Leaching ion adsorption rare earth by aluminum sulfate for increasing efficiency and lowering the environmental impact
|
摘要
The leaching efficiency(LE) of ion adsorption rare earth(IARE) by the sulfate and chloride of ammonium,magnesium and aluminum were comparatively determined using column leaching method. It is found that at equal equivalent concentration of cation, the LE of IARE by aluminum sulfate is the highest, and the zeta potential of clay mineral particles in the tailing is near to zero, which means a lower risk of landslide and pollutant emission. Furthermore, the optimum concentration of aluminum sulfate is determined to be0.02 mol/L, which is much lower than that of ammonium sulfate and magnesium sulfate. To reduce the production cost and environmental impact, we proposed a multi-stage leaching process, which was firstly leaching with ammonium sulfate and then with aluminum sulfate, following by water washing and lime neutralizing. With the ratio of ammonium sulfate to aluminum sulfate varying from 1:0 to 0.5:0.5, the residual ammonium in tailing decreases from 11.2% to 0.6%, however, the LE of RE shows an optimum value at 0.8:0.2. By neutralizing the pH of tailing with lime water to over 6, the ion concentration in water rinsing solution can meet the requirement for water discharge. At the same time, the zeta potential of clay particles is found to be around-5 mV, means a relatively lower risk of landslide. These facts indicate that the LE of IARE can be increased and the danger caused by tailings landslides and pollutant emissions can be reduced by replacing ammonium sulfate with aluminum sulfate as leaching reagent.
The leaching efficiency(LE) of ion adsorption rare earth(IARE) by the sulfate and chloride of ammonium,magnesium and aluminum were comparatively determined using column leaching method. It is found that at equal equivalent concentration of cation, the LE of IARE by aluminum sulfate is the highest, and the zeta potential of clay mineral particles in the tailing is near to zero, which means a lower risk of landslide and pollutant emission. Furthermore, the optimum concentration of aluminum sulfate is determined to be0.02 mol/L, which is much lower than that of ammonium sulfate and magnesium sulfate. To reduce the production cost and environmental impact, we proposed a multi-stage leaching process, which was firstly leaching with ammonium sulfate and then with aluminum sulfate, following by water washing and lime neutralizing. With the ratio of ammonium sulfate to aluminum sulfate varying from 1:0 to 0.5:0.5, the residual ammonium in tailing decreases from 11.2% to 0.6%, however, the LE of RE shows an optimum value at 0.8:0.2. By neutralizing the pH of tailing with lime water to over 6, the ion concentration in water rinsing solution can meet the requirement for water discharge. At the same time, the zeta potential of clay particles is found to be around-5 mV, means a relatively lower risk of landslide. These facts indicate that the LE of IARE can be increased and the danger caused by tailings landslides and pollutant emissions can be reduced by replacing ammonium sulfate with aluminum sulfate as leaching reagent.
The leaching efficiency(LE) of ion adsorption rare earth(IARE) by the sulfate and chloride of ammonium,magnesium and aluminum were comparatively determined using column leaching method. It is found that at equal equivalent concentration of cation, the LE of IARE by aluminum sulfate is the highest, and the zeta potential of clay mineral particles in the tailing is near to zero, which means a lower risk of landslide and pollutant emission. Furthermore, the optimum concentration of aluminum sulfate is determined to be0.02 mol/L, which is much lower than that of ammonium sulfate and magnesium sulfate. To reduce the production cost and environmental impact, we proposed a multi-stage leaching process, which was firstly leaching with ammonium sulfate and then with aluminum sulfate, following by water washing and lime neutralizing. With the ratio of ammonium sulfate to aluminum sulfate varying from 1:0 to 0.5:0.5, the residual ammonium in tailing decreases from 11.2% to 0.6%, however, the LE of RE shows an optimum value at 0.8:0.2. By neutralizing the pH of tailing with lime water to over 6, the ion concentration in water rinsing solution can meet the requirement for water discharge. At the same time, the zeta potential of clay particles is found to be around-5 mV, means a relatively lower risk of landslide. These facts indicate that the LE of IARE can be increased and the danger caused by tailings landslides and pollutant emissions can be reduced by replacing ammonium sulfate with aluminum sulfate as leaching reagent.
引文
1. Li YX. Ion adsorption rare earth resources and their green extraction. Beijing:Chemical Industry Press; 2014.
2. Chi RA, Tian J. Hydrometallurgy of the weathered crust elution-deposited rare earth ores. Beijing:Science Press; 2006.
3. He LY, Feng TZ, Fu SX, Zhu DS. Study on Extraction of rare earth from ion type rare earth ore by ammonium sulfate leaching. Chin Rare Earths(in Chin.).1983;4(3):1.
4. Xu QH, Sun YY, Zhou XZ, Liu YZ, Li J, Li YX. Green extraction of ion-adsorption rare earth resources. J Chin Soc Rare Earths(in Chin.). 2016;34(6):650.
5. Xiao YF, Chen YY, Feng ZY, Huang XW, Huang L, Long ZQ, et al. Leaching characteristics of ion-adsorption type rare earths ore with Magnesium sulfate.Trans Nonferrous Met Soc China. 2015;11:3784.
6. Yin S, Pei J, Jiang F, Li SW, Peng JH, Zhang LB, et al. Ultrasound-assisted leaching of rare earths from the weathered crustelution-deposited ore using magnesium sulfate without ammonia-nitrogen pollution. Ultrason Sonochem.2018;41:1-56.
7. Huang XW, Yu Y, Feng ZY, Zhao N. A method for recovery of rare earth from ionic rare earth ore. China Patent, CN201010128302.9, 2011.
8. Huang XW, Wang LS, Feng ZY, Huang L, Wang M, Xiao YF, et al. Extraction and recovery of rare earth from low concentration solution of rare earth. 2015. China Patent, CN201310303722.X.
9. Huang XW, Dong JS, Wang LS, Feng ZY, Xue QN, Meng XL, Selective recovery of rare earth elements from ion-adsorption rare earth element ores by stepwise extraction with HEH(EHP)and HDEHP. Green Chem. 2017;19(5):1345.
10. Jia JT, Zhang YW, Wu S, Liao CS, Yan CH, Liu JY, et al. Study on the distribution and separation of aluminum inrare earth extraction separation process(I). Chin Rare Earths(in Chin.). 2001;22(2):10.
11. Wu WY, Li D, Zhao ZH, Jian JL, Zhang FY, Yin SH. Formation mechanism of micro emulsion on aluminum and lanthanum extraction in P507-HC1 system.J Rare Earths. 2010;28(s1):174.
12. Liu ZQ, Zhu W, Guo QS. Study on process of extracting aluminum from highalumina rare earth solution. Materals Res Appl. 2012;6(4):256.
13. Li JH, Zhang X. Distribution ratio and separation coefficient of single rare earth and aluminium in chloronaphthenic acid system. Chin J Rare Metals(in Chin.).2010;34(5):776.
14. Yang XL, Qiu TS. Influence of aluminum ions distribution on the removal of aluminum from rare earth solutions using saponified naphthenic acid. Sep Purif Technol. 2017;186:290.
15. Qiu TS, Fang XH, Wu HQ, Zeng QH, Zhu DM. Leaching behaviors of iron and aluminum elements of ion-absorbed-rare-earth ore with a new impurity depressant. Trans Nonferrous Met Soc China. 2014;24(9):2986.
16. He ZY, Zhang ZY, Yu JX, Chi RA. Study on the behavior of rare earth and aluminum and ammonium in the leaching ofrare earth ores in weathering crust. Chin Rare Earths(in Chin.). 2015;36(6):18.
17. He Z, Zhang ZY, Yu JX, Xu ZG, Chen Z, Chi RA. Kinetics of column leaching of rare earth and aluminum from weathered crust elution-deposited rare earth ore with ammonium salt solutions. Hydrometallurgy. 2016;163(2016):33.
18. Tian J, Chi RA, Zhu GC, Zhang ZG, Xu SM. Occurrence of aluminum in rare earth mine in southern China. Nonferrous Met. 2000;52(3):58.
19. Ouyang KX, Rao GH, Qin HR, Mao YH. Study of southern RE ore leaching by aluminum inhibition. Rare Met Cem Carbides. 2003;31(4):1.
20. Zhao ZH, Xiao XY, Zhang WB, Hao GH, Duan CK, Li D. Application of centrifuging sedimentation on removing aluminum and iron from rare earth solution. Chin Rare Earths(in Chin.). 2007;28(6):95.
21. He ZY, Zhang ZY, Chi RA, Xu ZG, Yu JX, Wu M, et al. Leaching hydrodynamics of weathered elution-deposited rare earth ore with ammonium salts solution.J Rare Earths. 2017;35(8):824.
22. Xiao YF, Feng ZY, Hu GH, Huang L, Huang XW, Chen YY, et al. Reduction leaching of rare earth from ion-adsorption type rare earths ore with ferrous sulfate. J Rare Earths. 2016;34(9):917.
23. Xiao YF, Huang L, Long ZQ, Feng ZY, Wang LS.Adsorption ability of rare earth elements on clay minerals and its practical performance. J Rare Earths.2016;34(5):543.
24. Xiao YF, Liu XS, Feng ZY, Huang XW, Huang L, Chen YY, et al. Role of minerals properties on leaching process of weathered crust elution-deposited rare earth ore. J Rare Earths. 2015;33(5):545.
25. Wang L, Liao CF, Yang YM, Xu HB, Xiao YF, Yan CH. Effects of organic acids on the leaching process of ion-adsorption type rare earth ore. J Rare Earths.2017;35:1233.
26. Tian J, Yin J, Tang XK, Chen J, Luo XP, Rao GH. Enhanced leaching process of a low-grade weathered crust elution-deposited rare earth ore with carboxymethyl sesbania gum. Hydrometallurgy. 2013;139(3):124.
27. Xu QH, Yang LF, Zhang L, Li CC, Wang DS, Zhou XM, et al. Classification and high efficient leaching of ion adsorption rare earth based on its pH dependence. Chin J Inorg Chem. 2018;30(1):112.
28. Li YX, Yang LF, Li CC, Xu QH, Zhang L, Wang Y, et al. Extraction of rare earths from low content rare earth solution with primary amine extractant. China Patent:CN201610821052.4, 2017.
29. Li YX, Xu QH, Wang Y, Xie AL, Hou X, Zhou XZ, et al. A method to improve the extraction rate of ionic rare earth and the safety of tailings. China Patent,CN201310594438.2, 2014.
30. Hidayah NN, Abidin SZ. The evolution of mineral processing in extraction of rare earth elements using liquid-liquid extraction:a review. Miner Eng.2018;121:146.
31. Li YX, Yang LF, Li CC, Xu QH, Zhang L, Wang Y, et al. Method for the high efficiency leaching of ion adsorption rare earths using aluminum sulfate as leaching reagent. China Patent, CN201610821052.4, 2016.
32. Li DQ. Extraction and separation of rare earth. In:Xu GX, ed. Rare Earths. 2nd ed. Beijing:Metallurgy Industry Press; 1995:563.
33. Yang LF, Wang DS, Li CC, Sun YY, Zhou XZ, Li YX. Searching for a high efficiency and environmental benign reagent to leach ion-adsorption rare earths based on the zeta potential of clay particles. Green Chem. 2018;20:4528.
34. Hou X, Xu QH, Sun YY, Wang Y, Li J, Zhou XM, et al. The distribution and significance of rare earth and ammonium in ion absorbed rare earth leaching tailings. Chin Rare Earths(in Chin.). 2016;37(4):1.
35. Jing QX, Chai LY, Huang XD, Tang CJ, Guo H, Wang W. Behavior of ammonium adsorption by clay mineral halloysite. Trans Nonferrous Met Soc China.2017;27(7):1627.
2. Chi RA, Tian J. Hydrometallurgy of the weathered crust elution-deposited rare earth ores. Beijing:Science Press; 2006.
3. He LY, Feng TZ, Fu SX, Zhu DS. Study on Extraction of rare earth from ion type rare earth ore by ammonium sulfate leaching. Chin Rare Earths(in Chin.).1983;4(3):1.
4. Xu QH, Sun YY, Zhou XZ, Liu YZ, Li J, Li YX. Green extraction of ion-adsorption rare earth resources. J Chin Soc Rare Earths(in Chin.). 2016;34(6):650.
5. Xiao YF, Chen YY, Feng ZY, Huang XW, Huang L, Long ZQ, et al. Leaching characteristics of ion-adsorption type rare earths ore with Magnesium sulfate.Trans Nonferrous Met Soc China. 2015;11:3784.
6. Yin S, Pei J, Jiang F, Li SW, Peng JH, Zhang LB, et al. Ultrasound-assisted leaching of rare earths from the weathered crustelution-deposited ore using magnesium sulfate without ammonia-nitrogen pollution. Ultrason Sonochem.2018;41:1-56.
7. Huang XW, Yu Y, Feng ZY, Zhao N. A method for recovery of rare earth from ionic rare earth ore. China Patent, CN201010128302.9, 2011.
8. Huang XW, Wang LS, Feng ZY, Huang L, Wang M, Xiao YF, et al. Extraction and recovery of rare earth from low concentration solution of rare earth. 2015. China Patent, CN201310303722.X.
9. Huang XW, Dong JS, Wang LS, Feng ZY, Xue QN, Meng XL, Selective recovery of rare earth elements from ion-adsorption rare earth element ores by stepwise extraction with HEH(EHP)and HDEHP. Green Chem. 2017;19(5):1345.
10. Jia JT, Zhang YW, Wu S, Liao CS, Yan CH, Liu JY, et al. Study on the distribution and separation of aluminum inrare earth extraction separation process(I). Chin Rare Earths(in Chin.). 2001;22(2):10.
11. Wu WY, Li D, Zhao ZH, Jian JL, Zhang FY, Yin SH. Formation mechanism of micro emulsion on aluminum and lanthanum extraction in P507-HC1 system.J Rare Earths. 2010;28(s1):174.
12. Liu ZQ, Zhu W, Guo QS. Study on process of extracting aluminum from highalumina rare earth solution. Materals Res Appl. 2012;6(4):256.
13. Li JH, Zhang X. Distribution ratio and separation coefficient of single rare earth and aluminium in chloronaphthenic acid system. Chin J Rare Metals(in Chin.).2010;34(5):776.
14. Yang XL, Qiu TS. Influence of aluminum ions distribution on the removal of aluminum from rare earth solutions using saponified naphthenic acid. Sep Purif Technol. 2017;186:290.
15. Qiu TS, Fang XH, Wu HQ, Zeng QH, Zhu DM. Leaching behaviors of iron and aluminum elements of ion-absorbed-rare-earth ore with a new impurity depressant. Trans Nonferrous Met Soc China. 2014;24(9):2986.
16. He ZY, Zhang ZY, Yu JX, Chi RA. Study on the behavior of rare earth and aluminum and ammonium in the leaching ofrare earth ores in weathering crust. Chin Rare Earths(in Chin.). 2015;36(6):18.
17. He Z, Zhang ZY, Yu JX, Xu ZG, Chen Z, Chi RA. Kinetics of column leaching of rare earth and aluminum from weathered crust elution-deposited rare earth ore with ammonium salt solutions. Hydrometallurgy. 2016;163(2016):33.
18. Tian J, Chi RA, Zhu GC, Zhang ZG, Xu SM. Occurrence of aluminum in rare earth mine in southern China. Nonferrous Met. 2000;52(3):58.
19. Ouyang KX, Rao GH, Qin HR, Mao YH. Study of southern RE ore leaching by aluminum inhibition. Rare Met Cem Carbides. 2003;31(4):1.
20. Zhao ZH, Xiao XY, Zhang WB, Hao GH, Duan CK, Li D. Application of centrifuging sedimentation on removing aluminum and iron from rare earth solution. Chin Rare Earths(in Chin.). 2007;28(6):95.
21. He ZY, Zhang ZY, Chi RA, Xu ZG, Yu JX, Wu M, et al. Leaching hydrodynamics of weathered elution-deposited rare earth ore with ammonium salts solution.J Rare Earths. 2017;35(8):824.
22. Xiao YF, Feng ZY, Hu GH, Huang L, Huang XW, Chen YY, et al. Reduction leaching of rare earth from ion-adsorption type rare earths ore with ferrous sulfate. J Rare Earths. 2016;34(9):917.
23. Xiao YF, Huang L, Long ZQ, Feng ZY, Wang LS.Adsorption ability of rare earth elements on clay minerals and its practical performance. J Rare Earths.2016;34(5):543.
24. Xiao YF, Liu XS, Feng ZY, Huang XW, Huang L, Chen YY, et al. Role of minerals properties on leaching process of weathered crust elution-deposited rare earth ore. J Rare Earths. 2015;33(5):545.
25. Wang L, Liao CF, Yang YM, Xu HB, Xiao YF, Yan CH. Effects of organic acids on the leaching process of ion-adsorption type rare earth ore. J Rare Earths.2017;35:1233.
26. Tian J, Yin J, Tang XK, Chen J, Luo XP, Rao GH. Enhanced leaching process of a low-grade weathered crust elution-deposited rare earth ore with carboxymethyl sesbania gum. Hydrometallurgy. 2013;139(3):124.
27. Xu QH, Yang LF, Zhang L, Li CC, Wang DS, Zhou XM, et al. Classification and high efficient leaching of ion adsorption rare earth based on its pH dependence. Chin J Inorg Chem. 2018;30(1):112.
28. Li YX, Yang LF, Li CC, Xu QH, Zhang L, Wang Y, et al. Extraction of rare earths from low content rare earth solution with primary amine extractant. China Patent:CN201610821052.4, 2017.
29. Li YX, Xu QH, Wang Y, Xie AL, Hou X, Zhou XZ, et al. A method to improve the extraction rate of ionic rare earth and the safety of tailings. China Patent,CN201310594438.2, 2014.
30. Hidayah NN, Abidin SZ. The evolution of mineral processing in extraction of rare earth elements using liquid-liquid extraction:a review. Miner Eng.2018;121:146.
31. Li YX, Yang LF, Li CC, Xu QH, Zhang L, Wang Y, et al. Method for the high efficiency leaching of ion adsorption rare earths using aluminum sulfate as leaching reagent. China Patent, CN201610821052.4, 2016.
32. Li DQ. Extraction and separation of rare earth. In:Xu GX, ed. Rare Earths. 2nd ed. Beijing:Metallurgy Industry Press; 1995:563.
33. Yang LF, Wang DS, Li CC, Sun YY, Zhou XZ, Li YX. Searching for a high efficiency and environmental benign reagent to leach ion-adsorption rare earths based on the zeta potential of clay particles. Green Chem. 2018;20:4528.
34. Hou X, Xu QH, Sun YY, Wang Y, Li J, Zhou XM, et al. The distribution and significance of rare earth and ammonium in ion absorbed rare earth leaching tailings. Chin Rare Earths(in Chin.). 2016;37(4):1.
35. Jing QX, Chai LY, Huang XD, Tang CJ, Guo H, Wang W. Behavior of ammonium adsorption by clay mineral halloysite. Trans Nonferrous Met Soc China.2017;27(7):1627.