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系統識別號 U0026-2801201409175100
論文名稱(中文) 利用資源化鐵氧化物吸附鍶:共離子競爭效應與動力學探討
論文名稱(英文) Application of recovered iron oxide for adsorptive removal of Sr: Kinetic study and effect of coexisting ion
校院名稱 成功大學
系所名稱(中) 地球科學系
系所名稱(英) Department of Earth Sciences
學年度 102
學期 1
出版年 103
研究生(中文) 陳怡如
研究生(英文) Yi-Ru Chen
學號 L46001175
學位類別 碩士
語文別 中文
論文頁數 96頁
口試委員 指導教授-游鎮烽
共同指導教授-黃耀輝
口試委員-楊懷仁
中文關鍵字 選擇性吸附  流體化床  針鐵礦  共離子競爭 
英文關鍵字 Selectivity  Fluidized-bed  Goethite  Competitive adsorption 
學科別分類
中文摘要 在311東日本大地震發生後,大量的含鍶90廢水流入海中,隨著洋流漂流到世界各地,鍶90的半衰期約29年,放射性鍶容易進入人體骨髓,引發白血病和骨癌,對人類健康造成影響。
本研究使用實廠流體化床Fenton反應槽所產出的固體副產物,稱為BT鐵氧化物系列,已證實為大比表面積(150-250 m2g-1)之針鐵礦(Goethite, α-FeOOH, 0.25-1.5mm),經氫氧化鈉溶液鹼洗後,透過吸附技術來處理水中的鍶。利用X光繞射分析儀、掃描式電子顯微鏡、比表面積分析儀,進行吸附材表面分析,解析吸附材表面性質對吸附除鍶結果的影響,並利用感應耦合電漿原子發射光譜分析儀分析溶液中各金屬離子濃度。
吸附鍶實驗結果顯示,ΔG在15、30、50℃吸附實驗下皆為負值,此代表BT9在這三個溫度下,吸附鍶皆為自發性的反應;而ΔH為正值反映了此系統為吸熱反應。在30℃時BT9的最大吸附量為28.01 mg/g。
BT9對於帶1價的K離子幾乎不吸附,只吸附帶2價電的鹼土族離子。且經過24小時的吸附實驗後, BT9對各離子的去除率由高到低的順序為:Mg > Sr > Ba > Ca,此順序與水合離子數(N, the number of waters of hydration)和水合半徑(RH , the order of the hydrated radius)的比值一致。無論是含Ca、Sr共同離子吸附或是含Mg、Sr共同離子吸附及Ba、Sr共同離子吸附,皆符合二階動力式或擬二階動力式。當IMR=1時,Ca和Ba對於移除Sr沒有太大影響,當IMR=100時,所有的鹼土族離子大大降低了Sr的去除率,表示當溶液中共離子濃度增加時,離子間的競爭效應會明顯顯現,而海水中Ca和Mg濃度很高,因此BT9在Ca、Mg濃度很高的條件下將大幅降低對Sr的移除效率。
英文摘要 After the 311 earthquake in eastern Japan, huge amount of waste water with 90Sr was discharged into the sea, and spread to the worldwide by the current. The half-life of 90Sr is about 29 years and the radioactive Sr enters human bone marrow easily then causing leukemia and bone cancer.
The experiment applied as a waste iron oxide adsorbent, named BT series, for the strontium removal from the aqueous solutions; BT was recovered from real fluidized-bed Fenton equipment and was composed of a homogeneous goethite (α-FeOOH). BT has a high specific surface area (150-250m2g-1) and 0.25-1.5 mm in size, after modification, through adsorption of strontium to deal with strontium in the water. Using X-ray diffraction, scanning electron microscopy, surface area analyzers to proessive the adsorption material surface analysis and adsorb material surface properties on the adsorption results in the impact of strontium and using inductively coupled plasma atomic emission spectrometer analysis solution each metal ion concentration.
The experiment of strontium adsorption results show thatΔG at 15, 30, 50℃ under test are negative adsorption. It means that BT9 under three temperatures, the adsorption reactions of strontium are spontaneous. ΔH is positive reflection of this system is an endothermic reaction. The maximum adsorption capacity is 28.01 mg /g on BT9 at 30℃.
BT9 almost does not adsorb potassium ions and only adsorbs alkaline earth ions. After 24 hours, the adsorption experiment, the order of BT9 removal of various ions is Mg > Sr > Ba > Ca. The order is the same with the ratio of the number of waters of hydration and the order of the hydrated radius.
Whether containing Ca, Sr common ion adsorption or containing Mg, Sr common ion adsorption and Ba, Sr common ion adsorption, are in compliance with second order rate equation or pseudo second rate equatio. When IMR equal 1, Ca and Ba do not effect the removal of Sr, when IMR equal 100, all the alkaline earth ion greatly effect the removal of Sr. It means when the concentrations of the alkaline earth ion are high in the solution, the competitive effects will be obiviously. The concentration of Ca and Mg in the seawater is very high, therefore BT9 in conditions of high Ca and Mg concentration will reduce substantially the removal efficiency of Sr.

論文目次 第一章 前言 1
1-1 緣起及目的 1
1-2 研究內容 3
第二章 文獻回顧 4
2-1 鍶90特性概述 4
2-2 鐵氧化物特性與應用 5
2-2-1 鐵氧化物的種類 5
2-2-2 鐵氧化物表面化學特性 6
2-2-3 鐵氧化物BT系列之性質介紹 13
2-2-4 鐵氧化物-針鐵礦(Goethite)吸附材 18
2-2-5 鐵氧化物之應用 20
2-3-1 吸附作用 22
2-3-2 物理吸附 24
2-3-3 化學吸附 25
2-3-4 等溫吸附模式 25
2-3-5 影響吸附的因素 30
2-3-6 背景電解質對吸附反應之影響 31
2-3-7 陽離子之吸附反應 32
2-3-8 陰離子之吸附反應 33
2-3-9 共離子吸附 34
第三章 實驗 36
3-1 實驗架構 36
3-2 純化BT9 38
3-3 吸附材料基本性質鑑定 39
3-3-1 比表面積與孔隙分佈 39
3-3-2 表面型態觀察 39
3-3-3 表面元素分析 40
3-3-4 晶相分析 40
3-4 吸附實驗 42
3-4-1 實驗裝置及步驟 42
3-4-2 濃度分析 42
第四章 結果與討論 44
4-1 基本性質與鑑定分析 44
4-1-1 BT9材料基本性質 44
4-1-2 BT9晶相分析 45
4-1-3 表面型態觀察與元素分析 45
4-2 吸附實驗 48
4-2-1 吸附量與pH值之關係 48
4-2-2 溫度對吸附現象之影響 51
4-2-3 等溫吸附模式 55
4-2-4 含Sr、Ca、Mg、Ba、K之共同離子效應 58
4-2-5 含Sr、Ca共同離子效應吸附及動力學探討 61
4-2-6 含Sr、Mg共同離子效應吸附及動力學探討 68
4-2-7 含Sr、Ba共同離子效應吸附及動力學探討 73
4-2-8 共離子競爭效應 78
第五章 結論與建議 80
5-1 結論 80
5-2 建議 82
第六章 參考文獻 83
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