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研究生:蔡弘昇
研究生(外文):Hung-Sheng Tsai
論文名稱:以有機磷萃取劑萃取及中空纖維液膜分離鎵(III)與銦(III)之研究
論文名稱(外文):The Extraction and Separation of Gallium(III) and Indium(III) Using Organophosphorus Extractants and Hollow Fiber Liquid Membranes
指導教授:蔡德華
口試委員:陳奕宏方旭偉郭文正劉豫川張裕祺莊瑞鑫
口試日期:2012-07-30
學位類別:博士
校院名稱:國立臺北科技大學
系所名稱:工程科技研究所
學門:工程學門
學類:材料工程學類
論文種類:學術論文
論文出版年:2012
畢業學年度:100
語文別:中文
論文頁數:224
中文關鍵詞:溶劑萃取中空纖維液膜有機磷萃取劑二(2-乙基己基)磷酸2-乙基己基膦酸單-2-乙基己基酯二(244-三甲基戊基)次膦酸
外文關鍵詞:Solvent ExtractionHollow Fiber Liquid MembranesGalliumIndiumOrganophosphorus ExtractantsDi(2-ethylhexyl)phosphoric Acid2-Ethylhexyl Phosphonic Acid Mono-2-ethylhexyl EsterBis(244-trimethylpentyl)phosphinic Acid
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本論文以有機磷萃取劑,在25℃下以煤油為稀釋劑,研究硝酸水溶液中鎵(III)與銦(III)之萃取平衡,並將實驗所得的萃取平衡數據,應用於中空纖維液膜之理論分析上,解析鎵(III)與銦(III)在中空纖維液膜分離程序中之傳送行為。
首先探討分別以有機磷萃取劑二(2-乙基己基)磷酸(D2EHPA)、2-乙基己基膦酸單-2-乙基己基酯(PC-88A)及二(2,4,4-三甲基戊基)次膦酸(Cyanex 272)自硝酸水溶液中各別萃取鎵(III)與銦(III)之萃取平衡,實驗結果顯示鎵(III)與銦(III)在有機相和水相間的萃取分配比隨有機磷萃取劑D2EHPA、PC-88A及Cyanex 272濃度和pH值之增加而增加。並經由圖解和數值分析,有機相In-D2EHPA錯合物的組成為 ,其萃取平衡常數為127.34 (kmol/m3)3/2。而有機相Ga-D2EHPA錯合物的組成為 ,其萃取平衡常數為0.28 (kmol/m3)3/2;有機相In-PC-88A錯合物的組成為 和 ,其萃取平衡常數分別為13.79 (kmol/m3)3/2和175.09 kmol/m3。而有機相Ga-PC-88A錯合物的組成為 ,其萃取平衡常數為1.75 × 10?2 (kmol/m3)3/2;有機相In-Cyanex 272錯合物的組成為 ,其萃取平衡常數為0.72 (kmol/m3)3/2。
以D2EHPA、PC-88A 及Cyanex 272分別自含鎵(III)之硝酸水溶液中萃取銦(III)之研究上,銦(III)的萃取分配比皆隨萃取劑濃度和pH值之增加而增加。經由圖解和數值分析,有機相In-D2EHPA錯合物的組成為 ,其萃取平衡常數為87.30 (kmol/m3)3/2;有機相In-PC-88A錯合物的組成為 和 ,其萃取平衡常數分別為7.12 (kmol/m3)3/2和86.01 kmol/m3;有機相In-Cyanex 272錯合物的組成為 ,其萃取平衡常數為0.56 (kmol/m3)3/2。
本研究以polypropylene為膜材之中空纖維膜為支撐膜,並以D2EHPA為載劑,進行中空纖維液膜分離鎵(III)與銦(III)的研究。當中空纖維膜中進料液的體積流率到達4.74 × 10?4 m3/min (500 rpm)時,其水相邊界層的厚度減至最小。鎵(III)與銦(III)的透過係數隨載劑濃度之增加而增加,但隨進料液中鎵(III)與銦(III)之濃度的增加而降低。

The extraction and the separation of gallium(III), indium(III) and mixtures of gallium(III) and indium(III) using solvent extraction and hollow fiber liquid membranes methods were investigated at 25°C. The organophosphorus extractants of di(2-ethylhexyl)phosphoric acid (D2EHPA), 2-ethylhexyl phosphonic acid mono-2-ethylhexyl ester (PC-88A), and bis(2,4,4-trimethylpentyl) phosphinic acid (Cyanex 272) were used. The extraction equilibria of gallium(III) and indium(III) in extractants and kerosene solutions and in extractants and water solutions were studied, respectively. Based on these extraction equilibria information, the permeation rates of gallium(III) and indium(III) across a hollow fiber liquid membrane (HFLM) were determined experimentally. The relevant transport phenomena were also analyzed.
First, the extraction equilibria of gallium(III) and indium(III) from an aqueous nitric acid medium with D2EHPA, PC-88A and Cyanex 272 as the organophosphorus extractant were studied. The experimental results indicated that the distribution coefficients for the extraction of gallium(III) and indium(III) increased with increasing either concentrations of extractant in the organic phase or equilibrium pH values in the aqueous phase. The composition of In-D2EHPA complex formed in the organic phase was determined by graphical method and numerical analysis. The composition was , and the equilibrium constant was 127.34 (kmol/m3)3/2. The composition of Ga-D2EHPA complex in the organic phase was , and the equilibrium constant was 0.28 (kmol/m3)3/2. The compositions of In-PC-88A complexes in the organic phase were found to be and , and their corresponding equilibrium constants were 13.79 (kmol/m3)3/2 and 175.09 kmol/m3. The composition of Ga-PC-88A complex in the organic phase was , and the equilibrium constant was 1.75 × 10?2 (kmol/m3)3/2. The composition of In-Cyanex 272 complex in the organic phase was , and the equilibrium constant was 0.72 (kmol/m3)3/2.
Then, the extraction equilibria of indium(III) from an aqueous nitric acid medium containing gallium(III) ions with D2EHPA、PC-88A or Cyanex 272 as the organophosphorus extractant were investigated. The distribution coefficients for the extraction of indium(III) increased with increasing either concentrations of extractant in the organic phase or equilibrium pH value in the aqueous phase. Based on graphical and numerical analysis, the composition of In-D2EHPA complex formed in the organic phase was found to be , and the equilibrium constant was 87.30 (kmol/m3)3/2. The compositions of In-PC-88A complexes in the organic phase were and , and their corresponding equilibrium constants were 7.12 (kmol/m3)3/2 and 86.01 kmol/m3. The composition of In-Cyanex 272 complex in the organic phase was , and the equilibrium constant was 0.56 (kmol/m3)3/2.
A supported liquid membrane based on microporous polyprolylene hollow fiber membrane was used to investigate the permeation rates of gallium(III) and indium(III) through hollow fiber liquid membrane with D2EHPA as a carrier. The experimental results indicated that the thickness of the aqueous boundary diffusion layers reaches its minimum value at the flow rate of 4.74 × 10?4 m3/min (500 rpm). The experimental data also show that the permeability of gallium(III) and indium(III) increased when the carrier concentration in the hollow fiber liquid membrane increased. The permeability of gallium(III) and indium(III) decreased when the metal ion concentrations in the feed solutions increased.

中文摘要 i
英文摘要 iii
誌謝 vi
目錄 vii
表目錄 ix
圖目錄 xii
第一章 緒論 1
1.1 前言 1
1.2 溶劑萃取技術 3
1.2.1 溶劑萃取的原理 3
1.2.2 萃取劑的選擇 6
1.2.3 萃取劑的分類 7
1.2.4 稀釋劑的用途及選擇 17
1.3 液膜分離技術 18
1.3.1 液膜分離程序的傳送模式 20
1.3.2 支撐液膜 22
1.3.3 複合支撐液膜 24
1.3.4 中空纖維液膜 27
1.3.5 乳化液膜 28
1.4 研究動機與目的 30
第二章 實驗部分 39
2.1 實驗儀器及藥品 39
2.1.1 實驗藥品 39
2.1.2 實驗器材及儀器 43
2.2 實驗方法 44
2.2.1 萃取平衡實驗 44
2.2.2 中空纖維液膜分離實驗 44
2.2.3 濃度校正 46
第三章 以二(2-乙基己基)磷酸、2-乙基己基膦酸單-2-乙基己基酯及二(2,4,4-三甲基戊基)次膦酸自硝酸水溶液中萃取鎵(III)與銦(III)之研究 47
3.1 銦(III)之萃取平衡 47
3.2 鎵(III)之萃取平衡 65
3.3 鎵(III)與銦(III)萃取平衡之再確認 77
3.3.1 銦(III)萃取平衡之再確認 77
3.3.2 鎵(III)萃取平衡之再確認 98
第四章 以二(2-乙基己基)磷酸、2-乙基己基膦酸單-2-乙基己基酯及二(2,4,4-三甲基戊基)次膦酸自含鎵(III)的硝酸水溶液中萃取銦(III)之研究 112
4.1 銦(III)之萃取平衡 112
4.2 銦(III)萃取平衡之再確認 125
第五章 以二(2-乙基己基)磷酸為載劑之中空纖維液膜自硝酸水溶液中分離鎵(III)與銦(III)之研究 147
5.1 中空纖維液膜傳送原理 147
5.2 溶液體積流率之影響 161
5.3 載劑濃度之影響 166
5.4 鎵(III)與銦(III)質量傳送參數之測定 166
5.5 進料液鎵(III)與銦(III)離子濃度之影響 179
第六章 結論 185
參考文獻 187
符號說明 220
作者簡介 224

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