of As(V) are considered an important strategy for treating arsenic contaminated sites. Fenton reaction, a well-known pathway of producing the OH radicals through the interaction of Fe(II) with H2O2 at an acidic solution, had been previously used to oxidize As(III). Recently, studies also find that zero-valent aluminum (ZVAl) exhibits an excellent efficiency of oxidizing As(III) in an aerobic system via a Fenton-like reaction. However, the presence of oxide layers on the surfaces of ZVAl would inhibit the OH radical productions, and a catalyst of polyoxometalates (POM) was used to remove the oxide layer and enhance the oxidant formation. The technique still needs some modifications because the POM is expensive and difficult to be recycled and reused. Thus, in the study, we tried to replace POM by Fe ions, including Fe(III) and Fe(III), in the ZVAl/O2 system to promote the Fenton-like reaction and enhance As(III) oxidation. In addition, Al beverage can (ABC) was also used as a substitute for ZVAl to investigate its potential efficiency for As(III) oxidation. Results showed that As(III) oxidation was indiscernible in the ZVAl/O2 system within the 360 min reaction; however, 80 μM As(III) could be completely oxidized in the ABC/O2 system within 120 and 360 min at pH 1 and 2, respectively. With the addition of Fe, 80 μM As(III) would be rapidly oxidized in both ZVAl/Fe(II)/O2 and ZVAl/Fe(III)/O2 system, and As(III) oxidation increased with an increase in Fe concentrations. During As(III) oxidation, the H2O2 accumulation was inhibited, a result demonstrating that Fe(III) could be reduced and reacted rapidly with H2O2 to promote As(III) oxidation. Besides, compared to ZVAl/Fe/O2 system, ABC/Fe(II)/O2 and ABC/Fe(III)/O2 system exhibited a higher oxidative ability at pH 1 and 2 because OH radicals could be produced through both Fenton and Fenton-like (i.e., H2O2 react directly with ABC) reactions. After As(III) oxidation, Al and Fe would co-precipitate with As(V), and 100% As(V) removal could be achieved when the solution pH was increased to 6.0. Because As associates commonly with Fe in the groundwater, the current results may provide a cost-effective method for treating As in the water body.

環境中的砷(As)尤其是無機砷(包括As(III)與As(V))的汙染問題是全球關注的環境議題之一,由於As(III)比As(V)有著較高的毒性與移動性,因此如何將As(III)氧化成As(V)並進一步移除已成為受砷汙染地區整治時的主要目標。過去已有許多氧化As(III)的相關報導,其中又以Fenton法最受重視,此法主要是利用Fe(II)與過氧化氫在酸性條件下生成具有高氧化能力的氫氧自由基(OH radical)來氧化As(III)。最近的文獻亦發現使用零價鋁(ZVAl)做為電子來源,在酸性通氧條件下同樣能進行Fenton-like反應產生OH radicals來進行As(III)的氧化,然而ZVAl表面常含有一層金屬氧化層,會抑制該氧化劑的產生,需使用polyoxometalates(POM)來消除此氧化層並促進反應進行,但因POM較為昂貴且有回收上的疑慮,故本實驗擬在ZVAl系統中嘗試加入Fe(III)或Fe(II)來取代POM並促進Fenton-like反應之效率及增強As(III)的氧化,同時也使用生活中常見之鋁罐代替ZVAl作為電子提供者,了解鋁罐系統對於As(III)氧化之效率。結果顯示,在酸性通N2環境下,ZVAl及鋁罐系統均有還原溶液中Fe(III)的能力。在As(III)氧化的實驗中,ZVAl/O2系統無論在pH 1.0或2.0下,360 min內均觀察不到As(III)的氧化;而鋁罐/O2系統在pH 1.0或2.0分別可在120 min及360 min內將80 μM的As(III)完全氧化。當加入Fe離子時,ZVAl/Fe(II)/O2系統及ZVAl/Fe(III)/O2系統均能有效氧化80 μM的As(III),反應速率隨著Fe的添加量而提高,且過程中雙氧水的累積明顯受到抑制,證明無論是Fe(II)或是Fe(III)均較不受氧化層的影響,可迅速生成OH radical氧化As(III)。而鋁罐/Fe(II)/O2系統及鋁罐/Fe(III)/O2系統無論在pH 1.0及2.0下均顯示了非常高之氧化效率,此因鋁罐本身和額外添加之Fe兩者能同時利用雙氧水產生氧化劑,因此有非常高之氧化效率。當As(III)被完全氧化之後,將各反應溶液之pH調整至6.0附近,使Fe/Al產生(氫)氧化物沉澱,並同時移除水溶液中之As(V),結果顯示,所有加入Fe離子的ZVAl與鋁罐通氧系統均能達到100 %之砷移除率,因地下水中鐵與砷常共同存在,此技術未來可利用於處理受地下水砷污染地區的一個便宜有效的方法。
URI: http://hdl.handle.net/11455/90140
Rights: 同意授權瀏覽/列印電子全文服務,2018-08-14起公開。
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