308.2 K三元体系KCl+PEG10000/20000+H2O相平衡及热力学计算

doi:10.11949/0438-1157.20200933

摘要/Abstract

摘要：

采用等温溶解平衡法和浊点法分别测定了308.2 K时三元体系KCl+PEG10000/20000+H₂O的固液平衡组成和液液平衡组成，同时测定了固液平衡时体系的密度和折射率。根据实验数据，绘制了两个三元体系308.2 K时的完整相图、双液线对比图和结线-组成图。研究发现：三元体系KCl+PEG10000/20000+H₂O 308.2 K时的完整相图均包含6个区域：不饱和液相区（L），2个一固一液区（L+S），双液相区（2L），两液一固区（2L+S），两固一液区（L+2S）；其中，一液两固区（L+2S）中的两种固相分别为KCl和PEG10000/20000。在完整相图中，一固一液区面积最大，双液相区面积最小。对比308.2 K时聚乙二醇分子量为1000、4000、6000、10000和20000的KCl+PEG+H₂O体系可知：分子量为1000、4000和6000时，体系中仅存在固液相平衡关系；分子量为10000和20000时，体系中同时存在固液和液液相平衡关系，且随着聚乙二醇分子量的增加，双液线向原点移动，双液相区（2L）和两液一固区（2L+S）增大，不饱和液相区（L）和一固一液区（L+S）均减小。采用Chen-NRTL-PDH热力学模型进行了液液相平衡计算，计算结果与实验数据吻合较好。

关键词: 相平衡, 热力学性质, 溶解性, 聚合物, Chen-NRTL-PDH模型

Abstract:

For the ternary systems KCl+PEG10000/20000+ H₂O at 308.2 K, the composition of equilibrium liquid at solid-liquid equilibrium was measured by the isothermal dissolution method, and turbidimetric method was adopted for liquid-liquid equilibrium. Meanwhile, the density and refractive index of the equilibrated solution were also determined. According to the experimental data, the phase diagrams, comparison diagram of binodal curve, and tie-line diagrams were plotted. In terms of phase diagrams of both ternary systems mentioned above, they were all consisted of 6 regions which respectively were region of unsaturated liquid phase (L), two regions of one liquid and one solid phase KCl (L+S), region of two-liquids phase (2L), two liquids with one solid KCl (2L+S), and region of one liquid with two solids of KCl and PEG10000/20000 (L+2S). Among those regions, the area of (L+S) was the largest, and the area of (2L) was the smallest. Also, this paper compared phase diagrams of ternary systems KCl+PEG+H₂O where the molecular weight of PEG respectively was 1000, 4000, 6000, 10000, and 20000 at 308.2 K, respectively. The results showed that there was only solid-liquid equilibrium when the mixed solvents were composed of PEG1000, PEG4000, or PEG6000 in ternary systems at 308.2 K, while the solid-liquid equilibrium and liquid-liquid equilibrium coexisted in the systems containing PEG10000 or PEG20000 at 308.2 K. It also could be found that with an increase of the molecular weight of PEG, the binodal curve was closer to the original point, the region of two-liquids phase (2L) and two liquids with one solid KCl (2L+S) enlarged, while the region of unsaturated liquid phase (L) and two regions of one liquid and one solid phase KCl (L+S) shrank. The Chen-NRTL-PDH thermodynamic model is used to calculate the liquid-liquid equilibrium, and the calculated results are in good agreement with the experimental data.

Key words: phase equilibria, thermodynamic properties, solubility, polymers, Chen-NRTL-PDH model

中图分类号:

O 642.4

黄琴, 于旭东, 李茂兰, 郑洪, 曾英. 308.2 K三元体系KCl+PEG10000/20000+H₂O相平衡及热力学计算[J]. 化工学报, 2021, 72(4): 1895-1905.

HUANG Qin, YU Xudong, LI Maolan, ZHENG Hong, ZENG Ying. Experimental and thermodynamic simulation for ternary systems KCl+PEG10000/20000+ H₂O at 308.2 K[J]. CIESC Journal, 2021, 72(4): 1895-1905.

图/表 11

参考文献 42

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三元体系	a	b	c	R²
KCl+PEG10000+H₂O	-9.0880	22.0649	-303.6913	0.9984
KCl+PEG20000+H₂O	-7.9581	21.2533	-412.8902	0.9989

三元体系	a	b	c	R²
KCl+PEG10000+H₂O	-9.0880	22.0649	-303.6913	0.9984
KCl+PEG20000+H₂O	-7.9581	21.2533	-412.8902	0.9989

No.	Density(ρ)/ (g?cm^-3)	Refractive index (n_D)	Composition of equilibrated solution		Composition of wet solid phase		Equilibrated solid phase
No.	Density(ρ)/ (g?cm^-3)	Refractive index (n_D)	w_KCl	w_PEG	w_KCl	w_PEG	Equilibrated solid phase
KCl+PEG10000+ H₂O
1,A	1.1847	1.3692	0.2851	0.0000	－	－	－
2	1.1816	1.3722	0.2739	0.0197	0.6487	0.0095	KCl
3	1.1611	1.3904	0.2012	0.1997	0.6890	0.0778	KCl
4	1.1564	1.3941	0.1803	0.2459	0.6803	0.0959	KCl
5	1.1540	1.3995	0.1677	0.2913	0.6138	0.1352	KCl
6	1.1500	1.4050	0.1502	0.3399	0.6433	0.1427	KCl
7	1.1486	1.4105	0.1323	0.3905	0.5791	0.1894	KCl
8	1.1466	1.4164	0.1145	0.4428	0.5315	0.2343	KCl
9	1.1439	1.4221	0.0971	0.4966	0.4907	0.2801	KCl
10	1.1407	1.4280	0.0809	0.5515	0.3797	0.3722	KCl
11,B	1.1060	1.4334	0.0000	0.7017	－	－	－
KCl+PEG20000+ H₂O
12, C	1.1847	1.3692	0.2851	0.0000	－	－	－
13	1.1581	1.3939	0.1811	0.2457	0.5370	0.1389	KCl
14	1.1538	1.3995	0.1595	0.2942	0.4868	0.1796	KCl
15	1.1500	1.4040	0.1439	0.3424	0.4829	0.2068	KCl
16	1.1417	1.4087	0.1190	0.3964	0.4494	0.2478	KCl
17	1.1404	1.4144	0.1032	0.4484	0.3937	0.3031	KCl
18	1.1272	1.4200	0.0794	0.5063	0.2966	0.3869	KCl
19	1.1235	1.4260	0.0517	0.5690	0.2295	0.4623	KCl
20, D	1.1012	1.4280	0.0000	0.6742	－	－	－

No.	Density(ρ)/ (g?cm^-3)	Refractive index (n_D)	Composition of equilibrated solution		Composition of wet solid phase		Equilibrated solid phase
No.	Density(ρ)/ (g?cm^-3)	Refractive index (n_D)	w_KCl	w_PEG	w_KCl	w_PEG	Equilibrated solid phase
KCl+PEG10000+ H₂O
1,A	1.1847	1.3692	0.2851	0.0000	－	－	－
2	1.1816	1.3722	0.2739	0.0197	0.6487	0.0095	KCl
3	1.1611	1.3904	0.2012	0.1997	0.6890	0.0778	KCl
4	1.1564	1.3941	0.1803	0.2459	0.6803	0.0959	KCl
5	1.1540	1.3995	0.1677	0.2913	0.6138	0.1352	KCl
6	1.1500	1.4050	0.1502	0.3399	0.6433	0.1427	KCl
7	1.1486	1.4105	0.1323	0.3905	0.5791	0.1894	KCl
8	1.1466	1.4164	0.1145	0.4428	0.5315	0.2343	KCl
9	1.1439	1.4221	0.0971	0.4966	0.4907	0.2801	KCl
10	1.1407	1.4280	0.0809	0.5515	0.3797	0.3722	KCl
11,B	1.1060	1.4334	0.0000	0.7017	－	－	－
KCl+PEG20000+ H₂O
12, C	1.1847	1.3692	0.2851	0.0000	－	－	－
13	1.1581	1.3939	0.1811	0.2457	0.5370	0.1389	KCl
14	1.1538	1.3995	0.1595	0.2942	0.4868	0.1796	KCl
15	1.1500	1.4040	0.1439	0.3424	0.4829	0.2068	KCl
16	1.1417	1.4087	0.1190	0.3964	0.4494	0.2478	KCl
17	1.1404	1.4144	0.1032	0.4484	0.3937	0.3031	KCl
18	1.1272	1.4200	0.0794	0.5063	0.2966	0.3869	KCl
19	1.1235	1.4260	0.0517	0.5690	0.2295	0.4623	KCl
20, D	1.1012	1.4280	0.0000	0.6742	－	－	－

No.	Composition of binodal curve		No.	Composition of binodal curve		No.	Composition of binodal curve
No.	w_KCl	w_PEG	No.	w_KCl	w_PEG	No.	w_KCl	w_PEG
KCl+PEG10000+H₂O			KCl+PEG20000+H₂O			KCl+PEG20000+H₂O
1,E	0.2637	0.0390	1,G	0.2729	0.0059	20	0.2288	0.0637
2	0.2618	0.0398	2	0.2806	0.0057	21	0.2263	0.0706
3	0.2598	0.0418	3	0.2820	0.0056	22	0.2241	0.0765
4	0.2577	0.0444	4	0.2841	0.0054	23	0.2230	0.0809
5	0.2553	0.0479	5	0.2729	0.0059	24	0.2220	0.0852
6	0.2531	0.0523	6	0.2693	0.0083	25	0.2205	0.0909
7	0.2495	0.0611	7	0.2632	0.0091	26	0.2181	0.0965
8	0.2460	0.0700	8	0.2605	0.0100	27	0.2170	0.1052
9	0.2420	0.0803	9	0.2588	0.0110	28	0.2141	0.1149
10	0.2383	0.0898	10	0.2571	0.0119	29	0.2118	0.1225
11	0.2347	0.0990	11	0.2548	0.0160	30	0.2101	0.1309
12	0.2314	0.1080	12	0.2491	0.0250	31	0.2076	0.1402
13	0.2286	0.1150	13	0.2464	0.0275	32	0.2039	0.1521
14	0.2250	0.1234	14	0.2446	0.0308	33	0.2016	0.1632
15	0.2219	0.1317	15	0.2430	0.0329	34	0.1986	0.1790
16	0.2186	0.1405	16	0.2403	0.0399	35,H	0.1951	0.1970
17	0.2168	0.1498	17	0.2376	0.0459
18	0.2141	0.1581	18	0.2343	0.0544
19,F	0.2106	0.1648	19	0.2318	0.0581

308.2 K三元体系KCl+PEG10000/20000+H₂O相平衡及热力学计算

Experimental and thermodynamic simulation for ternary systems KCl+PEG10000/20000+ H₂O at 308.2 K

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No.	K_pc	TLL	STL	Composition of original solution		Composition of top phase		Composition of bottom phase
No.	K_pc	TLL	STL	w_KCl	w_PEG	w_KCl	w_PEG	w_KCl	w_PEG
KCl+PEG10000+H₂O
1	0.85	0.1009	-2.4945	0.2386	0.0900	0.2195	0.1407	0.2570	0.0470
2	0.84	0.1130	-2.4703	0.2393	0.0903	0.2171	0.1473	0.2595	0.0426
3	0.82	0.1273	-2.4229	0.2409	0.0909	0.2146	0.1544	0.2632	0.0367
4	0.81	0.1336	-2.4022	0.2405	0.0908	0.2135	0.1576	0.2648	0.0343
KCl+PEG20000+H₂O
1	0.80	0.1525	-2.7691	0.2400	0.0470	0.2026	0.1611	0.2544	0.0177
2	0.75	0.1877	-2.6375	0.2443	0.0490	0.1972	0.1854	0.2637	0.0099
3	0.72	0.2067	-2.5874	0.2487	0.0510	0.1939	0.2000	0.2684	0.0072
4	0.71	0.2146	-2.5858	0.2509	0.0520	0.1924	0.2067	0.2698	0.0066
5	0.68	0.2354	-2.5022	0.2531	0.0530	0.1888	0.2227	0.2761	0.0042

Solvent	Molecular weight (M)^①	Molar volume (V)/ (m³·mol^-1)	Dielectric constant (D)	Segment number (r)
PEG10000	10251.00	8.25×10^-3	2.20	227
PEG20000	21245.00	1.65×10^-2	2.20	482
H₂O	18.02	18.13×10^-6	74.83	1

PEG10000/20000	τ₁₂	τ₂₁	τ₁₃	τ₃₁	τ₂₃	τ₃₂	σ
PEG10000	-95.8304	0.4592	5.1452	-5.85×10^-5	1.2935	-103.4504	3.27×10^-6
PEG20000	-158.4585	-0.2582	8.1035	0.4067	3.0293	-165.1540	8.04×10^-7

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No.	Composition of top phase			Composition of bottom phase
No.	w_KCl	w_PEG	w_w	w_KCl	w_PEG	w_w
KCl+PEG10000+H₂O
1	0.2204	0.1418	0.6378	0.2560	0.0471	0.6969
2	0.2184	0.1487	0.6329	0.2581	0.0426	0.6993
3	0.2164	0.1559	0.6256	0.2624	0.0339	0.7037
4	0.2156	0.1588	0.6277	0.2613	0.0364	0.7023
KCl+PEG20000+H₂O
1	0.2029	0.1613	0.6358	0.2538	0.0176	0.7286
2	0.1979	0.1855	0.6166	0.2628	0.0099	0.7273
3	0.2001	0.1949	0.6050	0.2673	0.0072	0.7255
4	0.2068	0.1934	0.5998	0.2687	0.0065	0.7248
5	0.2227	0.1905	0.5868	0.2746	0.0041	0.7213

No.	Composition of top phase			Composition of bottom phase
No.	w_KCl	w_PEG	w_w	w_KCl	w_PEG	w_w
KCl+PEG10000+H₂O
1	0.2204	0.1418	0.6378	0.2560	0.0471	0.6969
2	0.2184	0.1487	0.6329	0.2581	0.0426	0.6993
3	0.2164	0.1559	0.6256	0.2624	0.0339	0.7037
4	0.2156	0.1588	0.6277	0.2613	0.0364	0.7023
KCl+PEG20000+H₂O
1	0.2029	0.1613	0.6358	0.2538	0.0176	0.7286
2	0.1979	0.1855	0.6166	0.2628	0.0099	0.7273
3	0.2001	0.1949	0.6050	0.2673	0.0072	0.7255
4	0.2068	0.1934	0.5998	0.2687	0.0065	0.7248
5	0.2227	0.1905	0.5868	0.2746	0.0041	0.7213