柴达木盆地一里坪盐湖卤水水化学及夏季蒸发中钾、锂、硼行为
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摘要
本文综合利用Na~+,K~+,Mg~(2+)//Cl~-,SO_4~(2-)-H_2O五元体系干基图、水图、钠图,研究柴达木盆地一里坪盐湖硫酸盐型卤水水化学特征受外来淡水补给掺杂、选择性溶解、年温差等多因素影响产生的季节性变化,其中温度为主要因素.当卤水温度降低至0℃,开始析出芒硝,水化学变质系数MgSO_4/MgCl_2比值急剧下降,水化学特征由硫酸镁亚型向氯化物型转化过渡.通过20～25℃晶间卤水L10和L20蒸发实验研究,确定了一里坪卤水蒸发路线、液固相组成、物相鉴定、水化学特征系数、离子行为等变化及成盐特征,并与25℃Na~+,K~+,Mg~(2+)//Cl~-,SO_4~(2-)-H_2O五元体系介稳相图理论预测计算综合对比,二者吻合性比较好,整体相对误差能控制在5%范围内,利用相图理论计算能够很好地指导实际硫酸盐型卤水蒸发析盐.利用水化学特征系数KCl/MgCl_2、MgSO_4/MgCl_2,研究了25℃硫酸盐型盐湖卤水钾盐成盐特征,当变质系数MgSO_4/MgCl_2高于0.13时,卤水钾盐矿物析出的同时,伴随有泻利盐共同析出.利用含Li~+、borate、Mg~(2+)水盐体系相图,研究一里坪老卤水深度蒸发中Li、B的行为,理论预测计算结果,剩余老卤水Mg~(2+)/Li~+比值降至27时,卤水中的Li、B始终以离子形式赋存于卤水中继续富集,此时卤水的累积成卤率仅为2.50%～3.20%,须引入新的工艺技术进行Li、B提取.研究结果为极高镁锂比、高镁硼比的硫酸盐型卤水的综合开发利用提供了理论支持.
Combining with the metastable phase diagram of reciprocal quinary system Na~+,K~+,Mg~(2+)//Cl-,SO_4~(2-)-H_2O,the projection phase diagram of water and sodium,this paper studied hydrochemical characteristics of the sulfate-type brine from Yiliping salt lake in Qaidam Basin. They were changed seasonally due to freshwater mixation,selective leaching,and annual temperature difference as the most important factor. While the brine temperature lowered to 0℃,mirabilite crystallized from the brine,the metamorphic coefficient MgSO_4/MgCl_2 declined sharply,and the hydrochemical characteristic transitioned from magnesium sulfate-type to chloride-type. In this paper,the evaporation experiment of Yiliping brine L10 and L20 had been operated at 20-25℃,and experimental results had been compared with theoretical calculations in the following ways including the evaporation route,chemical compositions of liquid and solid phase,XRD patter analysis,hydrochemical characteristic coefficients,ion behaviors,salt-forming characteristics,and so on. As a result,they were in good agreement with the relative error < 5%. Theoretical calculations of the metastable phase diagram Na~+,K~+,Mg~(2+)//Cl-,SO_4~(2-)-H_2O could be used to guide the actual sulfatetype-brine evaporation better.Then,this paper studied the potash-forming characteristic from the magnesium sulfate-type salt lake brine at 25℃ combining with hydrochemical characteristic coefficients KCl/MgCl_2 and MgSO_4/MgCl_2. While the metamorphic coefficient MgSO_4/MgCl_2 is above0.13,epsomite has crystallized together with potash. Finally,the behavior of Li and B during further evaporation of brine had been theoretical calculated by using several phase diagrams including Li~+,borate,and Mg~(2+)ions. While the mass ratio of Mg~(2+)/Li~+in the brine was above 27,it was considered that Li and B had accumulated fully in the concentrated brine in the deposition stage of bischofite and epsomite,and the brine accumulated rate declined to 2.50%-3.20%. So it's necessary to extract Li and B from the brine by utilizing new technologies. This results provide theoretical support for the exploitation and comprehensive utilization of the very high Mg~(2+)/Li~+and Mg~(2+)/B_2O_3 mass ratio sulfatetype-brine.
Combining with the metastable phase diagram of reciprocal quinary system Na~+,K~+,Mg~(2+)//Cl-,SO_4~(2-)-H_2O,the projection phase diagram of water and sodium,this paper studied hydrochemical characteristics of the sulfate-type brine from Yiliping salt lake in Qaidam Basin. They were changed seasonally due to freshwater mixation,selective leaching,and annual temperature difference as the most important factor. While the brine temperature lowered to 0℃,mirabilite crystallized from the brine,the metamorphic coefficient MgSO_4/MgCl_2 declined sharply,and the hydrochemical characteristic transitioned from magnesium sulfate-type to chloride-type. In this paper,the evaporation experiment of Yiliping brine L10 and L20 had been operated at 20-25℃,and experimental results had been compared with theoretical calculations in the following ways including the evaporation route,chemical compositions of liquid and solid phase,XRD patter analysis,hydrochemical characteristic coefficients,ion behaviors,salt-forming characteristics,and so on. As a result,they were in good agreement with the relative error < 5%. Theoretical calculations of the metastable phase diagram Na~+,K~+,Mg~(2+)//Cl-,SO_4~(2-)-H_2O could be used to guide the actual sulfatetype-brine evaporation better.Then,this paper studied the potash-forming characteristic from the magnesium sulfate-type salt lake brine at 25℃ combining with hydrochemical characteristic coefficients KCl/MgCl_2 and MgSO_4/MgCl_2. While the metamorphic coefficient MgSO_4/MgCl_2 is above0.13,epsomite has crystallized together with potash. Finally,the behavior of Li and B during further evaporation of brine had been theoretical calculated by using several phase diagrams including Li~+,borate,and Mg~(2+)ions. While the mass ratio of Mg~(2+)/Li~+in the brine was above 27,it was considered that Li and B had accumulated fully in the concentrated brine in the deposition stage of bischofite and epsomite,and the brine accumulated rate declined to 2.50%-3.20%. So it's necessary to extract Li and B from the brine by utilizing new technologies. This results provide theoretical support for the exploitation and comprehensive utilization of the very high Mg~(2+)/Li~+and Mg~(2+)/B_2O_3 mass ratio sulfatetype-brine.
引文
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[3]Zheng XY.Comprehensive utilization of salt lake resources over Qinghai-Xizang(Tibet)Plateau.J Lake Sci,1994,6(3):267-275.DOI:10.18307/1994.0310.[郑喜玉.青藏高原盐湖资源的开发利用.湖泊科学,1994,6(3):267-275.]
[4]Gao SY,Song PS,Xia SP eds.Chemistry of salt lakes.Beijing:Science Press,2007:26-35.[高世扬,宋彭生,夏树屏等.盐湖化学.北京:科学出版社,2007:26-35.]
[5]Zhou Y,Li LJ,Wu ZJ et al.Exploitation and comprehensive utilization of Qinghai salt lakes.Progress in Chemistry,2013,25(10):1613-1624.[周园,李丽娟,吴志坚等.青海盐湖资源开发及综合利用.化学进展,2013,25(10):1613-1624.]
[6]Zhang PX ed.Salt lakes in Qaidam basin.Beijing:Science Press,1987:209-211.[张彭熹.柴达木盆地盐湖.北京:科学出版社,1987:209-211.]
[7]Zhu YZ,Li WS,Wu BH et al.New recognition on the geology of the Yiliping Lake and the east and west taijinar lakes in the Qaidam basin,Qinghai province.Geological Review,1989,35(6):558-565.[朱允铸,李文生,吴必豪等.青海省柴达木盆地一里坪和东、西台吉乃尔湖地质新认识.地质论评,1989,35(6):558-565.]
[8]Zhan DP,Yu JQ,Gao CL et al.Hydrogeochemical conditions and lithium brine formation in the four salt lakes of Qaidam basin.J Lake Sci,2010,22(5):783-792.DOI:10.18307/2010.0522.[展大鹏,余俊清,高春亮等.柴达木盆地四盐湖卤水锂资源形成的水文地球化学条件.湖泊科学,2010,22(5):783-792.]
[9]Zhang PX,Zhang MG,Xu C eds.China salt lake scripts.Beijing:Science Press,2002:162-167.[张彭熹,张明刚,徐昶等.中国盐湖志.北京:科学出版社,2002:162-167.]
[10]Yao Y,Song PS,Zhang Q.Prediction of osmotic and activity coefficients and saturation degrees of a salt lake brine yiliping,Qinghai Li-Na-K-Mg-Cl-SO4-H2O system at 25℃.Oceanologia et Limnologia Sinica,1999,30(1):6-13.[姚燕,宋彭生,张契.青海一里平盐湖卤水Li-Na-K-Mg-Cl-SO4-H2O体系25℃时渗透系数、活度系数和饱和度的预测.海洋与湖沼,1999,30(1):6-13.]
[11]Li JD,Shi TC,Wang YX et al.Research on natural evaporation of brine in yiliping mining area.Journal of Salt Lake Science,2008,16(4):32-36,65.[李俊德,石天成,王英孝等.一里坪矿区卤水自然蒸发试验研究.盐湖研究,2008,16(4):32-36,65.]
[12]Bi SF.Study on natural and freezing evaporation of Yiliping brine[Dissertation].Xining:Qinghai University,2016.[毕思峰.一里坪盐湖卤水的自然及冷冻蒸发实验[学位论文].西宁:青海大学,2016.]
[13]Yang CJ,Zhang DY,Wang QY et al.Study on natural evaporation of brine in Yiliping Salt Lake in winter.Industrial Minerals&Processing,2014,43(12):29-31.[杨春节,张大义,汪全义等.一里坪盐湖冬季卤水自然蒸发试验研究.化工矿物与加工,2014,43(12):29-31.]
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