铝酸钠溶液中锂离子的平衡浓度（英文）
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摘要
氧化铝中过量的锂不利于铝电解。本文研究了含锂铝酸钠溶液中锂离子平衡浓度的变化。研究表明,升高温度、增大苛性碱浓度、减小氧化铝浓度或升高苛性比值(a_k)将有助于提高铝酸钠溶液中锂离子的浓度。搅拌速率对锂离子浓度影响很小。在拜耳溶出过程中,当铝酸钠溶液中锂离子平衡浓度超过0.65 g/L时,在晶种分解9 h后,铝酸钠溶液中锂离子浓度仅为35 mg/L。进一步研究发现,勃姆石或硬水铝石的溶出过程到晶种分解过程锂离子的平衡浓度急剧下降,大约有95%的锂会进入赤泥和氢氧化铝中。本文为氧化铝厂铝酸钠溶液中高效去除锂或回收锂提供了依据。
Excess lithium in alumina is significantly bad for aluminum reduction. In this study, the concentration variation of lithium ion in sodium aluminate solution with addition of synthetic lithium aluminate was investigated.Elevating temperature, increasing caustic soda concentration, reducing alumina concentration or raising molar ratio ?k improved equilibrium concentration of lithium ion in sodium aluminate solution. Agitation speed had a minimal effect on lithium ion concentration. Over 0.65 g/L lithium ion equilibrium concentration was observed in digestion process,whereas 35 mg/L lithium ion concentration remained in solution after precipitation time of 9 h. Moreover, equilibrium concentration decreased sharply from digestion of boehmite or diaspore to seed precipitation, about 95% lithium was precipitated into red mud(bauxite residue) and aluminum hydroxide. This study provides a valuable perspective in removal or extraction of lithium from sodium aluminate solution in alumina refineries.
Excess lithium in alumina is significantly bad for aluminum reduction. In this study, the concentration variation of lithium ion in sodium aluminate solution with addition of synthetic lithium aluminate was investigated.Elevating temperature, increasing caustic soda concentration, reducing alumina concentration or raising molar ratio ?k improved equilibrium concentration of lithium ion in sodium aluminate solution. Agitation speed had a minimal effect on lithium ion concentration. Over 0.65 g/L lithium ion equilibrium concentration was observed in digestion process,whereas 35 mg/L lithium ion concentration remained in solution after precipitation time of 9 h. Moreover, equilibrium concentration decreased sharply from digestion of boehmite or diaspore to seed precipitation, about 95% lithium was precipitated into red mud(bauxite residue) and aluminum hydroxide. This study provides a valuable perspective in removal or extraction of lithium from sodium aluminate solution in alumina refineries.
引文
[1]HUANG Hai-bo,QIU Shi-lin.Influences of rich-lithium alumina on aluminum reduction production[J].Light Metals,2014(8):26-28.(in Chinese)
[2]DANIELIK V,FELLNER P,THONSTAD J.Content of sodium and lithium in aluminium during electrolysis of cryolite-based melts[J].Journal of Applied Electrochemistry,1998,28(11):1265-1268.
[3]TABEREAUX A T,ALCORN T R,TREMBLEY L.Lithium-modified low ratio electrolyte chemistry for improved performance in modern reduction cells[M]//Essential Readings in Light Metals.Cham:Springer,2016:83-88.
[4]MESHRAM P,PANDEY B D,MANKHAND T R.Extraction of lithium from primary and secondary sources by pre-treatment,leaching and separation:A comprehensive review[J].Hydrometallurgy,2014,150:192-208.
[5]SWAIN B.Recovery and recycling of lithium:A review[J].Separation and Purification Technology,2017,172:388-403.
[6]CHAGNES A,POSPIECH B.A brief review on hydrometallurgical technologies for recycling spent lithium-ion batteries[J].Journal of Chemical Technology and Biotechnology,2013,88(7):1191-1199.
[7]XUE Sheng-guo,ZHU Feng,KONG Xiang-feng,WUChuan,HUANG Ling,HUANG Nan,HARTLEY W.Areview of the characterization and revegetation of bauxite residues(Red mud)[J].Environmental Science and Pollution Research,2016,23(2):1120-1132.
[8]ZHU Feng,CHENG Qing-yu,XUE Sheng-guo,LI Chu-xuan,HARTLEY W,WU Chuan,TIAN Tao.Influence of natural regeneration on fractal features of residue microaggregates in bauxite residue disposal areas[J].Land Degradation and Development,2018,29(1):138-149.
[9]FURUKAWA T,HIAKAWA Y,KONDO H,KANEMURA T.Dissolution behavior of lithium compounds in ethanol[J].Nuclear Materials and Energy,2016,9:286-291.
[10]FURUKAWA T,HIRAKAWA Y,KONDO H,KANEMURAT,WAKAI E.Chemical reaction of lithium with room temperature atmosphere of various humidities[J].Fusion Engineering and Design,2015,98:2138-2141.
[11]SILAMBARASAN A,RAJESH P,RAMASAMY P.Nucleation kinetics and growth aspects of negative solubility lithium sulphate monohydrate single crystal[J].Journal of Crystal Growth,2015,409:95-99.
[12]KIM T,OLEK J.The effects of lithium ions on chemical sequence of alkali-silica reaction[J].Cement and Concrete Research,2016,79:159-168.
[13]STEPHEN E F,MILLER P D.Solubility of lithium hydroxide in water and vapor pressure of solutions above220°F[J].Journal of Chemical and Engineering Data,1962,7(4):501-505.
[14]MONNIN C,DUBOIS M.Thermodynamics of the LiOH+H2O system[J].Journal of Chemical and Engineering Data,2005,50(4):1109-1113.
[15]PENSADO-RODRIGUEZ O,URQDIDI-MACDONALD M,MACDONALD D D.Electrochemical behavior of lithium in alkaline aqueous electrolytes.I.Thermodynamics[J].Journal of the Electrochemical Society,1999,146(4):1318-1325.
[16]van STRATEN H A,SCHOONEN M A A,de BRUVN P L.Precipitation from supersaturated aluminate solutions.III.Influence of alkali ions with special reference to Li+[J].Journal of Colloid and Interface Science,1985,103(2):493-507.
[17]LI Xian-bin,LONG Zhi-yuan.Studies of the process for producing lithium-bearing alumina[J].Mining and Metallurgical Engineering,1989(3):46-50.(in Chinese)
[18]VILYUGINA M D,MAKARENKOV V M,EREMIN N I.Lithium oxide solubility in aluminate solutions at elevated temperatures[J].Izvestiya Vysshikh Uchebnykh Zavedenii,Tsvetnaya Metallurgia,1983,5:72-74.(in Russian)
[19]CHENG Jian,GUO Lie-jin,XU Shi-sen,ZHANG Rui-yun.Submicronγ-LiAlO2 powder synthesized from boehmite[J].Chinese Journal of Chemical Engineering,2012,20(4):776-783.
[20]HEO S J,HU B,MANTHINA V,HILMI A,YUH C Y,SURENDRANATH A,SINGH P.Stability of lithium aluminate in reducing and oxidizing atmospheres at 700°C[J].International Journal of Hydrogen Energy,2016,41(41):18884-18892.
[21]LIU Gui-hua,LI Zheng,QI Tian-gui,ZHOU Qiu-sheng,PENG Zhi-hong,LI Xiao-bin.Continuous changes in electrical conductivity of sodium aluminate solution in seeded precipitation[J].Transactions of Nonferrous Metals Society of China,2015,25(12):4160-4166.
[22]XUE Sheng-guo,YE Yu-zhen,ZHU Feng,WANG Qiong-li,JIANG Jun,HARTLEY W.Changes in distribution and microstructure of bauxite residue aggregates following amendments addition[J].Journal of Environmental Sciences,2019,78:276-286.DOI:10.1016/j.jes.2018.10.010.
[23]ZHU Feng,LIAO Jia-xin,XUE Sheng-guo,HARTLEY W,ZOU Qi,WU Hao.Evaluation of aggregate microstructures following natural regeneration in bauxite residue as characterized by synchrotron-based X-ray micro-computed tomography[J].Science of the Total Environment,2016,573:155-163.
[2]DANIELIK V,FELLNER P,THONSTAD J.Content of sodium and lithium in aluminium during electrolysis of cryolite-based melts[J].Journal of Applied Electrochemistry,1998,28(11):1265-1268.
[3]TABEREAUX A T,ALCORN T R,TREMBLEY L.Lithium-modified low ratio electrolyte chemistry for improved performance in modern reduction cells[M]//Essential Readings in Light Metals.Cham:Springer,2016:83-88.
[4]MESHRAM P,PANDEY B D,MANKHAND T R.Extraction of lithium from primary and secondary sources by pre-treatment,leaching and separation:A comprehensive review[J].Hydrometallurgy,2014,150:192-208.
[5]SWAIN B.Recovery and recycling of lithium:A review[J].Separation and Purification Technology,2017,172:388-403.
[6]CHAGNES A,POSPIECH B.A brief review on hydrometallurgical technologies for recycling spent lithium-ion batteries[J].Journal of Chemical Technology and Biotechnology,2013,88(7):1191-1199.
[7]XUE Sheng-guo,ZHU Feng,KONG Xiang-feng,WUChuan,HUANG Ling,HUANG Nan,HARTLEY W.Areview of the characterization and revegetation of bauxite residues(Red mud)[J].Environmental Science and Pollution Research,2016,23(2):1120-1132.
[8]ZHU Feng,CHENG Qing-yu,XUE Sheng-guo,LI Chu-xuan,HARTLEY W,WU Chuan,TIAN Tao.Influence of natural regeneration on fractal features of residue microaggregates in bauxite residue disposal areas[J].Land Degradation and Development,2018,29(1):138-149.
[9]FURUKAWA T,HIAKAWA Y,KONDO H,KANEMURA T.Dissolution behavior of lithium compounds in ethanol[J].Nuclear Materials and Energy,2016,9:286-291.
[10]FURUKAWA T,HIRAKAWA Y,KONDO H,KANEMURAT,WAKAI E.Chemical reaction of lithium with room temperature atmosphere of various humidities[J].Fusion Engineering and Design,2015,98:2138-2141.
[11]SILAMBARASAN A,RAJESH P,RAMASAMY P.Nucleation kinetics and growth aspects of negative solubility lithium sulphate monohydrate single crystal[J].Journal of Crystal Growth,2015,409:95-99.
[12]KIM T,OLEK J.The effects of lithium ions on chemical sequence of alkali-silica reaction[J].Cement and Concrete Research,2016,79:159-168.
[13]STEPHEN E F,MILLER P D.Solubility of lithium hydroxide in water and vapor pressure of solutions above220°F[J].Journal of Chemical and Engineering Data,1962,7(4):501-505.
[14]MONNIN C,DUBOIS M.Thermodynamics of the LiOH+H2O system[J].Journal of Chemical and Engineering Data,2005,50(4):1109-1113.
[15]PENSADO-RODRIGUEZ O,URQDIDI-MACDONALD M,MACDONALD D D.Electrochemical behavior of lithium in alkaline aqueous electrolytes.I.Thermodynamics[J].Journal of the Electrochemical Society,1999,146(4):1318-1325.
[16]van STRATEN H A,SCHOONEN M A A,de BRUVN P L.Precipitation from supersaturated aluminate solutions.III.Influence of alkali ions with special reference to Li+[J].Journal of Colloid and Interface Science,1985,103(2):493-507.
[17]LI Xian-bin,LONG Zhi-yuan.Studies of the process for producing lithium-bearing alumina[J].Mining and Metallurgical Engineering,1989(3):46-50.(in Chinese)
[18]VILYUGINA M D,MAKARENKOV V M,EREMIN N I.Lithium oxide solubility in aluminate solutions at elevated temperatures[J].Izvestiya Vysshikh Uchebnykh Zavedenii,Tsvetnaya Metallurgia,1983,5:72-74.(in Russian)
[19]CHENG Jian,GUO Lie-jin,XU Shi-sen,ZHANG Rui-yun.Submicronγ-LiAlO2 powder synthesized from boehmite[J].Chinese Journal of Chemical Engineering,2012,20(4):776-783.
[20]HEO S J,HU B,MANTHINA V,HILMI A,YUH C Y,SURENDRANATH A,SINGH P.Stability of lithium aluminate in reducing and oxidizing atmospheres at 700°C[J].International Journal of Hydrogen Energy,2016,41(41):18884-18892.
[21]LIU Gui-hua,LI Zheng,QI Tian-gui,ZHOU Qiu-sheng,PENG Zhi-hong,LI Xiao-bin.Continuous changes in electrical conductivity of sodium aluminate solution in seeded precipitation[J].Transactions of Nonferrous Metals Society of China,2015,25(12):4160-4166.
[22]XUE Sheng-guo,YE Yu-zhen,ZHU Feng,WANG Qiong-li,JIANG Jun,HARTLEY W.Changes in distribution and microstructure of bauxite residue aggregates following amendments addition[J].Journal of Environmental Sciences,2019,78:276-286.DOI:10.1016/j.jes.2018.10.010.
[23]ZHU Feng,LIAO Jia-xin,XUE Sheng-guo,HARTLEY W,ZOU Qi,WU Hao.Evaluation of aggregate microstructures following natural regeneration in bauxite residue as characterized by synchrotron-based X-ray micro-computed tomography[J].Science of the Total Environment,2016,573:155-163.