化工学报 ›› 2019, Vol. 70 ›› Issue (11): 4123-4130.DOI: 10.11949/0438-1157.20190647
收稿日期:
2019-06-10
修回日期:
2019-08-22
出版日期:
2019-11-05
发布日期:
2019-11-05
通讯作者:
王敏
作者简介:
戈海文(1984—),男,硕士,助理研究员,基金资助:
Haiwen GE1,2(),Huaiyou WANG1,2,Min WANG1,2()
Received:
2019-06-10
Revised:
2019-08-22
Online:
2019-11-05
Published:
2019-11-05
Contact:
Min WANG
摘要:
采用等温溶解平衡法开展碳酸锂在碳酸钠溶液中(278.15~358.15 K)的溶解平衡实验研究,测定平衡体系碳酸锂溶解度和平衡溶液密度,利用E-DH方程对碳酸锂溶解度实验数据进行关联,标准偏差小于0.01;利用Connaughton方程对液相密度数据进行关联,标准偏差小于2×10-3。实验和计算研究结果表明:在同离子和盐效应协同影响下,碳酸锂在Na2CO3-H2O体系中溶解度随碳酸钠浓度增加先降低后降低趋势变缓,在278.15~358.15 K温度范围内,溶解度转变折点为碳酸钠浓度约为0.1 mol·kg-1;通过溶解热力学计算,得到碳酸锂在碳酸钠中的溶解焓变(ΔHd)、熵变(ΔSd)和Gibbs自由能变(ΔGd),结果表明溶解过程为放热、熵减的非自发过程,溶解焓变和熵变随着碳酸钠浓度增加而增加,Gibbs自由能变在0.6 mol·kg-1出现最大值,且溶解过程为熵控制过程。研究结果将为卤水提锂碳化沉锂过程设计提供基础数据。
中图分类号:
戈海文, 王怀有, 王敏. 碳酸锂在碳酸钠溶液中的溶解度与热力学[J]. 化工学报, 2019, 70(11): 4123-4130.
Haiwen GE, Huaiyou WANG, Min WANG. Solubility and thermodynamics of lithium carbonate in sodium carbonate solution[J]. CIESC Journal, 2019, 70(11): 4123-4130.
(mol·kg-1) | (mol·kg-1) | ρ/(g·cm-3) | (mol·kg-1) | (mol·kg-1) | ρ/(g·cm-3) | (mol·kg-1) | (mol·kg-1) | ρ/(g·cm-3) |
---|---|---|---|---|---|---|---|---|
278.15 K | 308.15 K | 338.15 K | ||||||
0 0.0100 0.0203 0.0500 0.0699 0.1000 0.2869 0.4789 0.6521 0.8244 0.9938 1.1473 1.2808 1.4041 1.5801 1.6970 | 0.2122 0.2092 0.2066 0.2026 0.2007 0.1978 0.1887 0.1832 0.1795 0.1758 0.1723 0.1703 0.1689 0.1679 0.1667 0.1661 | 1.01319 1.01423 1.01502 1.01771 1.01939 1.02206 1.04224 1.05625 1.07596 1.09412 1.11250 1.12993 1.14522 1.16051 1.18297 1.19884 | 0 0.0100 0.0203 0.0500 0.0699 0.1000 0.2999 0.4697 0.6662 0.7975 0.9915 1.1504 1.2664 1.3503 1.4389 1.6734 | 0.1460 0.1448 0.1436 0.1416 0.1393 0.1377 0.1310 0.1287 0.1262 0.1251 0.1231 0.1217 0.1205 0.1198 0.1189 0.1167 | 1.00924 1.00981 1.01067 1.01260 1.01392 1.01614 1.03623 1.05277 1.07093 1.08600 1.10502 1.12462 1.13800 1.14748 1.15598 1.18412 | 0 0.0137 0.0225 0.0539 0.0691 0.0994 0.2808 0.3860 0.6659 0.8582 0.9944 1.0856 1.3309 1.4766 1.5863 1.7003 | 0.1118 0.1112 0.1102 0.1090 0.1076 0.1056 0.1036 0.1015 0.0998 0.0982 0.0974 0.0969 0.0965 0.0962 0.0959 0.0956 | 1.01021 1.01122 1.01190 1.01493 1.01629 1.01865 1.03587 1.04674 1.07783 1.09537 1.11162 1.12096 1.14863 1.16713 1.18202 1.19403 |
288.15 K | 318.15 K | 348.15 K | ||||||
0 0.0100 0.0203 0.0500 0.0699 0.1000 0.2928 0.4807 0.6544 0.8328 0.9784 1.1560 1.2875 1.4490 1.5967 1.6958 | 0.1844 0.1826 0.1819 0.1799 0.1786 0.1766 0.1696 0.1652 0.1621 0.1595 0.1578 0.1558 0.1544 0.1528 0.1511 0.1502 | 0.99972 1.00068 1.00105 1.00411 1.00636 1.00809 1.02755 1.04397 1.06560 1.08103 1.09713 1.11942 1.13652 1.15176 1.16646 1.18660 | 0 0.0100 0.0203 0.0500 0.0699 0.1000 0.2999 0.4653 0.6580 0.7968 0.9975 1.1458 1.2717 1.3928 1.4461 1.6589 | 0.1313 0.1306 0.1293 0.1266 0.1252 0.1232 0.1204 0.1166 0.1145 0.1124 0.1111 0.1102 0.1098 0.1088 0.1084 0.1076 | 1.01180 1.01233 1.01326 1.01559 1.01740 1.01982 1.03942 1.05491 1.07592 1.09010 1.11190 1.12842 1.14393 1.15889 1.16700 1.19354 | 0 0.0122 0.0208 0.0549 0.0737 0.1022 0.2971 0.4153 0.6759 0.8569 1.0001 1.1851 1.3570 1.4941 1.6229 1.7651 | 0.1047 0.1036 0.1026 0.1012 0.1003 0.0981 0.0956 0.0924 0.0906 0.0890 0.0881 0.0873 0.0866 0.0861 0.0855 0.0849 | 1.01272 1.01350 1.01428 1.01740 1.01935 1.02091 1.03921 1.04953 1.07591 1.09373 1.10803 1.12868 1.14703 1.16309 1.17915 1.19600 |
298.15 K | 328.15 K | 358.15 K | ||||||
0 0.0100 0.0203 0.0500 0.0699 0.1000 0.2999 0.4835 0.6689 0.8290 0.9987 1.1482 1.2904 1.4423 1.5847 1.7555 | 0.1643 0.1633 0.1618 0.1583 0.1560 0.1547 0.1484 0.1442 0.1408 0.1385 0.1361 0.1338 0.1327 0.1320 0.1312 0.1303 | 1.00455 1.00675 1.00740 1.00981 1.01393 1.01569 1.03510 1.05051 1.06890 1.08956 1.10256 1.12147 1.13787 1.15559 1.17257 1.19856 | 0 0.0159 0.0256 0.0511 0.0717 0.0975 0.2889 0.4551 0.6409 0.8074 0.9797 1.1256 1.2576 1.3728 1.5014 1.6558 | 0.1194 0.1184 0.1167 0.1157 0.1149 0.1126 0.1086 0.1071 0.1057 0.1047 0.1039 0.1033 0.1027 0.1025 0.1020 0.1016 | 1.01822 1.01927 1.02022 1.02325 1.02596 1.02867 1.05062 1.06883 1.08990 1.10916 1.13009 1.14910 1.16623 1.18240 1.20047 1.22193 | 0 0.0109 0.0199 0.0560 0.0723 0.1036 0.2932 0.4840 0.6559 0.8366 0.9871 1.1468 1.3385 1.4540 1.5811 1.7287 | 0.09532 0.09475 0.09337 0.09149 0.08955 0.08733 0.08459 0.08210 0.08052 0.07954 0.07892 0.07847 0.07802 0.07761 0.07730 0.07701 | 1.01048 1.01080 1.01143 1.01460 1.01586 1.01869 1.03549 1.05297 1.07208 1.08993 1.10670 1.12165 1.14762 1.15965 1.17548 1.19353 |
表1 278.15~358.15 K时碳酸锂在碳酸钠溶液中溶解度以及密度
Table 1 Solubility and density of lithium carbonate in sodium carbonate solution at 278.15—358.15 K
(mol·kg-1) | (mol·kg-1) | ρ/(g·cm-3) | (mol·kg-1) | (mol·kg-1) | ρ/(g·cm-3) | (mol·kg-1) | (mol·kg-1) | ρ/(g·cm-3) |
---|---|---|---|---|---|---|---|---|
278.15 K | 308.15 K | 338.15 K | ||||||
0 0.0100 0.0203 0.0500 0.0699 0.1000 0.2869 0.4789 0.6521 0.8244 0.9938 1.1473 1.2808 1.4041 1.5801 1.6970 | 0.2122 0.2092 0.2066 0.2026 0.2007 0.1978 0.1887 0.1832 0.1795 0.1758 0.1723 0.1703 0.1689 0.1679 0.1667 0.1661 | 1.01319 1.01423 1.01502 1.01771 1.01939 1.02206 1.04224 1.05625 1.07596 1.09412 1.11250 1.12993 1.14522 1.16051 1.18297 1.19884 | 0 0.0100 0.0203 0.0500 0.0699 0.1000 0.2999 0.4697 0.6662 0.7975 0.9915 1.1504 1.2664 1.3503 1.4389 1.6734 | 0.1460 0.1448 0.1436 0.1416 0.1393 0.1377 0.1310 0.1287 0.1262 0.1251 0.1231 0.1217 0.1205 0.1198 0.1189 0.1167 | 1.00924 1.00981 1.01067 1.01260 1.01392 1.01614 1.03623 1.05277 1.07093 1.08600 1.10502 1.12462 1.13800 1.14748 1.15598 1.18412 | 0 0.0137 0.0225 0.0539 0.0691 0.0994 0.2808 0.3860 0.6659 0.8582 0.9944 1.0856 1.3309 1.4766 1.5863 1.7003 | 0.1118 0.1112 0.1102 0.1090 0.1076 0.1056 0.1036 0.1015 0.0998 0.0982 0.0974 0.0969 0.0965 0.0962 0.0959 0.0956 | 1.01021 1.01122 1.01190 1.01493 1.01629 1.01865 1.03587 1.04674 1.07783 1.09537 1.11162 1.12096 1.14863 1.16713 1.18202 1.19403 |
288.15 K | 318.15 K | 348.15 K | ||||||
0 0.0100 0.0203 0.0500 0.0699 0.1000 0.2928 0.4807 0.6544 0.8328 0.9784 1.1560 1.2875 1.4490 1.5967 1.6958 | 0.1844 0.1826 0.1819 0.1799 0.1786 0.1766 0.1696 0.1652 0.1621 0.1595 0.1578 0.1558 0.1544 0.1528 0.1511 0.1502 | 0.99972 1.00068 1.00105 1.00411 1.00636 1.00809 1.02755 1.04397 1.06560 1.08103 1.09713 1.11942 1.13652 1.15176 1.16646 1.18660 | 0 0.0100 0.0203 0.0500 0.0699 0.1000 0.2999 0.4653 0.6580 0.7968 0.9975 1.1458 1.2717 1.3928 1.4461 1.6589 | 0.1313 0.1306 0.1293 0.1266 0.1252 0.1232 0.1204 0.1166 0.1145 0.1124 0.1111 0.1102 0.1098 0.1088 0.1084 0.1076 | 1.01180 1.01233 1.01326 1.01559 1.01740 1.01982 1.03942 1.05491 1.07592 1.09010 1.11190 1.12842 1.14393 1.15889 1.16700 1.19354 | 0 0.0122 0.0208 0.0549 0.0737 0.1022 0.2971 0.4153 0.6759 0.8569 1.0001 1.1851 1.3570 1.4941 1.6229 1.7651 | 0.1047 0.1036 0.1026 0.1012 0.1003 0.0981 0.0956 0.0924 0.0906 0.0890 0.0881 0.0873 0.0866 0.0861 0.0855 0.0849 | 1.01272 1.01350 1.01428 1.01740 1.01935 1.02091 1.03921 1.04953 1.07591 1.09373 1.10803 1.12868 1.14703 1.16309 1.17915 1.19600 |
298.15 K | 328.15 K | 358.15 K | ||||||
0 0.0100 0.0203 0.0500 0.0699 0.1000 0.2999 0.4835 0.6689 0.8290 0.9987 1.1482 1.2904 1.4423 1.5847 1.7555 | 0.1643 0.1633 0.1618 0.1583 0.1560 0.1547 0.1484 0.1442 0.1408 0.1385 0.1361 0.1338 0.1327 0.1320 0.1312 0.1303 | 1.00455 1.00675 1.00740 1.00981 1.01393 1.01569 1.03510 1.05051 1.06890 1.08956 1.10256 1.12147 1.13787 1.15559 1.17257 1.19856 | 0 0.0159 0.0256 0.0511 0.0717 0.0975 0.2889 0.4551 0.6409 0.8074 0.9797 1.1256 1.2576 1.3728 1.5014 1.6558 | 0.1194 0.1184 0.1167 0.1157 0.1149 0.1126 0.1086 0.1071 0.1057 0.1047 0.1039 0.1033 0.1027 0.1025 0.1020 0.1016 | 1.01822 1.01927 1.02022 1.02325 1.02596 1.02867 1.05062 1.06883 1.08990 1.10916 1.13009 1.14910 1.16623 1.18240 1.20047 1.22193 | 0 0.0109 0.0199 0.0560 0.0723 0.1036 0.2932 0.4840 0.6559 0.8366 0.9871 1.1468 1.3385 1.4540 1.5811 1.7287 | 0.09532 0.09475 0.09337 0.09149 0.08955 0.08733 0.08459 0.08210 0.08052 0.07954 0.07892 0.07847 0.07802 0.07761 0.07730 0.07701 | 1.01048 1.01080 1.01143 1.01460 1.01586 1.01869 1.03549 1.05297 1.07208 1.08993 1.10670 1.12165 1.14762 1.15965 1.17548 1.19353 |
T/K | A | Ba | C | D | σ |
---|---|---|---|---|---|
278.15 288.15 298.15 308.15 318.15 328.15 338.15 348.15 358.15 | 0.56776 0.52846 0.51160 0.48690 0.46413 0.44307 0.42357 0.40545 0.38859 | 24.19 25.66 28.58 28.32 30.95 35.60 42.61 50.17 54.66 | -0.3154 -0.3636 -0.3621 -0.4050 -0.4273 -0.4465 -0.4499 -0.4438 -0.4551 | 0.02800 0.03444 0.03407 0.04128 0.04422 0.04593 0.04560 0.04510 0.04678 | 0.008213 0.009855 0.009934 0.008765 0.009765 0.009440 0.01059 0.01061 0.009062 |
表2 不同温度下的Debye-Hückel延展模型参数和标准偏差
Table 2 Model parameters and standard deviation of extended Debye-Hückel model at different temperatures
T/K | A | Ba | C | D | σ |
---|---|---|---|---|---|
278.15 288.15 298.15 308.15 318.15 328.15 338.15 348.15 358.15 | 0.56776 0.52846 0.51160 0.48690 0.46413 0.44307 0.42357 0.40545 0.38859 | 24.19 25.66 28.58 28.32 30.95 35.60 42.61 50.17 54.66 | -0.3154 -0.3636 -0.3621 -0.4050 -0.4273 -0.4465 -0.4499 -0.4438 -0.4551 | 0.02800 0.03444 0.03407 0.04128 0.04422 0.04593 0.04560 0.04510 0.04678 | 0.008213 0.009855 0.009934 0.008765 0.009765 0.009440 0.01059 0.01061 0.009062 |
T/K | a1 | b1 | a2 | b2 | σ |
---|---|---|---|---|---|
278.15 288.15 298.15 308.15 318.15 328.15 338.15 348.15 358.15 | 0.7326 0.3796 1.558 0.1412 0.7893 2.095 0.8836 1.597 1.529 | -1.461 -0.8787 -3.729 -0.1025 -1.730 -5.298 -1.852 -3.823 -3.545 | 0.05298 0.06969 0.03699 0.08134 0.06800 0.07174 0.08070 0.06645 0.06883 | 0.03858 0.02718 0.04579 0.01922 0.03088 0.03559 0.02107 0.02659 0.0281 | 0.9615×10-3 1.894×10-3 1.479×10-3 0.7667×10-3 0.6910×10-3 0.5967×10-3 0.8899×10-3 0.5291×10-3 0.8378×10-3 |
表3 不同温度下的Connaughton方程参数和标准偏差
Table 3 Model parameters and standard deviation of Connaughton equation at different temperatures
T/K | a1 | b1 | a2 | b2 | σ |
---|---|---|---|---|---|
278.15 288.15 298.15 308.15 318.15 328.15 338.15 348.15 358.15 | 0.7326 0.3796 1.558 0.1412 0.7893 2.095 0.8836 1.597 1.529 | -1.461 -0.8787 -3.729 -0.1025 -1.730 -5.298 -1.852 -3.823 -3.545 | 0.05298 0.06969 0.03699 0.08134 0.06800 0.07174 0.08070 0.06645 0.06883 | 0.03858 0.02718 0.04579 0.01922 0.03088 0.03559 0.02107 0.02659 0.0281 | 0.9615×10-3 1.894×10-3 1.479×10-3 0.7667×10-3 0.6910×10-3 0.5967×10-3 0.8899×10-3 0.5291×10-3 0.8378×10-3 |
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