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研究生:鄭富吉
研究生(外文):Fu-ChiCheng
論文名稱:以過錳酸鉀改質鐵氧化物對砷吸附之研究
論文名稱(外文):Study on the Adsorption of Arsenic by Using Iron Oxide Modified by KMnO4
指導教授:黃耀輝黃耀輝引用關係
指導教授(外文):Yao-Hui Huang
學位類別:碩士
校院名稱:國立成功大學
系所名稱:化學工程學系碩博士班
學門:工程學門
學類:化學工程學類
論文種類:學術論文
論文出版年:2010
畢業學年度:98
語文別:中文
論文頁數:104
中文關鍵詞:鐵氧化物吸附三價砷
外文關鍵詞:iron oxideadsorptionarsenite
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本研究以KMnO4改質鐵氧化物(BT4),製備出吸附材(MBT4),對三價砷(As(III))進行吸附研究,藉由觀察水中的錳離子和砷離子濃度變化來推倒MBT4對三價砷的吸附機制。
對鐵氧化物(BT4)顆粒進行鑑定與分析,由XRD的鑑定BT4為含微量結晶的α-FeOOH,粒徑為0.125~0.25mm,由BET分析出比表面積為154m2/g。
吸附材改質實驗結果顯示,MBT材料上的錳負載量隨著進料鐵/錳莫耳比(FeCl2/KMnO4)的增加而下降,並發現BT4本身即可與MnO4-反應,不需外加FeCl2 ,反應24小時後,MBT4的錳負載量可達1.24 mg/g。
吸附砷實驗結果顯示,MBT4對As(III)吸附量為12.82 mg/g大於未改質BT4對As(III)吸附量(10.87 mg/g)。在吸附動力方面,以一階動?模式、擬二階動?模式和二階動力模式來模擬,發現MBT4對As(III)的吸附較符合擬二階動?模式和二階動力模式。在等溫吸附實驗方面,以Langmuir Model與Freundlich Model來討論,發現較符合Freundlich Model。最後,討論陰離子對MBT4吸附As(III)的干擾,以磷酸鹽的影響最大,硫酸鹽次之,硝酸鹽影響很小。在MBT4對As(III)的吸附機制的探討上,本研究推測為As(III) 先與MBT4的含錳有效活性座進行氧化反應,將As(III)被氧化為As(V),MBT4再將As(V)吸附移除,故提高近二成的As吸附量。

In this study, we modified iron oxide (BT4) by using KMnO4 to prepare a new adsorbent-MBT4 which was used to removal arsenite (As(III)) from water solution. We detected the concentration variation of As(III) and Mn in the solution to investigate the adsorption mechanism.
We take appraisement and analysis for iron oxide (BT4). The result of XRD showed that BT4 contained lots of amorphous goethite (α-FeOOH). The particle size range was 0.125~0.25 mm.The Specific surface area of BT4 was 154 m2/g by using BET analysis.
When the feed Fe/Mn molar ratio (FeCl2/KMnO4) increased, the capacity of Mn loading on MBT4 decreased. We also found that BT4 could react with MnO4- by itself. The capacity of Mn loading on MBT4 was 1.24 mg/g after 24 hours of the reaction.
The As adsorption capacity of MBT4 was 12.82 mg/g which is higher than that of BT4 (10.87 mg/g). Three models were used to describe the adsorption kinetics. Pseudo-second-order rate equation and the second-order rate equation were more suitable than the first-order Lagergren equation . For adsorption isotherm, Freundlich Model was better than Langmuir Model. The competition of nitrate, sulfate and phosphate with arsenate was also studied. Phosphate and sulfate decreased the arsenate removal efficiency. Nitrate had no obvious effect on the adsorption of arsenite. The mechanism of removal As(III) by MBT4 was proposed. Intially, As(III) was oxidateed by Mn oxide on MBT4. As(III) was transformed into As(V).Finally, MBT4 adsorbed As(V).

中文摘要 I
Abstract II
誌謝 III
目錄 IV
表目錄 VI
圖目錄 VII
第一章緒論 1
1-1研究動機 1
1-2研究目的與內容 2
第二章文獻回顧 3
2-1砷的介紹 3
2-1-1砷的來源 3
2-1-2砷的特性 7
2-1-3砷對人體的危害 10
2-1-4水中砷的去除方法 11
2-2 氧化鐵的種類與應用 14
2-2-1 氧化鐵的種類 14
2-2-2 鐵氧化物表面化學特性 16
2-3 吸附理論 23
2-3-1 物理吸附理論 24
2-3-2 化學吸附理論 24
2-3-3 特定吸附與非特定吸附 25
2-3-4 等溫吸附模式 26
2-4 鐵系材料對砷吸附之討論 29
第三章實驗設備材料與方法 33
3-1 研究架構及流程 33
3-2 吸附材料基本性質鑑定 35
3-2-1 XRD晶相分析 35
3-2-2 SEM表面形態觀察 37
3-2-3 EDS表面元素分析 39
3-2-4 比表面積與孔隙分佈 41
3-2-5 化學結構分析 41
3-2-6 覆膜總鐵量和總錳量分析 42
3-2-7 零電位點(Zero-point surface charge, pHzpc) 常數測定 43
3-2-8 真密度與孔隙率量測 44
3-3 吸附實驗 45
3-3-1 實驗藥品 45
3-3-2 實驗設備 45
3-3-3 實驗步驟 46
3-3-4 水樣分析 48
第四章 實驗結果與討論 51
4-1 BT4材料基本性質與鑑定分析 51
4-1-1 BT4材料基本性質 51
4-1-2 BT4晶相分析 52
4-1-3 表面形態觀察與元素分析 54
4-1-4 BT4之比表面積 57
4-1-5 化學結構分析 59
4-2 BT4吸附砷 61
4-3 KMnO4改質BT4 63
4-3-1 Fe/Mn莫耳比對錳負載之影響 63
4-3-2 KMnO4濃度對錳負載量之影響 66
4-4 MBT4處理As(III)之探討 68
4-4-1 錳覆膜量對吸附As (III)之影響 68
4-4-2 吸附劑量對吸附As(III)之影響 76
等溫吸附曲線 82
4-5 等溫吸附曲線 82
4-6 陰離子效應 85
第五章 結論與建議 87
5-1 結論 87
5-2 建議 89
參考文獻 90
附錄A-鐵氧化物BT4來源描述與pHzpc實驗 96
附錄B-鐵氧化物BT4對As(V)的吸附討論 99


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