CIESC Journal ›› 2021, Vol. 72 ›› Issue (9): 4796-4807.DOI: 10.11949/0438-1157.20201770
• Separation engineering • Previous Articles Next Articles
Chuang LI1(),Yang ZHANG1(),Xiaojuan LIU1,Xuezhong WANG2()
Received:
2020-12-09
Revised:
2021-08-02
Online:
2021-09-05
Published:
2021-09-05
Contact:
Yang ZHANG,Xuezhong WANG
通讯作者:
张扬,王学重
作者简介:
李闯(1994—),男,硕士研究生,基金资助:
CLC Number:
Chuang LI, Yang ZHANG, Xiaojuan LIU, Xuezhong WANG. Modeling and experimental study of additives on solution crystallization of aspirin[J]. CIESC Journal, 2021, 72(9): 4796-4807.
李闯, 张扬, 刘小娟, 王学重. 添加剂作用下阿司匹林结晶模拟和实验研究[J]. 化工学报, 2021, 72(9): 4796-4807.
Face | Multiplicity | 面积占比/% |
---|---|---|
(1 0 0) | 2 | 51.93 |
(1 1 0) | 4 | 10.42 |
(0 1 1) | 4 | 11.44 |
(0 0 2) | 2 | 25.39 |
(1 1 -1) | 4 | 0.60 |
(1 1 1) | 4 | 0.22 |
Table 1 Theoretical crystal habits and percentage of total crystal plane area obtained from AE model
Face | Multiplicity | 面积占比/% |
---|---|---|
(1 0 0) | 2 | 51.93 |
(1 1 0) | 4 | 10.42 |
(0 1 1) | 4 | 11.44 |
(0 0 2) | 2 | 25.39 |
(1 1 -1) | 4 | 0.60 |
(1 1 1) | 4 | 0.22 |
添加剂(聚合度) | Eads/(kcal/mol) | |||||
---|---|---|---|---|---|---|
(1 0 0) | (1 1 0) | (0 1 1) | (0 0 2) | (1 1 -1) | (1 1 1) | |
PVP(45) | -122.35 | -135.69 | -159.11 | -129.30 | -120.90 | -90.74 |
PVP(90) | -220.06 | -237.32 | -277.11 | -207.90 | -180.92 | -148.76 |
PVP(135) | -260.23 | -303.76 | -338.57 | -256.32 | -222.13 | -195.33 |
HPMC(100) | -301.15 | -211.30 | -197.18 | -311.26 | -268.76 | -268.81 |
Table 2 Adsorption energy of additives on different crystal faces of aspirin
添加剂(聚合度) | Eads/(kcal/mol) | |||||
---|---|---|---|---|---|---|
(1 0 0) | (1 1 0) | (0 1 1) | (0 0 2) | (1 1 -1) | (1 1 1) | |
PVP(45) | -122.35 | -135.69 | -159.11 | -129.30 | -120.90 | -90.74 |
PVP(90) | -220.06 | -237.32 | -277.11 | -207.90 | -180.92 | -148.76 |
PVP(135) | -260.23 | -303.76 | -338.57 | -256.32 | -222.13 | -195.33 |
HPMC(100) | -301.15 | -211.30 | -197.18 | -311.26 | -268.76 | -268.81 |
T/K | b1 | b2 | b3 | b4 | b5 | 最大溶解度Cmax×10-2/(g/g) | w×10-2 | RMSD×10-2 |
---|---|---|---|---|---|---|---|---|
278.15 | -2.105 | 1.990 | -13.57 | 18.80 | -16.62 | 13.21 | 8.772 | 0.1761 |
283.15 | -1.921 | 1.953 | -11.01 | 13.53 | -13.98 | 16.14 | 10.66 | 0.0716 |
293.15 | -1.538 | 1.895 | -7.609 | 1.179 | -0.708 | 24.20 | 12.80 | 0.1114 |
298.15 | -1.349 | 2.144 | -9.451 | 7.815 | -7.170 | 29.65 | 13.15 | 0.1393 |
303.15 | -1.130 | 1.716 | -6.801 | 2.970 | -3.928 | 36.17 | 13.53 | 0.1843 |
313.15 | -0.790 | 1.934 | -6.496 | 3.221 | -4.178 | 52.91 | 16.31 | 0.2273 |
323.15 | -0.436 | 2.340 | -9.745 | 17.81 | -17.69 | 78.37 | 20.21 | 0.3460 |
333.15 | -0.082 | 0.551 | 4.396 | -13.09 | 6.882 | 121.0 | 34.97 | 0.6620 |
Table 3 Mass solubility fitting parameters and maximum solubility of aspirin
T/K | b1 | b2 | b3 | b4 | b5 | 最大溶解度Cmax×10-2/(g/g) | w×10-2 | RMSD×10-2 |
---|---|---|---|---|---|---|---|---|
278.15 | -2.105 | 1.990 | -13.57 | 18.80 | -16.62 | 13.21 | 8.772 | 0.1761 |
283.15 | -1.921 | 1.953 | -11.01 | 13.53 | -13.98 | 16.14 | 10.66 | 0.0716 |
293.15 | -1.538 | 1.895 | -7.609 | 1.179 | -0.708 | 24.20 | 12.80 | 0.1114 |
298.15 | -1.349 | 2.144 | -9.451 | 7.815 | -7.170 | 29.65 | 13.15 | 0.1393 |
303.15 | -1.130 | 1.716 | -6.801 | 2.970 | -3.928 | 36.17 | 13.53 | 0.1843 |
313.15 | -0.790 | 1.934 | -6.496 | 3.221 | -4.178 | 52.91 | 16.31 | 0.2273 |
323.15 | -0.436 | 2.340 | -9.745 | 17.81 | -17.69 | 78.37 | 20.21 | 0.3460 |
333.15 | -0.082 | 0.551 | 4.396 | -13.09 | 6.882 | 121.0 | 34.97 | 0.6620 |
添加剂 | 统计数目 | 平均长径比 |
---|---|---|
0 | 60 | 1.93±0.32 |
0.05% PVP K13-18 | 60 | 1.58±0.26 |
0.01% PVP K29-32 | 72 | 1.63±0.22 |
0.05% PVP K29-32 | 73 | 1.39±0.24 |
0.1% PVP K29-32 | 64 | 1.10±0.21 |
0.05% PVP K88-96 | 80 | 1.22±0.22 |
0.01% HPMC | 52 | 3.81±1.25 |
0.05% HPMC | 66 | 6.19±2.01 |
0.1% HPMC | 78 | 7.62±2.41 |
Table 4 Experimental aspirin crystal aspect ratio under different additives
添加剂 | 统计数目 | 平均长径比 |
---|---|---|
0 | 60 | 1.93±0.32 |
0.05% PVP K13-18 | 60 | 1.58±0.26 |
0.01% PVP K29-32 | 72 | 1.63±0.22 |
0.05% PVP K29-32 | 73 | 1.39±0.24 |
0.1% PVP K29-32 | 64 | 1.10±0.21 |
0.05% PVP K88-96 | 80 | 1.22±0.22 |
0.01% HPMC | 52 | 3.81±1.25 |
0.05% HPMC | 66 | 6.19±2.01 |
0.1% HPMC | 78 | 7.62±2.41 |
实验 编号 | 添加剂 浓度/% | 晶种量/% | 降温速率/ (K/min) | 搅拌速率/(r/min) | 加水速率/(ml/min) |
---|---|---|---|---|---|
1 | 0 | 1 | 0.3 | 250 | 5 |
2 | 0.01 | 1 | 0.3 | 250 | 5 |
3 | 0.05 | 1 | 0.3 | 250 | 5 |
4 | 0.10 | 1 | 0.3 | 250 | 5 |
5 | 0.05 | 0 | 0.3 | 250 | 5 |
6 | 0.05 | 0.5 | 0.3 | 250 | 5 |
7 | 0.05 | 3 | 0.3 | 250 | 5 |
8 | 0.05 | 1 | 0.1 | 250 | 5 |
9 | 0.05 | 1 | 0.5 | 250 | 5 |
10 | 0.05 | 1 | 0.3 | 150 | 5 |
11 | 0.05 | 1 | 0.3 | 350 | 5 |
12 | 0.05 | 1 | 0.3 | 250 | 20 |
13 | 0.05 | 1 | 0.3 | 250 | 一次性倾倒 |
Table 5 Summary of single factor experiment conditions
实验 编号 | 添加剂 浓度/% | 晶种量/% | 降温速率/ (K/min) | 搅拌速率/(r/min) | 加水速率/(ml/min) |
---|---|---|---|---|---|
1 | 0 | 1 | 0.3 | 250 | 5 |
2 | 0.01 | 1 | 0.3 | 250 | 5 |
3 | 0.05 | 1 | 0.3 | 250 | 5 |
4 | 0.10 | 1 | 0.3 | 250 | 5 |
5 | 0.05 | 0 | 0.3 | 250 | 5 |
6 | 0.05 | 0.5 | 0.3 | 250 | 5 |
7 | 0.05 | 3 | 0.3 | 250 | 5 |
8 | 0.05 | 1 | 0.1 | 250 | 5 |
9 | 0.05 | 1 | 0.5 | 250 | 5 |
10 | 0.05 | 1 | 0.3 | 150 | 5 |
11 | 0.05 | 1 | 0.3 | 350 | 5 |
12 | 0.05 | 1 | 0.3 | 250 | 20 |
13 | 0.05 | 1 | 0.3 | 250 | 一次性倾倒 |
实验编号 | D10/μm | D50/μm | D90/μm | 松装密度/(g/cm3) | 振实密度/(g/cm3) | 休止角/(°) | 收率/% | CV/% |
---|---|---|---|---|---|---|---|---|
1 | 201 | 544 | 1030 | 0.41 | 0.52 | 43 | 88.91 | 56.37 |
2 | 144 | 438 | 886 | 0.58 | 0.67 | 33 | 88.61 | 62.74 |
3 | 144 | 363 | 712 | 0.72 | 0.78 | 26 | 88.33 | 57.13 |
4 | 107 | 270 | 496 | 0.71 | 0.75 | 29 | 88.15 | 53.37 |
5 | 71.2 | 269 | 521 | 0.39 | 0.51 | 45 | 88.73 | 61.04 |
6 | 105 | 291 | 549 | 0.53 | 0.63 | 30 | 88.65 | 58.01 |
7 | 139 | 558 | 1040 | 0.65 | 0.73 | 28 | 87.85 | 56.83 |
8 | 279 | 579 | 1080 | 0.61 | 0.73 | 31 | 88.75 | 51.13 |
9 | 147 | 437 | 1170 | 0.53 | 0.68 | 35 | 87.35 | 86.71 |
10 | 35.3 | 472 | 1110 | 0.43 | 0.56 | 41 | 88.55 | 83.96 |
11 | 121 | 358 | 901 | 0.68 | 0.73 | 30 | 88.43 | 80.66 |
12 | 86.6 | 294 | 570 | 0.73 | 0.77 | 26 | 88.41 | 58.21 |
13 | 50.8 | 542 | 988 | 0.70 | 0.75 | 30 | 88.17 | 64.13 |
原料 | 74.5 | 459 | 916 | 0.43 | 0.55 | 40 | — | 67.81 |
Table 6 Summary of experimental results
实验编号 | D10/μm | D50/μm | D90/μm | 松装密度/(g/cm3) | 振实密度/(g/cm3) | 休止角/(°) | 收率/% | CV/% |
---|---|---|---|---|---|---|---|---|
1 | 201 | 544 | 1030 | 0.41 | 0.52 | 43 | 88.91 | 56.37 |
2 | 144 | 438 | 886 | 0.58 | 0.67 | 33 | 88.61 | 62.74 |
3 | 144 | 363 | 712 | 0.72 | 0.78 | 26 | 88.33 | 57.13 |
4 | 107 | 270 | 496 | 0.71 | 0.75 | 29 | 88.15 | 53.37 |
5 | 71.2 | 269 | 521 | 0.39 | 0.51 | 45 | 88.73 | 61.04 |
6 | 105 | 291 | 549 | 0.53 | 0.63 | 30 | 88.65 | 58.01 |
7 | 139 | 558 | 1040 | 0.65 | 0.73 | 28 | 87.85 | 56.83 |
8 | 279 | 579 | 1080 | 0.61 | 0.73 | 31 | 88.75 | 51.13 |
9 | 147 | 437 | 1170 | 0.53 | 0.68 | 35 | 87.35 | 86.71 |
10 | 35.3 | 472 | 1110 | 0.43 | 0.56 | 41 | 88.55 | 83.96 |
11 | 121 | 358 | 901 | 0.68 | 0.73 | 30 | 88.43 | 80.66 |
12 | 86.6 | 294 | 570 | 0.73 | 0.77 | 26 | 88.41 | 58.21 |
13 | 50.8 | 542 | 988 | 0.70 | 0.75 | 30 | 88.17 | 64.13 |
原料 | 74.5 | 459 | 916 | 0.43 | 0.55 | 40 | — | 67.81 |
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