田口实验设计法优化碳酸锂反应结晶制备工艺

doi:10.19964/j.issn.1006-4990.2020-0527

Abstract

Abstract:

Single-factor experiment cannot comprehensively and reliably study the influence of various factors on the pre-paration of high-quality lithium carbonate during the reaction crystallization process.Taguchi′s design is conducive to the comprehensive study of various factors to prepare high-quality lithium carbonate.The experiment cycle is shorter and the experiment cost is lower.Using the refined brine of Dongtai Jinel Salt Lake as the raw material,Taguchi experiment was designed,and the focused beam reflection measuring instrument FBRM G400 was used to study effect of the reaction temperature,stirring rate,brine feed rate,Na₂CO₃ concentration and other factors on the reaction crystallization process in real-time on-line study of the lithium carbonate particle size and purity.Taguchi experiments showed that the stirring rate had the greatest influence on the particle size of lithium carbonate,and the purity of lithium carbonate was most sensitive to the reaction temperature.The results of the study showed that when the reaction temperature was 85 ℃,the stirring rate was 200 r/min,the brine feed rate was 2 mL/min,and the mass concentration of Na₂CO₃ was 201.6 g/L,the quality of obtained lithium carbonate was the best with particle size of 3.71 μm and purity of 99.62%.

Key words: Li₂CO₃, reaction crystallization, Taguchi experimental design method, particle size, purity

CLC Number:

TQ131.11

Wang Bin,Deng Xiaochuan,Shi Yifei,Dong Chaochao,Fan Faying,Zhu Chaoliang,Fan Jie,Ma Wanxia,Zuo Fangtao. Optimizing preparation process of lithium carbonate reaction crystallization by Taguchi experimental design method[J]. Inorganic Chemicals Industry, 2021, 53(8): 60-65.

Figures/Tables 16

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References 16

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水平	因素
水平	A 反应温度/ ℃	B 搅拌速率/ （r·min^-1）	C 卤水加料速度/ （mL·min^-1）	D Na₂CO₃ 质量浓度/ （g·L^-1）
1	55	200	2	183.3
2	70	400	3	201.6
3	85	600	6	219.9

实验序号	A 反应温度/℃	B 搅拌速率/ （r·min^-1）	C 卤水加料速度/（mL·min^-1）	D Na₂CO₃ 质量浓度/ （g·L^-1）	粒径/ μm	纯度/ %	实验序号	A 反应温度/℃	B 搅拌速率/ （r·min^-1）	C 卤水加料速度/（mL·min^-1）	D Na₂CO₃质量浓度/ （g·L^-1）	粒径/ μm	纯度/ %
1	55	200	6	183.3	4.25	98.60	23	70	400	2	183.3	8.57	99.15
10	55	200	6	183.3	6.46	98.59	6	70	600	6	201.6	9.05	99.02
19	55	200	6	183.3	4.05	98.59	15	70	600	6	201.6	9.75	98.96
2	55	400	3	201.6	9.71	98.74	24	70	600	6	201.6	8.84	98.82
11	55	400	3	201.6	5.31	98.56	7	85	200	2	201.6	3.44	99.46
20	55	400	3	201.6	6.94	98.68	16	85	200	2	201.6	3.74	99.62
3	55	600	2	219.9	9.24	98.60	25	85	200	2	201.6	3.96	99.48
12	55	600	2	219.9	9.86	98.75	8	85	400	6	219.9	9.47	99.35
21	55	600	2	219.9	8.00	99.10	17	85	400	6	219.9	10.75	99.50
4	70	200	3	219.9	3.68	98.70	26	85	400	6	219.9	12.69	99.14
13	70	200	3	219.9	3.18	99.23	9	85	600	3	183.3	10.56	99.46
22	70	200	3	219.9	3.55	99.04	18	85	600	3	183.3	10.22	99.44
5	70	400	2	183.3	9.74	99.60	27	85	600	3	183.3	9.35	99.68
14	70	400	2	183.3	8.57	99.29

水平	粒径均值/μm
水平	A 反应温度	B 搅拌速率	C 卤水加料速度	D Na₂CO₃浓度
1	7.091	4.034	7.236	7.974
2	7.214	9.083	6.944	6.749
3	8.242	9.430	8.368	7.824
Delta	1.151	5.396	1.423	1.226
排秩	4	1	2	3

来源	自由度	离差平方和SS（Adj）	均方MS （Adj）	F值	P值
A 反应温度	2	7.190	3.595	2.82	0.086
B 搅拌速率	2	164.2	82.09	64.41	0.000
C 卤水加料速度	2	10.18	5.089	3.99	0.037
D Na₂CO₃浓度	2	8.044	4.022	3.16	0.067
误差	18	22.94	1.275
合计	26	212.5

来源	自由度	离差平方和SS（Adj）	均方MS （Adj）	F值	P值
A 反应温度	2	2.662	1.331	44.70	0.000
B 搅拌速率	2	0.029	0.015	0.49	0.619
C 卤水加料速度	2	0.348	0.174	5.84	0.011
D Na₂CO₃浓度	2	0.078	0.039	1.31	0.294
误差	18	0.536	0.030
合计	26	3.653

National Inorganic Salts Information Center

Inorganic Acid-Base-Salt Committee of CIESC

Optimizing preparation process of lithium carbonate reaction crystallization by Taguchi experimental design method

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实验	w（Li₂CO₃）	w（Cl^-）	w（SO₄^2-）	w（Na⁺）	w（K⁺）	w（Ca²⁺）	w（Mg²⁺）	w（Fe）
A₃B₂C₁D₁	99.73	20×10^-3	4.3×10^-3	43×10^-3	1.4×10^-3	21×10^-3	6.3×10^-3	5.6×10^-3
实验16	99.62	33×10^-3	5.3×10^-3	50×10^-3	1.6×10^-3	25×10^-3	7.4×10^-3	8.0×10^-3
实验23	99.15	18×10^-3	5.7×10^-3	53×10^-3	2.2×10^-3	27×10^-3	8.6×10^-3	6.7×10^-3
实验20	98.68	26×10^-3	4.9×10^-3	83×10^-3	4.1×10^-3	30×10^-3	9.7×10^-3	11.4×10^-3

考察指标	粒径			纯度			最佳综合工艺条件
考察指标	P值	显著性	最优条件	P值	显著性	最优条件	最佳综合工艺条件
A 反应温度	0.086	有影响	55 ℃	0.000	**	85 ℃	85 ℃
B 搅拌速率	0.000	**	200 r/min	0.619	不显著	400 r/min	200 r/min
C 卤水加料速度	0.037	*	3 mL/min	0.011	**	2 mL/min	2 mL/min
D Na₂CO₃浓度	0.067	有影响	201.6 g/L	0.294	不显著	183.3 g/L	201.6 g/L

实验	粒径/μm	w（Li₂CO₃）/%	w（Cl^-）/%	w（SO₄^2-）/%	w（Na⁺）/%	w（K⁺）/%	w（Ca²⁺）/%	w（Mg²⁺）/%	w（Fe）/%
实验 7	3.44	99.46	12×10^-3	4.6×10^-3	70×10^-3	1.8×10^-3	24×10^-3	8.6×10^-3	6.3×10^-3
实验16	3.74	99.62	10×10^-3	5.3×10^-3	62×10^-3	1.5×10^-3	21×10^-3	8.1×10^-3	5.6×10^-3
实验25	3.96	99.48	13×10^-3	4.9×10^-3	73×10^-3	2.1×10^-3	23×10^-3	9.2×10^-3	7.1×10^-3

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水平	碳酸锂纯度均值/%
水平	A 反应温度	B 搅拌速率	C 卤水加料速度	D Na₂CO₃浓度
1	98.69	99.03	99.23	99.16
2	99.09	99.11	99.06	99.04
3	99.46	99.09	98.95	99.05
Delta	0.77	0.08	0.28	0.12
排秩	1	4	2	3