KCl-PEG4000-H2O三元体系288、298、308 K相平衡测定及计算

doi:10.11949/j.issn.0438-1157.20181154

摘要/Abstract

摘要：

采用等温溶解平衡法研究了288、298、308 K下三元体系KCl-PEG4000-H₂O的相平衡关系，绘制了相应的相图、密度-组成图和折射率-组成图。研究发现：288、298、308 K下，三元体系KCl-PEG4000-H₂O无分层现象，只存在固液相平衡关系，其平衡相图由不饱和液相区(L)、一固一液区(S+L)和两固一液区(2S+L)构成，且两固一液区随温度升高减小。KCl溶解度随着溶液中PEG4000含量不断增加而减小。溶液中PEG4000含量小于0.50时，盐析率受温度影响较小；含量大于0.50时，盐析率随着温度升高呈减小趋势。采用修正后的Pitzer方程进行了三元体系KCl-PEG4000-H₂O (288、298、308 K)溶解度计算，对比发现，理论计算值与实验值吻合较好。

关键词: 相平衡, 热力学性质, 溶解性, 混合溶剂, Pitzer方程

Abstract:

The phase equilibrium relationship of the ternary system KCl-PEG4000-H₂O at 288, 298 and 308 K was studied by isothermal dissolution equilibrium method. The corresponding phase diagram, density-composition diagram and refractive index-composition diagram were drawn. The results show that over the entire PEG 4000 composition rang studied only one liquid phase is obtained, without the biphase region formed at 288, 298 and 308 K. The phase diagram of system KCl-PEG4000-H₂O consists of one homogeneous area with unsaturated liquid (L), an equilibrium area containing the solid phase of KCl and saturated liquid phase (S+L), one area with one liquid phase and two solid phases(2S+L). The area of (2S+L) decrease with the increasing of temperature, while the areas of (L) and (S+L) increase with the increasing of temperature. The solubility of KCl decreases with the addition of PEG 4000 at 288, 298 and 308 K. When w_PEG4000 in the solution is less than 0.50, the temperature has little effect on the salting-out ratio of the system, while when w_PEG4000 is higher than 0.50, the salting-out ratio of the system decreases with the increasing of temperature. The thermodynamics calculation of equilibrium data of system KCl-PEG4000-H₂O at 288, 298 and 308 K was carried out by using the modified Pitzer equation, it can be seen from the comparison of experimental and calculation diagrams that the predictive solubilities agree well with the experimental values.

Key words: phase equilibria, thermodynamic properties, solubility, mixed solvents, Pitzer equation

中图分类号:

O 642

于旭东, 黄琴, 王林, 李茂兰, 郑洪, 曾英. KCl-PEG4000-H₂O三元体系288、298、308 K相平衡测定及计算[J]. 化工学报, 2019, 70(3): 830-839.

Xudong YU, Qin HUANG, Lin WANG, Maolan LI, Hong ZHENG, Ying ZENG. Measurements and simulation for ternary system KCl-PEG4000-H₂O at 288, 298 and 308 K[J]. CIESC Journal, 2019, 70(3): 830-839.

图/表 10

图1 288、298、308 K时KCl在水中的溶解度对比

Fig.1 Solubility for KCl in pure water at 288，298 and 308 K: ●，▲，■ solubility for KCl at 288，298 and 308 K by this work，○，Δ，□ solubility for KCl at 288，298 and 308 K from literatures[23,24,25,26,27,28]

表1 288、298、308 K时KCl在水中的溶解度

Table 1 Solubility of KCl in pure water at 288，298 and 308 K

T/K	Solubility/(g/g)		Relative deviation(RD)^①
T/K	This work	Ref.	Relative deviation(RD)^①
288	0.2485	0.2482^[23]	–0.0012
288	0.2485	0.2484^[24]	–0.0004
298	0.2639	0.2642^[25]	0.0011
		0.2645^[26]	0.0023
		0.2630^[27]	–0.0034
308	0.2851	0.2824^[23]	–0.0095
308	0.2851	0.2863^[28]	0.0042

表2 三元体系KCl-PEG4000-H2O 在288、298和308 K下的溶解度、密度、折射率和盐析率数据

No.	Density，ρ/ (g?cm^–3)	Refractive index，n_D	Composition of equilibrated solution		R	Composition of wet solid phase			Equilibrated solid phase
No.	Density，ρ/ (g?cm^–3)	Refractive index，n_D	w(KCl)	w(PEG4000)	R	w(KCl)		w(PEG4000)	Equilibrated solid phase
T=288 K
1A	1.1671	1.3680	0.2485	0.0000	0.0000	－	－		KCl
2	1.1649	1.3723	0.2387	0.0381	0.0396	0.8875	0.0056		KCl
3	1.1622	1.3764	0.2219	0.0778	0.1070	0.8694	0.0131		KCl
4	1.1592	1.3807	0.2073	0.1188	0.1656	0.8615	0.0208		KCl
5	1.1569	1.3852	0.1899	0.1619	0.2357	0.7081	0.0583		KCl
6	1.1548	1.3898	0.1758	0.2061	0.2924	0.7530	0.0618		KCl
7	1.1520	1.3950	0.1613	0.2517	0.3507	0.6919	0.0925		KCl
8	1.1510	1.4003	0.1448	0.2993	0.4174	0.6924	0.1077		KCl
9	1.1507	1.4061	0.1300	0.3478	0.4768	0.6974	0.1210		KCl
10	1.1509	1.4122	0.1188	0.3966	0.5221	0.7025	0.1339		KCl
11	1.1516	1.4174	0.1056	0.4468	0.5751	0.6464	0.1766		KCl
12	1.1496	1.4240	0.0893	0.5010	0.6406	0.6672	0.1831		KCl
13	1.1364	1.4282	0.0389	0.5767	0.8434	0.7232	0.1661		KCl
14B	1.1071	1.4281	0.0000	0.6485	1.0000	－	－		－
T=298 K
15C	1.1798	1.3704	0.2639	0.0000	0.0000	－	－		KCl
16	1.1746	1.3735	0.2532	0.0374	0.0446	0.8688	0.0066		KCl
17	1.1712	1.3775	0.2382	0.0762	0.1013	0.9442	0.0056		KCl
18	1.1675	1.3820	0.2238	0.1164	0.1555	0.8957	0.0156		KCl
19	1.1641	1.3861	0.2073	0.1584	0.2178	0.8541	0.0292		KCl
20	1.1612	1.3906	0.1903	0.2025	0.2818	0.7349	0.0663		KCl
21	1.1587	1.3956	0.1744	0.2478	0.3418	0.7347	0.0796		KCl
22	1.1561	1.4002	0.1581	0.2947	0.4033	0.7318	0.0939		KCl
23	1.1539	1.4059	0.1409	0.3435	0.4684	0.7328	0.1068		KCl
24	1.1523	1.4114	0.1258	0.3934	0.5254	0.7340	0.1197		KCl
25	1.1516	1.4173	0.1087	0.4453	0.5896	0.7189	0.1404		KCl
26	1.1490	1.4229	0.0929	0.4990	0.6496	0.6976	0.1664		KCl
27	1.1431	1.4282	0.0669	0.5600	0.7477	0.6789	0.1927		KCl
28	1.1428	1.4340	0.0548	0.6130	0.7933	0.7376	0.1702		KCl
29D	1.1118	1.4314	0.0000	0.6990	1.0000	－	－		－
T=308 K
30E	1.1847	1.3692	0.2851	0.0000	0.0000	－	－		KCl
31	1.1794	1.3744	0.2680	0.0367	0.0598	0.9781	0.0011		KCl
32	1.1748	1.3780	0.2510	0.0749	0.1196	0.9224	0.0078		KCl
33	1.1707	1.3829	0.2371	0.1144	0.1685	0.9498	0.0075		KCl
34	1.1658	1.3861	0.2185	0.1562	0.2336	0.9496	0.0101		KCl
35	1.1629	1.3905	0.2030	0.1993	0.2880	0.8288	0.0428		KCl
36	1.1589	1.3945	0.1841	0.2449	0.3544	0.8756	0.0373		KCl
37	1.1559	1.4000	0.1680	0.2912	0.4109	0.7442	0.0895		KCl
38	1.1522	1.4050	0.1490	0.3402	0.4772	0.7634	0.0946		KCl
39	1.1497	1.4101	0.1323	0.3905	0.5360	0.7283	0.1222		KCl
40	1.1464	1.4159	0.1153	0.4420	0.5957	0.7034	0.1482		KCl
41	1.1441	1.4215	0.0973	0.4966	0.6586	0.7191	0.1545		KCl
42	1.1421	1.4272	0.0796	0.5523	0.7208	0.7530	0.1482		KCl
43	1.1356	1.4321	0.0592	0.6101	0.7923	0.7134	0.1859		KCl
44	1.1308	1.4337	0.0441	0.6689	0.8453	0.1845	0.5707		KCl
45	1.1274	1.4376	0.0400	0.7191	0.8599	0.1704	0.6214		KCl
46F	1.1089	1.4445	0.0000	0.7800	1.0000	－	－		－

表2 三元体系KCl-PEG4000-H2O 在288、298和308 K下的溶解度、密度、折射率和盐析率数据

No.	Density，ρ/ (g?cm^–3)	Refractive index，n_D	Composition of equilibrated solution		R	Composition of wet solid phase			Equilibrated solid phase
No.	Density，ρ/ (g?cm^–3)	Refractive index，n_D	w(KCl)	w(PEG4000)	R	w(KCl)		w(PEG4000)	Equilibrated solid phase
T=288 K
1A	1.1671	1.3680	0.2485	0.0000	0.0000	－	－		KCl
2	1.1649	1.3723	0.2387	0.0381	0.0396	0.8875	0.0056		KCl
3	1.1622	1.3764	0.2219	0.0778	0.1070	0.8694	0.0131		KCl
4	1.1592	1.3807	0.2073	0.1188	0.1656	0.8615	0.0208		KCl
5	1.1569	1.3852	0.1899	0.1619	0.2357	0.7081	0.0583		KCl
6	1.1548	1.3898	0.1758	0.2061	0.2924	0.7530	0.0618		KCl
7	1.1520	1.3950	0.1613	0.2517	0.3507	0.6919	0.0925		KCl
8	1.1510	1.4003	0.1448	0.2993	0.4174	0.6924	0.1077		KCl
9	1.1507	1.4061	0.1300	0.3478	0.4768	0.6974	0.1210		KCl
10	1.1509	1.4122	0.1188	0.3966	0.5221	0.7025	0.1339		KCl
11	1.1516	1.4174	0.1056	0.4468	0.5751	0.6464	0.1766		KCl
12	1.1496	1.4240	0.0893	0.5010	0.6406	0.6672	0.1831		KCl
13	1.1364	1.4282	0.0389	0.5767	0.8434	0.7232	0.1661		KCl
14B	1.1071	1.4281	0.0000	0.6485	1.0000	－	－		－
T=298 K
15C	1.1798	1.3704	0.2639	0.0000	0.0000	－	－		KCl
16	1.1746	1.3735	0.2532	0.0374	0.0446	0.8688	0.0066		KCl
17	1.1712	1.3775	0.2382	0.0762	0.1013	0.9442	0.0056		KCl
18	1.1675	1.3820	0.2238	0.1164	0.1555	0.8957	0.0156		KCl
19	1.1641	1.3861	0.2073	0.1584	0.2178	0.8541	0.0292		KCl
20	1.1612	1.3906	0.1903	0.2025	0.2818	0.7349	0.0663		KCl
21	1.1587	1.3956	0.1744	0.2478	0.3418	0.7347	0.0796		KCl
22	1.1561	1.4002	0.1581	0.2947	0.4033	0.7318	0.0939		KCl
23	1.1539	1.4059	0.1409	0.3435	0.4684	0.7328	0.1068		KCl
24	1.1523	1.4114	0.1258	0.3934	0.5254	0.7340	0.1197		KCl
25	1.1516	1.4173	0.1087	0.4453	0.5896	0.7189	0.1404		KCl
26	1.1490	1.4229	0.0929	0.4990	0.6496	0.6976	0.1664		KCl
27	1.1431	1.4282	0.0669	0.5600	0.7477	0.6789	0.1927		KCl
28	1.1428	1.4340	0.0548	0.6130	0.7933	0.7376	0.1702		KCl
29D	1.1118	1.4314	0.0000	0.6990	1.0000	－	－		－
T=308 K
30E	1.1847	1.3692	0.2851	0.0000	0.0000	－	－		KCl
31	1.1794	1.3744	0.2680	0.0367	0.0598	0.9781	0.0011		KCl
32	1.1748	1.3780	0.2510	0.0749	0.1196	0.9224	0.0078		KCl
33	1.1707	1.3829	0.2371	0.1144	0.1685	0.9498	0.0075		KCl
34	1.1658	1.3861	0.2185	0.1562	0.2336	0.9496	0.0101		KCl
35	1.1629	1.3905	0.2030	0.1993	0.2880	0.8288	0.0428		KCl
36	1.1589	1.3945	0.1841	0.2449	0.3544	0.8756	0.0373		KCl
37	1.1559	1.4000	0.1680	0.2912	0.4109	0.7442	0.0895		KCl
38	1.1522	1.4050	0.1490	0.3402	0.4772	0.7634	0.0946		KCl
39	1.1497	1.4101	0.1323	0.3905	0.5360	0.7283	0.1222		KCl
40	1.1464	1.4159	0.1153	0.4420	0.5957	0.7034	0.1482		KCl
41	1.1441	1.4215	0.0973	0.4966	0.6586	0.7191	0.1545		KCl
42	1.1421	1.4272	0.0796	0.5523	0.7208	0.7530	0.1482		KCl
43	1.1356	1.4321	0.0592	0.6101	0.7923	0.7134	0.1859		KCl
44	1.1308	1.4337	0.0441	0.6689	0.8453	0.1845	0.5707		KCl
45	1.1274	1.4376	0.0400	0.7191	0.8599	0.1704	0.6214		KCl
46F	1.1089	1.4445	0.0000	0.7800	1.0000	－	－		－

图2 KCl-PEG4000-H2O三元体系288、298、308 K相图

Fig.2 Phase diagram of KCl-PEG4000-H2O at 288，298 and 308 K

图3 KCl-PEG4000-H2O 288、298、308 K盐析率曲线

Fig.3 Salting-out ratio(R) for KCl-PEG4000-H2O at 288，298 and 308 K

图4 KCl-PEG4000-H2O三元体系288、298、308 K相图

Fig.4 Phase diagram of KCl-PEG4000-H2O at 288，298 and 308 K

图5 KCl-PEG4000-H2O 298 K文献[16]和实验相图对比

Fig.5 Comparison of phase diagrams of Ref.[16] and experimental for KCl-PEG4000-H2O at 298 K

图6 KCl-PEG4000-H2O三元体系288、298、308 K密度/折射率-组成图

Fig.6 Diagrams of density vs composition and refractive index vs composition for system KCl-PEG4000-H2O at 288，298 and 308 K

表3 三元体系KCl-PEG4000-H2O在288，298和308 K下的二元参数和交互作用参数

Table 3 Binary parameters and cross parameters for ternary system KCl-PEG4000-H2O at 288，298 and 308 K

二元参数
T/K	B₁₁×10²	C₁₁₁×10⁵	$β 220 × 102$	$β 221 × 102$	$C 222 ? × 103$	N_p	σ×10²
288	0.7088^[19]	1.296^[19]	–0.4398	–1.095	0.7345	11	0.3129
298	0.7088^[19]	1.296^[19]	0.7523	–0.8338	0.9664	16	0.4356
308	0.7088^[19]	1.296^[19]	0.9950	–1.053	1.981	14	0.2434
交互作用参数
T/K	$β 120$	$β 121$	C₁₁₂	C₁₂₂	N_p	σ
288	0.101683	–0.09897	0.000586	–0.00325	13	0.26
298	0.114476	–0.10325	–0.00015	–0.00294	13	0.09
308	0.110781	0.056002	–0.0007	–0.00233	15	0.20

表3 三元体系KCl-PEG4000-H2O在288，298和308 K下的二元参数和交互作用参数

Table 3 Binary parameters and cross parameters for ternary system KCl-PEG4000-H2O at 288，298 and 308 K

二元参数
T/K	B₁₁×10²	C₁₁₁×10⁵	$β 220 × 102$	$β 221 × 102$	$C 222 ? × 103$	N_p	σ×10²
288	0.7088^[19]	1.296^[19]	–0.4398	–1.095	0.7345	11	0.3129
298	0.7088^[19]	1.296^[19]	0.7523	–0.8338	0.9664	16	0.4356
308	0.7088^[19]	1.296^[19]	0.9950	–1.053	1.981	14	0.2434
交互作用参数
T/K	$β 120$	$β 121$	C₁₁₂	C₁₂₂	N_p	σ
288	0.101683	–0.09897	0.000586	–0.00325	13	0.26
298	0.114476	–0.10325	–0.00015	–0.00294	13	0.09
308	0.110781	0.056002	–0.0007	–0.00233	15	0.20

图7 KCl-PEG4000-H2O三元体系288、298、308 K理论和实验相图

Fig.7 Experimental and calculation phase diagram of KCl-PEG4000-H2O at 288，298 and 308 K

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KCl-PEG4000-H₂O三元体系288、298、308 K相平衡测定及计算

Measurements and simulation for ternary system KCl-PEG4000-H₂O at 288, 298 and 308 K

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