298.2 K四元体系MgCl2-SrCl2-AlCl3-H2O相平衡实验及溶解度计算

doi:10.11949/0438-1157.20200420

摘要/Abstract

摘要：

采用等温溶解平衡法研究了298.2 K四元体系MgCl₂-SrCl₂-AlCl₃-H₂O的相平衡关系，测定了该体系的溶解度和平衡溶液的密度、折射率。根据实验数据，分别绘制了298.2 K该四元体系的空间立体图、相图、水图、密度-组成图和折射率-组成图。研究发现：298.2 K下，四元体系MgCl₂-SrCl₂-AlCl₃-H₂O无复盐或固溶体生成，稳定相图由2个共饱点、5条单变量曲线和4个结晶区组成。四个结晶区分别为MgCl₂·6H₂O、SrCl₂·6H₂O、SrCl₂·2H₂O和AlCl₃·6H₂O，其中SrCl₂·6H₂O结晶区最大，SrCl₂·2H₂O结晶区最小，说明SrCl₂·6H₂O更容易结晶析出。平衡液相的密度和折射率随着J（MgCl₂）的变化呈规律性变化。采用Pitzer模型进行了298.2 K四元体系MgCl₂-SrCl₂-AlCl₃-H₂O溶解度计算，对比发现，计算结果与实验结果基本吻合。

关键词: 相平衡, 热力学性质, 溶解性, 水合物, Pitzer模型

Abstract:

Solid-liquid equilibria of the aqueous quaternary system MgCl₂-SrCl₂-AlCl₃-H₂O at 298.2 K was studied by using the isothermal dissolution equilibrium method. The solubility, density, and refractive index of the aqueous quaternary system were measured. The corresponding space diagram, stable phase diagram, water content diagram, and the diagrams of density vs composition, refractive index vs composition were constructed based on the experimental data. The results show that there is no double that salt or solid solution was formed in the quaternary system. The stable phase diagram of the quaternary system MgCl₂-SrCl₂-AlCl₃-H₂O at 298.2 K consists of two invariant points, five isothermal dissolution curves, and four crystallization regions. The four crystallization regions correspond to four single hydrate salts magnesium chloride hexahydrate (MgCl₂·6H₂O), strontium chloride hexahydrate (SrCl₂·6H₂O), strontium chloride dihydrate (SrCl₂·2H₂O), and aluminum chloride hexahydrate (AlCl₃·6H₂O). With a view to the crystallization regions, the crystallization region of salt SrCl₂·2H₂O is the smallest, while the crystallization region of salt SrCl₂·6H₂O is the largest, meaning SrCl₂·6H₂O can be more easily separated from solution than other coexisting salts in this system at 298.2 K. The densities and refractive indices of the solution at equilibrium change regularly with the change of J(MgCl₂) of the solution. The Pitzer model is used to calculate the solubility of the 298.2 K quaternary system MgCl₂-SrCl₂-AlCl₃-H₂O. The comparison found that the calculated results are basically consistent with the experimental results.

Key words: phase equilibria, thermodynamic properties, solubility, hydrate, Pitzer model

中图分类号:

O 642.4

郑秋风,罗军,陈帅,陈念粗,于旭东,曾英. 298.2 K四元体系MgCl₂-SrCl₂-AlCl₃-H₂O相平衡实验及溶解度计算[J]. 化工学报, 2020, 71(12): 5443-5451.

ZHENG Qiufeng,LUO Jun,CHEN Shuai,CHEN Niancu,YU Xudong,ZENG Ying. Measurements and simulation for aqueous quaternary system MgCl₂-SrCl₂-AlCl₃-H₂O at 298.2 K[J]. CIESC Journal, 2020, 71(12): 5443-5451.

图/表 14

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No.	Composition of equilibrium solution, w(B)/%				J?necke index of dry salt, J(B)/(g/100 g salt)				Equilibrated solid phase
	Composition of equilibrium solution, w(B)/%				J(MgCl₂)+J(SrCl₂)+J(AlCl₃)=100
	w(MgCl₂)	w(SrCl₂)	w(AlCl₃)	w(H₂O)	J(MgCl₂)	J(SrCl₂)	J(AlCl₃)	J(H₂O)
1, A	34.75	1.42	0.00	63.83	96.07	3.93	0.00	176.47	Bis + S₂
2	33.98	1.33	0.83	63.86	94.02	3.68	2.30	176.70	Bis + S₂
3	32.94	1.27	1.75	64.04	91.60	3.53	4.87	178.09	Bis + S₂
4	33.01	1.31	2.53	63.15	89.58	3.55	6.87	171.37	Bis + S₂
5	31.87	1.33	3.50	63.30	86.84	3.62	9.54	172.48	Bis + S₂
6	30.37	1.39	4.57	63.67	83.59	3.83	12.58	175.25	Bis + S₂
7, E₁	29.49	1.32	5.47	63.72	81.28	3.64	15.08	175.63	Bis + S₂ + AC
8	28.80	1.23	6.19	63.78	79.51	3.40	17.09	176.09	S₂ + AC
9, E₂	27.36	1.39	7.28	63.97	75.93	3.86	20.21	177.55	S₆ + S₂ + AC
10, B	33.16	2.22	0.00	64.62	93.73	6.27	0.00	182.65	S₆ + S₂
11	32.01	1.98	1.84	64.17	89.33	5.53	5.14	179.10	S₆ + S₂
12	30.74	2.10	2.89	64.27	86.03	5.88	8.09	179.88	S₆ + S₂
13	29.27	2.12	4.04	64.57	82.62	5.98	11.40	182.25	S₆ + S₂
14	28.45	2.11	4.90	64.54	80.23	5.95	13.82	182.01	S₆ + S₂
15	28.23	1.96	5.52	64.29	79.05	5.49	15.46	180.03	S₆ + S₂
16	27.73	1.53	6.55	64.19	77.44	4.27	18.29	179.25	S₆ + S₂
17, C	30.45	0.00	5.65	63.90	84.35	0.00	15.65	177.01	Bis + AC
18	30.08	0.90	5.29	63.73	82.93	2.48	14.59	175.71	Bis + AC
19	29.46	1.14	5.36	64.04	81.92	3.17	14.91	178.09	Bis + AC
20, D	0.00	1.95	30.12	67.93	0.00	6.08	93.92	211.82	S₆ + AC
21	5.34	1.82	25.76	67.08	16.22	5.53	78.25	203.77	S₆ + AC
22	9.85	1.71	22.00	66.44	29.35	5.10	65.55	197.97	S₆ + AC
23	13.74	1.59	18.73	65.94	40.34	4.67	54.99	193.60	S₆ + AC
24	16.99	1.49	16.06	65.46	49.19	4.31	46.50	189.52	S₆ + AC
25	19.76	1.40	13.67	65.17	56.73	4.02	39.25	187.11	S₆ + AC
26	22.68	1.38	11.42	64.52	63.92	3.89	32.19	181.85	S₆ + AC
27	25.02	1.39	9.39	64.20	69.89	3.88	26.23	179.33	S₆ + AC

No.	Composition of equilibrium solution, w(B)/%				J?necke index of dry salt, J(B)/(g/100 g salt)				Equilibrated solid phase
	Composition of equilibrium solution, w(B)/%				J(MgCl₂)+J(SrCl₂)+J(AlCl₃)=100
	w(MgCl₂)	w(SrCl₂)	w(AlCl₃)	w(H₂O)	J(MgCl₂)	J(SrCl₂)	J(AlCl₃)	J(H₂O)
1, A	34.75	1.42	0.00	63.83	96.07	3.93	0.00	176.47	Bis + S₂
2	33.98	1.33	0.83	63.86	94.02	3.68	2.30	176.70	Bis + S₂
3	32.94	1.27	1.75	64.04	91.60	3.53	4.87	178.09	Bis + S₂
4	33.01	1.31	2.53	63.15	89.58	3.55	6.87	171.37	Bis + S₂
5	31.87	1.33	3.50	63.30	86.84	3.62	9.54	172.48	Bis + S₂
6	30.37	1.39	4.57	63.67	83.59	3.83	12.58	175.25	Bis + S₂
7, E₁	29.49	1.32	5.47	63.72	81.28	3.64	15.08	175.63	Bis + S₂ + AC
8	28.80	1.23	6.19	63.78	79.51	3.40	17.09	176.09	S₂ + AC
9, E₂	27.36	1.39	7.28	63.97	75.93	3.86	20.21	177.55	S₆ + S₂ + AC
10, B	33.16	2.22	0.00	64.62	93.73	6.27	0.00	182.65	S₆ + S₂
11	32.01	1.98	1.84	64.17	89.33	5.53	5.14	179.10	S₆ + S₂
12	30.74	2.10	2.89	64.27	86.03	5.88	8.09	179.88	S₆ + S₂
13	29.27	2.12	4.04	64.57	82.62	5.98	11.40	182.25	S₆ + S₂
14	28.45	2.11	4.90	64.54	80.23	5.95	13.82	182.01	S₆ + S₂
15	28.23	1.96	5.52	64.29	79.05	5.49	15.46	180.03	S₆ + S₂
16	27.73	1.53	6.55	64.19	77.44	4.27	18.29	179.25	S₆ + S₂
17, C	30.45	0.00	5.65	63.90	84.35	0.00	15.65	177.01	Bis + AC
18	30.08	0.90	5.29	63.73	82.93	2.48	14.59	175.71	Bis + AC
19	29.46	1.14	5.36	64.04	81.92	3.17	14.91	178.09	Bis + AC
20, D	0.00	1.95	30.12	67.93	0.00	6.08	93.92	211.82	S₆ + AC
21	5.34	1.82	25.76	67.08	16.22	5.53	78.25	203.77	S₆ + AC
22	9.85	1.71	22.00	66.44	29.35	5.10	65.55	197.97	S₆ + AC
23	13.74	1.59	18.73	65.94	40.34	4.67	54.99	193.60	S₆ + AC
24	16.99	1.49	16.06	65.46	49.19	4.31	46.50	189.52	S₆ + AC
25	19.76	1.40	13.67	65.17	56.73	4.02	39.25	187.11	S₆ + AC
26	22.68	1.38	11.42	64.52	63.92	3.89	32.19	181.85	S₆ + AC
27	25.02	1.39	9.39	64.20	69.89	3.88	26.23	179.33	S₆ + AC

No.	J(MgCl₂)/ (g/100 g salt)	Density, ρ/ (g/cm³)	Refractive index, n_D	No.	J(MgCl₂)/ (g/100 g salt)	Density, ρ/ (g/cm³)	Refractive index, n_D
1, A	96.07	1.3332	1.4339	15	79.05	1.3266	1.4324
2	94.02	1.3368	1.4337	16	77.44	1.3282	1.4341
3	91.60	1.3352	1.4338	17, C	84.35	1.3403	1.4347
4	89.58	1.3329	1.4339	18	82.93	1.3266	1.4343
5	86.84	1.3299	1.4338	19	81.92	1.3265	1.4341
6	83.59	1.3293	1.4336	20, D	0.00	1.3027	1.4346
7, E₁	81.28	1.3261	1.4333	21	16.22	1.3100	1.4331
8	79.51	1.3295	1.4344	22	29.35	1.3133	1.4330
9, E₂	75.93	1.3295	1.4350	23	40.34	1.3142	1.4330
10, B	93.73	1.3147	1.4301	24	49.19	1.3206	1.4331
11	89.33	1.3235	1.4305	25	56.73	1.3259	1.4338
12	86.03	1.3241	1.4310	26	63.92	1.3286	1.4340
13	82.62	1.3245	1.4312	27	69.89	1.3290	1.4342
14	80.23	1.3255	1.4315

No.	J(MgCl₂)/ (g/100 g salt)	Density, ρ/ (g/cm³)	Refractive index, n_D	No.	J(MgCl₂)/ (g/100 g salt)	Density, ρ/ (g/cm³)	Refractive index, n_D
1, A	96.07	1.3332	1.4339	15	79.05	1.3266	1.4324
2	94.02	1.3368	1.4337	16	77.44	1.3282	1.4341
3	91.60	1.3352	1.4338	17, C	84.35	1.3403	1.4347
4	89.58	1.3329	1.4339	18	82.93	1.3266	1.4343
5	86.84	1.3299	1.4338	19	81.92	1.3265	1.4341
6	83.59	1.3293	1.4336	20, D	0.00	1.3027	1.4346
7, E₁	81.28	1.3261	1.4333	21	16.22	1.3100	1.4331
8	79.51	1.3295	1.4344	22	29.35	1.3133	1.4330
9, E₂	75.93	1.3295	1.4350	23	40.34	1.3142	1.4330
10, B	93.73	1.3147	1.4301	24	49.19	1.3206	1.4331
11	89.33	1.3235	1.4305	25	56.73	1.3259	1.4338
12	86.03	1.3241	1.4310	26	63.92	1.3286	1.4340
13	82.62	1.3245	1.4312	27	69.89	1.3290	1.4342
14	80.23	1.3255	1.4315

System	β⁽⁰⁾	β⁽¹⁾	C^f	Ref.
MgCl₂-H₂O	0.3511	1.6512	0.0065	[37,38]
AlCl₃-H₂O	0.7153	5.6509	–0.0042	[37,38]
SrCl₂-H₂O	0.2827	1.5625	–0.0023	[39]

298.2 K四元体系MgCl₂-SrCl₂-AlCl₃-H₂O相平衡实验及溶解度计算

Measurements and simulation for aqueous quaternary system MgCl₂-SrCl₂-AlCl₃-H₂O at 298.2 K

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C	C′	θ_CC′	ψ_CC′Cl	Ref.
Mg²⁺	Sr²⁺	–0.1965	0.0305	[22]
Sr²⁺	Al³⁺	0.1244	–0.0161	[23]
Mg²⁺	Al³⁺	0.0341	–0.0053	this work

Species	ln K_sp	Ref.
MgCl₂·6H₂O	10.60	[37]
AlCl₃·6H₂O	16.05	[38]
SrCl₂·6H₂O	4.33	[39]
SrCl₂·2H₂O	8.46	[40]

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No.	J?necke index of dry salt, J(B)/(g/100 g)				No.	J?necke index of dry salt, J(B)/(g/100 g)
No.	J(MgCl₂)	J(SrCl₂)	J(AlCl₃)	J(H₂O)	No.	J(MgCl₂)	J(SrCl₂)	J(AlCl₃)	J(H₂O)
1, C	84.56	0.00	15.44	177.70	13	86.50	6.11	7.39	184.64
2	83.93	0.84	15.23	176.91	14	79.34	5.80	14.86	185.78
3, E₁	83.04	2.03	14.93	175.78	15	72.02	5.54	22.44	186.98
4	69.91	3.54	26.55	183.55	16	64.58	5.30	30.12	188.25
5, E₂	55.87	5.07	39.06	189.78	17, E₂	55.87	5.07	39.06	189.78
6, A	97.13	2.87	0.00	176.52	18	46.27	5.34	48.39	194.40
7	93.81	2.66	3.53	176.43	19	37.76	5.50	56.74	198.29
8	90.49	2.46	7.05	176.30	20	28.88	5.63	65.49	202.19
9	87.16	2.27	10.57	176.10	21	19.63	5.71	74.66	206.14
10	83.85	2.08	14.07	175.85	22	10.01	5.75	84.24	210.16
11, E₁	83.04	2.03	14.93	175.78	23, D	0.00	5.76	94.24	214.27
12, B	93.54	6.46	0.00	183.54

No.	J?necke index of dry salt, J(B)/(g/100 g)				No.	J?necke index of dry salt, J(B)/(g/100 g)
No.	J(MgCl₂)	J(SrCl₂)	J(AlCl₃)	J(H₂O)	No.	J(MgCl₂)	J(SrCl₂)	J(AlCl₃)	J(H₂O)
1, C	84.56	0.00	15.44	177.70	13	86.50	6.11	7.39	184.64
2	83.93	0.84	15.23	176.91	14	79.34	5.80	14.86	185.78
3, E₁	83.04	2.03	14.93	175.78	15	72.02	5.54	22.44	186.98
4	69.91	3.54	26.55	183.55	16	64.58	5.30	30.12	188.25
5, E₂	55.87	5.07	39.06	189.78	17, E₂	55.87	5.07	39.06	189.78
6, A	97.13	2.87	0.00	176.52	18	46.27	5.34	48.39	194.40
7	93.81	2.66	3.53	176.43	19	37.76	5.50	56.74	198.29
8	90.49	2.46	7.05	176.30	20	28.88	5.63	65.49	202.19
9	87.16	2.27	10.57	176.10	21	19.63	5.71	74.66	206.14
10	83.85	2.08	14.07	175.85	22	10.01	5.75	84.24	210.16
11, E₁	83.04	2.03	14.93	175.78	23, D	0.00	5.76	94.24	214.27
12, B	93.54	6.46	0.00	183.54