Phase equilibrium of Na2SO4-NH3-CO2-H2O system in preparation of sodium bicarbonate from sodium sulfate

doi:10.16085/j.issn.1000-6613.2023-0472

Abstract

Abstract:

It is of great significance to master the phase equilibrium law of Na₂SO₄-NH₃-CO₂-H₂O system to optimize the process of preparing sodium bicarbonate with high utilization of sodium sulfate. In this paper, the liquid-solid equilibrium relationship of Na₂SO₄-NH₃-CO₂-H₂O system and its sub-system Na₂SO₄-NH₃-H₂O was studied by isothermal solution equilibrium method at 303.15K, 323.15K and 343.15K at 101.3—1099.0kPa. The equilibrium law of SO $4 2 -$ , CO $3 2 -$ and HCO $3 -$ in the Na₂SO₄-NH₃-CO₂-H₂O system and the Na₂SO₄-NH₃-CO₂-H₂O system were obtained. The results showed that ammonia in the Na₂SO₄-NH₃-H₂O system had a strong salt-out effect on sodium sulfate. Under the action of ammonia, the equilibrium solid phase of the system existed in the form of anhydrous sodium sulfate when the temperature was lower than 305.55K. At the same time, the solution of sodium sulfate ammonia salt water could promote the dissolution of sodium sulfate by carbonation of carbon dioxide. Low temperature and high pressure could promote the carbonation of sodium sulfate ammonia brine solution and improve the conversion of sodium sulfate to sodium bicarbonate.

Key words: sodium sulfate, phase equilibrium, carbonation, ammonia, sodium bicarbonate

摘要：

Na₂SO₄-NH₃-CO₂-H₂O体系相平衡规律的掌握，对硫酸钠高值利用制备碳酸氢钠过程的工艺优化有重要意义。本文采用等温溶解平衡法在101.3～1099.0kPa下303.15K、323.15K和343.15K时研究了Na₂SO₄-NH₃-CO₂-H₂O体系以及其子体系Na₂SO₄-NH₃-H₂O的液-固相平衡关系，并获得了Na₂SO₄-NH₃-H₂O体系以及SO $4 2 -$ 、CO $3 2 -$ 和HCO $3 -$ 在Na₂SO₄-NH₃-CO₂-H₂O体系相平衡规律。研究结果表明，Na₂SO₄-NH₃-H₂O体系中氨对硫酸钠有强烈盐析作用，当温度低于305.55K时在氨的作用下，体系平衡固相以无水硫酸钠的形式存在。同时硫酸钠氨盐水溶液通入二氧化碳进行碳酸化可促进硫酸钠的溶解。低温、高压有利于促进硫酸钠氨盐水溶液的碳酸化，并提高硫酸钠向碳酸氢钠的转化率。

关键词: 硫酸钠, 相平衡, 碳酸化, 氨气, 碳酸氢钠

CLC Number:

TQ114.1

HU Hongyuan, ZHANG Yang, ZHANG Hedong, FAN Bingqiang, ZHENG Shili, TANG Jihai. Phase equilibrium of Na₂SO₄-NH₃-CO₂-H₂O system in preparation of sodium bicarbonate from sodium sulfate[J]. Chemical Industry and Engineering Progress, 2024, 43(3): 1621-1629.

胡洪远, 张洋, 张贺东, 范兵强, 郑诗礼, 汤吉海. 硫酸钠制备碳酸氢钠过程中Na₂SO₄-NH₃-CO₂-H₂O体系相平衡规律[J]. 化工进展, 2024, 43(3): 1621-1629.

Figures/Tables 14

点	T/K	ρ/g·cm^-3	液相组成（质量分数）/%			平衡固相
点	T/K	ρ/g·cm^-3	NH₃	Na₂SO₄	H₂O	平衡固相
F	303.15	1.2560	0.00	24.42	75.58	Na₂SO₄
	303.15	1.2500	1.09	24.17	74.74	Na₂SO₄
	303.15	1.2388	1.78	23.59	74.64	Na₂SO₄
	303.15	1.2020	2.65	22.22	75.13	Na₂SO₄
	303.15	1.1694	3.68	20.60	75.73	Na₂SO₄
	303.15	1.1434	4.89	18.99	76.12	Na₂SO₄
	303.15	1.1171	5.81	17.66	76.53	Na₂SO₄
	303.15	1.0815	8.09	14.37	77.54	Na₂SO₄
	303.15	1.0274	10.98	11.06	77.96	Na₂SO₄
	303.15	1.0023	13.15	7.84	79.01	Na₂SO₄
	303.15	0.9599	16.37	5.82	77.81	Na₂SO₄
	303.15	0.9435	20.10	3.95	75.95	Na₂SO₄
	303.15	0.9176	23.48	2.75	73.77	Na₂SO₄
	303.15	0.9140	26.01	2.08	71.90	Na₂SO₄
	303.15	0.9152	27.47	1.66	70.87	Na₂SO₄
	303.15	0.9043	28.35	1.53	70.13	Na₂SO₄
E	303.15	0.8926	29.00	1.59	69.41	Na₂SO₄
D	303.15	0.8954	29.20	0	70.80	—
F'	323.15	1.2808	0.00	25.64	74.36	Na₂SO₄
	323.15	1.2363	1.12	23.70	75.18	Na₂SO₄
	323.15	1.1244	4.87	18.09	77.04	Na₂SO₄
	323.15	1.0730	6.83	15.72	77.45	Na₂SO₄
	323.15	1.0475	8.03	14.00	77.97	Na₂SO₄
	323.15	1.0128	10.71	11.82	77.47	Na₂SO₄
	323.15	1.0072	11.17	10.87	77.96	Na₂SO₄
	323.15	0.9984	11.97	10.05	77.98	Na₂SO₄
	323.15	0.9891	12.68	9.67	77.65	Na₂SO₄
E'	323.15	0.9875	12.77	9.49	77.74	Na₂SO₄
	323.15	0.9862	13.12	8.93	77.95	—
	323.15	0.9732	13.68	8.90	77.42	—
	323.15	0.9610	14.89	7.54	77.57	—
	323.15	0.9542	15.93	5.65	78.42	—
	323.15	0.9402	16.56	4.68	78.76	—
	323.15	0.9367	17.35	2.43	80.22	—
D'	323.15	0.9252	18.37	0.00	81.63	—
F''	343.15	1.2804	0.00	24.71	75.29	Na₂SO₄
	343.15	1.2464	0.71	23.67	75.62	Na₂SO₄
	343.15	1.2034	2.06	22.05	75.89	Na₂SO₄
	343.15	1.1662	3.01	21.01	75.98	Na₂SO₄
	343.15	1.1583	3.18	20.54	76.28	Na₂SO₄
	343.15	1.1626	3.15	20.06	76.78	Na₂SO₄
E''	343.15	1.1631	3.15	19.94	76.91	Na₂SO₄
	343.15	1.1612	3.17	19.54	77.29	—
	343.15	1.1512	3.35	19.30	77.35	—
	343.15	1.0993	3.92	15.29	80.78	—
	343.15	1.0763	4.33	13.28	82.39	—
	343.15	1.0434	4.86	11.61	83.53	—
	343.15	1.0172	5.68	8.31	86.01	—
	343.15	0.9906	6.50	5.71	87.79	—
D''	343.15	0.9426	8.69	0.00	91.31	—

点	T/K	ρ/g·cm^-3	液相组成/g·L^-1					固相
点	T/K	ρ/g·cm^-3	SO $4 2 -$	OH^-	CO $3 2 -$	HCO $3 -$	NH $4 +$	固相
	303.15	1.1351	132	78	84	0	116	Na₂SO₄
	303.15	1.1700	151	66	97	0	117	Na₂SO₄
	303.15	1.2063	170	55	109	0	117	Na₂SO₄
	303.15	1.2235	184	43	124	0	118	Na₂SO₄
	303.15	1.2412	197	32	139	0	119	Na₂SO₄
	303.15	1.2543	209	16	150	0	118	Na₂SO₄
	303.15	1.2677	221	0	162	15	117	Na₂SO₄
G	303.15	1.2680	240	0	135	23	118	Na₂SO₄
G'	303.15	1.2695	259	0	109	31	119	Na₂SO₄+NaHCO₃
	303.15	1.2730	277	0	85	39	119	Na₂SO₄+NaHCO₃
	303.15	1.2767	295	0	62	47	119	Na₂SO₄+NaHCO₃
	323.15	1.1643	151	61	66	0	115	Na₂SO₄
	323.15	1.1905	164	54	78	0	115	Na₂SO₄
	323.15	1.2175	178	48	90	0	115	Na₂SO₄
	323.15	1.2340	195	37	106	0	115	Na₂SO₄
	323.15	1.2527	211	27	121	0	115	Na₂SO₄
	323.15	1.2515	219	13	136	0	115	Na₂SO₄
	323.15	1.2509	235	0	151	9	115	Na₂SO₄
H	323.15	1.2573	250	0	122	17	115	Na₂SO₄
H'	323.15	1.2627	264	0	93	26	114	Na₂SO₄+NaHCO₃
	323.15	1.2610	281	0	72	32	114	Na₂SO₄+NaHCO₃
	323.15	1.2590	297	0	50	38	114	Na₂SO₄+NaHCO₃
	343.15	1.1577	149	58	42	0	107	Na₂SO₄
	343.15	1.1833	168	49	54	0	107	Na₂SO₄
	343.15	1.2110	186	41	66	0	107	Na₂SO₄
	343.15	1.2250	197	33	81	0	107	Na₂SO₄
	343.15	1.2421	208	26	97	0	108	Na₂SO₄
	343.15	1.2450	223	13	109	0	108	Na₂SO₄
	343.15	1.2518	231	0	121	5	109	Na₂SO₄
	343.15	1.2554	249	0	103	11	109	Na₂SO₄
	343.15	1.2544	266	0	84	17	109	Na₂SO₄
J	343.15	1.2540	279	0	63	21	108	Na₂SO₄
J'	343.15	1.2522	291	0	42	25	108	Na₂SO₄+NaHCO₃

点	T/K	ρ/g·cm^-3	液相组成/g·L^-1					固相
点	T/K	ρ/g·cm^-3	SO $4 2 -$	OH^-	CO $3 2 -$	HCO $3 -$	NH $4 +$	固相
	303.15	1.1351	132	78	84	0	116	Na₂SO₄
	303.15	1.1700	151	66	97	0	117	Na₂SO₄
	303.15	1.2063	170	55	109	0	117	Na₂SO₄
	303.15	1.2235	184	43	124	0	118	Na₂SO₄
	303.15	1.2412	197	32	139	0	119	Na₂SO₄
	303.15	1.2543	209	16	150	0	118	Na₂SO₄
	303.15	1.2677	221	0	162	15	117	Na₂SO₄
G	303.15	1.2680	240	0	135	23	118	Na₂SO₄
G'	303.15	1.2695	259	0	109	31	119	Na₂SO₄+NaHCO₃
	303.15	1.2730	277	0	85	39	119	Na₂SO₄+NaHCO₃
	303.15	1.2767	295	0	62	47	119	Na₂SO₄+NaHCO₃
	323.15	1.1643	151	61	66	0	115	Na₂SO₄
	323.15	1.1905	164	54	78	0	115	Na₂SO₄
	323.15	1.2175	178	48	90	0	115	Na₂SO₄
	323.15	1.2340	195	37	106	0	115	Na₂SO₄
	323.15	1.2527	211	27	121	0	115	Na₂SO₄
	323.15	1.2515	219	13	136	0	115	Na₂SO₄
	323.15	1.2509	235	0	151	9	115	Na₂SO₄
H	323.15	1.2573	250	0	122	17	115	Na₂SO₄
H'	323.15	1.2627	264	0	93	26	114	Na₂SO₄+NaHCO₃
	323.15	1.2610	281	0	72	32	114	Na₂SO₄+NaHCO₃
	323.15	1.2590	297	0	50	38	114	Na₂SO₄+NaHCO₃
	343.15	1.1577	149	58	42	0	107	Na₂SO₄
	343.15	1.1833	168	49	54	0	107	Na₂SO₄
	343.15	1.2110	186	41	66	0	107	Na₂SO₄
	343.15	1.2250	197	33	81	0	107	Na₂SO₄
	343.15	1.2421	208	26	97	0	108	Na₂SO₄
	343.15	1.2450	223	13	109	0	108	Na₂SO₄
	343.15	1.2518	231	0	121	5	109	Na₂SO₄
	343.15	1.2554	249	0	103	11	109	Na₂SO₄
	343.15	1.2544	266	0	84	17	109	Na₂SO₄
J	343.15	1.2540	279	0	63	21	108	Na₂SO₄
J'	343.15	1.2522	291	0	42	25	108	Na₂SO₄+NaHCO₃

p/kPa	ρ/g·cm^-3	液相组成/g·L^-1					平衡固相
p/kPa	ρ/g·cm^-3	SO $4 2 -$	CO $3 2 -$	HCO $3 -$	NH $4 +$	Na⁺	平衡固相
115.0	1.2291	246	36	37	79	41	NaHCO₃
307.0	1.2278	244	33	40	79	39	NaHCO₃
563.0	1.2234	246	26	48	81	38	NaHCO₃
793.0	1.2244	243	23	54	81	35	NaHCO₃
1058.0	1.2248	245	18	60	81	34	NaHCO₃

p/kPa	ρ/g·cm^-3	液相组成/g·L^-1					平衡固相
p/kPa	ρ/g·cm^-3	SO $4 2 -$	CO $3 2 -$	HCO $3 -$	NH $4 +$	Na⁺	平衡固相
115.0	1.2291	246	36	37	79	41	NaHCO₃
307.0	1.2278	244	33	40	79	39	NaHCO₃
563.0	1.2234	246	26	48	81	38	NaHCO₃
793.0	1.2244	243	23	54	81	35	NaHCO₃
1058.0	1.2248	245	18	60	81	34	NaHCO₃

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Phase equilibrium of Na₂SO₄-NH₃-CO₂-H₂O system in preparation of sodium bicarbonate from sodium sulfate

硫酸钠制备碳酸氢钠过程中Na₂SO₄-NH₃-CO₂-H₂O体系相平衡规律

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