化工学报 ›› 2021, Vol. 72 ›› Issue (6): 3170-3178.DOI: 10.11949/0438-1157.20201690
收稿日期:
2020-11-25
修回日期:
2021-03-05
出版日期:
2021-06-05
发布日期:
2021-06-05
通讯作者:
王士强
作者简介:
李栋婵(1982—),女,博士,副教授,基金资助:
LI Dongchan1(),WANG Jiayu1,WANG Shiqiang1,2()
Received:
2020-11-25
Revised:
2021-03-05
Online:
2021-06-05
Published:
2021-06-05
Contact:
WANG Shiqiang
摘要:
采用等温溶解平衡法,开展四元体系Li+, Mg2+//Cl-, borate–H2O固液相平衡与相图研究,测定平衡溶液的液相组成、密度、折射率和pH。该四元体系相图中存在的盐类矿物为:LiCl·H2O、Li2B4O7·3H2O、 MgCl2·6H2O、Mg2B6O11·15H2O和锂光卤石LiCl·MgCl2·7H2O,其中锂光卤石LiCl·MgCl2·7H2O是异成分复盐,溶液中MgCl2存在下章氏硼镁石(MgB4O7·9H2O)不稳定,转化为多水硼镁石(Mg2B6O11·15H2O)。多水硼镁石结晶区最大,表明镁硼酸盐易于结晶析出,而锂光卤石结晶区最小。采用Pitzer热力学模型对该四元体系的溶解度进行理论预测,计算相图与实验相图吻合较好。该四元体系的稳定相平衡与相图研究,可为含锂硼盐湖老卤中锂、镁、硼产品开发及其综合利用提供理论依据。
中图分类号:
李栋婵, 王嘉宇, 王士强. 四元体系(Li+, Mg2+//Cl-, borate-H2O)308.15 K相平衡与相图研究[J]. 化工学报, 2021, 72(6): 3170-3178.
LI Dongchan, WANG Jiayu, WANG Shiqiang. Phase equilibria and phase diagram of the quaternary system (Li+, Mg2+//Cl-, borate-H2O) at 308.15 K[J]. CIESC Journal, 2021, 72(6): 3170-3178.
No. | Composition of liquid phase(w)/% | J?necke index(J) | Solid phase | ||||||
---|---|---|---|---|---|---|---|---|---|
Li+ | Mg2+ | Cl- | B4O72- | H2O | J(Mg2+) | J(B4O72-) | J(H2O) | ||
1,E1 | 0.28 | 0.01 | 0.00 | 3.20 | 96.51 | 2.00 | 100.15 | 26028.88 | Inderite+Lb |
2 | 0.30 | 0.01 | 0.51 | 2.31 | 96.87 | 1.87 | 67.57 | 24416.78 | Inderite+Lb |
3 | 0.33 | 0.01 | 0.88 | 1.88 | 96.90 | 1.70 | 50.08 | 22241.73 | Inderite+Lb |
4 | 0.44 | 0.01 | 1.55 | 1.65 | 96.35 | 1.28 | 33.10 | 16657.46 | Inderite+Lb |
5 | 0.50 | 0.02 | 1.99 | 1.35 | 96.14 | 2.23 | 23.60 | 14485.54 | Inderite+Lb |
6 | 0.64 | 0.03 | 2.89 | 1.02 | 95.42 | 2.61 | 13.88 | 11189.12 | Inderite+Lb |
7 | 0.86 | 0.05 | 4.12 | 0.92 | 94.05 | 3.21 | 9.26 | 8156.13 | Inderite+Lb |
8 | 1.47 | 0.09 | 7.51 | 0.58 | 90.35 | 3.38 | 3.41 | 4576.09 | Inderite+Lb |
9 | 2.08 | 0.10 | 10.70 | 0.40 | 86.72 | 2.67 | 1.67 | 3126.82 | Inderite+Lb |
10 | 2.88 | 0.10 | 14.88 | 0.27 | 81.87 | 1.94 | 0.82 | 2147.90 | Inderite+Lb |
11,F1 | 3.44 | 0.11 | 17.76 | 0.21 | 78.48 | 1.79 | 0.54 | 1726.44 | Inderite+Lb+Lc |
12 | 3.35 | 0.11 | 17.31 | 0.24 | 78.99 | 1.84 | 0.63 | 1783.48 | Lb+Lc |
13 | 4.04 | 0.10 | 20.83 | 0.18 | 74.85 | 1.39 | 0.39 | 1407.75 | Lb+Lc |
14,E2 | 6.55 | 0.00 | 33.36 | 0.18 | 59.91 | 0.00 | 0.25 | 704.81 | Lb+Lc |
15,E3 | 5.34 | 2.21 | 33.72 | 0.00 | 58.73 | 19.12 | 0.00 | 685.45 | Bis+Lc |
16 | 4.09 | 0.01 | 20.86 | 0.13 | 74.91 | 0.14 | 0.28 | 1409.36 | Inderite+Lc |
17 | 4.18 | 0.02 | 21.33 | 0.13 | 74.34 | 0.27 | 0.28 | 1366.70 | Inderite+Lc |
18 | 4.10 | 0.10 | 21.18 | 0.18 | 74.44 | 1.37 | 0.39 | 1379.83 | Inderite+Lc |
19 | 5.61 | 1.15 | 31.76 | 0.49 | 60.99 | 10.48 | 0.70 | 749.93 | Inderite+Lc |
20 | 6.47 | 1.70 | 37.79 | 0.50 | 53.54 | 13.05 | 0.60 | 554.45 | Inderite+Lc |
21 | 5.85 | 2.17 | 36.01 | 0.41 | 55.56 | 17.48 | 0.52 | 603.90 | Inderite+Lc |
22,F2 | 5.58 | 2.37 | 35.19 | 0.56 | 56.30 | 19.52 | 0.72 | 625.69 | Inderite+Lc+Lcar |
23 | 5.26 | 2.41 | 33.63 | 0.59 | 58.11 | 20.74 | 0.79 | 674.72 | Inderite+Lcar |
24,E4 | 4.93 | 2.84 | 33.44 | 0.00 | 58.79 | 24.76 | 0.00 | 691.41 | Bis+Lcar |
25,F3 | 4.85 | 2.68 | 32.14 | 0.96 | 59.37 | 23.99 | 1.35 | 716.98 | Inderite+Lcar+Bis |
26 | 3.99 | 4.12 | 31.84 | 1.19 | 58.86 | 37.10 | 1.68 | 715.03 | Inderite+Bis |
27 | 2.54 | 5.65 | 29.22 | 0.55 | 62.04 | 55.96 | 0.85 | 828.95 | Inderite+Bis |
28 | 2.07 | 6.34 | 28.75 | 0.70 | 62.14 | 63.63 | 1.10 | 841.36 | Inderite+Bis |
29 | 2.10 | 6.15 | 28.40 | 0.57 | 62.78 | 62.58 | 0.91 | 861.92 | Inderite+Bis |
30 | 1.37 | 4.96 | 21.23 | 0.51 | 71.93 | 67.40 | 1.09 | 1318.76 | Inderite+Bis |
31 | 0.83 | 4.24 | 16.39 | 0.46 | 78.08 | 74.47 | 1.27 | 1850.29 | Inderite+Bis |
32 | 0.41 | 3.66 | 12.57 | 0.44 | 82.92 | 83.60 | 1.57 | 2555.37 | Inderite+Bis |
33,E5 | 0.00 | 3.19 | 9.12 | 0.42 | 87.27 | 100.00 | 2.06 | 3690.87 | Inderite+Bis |
表1 卤水体系Li+, Mg2+//Cl-, borate–H2O在308.15 K的固液相平衡数据
Table 1 Solid-liquid phase equilibria of brine system (Li+, Mg2+//Cl-, borate–H2O) at 308.15 K
No. | Composition of liquid phase(w)/% | J?necke index(J) | Solid phase | ||||||
---|---|---|---|---|---|---|---|---|---|
Li+ | Mg2+ | Cl- | B4O72- | H2O | J(Mg2+) | J(B4O72-) | J(H2O) | ||
1,E1 | 0.28 | 0.01 | 0.00 | 3.20 | 96.51 | 2.00 | 100.15 | 26028.88 | Inderite+Lb |
2 | 0.30 | 0.01 | 0.51 | 2.31 | 96.87 | 1.87 | 67.57 | 24416.78 | Inderite+Lb |
3 | 0.33 | 0.01 | 0.88 | 1.88 | 96.90 | 1.70 | 50.08 | 22241.73 | Inderite+Lb |
4 | 0.44 | 0.01 | 1.55 | 1.65 | 96.35 | 1.28 | 33.10 | 16657.46 | Inderite+Lb |
5 | 0.50 | 0.02 | 1.99 | 1.35 | 96.14 | 2.23 | 23.60 | 14485.54 | Inderite+Lb |
6 | 0.64 | 0.03 | 2.89 | 1.02 | 95.42 | 2.61 | 13.88 | 11189.12 | Inderite+Lb |
7 | 0.86 | 0.05 | 4.12 | 0.92 | 94.05 | 3.21 | 9.26 | 8156.13 | Inderite+Lb |
8 | 1.47 | 0.09 | 7.51 | 0.58 | 90.35 | 3.38 | 3.41 | 4576.09 | Inderite+Lb |
9 | 2.08 | 0.10 | 10.70 | 0.40 | 86.72 | 2.67 | 1.67 | 3126.82 | Inderite+Lb |
10 | 2.88 | 0.10 | 14.88 | 0.27 | 81.87 | 1.94 | 0.82 | 2147.90 | Inderite+Lb |
11,F1 | 3.44 | 0.11 | 17.76 | 0.21 | 78.48 | 1.79 | 0.54 | 1726.44 | Inderite+Lb+Lc |
12 | 3.35 | 0.11 | 17.31 | 0.24 | 78.99 | 1.84 | 0.63 | 1783.48 | Lb+Lc |
13 | 4.04 | 0.10 | 20.83 | 0.18 | 74.85 | 1.39 | 0.39 | 1407.75 | Lb+Lc |
14,E2 | 6.55 | 0.00 | 33.36 | 0.18 | 59.91 | 0.00 | 0.25 | 704.81 | Lb+Lc |
15,E3 | 5.34 | 2.21 | 33.72 | 0.00 | 58.73 | 19.12 | 0.00 | 685.45 | Bis+Lc |
16 | 4.09 | 0.01 | 20.86 | 0.13 | 74.91 | 0.14 | 0.28 | 1409.36 | Inderite+Lc |
17 | 4.18 | 0.02 | 21.33 | 0.13 | 74.34 | 0.27 | 0.28 | 1366.70 | Inderite+Lc |
18 | 4.10 | 0.10 | 21.18 | 0.18 | 74.44 | 1.37 | 0.39 | 1379.83 | Inderite+Lc |
19 | 5.61 | 1.15 | 31.76 | 0.49 | 60.99 | 10.48 | 0.70 | 749.93 | Inderite+Lc |
20 | 6.47 | 1.70 | 37.79 | 0.50 | 53.54 | 13.05 | 0.60 | 554.45 | Inderite+Lc |
21 | 5.85 | 2.17 | 36.01 | 0.41 | 55.56 | 17.48 | 0.52 | 603.90 | Inderite+Lc |
22,F2 | 5.58 | 2.37 | 35.19 | 0.56 | 56.30 | 19.52 | 0.72 | 625.69 | Inderite+Lc+Lcar |
23 | 5.26 | 2.41 | 33.63 | 0.59 | 58.11 | 20.74 | 0.79 | 674.72 | Inderite+Lcar |
24,E4 | 4.93 | 2.84 | 33.44 | 0.00 | 58.79 | 24.76 | 0.00 | 691.41 | Bis+Lcar |
25,F3 | 4.85 | 2.68 | 32.14 | 0.96 | 59.37 | 23.99 | 1.35 | 716.98 | Inderite+Lcar+Bis |
26 | 3.99 | 4.12 | 31.84 | 1.19 | 58.86 | 37.10 | 1.68 | 715.03 | Inderite+Bis |
27 | 2.54 | 5.65 | 29.22 | 0.55 | 62.04 | 55.96 | 0.85 | 828.95 | Inderite+Bis |
28 | 2.07 | 6.34 | 28.75 | 0.70 | 62.14 | 63.63 | 1.10 | 841.36 | Inderite+Bis |
29 | 2.10 | 6.15 | 28.40 | 0.57 | 62.78 | 62.58 | 0.91 | 861.92 | Inderite+Bis |
30 | 1.37 | 4.96 | 21.23 | 0.51 | 71.93 | 67.40 | 1.09 | 1318.76 | Inderite+Bis |
31 | 0.83 | 4.24 | 16.39 | 0.46 | 78.08 | 74.47 | 1.27 | 1850.29 | Inderite+Bis |
32 | 0.41 | 3.66 | 12.57 | 0.44 | 82.92 | 83.60 | 1.57 | 2555.37 | Inderite+Bis |
33,E5 | 0.00 | 3.19 | 9.12 | 0.42 | 87.27 | 100.00 | 2.06 | 3690.87 | Inderite+Bis |
No. | J(Mg2+) | Density, ρ/(g·cm-3) | nD | pH |
---|---|---|---|---|
1,E1 | 2.00 | 1.0262 | 1.3400 | 9.195 |
2 | 1.87 | 1.0248 | 1.3421 | 9.173 |
3 | 1.70 | 1.022 | 1.3432 | 9.160 |
4 | 1.28 | 1.0241 | 1.3503 | 9.036 |
5 | 2.23 | 1.0267 | 1.3584 | 9.026 |
6 | 2.61 | 1.0281 | 1.3680 | 8.806 |
7 | 3.21 | 1.0300 | 1.3768 | 8.524 |
8 | 3.38 | 1.0484 | 1.3750 | 8.314 |
9 | 2.67 | 1.0694 | 1.3852 | 8.134 |
10 | 1.94 | 1.0957 | 1.4213 | 7.961 |
11,F1 | 1.79 | 1.1199 | 1.3400 | 7.669 |
12 | 1.84 | 1.1256 | 1.3421 | 7.791 |
13 | 1.39 | 1.1429 | 1.3432 | 6.826 |
14,E2 | 0.00 | 1.2498 | 1.3503 | 4.821 |
15,E3 | 19.12 | 1.3121 | 1.4354 | 3.992 |
16 | 0.14 | 1.1412 | 1.3849 | 6.066 |
17 | 0.27 | 1.1447 | 1.3861 | 5.762 |
18 | 1.37 | 1.1483 | 1.3871 | 5.914 |
19 | 10.48 | 1.2581 | 1.4217 | 4.409 |
20 | 13.05 | 1.3178 | 1.4369 | 4.071 |
21 | 17.48 | 1.3190 | 1.438 | 3.961 |
22,F2 | 19.52 | 1.3207 | 1.4365 | 3.971 |
23 | 20.74 | 1.3191 | 1.4362 | 3.962 |
24,E4 | 24.76 | 1.3090 | 1.4348 | 4.007 |
25,F3 | 23.99 | 1.3187 | 1.4351 | 3.946 |
26 | 37.10 | 1.3180 | 1.4331 | 3.952 |
27 | 55.96 | 1.3208 | 1.4353 | 4.021 |
28 | 63.63 | 1.3252 | 1.4373 | 3.986 |
29 | 62.58 | 1.3258 | 1.4375 | 3.967 |
30 | 67.40 | 1.3285 | 1.4389 | 4.001 |
31 | 74.47 | 1.3296 | 1.4398 | 4.012 |
32 | 83.60 | 1.3311 | 1.4407 | 4.023 |
33,E5 | 100.00 | 1.3375 | 1.4428 | 4.112 |
表2 四元体系Li+, Mg2+//Cl-, borate–H2O在308.15 K的物化性质
Table 2 Physiochemical property of the quaternary system (Li+, Mg2+//Cl-, borate–H2O) at 308.15 K
No. | J(Mg2+) | Density, ρ/(g·cm-3) | nD | pH |
---|---|---|---|---|
1,E1 | 2.00 | 1.0262 | 1.3400 | 9.195 |
2 | 1.87 | 1.0248 | 1.3421 | 9.173 |
3 | 1.70 | 1.022 | 1.3432 | 9.160 |
4 | 1.28 | 1.0241 | 1.3503 | 9.036 |
5 | 2.23 | 1.0267 | 1.3584 | 9.026 |
6 | 2.61 | 1.0281 | 1.3680 | 8.806 |
7 | 3.21 | 1.0300 | 1.3768 | 8.524 |
8 | 3.38 | 1.0484 | 1.3750 | 8.314 |
9 | 2.67 | 1.0694 | 1.3852 | 8.134 |
10 | 1.94 | 1.0957 | 1.4213 | 7.961 |
11,F1 | 1.79 | 1.1199 | 1.3400 | 7.669 |
12 | 1.84 | 1.1256 | 1.3421 | 7.791 |
13 | 1.39 | 1.1429 | 1.3432 | 6.826 |
14,E2 | 0.00 | 1.2498 | 1.3503 | 4.821 |
15,E3 | 19.12 | 1.3121 | 1.4354 | 3.992 |
16 | 0.14 | 1.1412 | 1.3849 | 6.066 |
17 | 0.27 | 1.1447 | 1.3861 | 5.762 |
18 | 1.37 | 1.1483 | 1.3871 | 5.914 |
19 | 10.48 | 1.2581 | 1.4217 | 4.409 |
20 | 13.05 | 1.3178 | 1.4369 | 4.071 |
21 | 17.48 | 1.3190 | 1.438 | 3.961 |
22,F2 | 19.52 | 1.3207 | 1.4365 | 3.971 |
23 | 20.74 | 1.3191 | 1.4362 | 3.962 |
24,E4 | 24.76 | 1.3090 | 1.4348 | 4.007 |
25,F3 | 23.99 | 1.3187 | 1.4351 | 3.946 |
26 | 37.10 | 1.3180 | 1.4331 | 3.952 |
27 | 55.96 | 1.3208 | 1.4353 | 4.021 |
28 | 63.63 | 1.3252 | 1.4373 | 3.986 |
29 | 62.58 | 1.3258 | 1.4375 | 3.967 |
30 | 67.40 | 1.3285 | 1.4389 | 4.001 |
31 | 74.47 | 1.3296 | 1.4398 | 4.012 |
32 | 83.60 | 1.3311 | 1.4407 | 4.023 |
33,E5 | 100.00 | 1.3375 | 1.4428 | 4.112 |
图4 四元体系(Li+, Mg2+//Cl-, borate–H2O) 308.15 K溶液物化性质
Fig.4 Physiochemical property diagram of the quaternary system (Li+, Mg2+//Cl-, borate–H2O) at 308.15 K
Species | β(0) | β(1) | β(2) | C? | θ | ψ |
---|---|---|---|---|---|---|
LiCl | 0.1469 | 0.3134 | — | -0.00324 | — | — |
MgCl2 | 0.3455 | 1.6987 | — | 0.05489 | — | — |
Li2B4O7 | 5.9118 | -37.298 | — | -7.3439 | — | — |
MgB4O7 | -1.7318 | 6.2356 | -139.94 | -1.4978 | — | — |
Li+, Mg2+ | — | — | — | — | -0.00743 | — |
Cl-, B4O72- | — | — | — | — | 0.05252 | — |
Li+,Mg2+,Cl- | — | — | — | — | — | 0.00 |
Li+,Mg2+,B4O72- | — | — | — | — | — | 0.00 |
Li+, Cl-,B4O72- | — | — | — | — | — | 1.0857 |
Mg2+,Cl-,B4O72- | — | — | — | — | — | 0.7383 |
表3 四元体系Li+, Mg2+//Cl-, borate–H2O在308.15 K模型参数
Table 3 Pitzer parameters of the system (Li+, Mg2+//Cl-, borate–H2O) at 308.15 K
Species | β(0) | β(1) | β(2) | C? | θ | ψ |
---|---|---|---|---|---|---|
LiCl | 0.1469 | 0.3134 | — | -0.00324 | — | — |
MgCl2 | 0.3455 | 1.6987 | — | 0.05489 | — | — |
Li2B4O7 | 5.9118 | -37.298 | — | -7.3439 | — | — |
MgB4O7 | -1.7318 | 6.2356 | -139.94 | -1.4978 | — | — |
Li+, Mg2+ | — | — | — | — | -0.00743 | — |
Cl-, B4O72- | — | — | — | — | 0.05252 | — |
Li+,Mg2+,Cl- | — | — | — | — | — | 0.00 |
Li+,Mg2+,B4O72- | — | — | — | — | — | 0.00 |
Li+, Cl-,B4O72- | — | — | — | — | — | 1.0857 |
Mg2+,Cl-,B4O72- | — | — | — | — | — | 0.7383 |
图5 四元体系(Li+, Mg2+//Cl-, borate–H2O) 308.15 K计算与实验相图对比
Fig.5 Comparison of the calculated and experimental phase diagram of the system (Li+, Mg2+//Cl-, borate–H2O) at 308.15 K
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