氯化铝中萃取铁工艺
|
摘要
采用萃取剂N,N,N',N'-四丁基丙二酰胺(TBMA)、N,N,N',N'-四辛基-3-氧戊二酰胺(TODGA)和甲基异丁基甲酮(MIBK)从氯化铝水溶液中萃取铁,以制备高纯氯化铝。研究结果表明,当氯化铝溶液中盐酸浓度在4 mol/L左右时,TBMA和MIBK的萃取率在90%以上。TODGA显示出优异的萃取分离性能。当氯化铝溶液中Al~(3+)浓度为2.0 mol/L,Fe~(3+)浓度为0.0036 mol/L(0.2 g/L),HCl浓度为1.2 mol/L时,0.20 mol/L TODGA的环己烷或环己烷有机相对铁的一次萃取率达到99.9%以上,多次萃取后溶液中的铁含量低于0.01 mg/L,能深度去除氯化铝中的铁杂质,在工业化生产中有极大的应用价值。
The extraction behaviors of Fe( Ⅲ) in the preparation of high purity aluminum chloride with N,N,N',N'-tetrabutyl malonamide( TBMA),N,N,N',N'-tetraoctyl-3-oxy-glutaramide( TODGA) and methyl isobutyl ketone( MIBK) have been investigated. The results show that the extraction efficiency of Fe( Ⅲ) with TBMA or MIBK is 90% when the concentration of hydrochloric acid in the aluminum chloride solution is4 mol/L. TODGA shows an excellent separation performance. When the concentrations of Al~(3+),Fe~(3+),and HCl are 2. 0 mol/L,0. 0036 mol/L(0. 2 g/L),and 1. 2 mol/L,respectively,in the solution of aluminum chloride,the extraction efficiency of Fe~(3+)is more than 99. 9% with 0. 20 mol/L TODGA in cyclohexane or n-dodecane. After several extractions,the iron impurities in the aluminum chloride can be deeply removed and the iron content in the solution is lower than 0. 01 mg/L,indicating that it has potential application in industrial production.
The extraction behaviors of Fe( Ⅲ) in the preparation of high purity aluminum chloride with N,N,N',N'-tetrabutyl malonamide( TBMA),N,N,N',N'-tetraoctyl-3-oxy-glutaramide( TODGA) and methyl isobutyl ketone( MIBK) have been investigated. The results show that the extraction efficiency of Fe( Ⅲ) with TBMA or MIBK is 90% when the concentration of hydrochloric acid in the aluminum chloride solution is4 mol/L. TODGA shows an excellent separation performance. When the concentrations of Al~(3+),Fe~(3+),and HCl are 2. 0 mol/L,0. 0036 mol/L(0. 2 g/L),and 1. 2 mol/L,respectively,in the solution of aluminum chloride,the extraction efficiency of Fe~(3+)is more than 99. 9% with 0. 20 mol/L TODGA in cyclohexane or n-dodecane. After several extractions,the iron impurities in the aluminum chloride can be deeply removed and the iron content in the solution is lower than 0. 01 mg/L,indicating that it has potential application in industrial production.
引文
[1]Cui L,Cheng F Q,Zhou J F.Preparation of High Purity Al Cl3·6H2O Crystals from Coal Mining Waste Based on Iron(Ⅲ)Removal Using Undiluted Ionic Liquids[J].Sep Purif Technol,2016,167:45-54.
[2]Kim,Su Tae.Method for Simultaneously Preparing High Purity Aluminum Chloride and Zinc:WO 2014208944 A1[P].2014-12-31.
[3]Shiroishi Akihiro,Sanuki Sumiko,Takikawa Shinichiro,et al.Method and Apparatus for Manufacturing High Purity Aluminum:JP 2004203713A[P].2004-07-22.
[4]GUO Yujie,LUAN Zhaokun,FAN Bin.Preparation Solution of Polymeric Aluminum Chloride with High Concentration of Al13[J].Chinese J Inorg Chem,2007,23(1):63-699(in Chinese).郭宇杰,栾兆坤,范彬.高浓度高Al13含量聚合氯化铝溶液的制备[J].无机化学学报,2007,23(1):63-69.
[5]Mishra R K,Rout P C,Sarangi K,et al.Solvent Extraction of Fe(Ⅲ)from the Chloride Leach Liquor of Low Grade Iron ore Tailings Using Aliquat 336[J].Hydrometallurgy,2011,108:93-99.
[6]Zhu Z,Zhang W,Cheng C Y.A Synergistic Solvent Extraction System for Separating Copper from Iron in High Chloride Concentration Solutions[J].Hydrometallurgy,2012,113/114:155-159.
[7]WEI Cundi,GUO Zhaohua,DONG Hong,et al.A Method for Extracting Iron from Aluminum Chloride Slurry:CN103435080B[P].2015-12-09(in Chinese).魏存弟,郭昭华,董宏,等.一种氯化铝浆液萃取除铁的方法:CN 103435080B[P].2015-12-09.
[8]Mishra R K,Rout P C,Sarangi K,et al.A Comparative Study on Extraction of Fe(Ⅲ)from Chloride Leach Liquor Using TBP,Cyanex 921 and Cyanex 923[J].Hydrometallurgy,2010,104:298-303.
[9]Wang X Y,Ma C,Liu J.Studies of Selective Removal of Iron(Ⅲ)from the Simulated Bauxite Hydrochloric Acid Leaching Liquor by Solvent Extraction[J].Adv Mater Res,2013,746:31-33.
[10]Li M Y,He Z M,Zhou L.Removal of Iron from Iindustrial Grade Aluminum Sulfate by Primary Amine Extraction System[J].Hydrometallurgy,2011,106:170-174.
[11]Paiva A P,Costa M C.Application of N,N'-Tetrasubstituted Malonamides to the Recovery of Iron(Ⅲ)from Chloride Solutions[J].Hydrometallurgy,2005,77:103-108.
[12]Zhu Z W,Karol Tulpatowicz,Yoko Pranolo,et al.Fe(Ⅲ)Removal from a Synthetic Chloride Leach Solution of Nickel Laterite by N,N-Diethyldodecanamide[J].Miner Eng,2014,61:47-53.
[13]LV Zijian,JIANG Yinshan,GUO Zhaohua,et al.A Method for Removing Iron from Aluminum Chloride Solution:CN101838004A[P].2010-09-22(in Chinese).吕子剑,蒋引珊,郭昭华,等.一种氯化铝溶液除铁的方法:CN101838004A[P].2010-09-22.
[14]KOU Xiaokang,GUO Zhaohua,FAN Wenmin,et al.Method for Removing Iron from Iron Containing Aluminum Chloride Solution:CN105016368A[P].2015-11-04(in Chinese).寇晓康,郭昭华,樊文岷,等.含铁氯化铝溶液除铁的方法:CN105016368A[P].2015-11-04.
[15]WU Xingke.Sublimation of Anhydrous Aluminum Chloride Under Vacuum Condition[J].Fine Chem,1988,5:27-30(in Chinese).吴兴科.无水氯化铝在真空条件下的升华研究[J].精细化工,1988,5:27-30.
[16]FENG Yuebin,DAI Yongnian,LIU Yongcheng,et al.The Production Process and Application of Anhydrous Aluminum Chloride and Aluminum Chloride Crystal[J].Chinese J Vac Sci Technol,2008,29(5):336-339(in Chinese).冯月斌,戴永年,刘永成,等.无水三氯化铝及结晶三氯化铝的生产工艺和应用[J].真空科学与技术学报,2008,29(5):336-339.
[17]JIANG Tao,SU Yuanfu.Removal of Iron from Zinc Chloride Solution by Solvent Extraction[J].J East China Inst Chem Technol,1988,14(5):537-543(in Chinese).江涛,苏元复.溶剂萃取法从氯化锌溶液中除铁(Ⅲ)[J].华东化工学院学报,1988,14(5):537-543.
[18]ZHAO Hongli,JU Xingsong,ZHAO Lixin,et al.Preparation of High Purity Fe2O3by Methyl Isobutyl Methanol Extraction[J].J Hefei Univ Technol,2006,29(9):1132-1135(in Chinese).赵红丽,琚行松,赵立新,等.甲基异丁基甲酮萃取制备高纯Fe2O3的研究[J].合肥工业大学学报,2006,29(9):1132-1135.
[19]YANG Quanning.Study on the Extraction of Iron and Rare Earth and Its Kinetics in Malonamide Hydrochloride[D].Ji'nan:Ji'nan University,2016(in Chinese).杨全宁.丙二酰胺盐酸体系中萃取铁和稀土及动力学研究[D].济南:济南大学,2016.
[20]WEI Bing.Study on Kinetics of Extraction of Rare Earth Elements by TODGA in HNO3[D].Ji'nan:Ji'nan University,2016(in Chinese).韦兵.N,N,N',N'-四辛基-3-氧戊二酰胺/HNO3萃取稀土元素的动力学研究[D].济南:济南大学,2016.
[21]HANG Zhizhong,LUO Liubao,ZHANG Shiyu,et al.Improvement on the Determination of Iron Condition by the Method of Phenanthroline[J].Sci Technol Chem Ind,2008,16(6):50-53(in Chinese).黄志中,罗六保,张世誉,等.邻二氮菲分光光度法测定铁条件选择实验的改进[J].化工科技,2008,16(6):50-53.
[22]LI Sihong,GUO Youhong.An Experimental Study on the Determination of Trace Iron by Phenanthroline[J].Strait Pharm J,2013,25(8):82-85(in Chinese).李丝红,郭幼红.邻二氮菲分光光度法测定微量铁实验探讨[J].海峡药学,2013,25(8):82-85.
[23]GB/T 3049-2006/ISO 6685:General Method for the Determination of Iron Content of Chemical Products Industry[S].1982(in Chinese).GB/T 3049-2006/ISO 6685:工业用化工产品铁含量测定的通用方法[S].1982.
[24]Zhang G Z,Chen D S,Wei G Y,et al.Extraction of Iron(Ⅲ)from Chloride Leaching Liquor with High Acidity Using Trin-butyl Phosphate and Synergistic Extraction Combined with Methyl Isobutyl Ketone[J].Sep Purif Technol,2015,150:132-138.
[25]Cai X C,Han J X,Pang M P,et al.Structural Effect of Diamide Extractants on the Extraction Behaviour of Fe(Ⅲ)from Hydrochloric Acid[J].Hydrometallurgy,2016,164:48-53.
[26]CAI Xucan.Study on the Synthesis and Extraction Performance of Bisamide Extractant[D].Ji'nan:Ji'nan University,2016(in Chinese).蔡绪灿.双酰胺萃取剂的合成及萃取性能研究[D].济南:济南大学,2016..
[2]Kim,Su Tae.Method for Simultaneously Preparing High Purity Aluminum Chloride and Zinc:WO 2014208944 A1[P].2014-12-31.
[3]Shiroishi Akihiro,Sanuki Sumiko,Takikawa Shinichiro,et al.Method and Apparatus for Manufacturing High Purity Aluminum:JP 2004203713A[P].2004-07-22.
[4]GUO Yujie,LUAN Zhaokun,FAN Bin.Preparation Solution of Polymeric Aluminum Chloride with High Concentration of Al13[J].Chinese J Inorg Chem,2007,23(1):63-699(in Chinese).郭宇杰,栾兆坤,范彬.高浓度高Al13含量聚合氯化铝溶液的制备[J].无机化学学报,2007,23(1):63-69.
[5]Mishra R K,Rout P C,Sarangi K,et al.Solvent Extraction of Fe(Ⅲ)from the Chloride Leach Liquor of Low Grade Iron ore Tailings Using Aliquat 336[J].Hydrometallurgy,2011,108:93-99.
[6]Zhu Z,Zhang W,Cheng C Y.A Synergistic Solvent Extraction System for Separating Copper from Iron in High Chloride Concentration Solutions[J].Hydrometallurgy,2012,113/114:155-159.
[7]WEI Cundi,GUO Zhaohua,DONG Hong,et al.A Method for Extracting Iron from Aluminum Chloride Slurry:CN103435080B[P].2015-12-09(in Chinese).魏存弟,郭昭华,董宏,等.一种氯化铝浆液萃取除铁的方法:CN 103435080B[P].2015-12-09.
[8]Mishra R K,Rout P C,Sarangi K,et al.A Comparative Study on Extraction of Fe(Ⅲ)from Chloride Leach Liquor Using TBP,Cyanex 921 and Cyanex 923[J].Hydrometallurgy,2010,104:298-303.
[9]Wang X Y,Ma C,Liu J.Studies of Selective Removal of Iron(Ⅲ)from the Simulated Bauxite Hydrochloric Acid Leaching Liquor by Solvent Extraction[J].Adv Mater Res,2013,746:31-33.
[10]Li M Y,He Z M,Zhou L.Removal of Iron from Iindustrial Grade Aluminum Sulfate by Primary Amine Extraction System[J].Hydrometallurgy,2011,106:170-174.
[11]Paiva A P,Costa M C.Application of N,N'-Tetrasubstituted Malonamides to the Recovery of Iron(Ⅲ)from Chloride Solutions[J].Hydrometallurgy,2005,77:103-108.
[12]Zhu Z W,Karol Tulpatowicz,Yoko Pranolo,et al.Fe(Ⅲ)Removal from a Synthetic Chloride Leach Solution of Nickel Laterite by N,N-Diethyldodecanamide[J].Miner Eng,2014,61:47-53.
[13]LV Zijian,JIANG Yinshan,GUO Zhaohua,et al.A Method for Removing Iron from Aluminum Chloride Solution:CN101838004A[P].2010-09-22(in Chinese).吕子剑,蒋引珊,郭昭华,等.一种氯化铝溶液除铁的方法:CN101838004A[P].2010-09-22.
[14]KOU Xiaokang,GUO Zhaohua,FAN Wenmin,et al.Method for Removing Iron from Iron Containing Aluminum Chloride Solution:CN105016368A[P].2015-11-04(in Chinese).寇晓康,郭昭华,樊文岷,等.含铁氯化铝溶液除铁的方法:CN105016368A[P].2015-11-04.
[15]WU Xingke.Sublimation of Anhydrous Aluminum Chloride Under Vacuum Condition[J].Fine Chem,1988,5:27-30(in Chinese).吴兴科.无水氯化铝在真空条件下的升华研究[J].精细化工,1988,5:27-30.
[16]FENG Yuebin,DAI Yongnian,LIU Yongcheng,et al.The Production Process and Application of Anhydrous Aluminum Chloride and Aluminum Chloride Crystal[J].Chinese J Vac Sci Technol,2008,29(5):336-339(in Chinese).冯月斌,戴永年,刘永成,等.无水三氯化铝及结晶三氯化铝的生产工艺和应用[J].真空科学与技术学报,2008,29(5):336-339.
[17]JIANG Tao,SU Yuanfu.Removal of Iron from Zinc Chloride Solution by Solvent Extraction[J].J East China Inst Chem Technol,1988,14(5):537-543(in Chinese).江涛,苏元复.溶剂萃取法从氯化锌溶液中除铁(Ⅲ)[J].华东化工学院学报,1988,14(5):537-543.
[18]ZHAO Hongli,JU Xingsong,ZHAO Lixin,et al.Preparation of High Purity Fe2O3by Methyl Isobutyl Methanol Extraction[J].J Hefei Univ Technol,2006,29(9):1132-1135(in Chinese).赵红丽,琚行松,赵立新,等.甲基异丁基甲酮萃取制备高纯Fe2O3的研究[J].合肥工业大学学报,2006,29(9):1132-1135.
[19]YANG Quanning.Study on the Extraction of Iron and Rare Earth and Its Kinetics in Malonamide Hydrochloride[D].Ji'nan:Ji'nan University,2016(in Chinese).杨全宁.丙二酰胺盐酸体系中萃取铁和稀土及动力学研究[D].济南:济南大学,2016.
[20]WEI Bing.Study on Kinetics of Extraction of Rare Earth Elements by TODGA in HNO3[D].Ji'nan:Ji'nan University,2016(in Chinese).韦兵.N,N,N',N'-四辛基-3-氧戊二酰胺/HNO3萃取稀土元素的动力学研究[D].济南:济南大学,2016.
[21]HANG Zhizhong,LUO Liubao,ZHANG Shiyu,et al.Improvement on the Determination of Iron Condition by the Method of Phenanthroline[J].Sci Technol Chem Ind,2008,16(6):50-53(in Chinese).黄志中,罗六保,张世誉,等.邻二氮菲分光光度法测定铁条件选择实验的改进[J].化工科技,2008,16(6):50-53.
[22]LI Sihong,GUO Youhong.An Experimental Study on the Determination of Trace Iron by Phenanthroline[J].Strait Pharm J,2013,25(8):82-85(in Chinese).李丝红,郭幼红.邻二氮菲分光光度法测定微量铁实验探讨[J].海峡药学,2013,25(8):82-85.
[23]GB/T 3049-2006/ISO 6685:General Method for the Determination of Iron Content of Chemical Products Industry[S].1982(in Chinese).GB/T 3049-2006/ISO 6685:工业用化工产品铁含量测定的通用方法[S].1982.
[24]Zhang G Z,Chen D S,Wei G Y,et al.Extraction of Iron(Ⅲ)from Chloride Leaching Liquor with High Acidity Using Trin-butyl Phosphate and Synergistic Extraction Combined with Methyl Isobutyl Ketone[J].Sep Purif Technol,2015,150:132-138.
[25]Cai X C,Han J X,Pang M P,et al.Structural Effect of Diamide Extractants on the Extraction Behaviour of Fe(Ⅲ)from Hydrochloric Acid[J].Hydrometallurgy,2016,164:48-53.
[26]CAI Xucan.Study on the Synthesis and Extraction Performance of Bisamide Extractant[D].Ji'nan:Ji'nan University,2016(in Chinese).蔡绪灿.双酰胺萃取剂的合成及萃取性能研究[D].济南:济南大学,2016..