化工进展 ›› 2023, Vol. 42 ›› Issue (1): 488-496.DOI: 10.16085/j.issn.1000-6613.2022-0542
范嘉昊1,2(), 张洋2(
), 范兵强2, 张贺东2, 郑诗礼2, 邹兴1
收稿日期:
2022-04-01
修回日期:
2022-06-06
出版日期:
2023-01-25
发布日期:
2023-02-20
通讯作者:
张洋
作者简介:
范嘉昊(1997—),男,硕士研究生,研究方向工业结晶。E-mail:g20198253@xs.ustb.edu.cn。
基金资助:
FAN Jiahao1,2(), ZHANG Yang2(
), FAN Binqiang2, ZHANG Hedong2, ZHENG Shili2, ZOU Xing1
Received:
2022-04-01
Revised:
2022-06-06
Online:
2023-01-25
Published:
2023-02-20
Contact:
ZHANG Yang
摘要:
湿法冶金、三元前体制备等过程均会产生含硫酸钠与硫酸铵的高盐废水。研究高盐废水中硫酸铵的结晶动力学,并考察常见金属离子的影响规律对高盐废水处理具有重要意义。本文以含硫酸钠与硫酸铵混合溶液中硫酸铵的结晶过程为例,系统考察了硫酸铵的结晶动力学及铁、铝、锰、铬对硫酸铵结晶的影响规律。含硫酸钠与硫酸铵混合溶液硫酸铵结晶动力学研究结果表明,硫酸铵生长速率和成核速率方程分别为为
中图分类号:
范嘉昊, 张洋, 范兵强, 张贺东, 郑诗礼, 邹兴. (NH4)2SO4和Na2SO4混合溶液中(NH4)2SO4结晶动力学及铁/铝/锰/铬等离子对(NH4)2SO4结晶的影响规律[J]. 化工进展, 2023, 42(1): 488-496.
FAN Jiahao, ZHANG Yang, FAN Binqiang, ZHANG Hedong, ZHENG Shili, ZOU Xing. Crystallization kinetics of (NH4)2SO4 in mixed solution of (NH4)2SO4 and Na2SO4 and the influence of Fe/Al/Mn/Cr ions on crystallization[J]. Chemical Industry and Engineering Progress, 2023, 42(1): 488-496.
取样编号 | m/kg | σ | |
---|---|---|---|
1 | 4.19×10-5 | 4.19 | 0.014 |
2 | 7.99×10-5 | 7.99 | 0.042 |
3 | 12.01×10-4 | 12.01 | 0.035 |
4 | 19.13×10-4 | 19.13 | 0.05 |
5 | 14.24×10-4 | 14.24 | 0.04 |
6 | 19.77×10-4 | 19.77 | 0.075 |
7 | 23.55×10-4 | 23.55 | 0.05 |
8 | 25.52×10-4 | 25.52 | 0.014 |
9 | 26.08×10-4 | 26.08 | 0.042 |
表1 硫酸铵悬浮密度及相对过饱和度
取样编号 | m/kg | σ | |
---|---|---|---|
1 | 4.19×10-5 | 4.19 | 0.014 |
2 | 7.99×10-5 | 7.99 | 0.042 |
3 | 12.01×10-4 | 12.01 | 0.035 |
4 | 19.13×10-4 | 19.13 | 0.05 |
5 | 14.24×10-4 | 14.24 | 0.04 |
6 | 19.77×10-4 | 19.77 | 0.075 |
7 | 23.55×10-4 | 23.55 | 0.05 |
8 | 25.52×10-4 | 25.52 | 0.014 |
9 | 26.08×10-4 | 26.08 | 0.042 |
粒度/μm | 累加百分数/% | ΔL/μm | nj /μm-4 | μ0j /μm-3 | μ1j /μm-2 | |
---|---|---|---|---|---|---|
0 | 0 | 50 | 25 | 0 | 0 | 0 |
50 | 0 | 50 | 75 | 0 | 0 | 0 |
100 | 1.8113208 | 50 | 125 | 4.39072×10-15 | 2.19536×10-13 | 2.7442×10-11 |
150 | 6.5660377 | 50 | 175 | 4.20031×10-15 | 2.10015×10-3 | 3.67527×10-11 |
200 | 6.5660377 | 50 | 225 | 0 | 0 | 0 |
250 | 10.0377358 | 50 | 275 | 7.90341×10-16 | 3.95171×10-14 | 1.08672×10-11 |
300 | 21.4339623 | 100 | 350 | 6.29213×10-16 | 6.29213×10-14 | 2.20225×10-11 |
400 | 26.7169811 | 100 | 450 | 1.37241×10-16 | 1.37241×10-14 | 6.17587×10-12 |
500 | 30.9433962 | 100 | 550 | 6.01347×10-17 | 6.01347×10-15 | 3.30741×10-12 |
600 | 43.3962264 | 100 | 650 | 1.07342×10-16 | 1.07342×10-14 | 6.97722×10-12 |
700 | 46.7924528 | 100 | 750 | 1.9057×10-17 | 1.9057×10-15 | 1.42927×10-12 |
800 | 46.7924528 | 100 | 850 | 0 | 0 | 0 |
900 | 58.5660377 | 100 | 950 | 3.25071×10-17 | 3.25071×10-15 | 3.08818×10-12 |
1000 | 83.8490566 | 500 | 1250 | 6.12872×10-18 | 3.06436×10-15 | 3.83045×10-12 |
1500 | 100 | 500 | 1750 | 1.42677×10-18 | 7.13386×10-16 | 1.24843×10-12 |
2000 | μ0=5.71396×10-13 | μ1=1.23141×10-10 |
表2 以1号结晶样品为例计算μ0和μ1
粒度/μm | 累加百分数/% | ΔL/μm | nj /μm-4 | μ0j /μm-3 | μ1j /μm-2 | |
---|---|---|---|---|---|---|
0 | 0 | 50 | 25 | 0 | 0 | 0 |
50 | 0 | 50 | 75 | 0 | 0 | 0 |
100 | 1.8113208 | 50 | 125 | 4.39072×10-15 | 2.19536×10-13 | 2.7442×10-11 |
150 | 6.5660377 | 50 | 175 | 4.20031×10-15 | 2.10015×10-3 | 3.67527×10-11 |
200 | 6.5660377 | 50 | 225 | 0 | 0 | 0 |
250 | 10.0377358 | 50 | 275 | 7.90341×10-16 | 3.95171×10-14 | 1.08672×10-11 |
300 | 21.4339623 | 100 | 350 | 6.29213×10-16 | 6.29213×10-14 | 2.20225×10-11 |
400 | 26.7169811 | 100 | 450 | 1.37241×10-16 | 1.37241×10-14 | 6.17587×10-12 |
500 | 30.9433962 | 100 | 550 | 6.01347×10-17 | 6.01347×10-15 | 3.30741×10-12 |
600 | 43.3962264 | 100 | 650 | 1.07342×10-16 | 1.07342×10-14 | 6.97722×10-12 |
700 | 46.7924528 | 100 | 750 | 1.9057×10-17 | 1.9057×10-15 | 1.42927×10-12 |
800 | 46.7924528 | 100 | 850 | 0 | 0 | 0 |
900 | 58.5660377 | 100 | 950 | 3.25071×10-17 | 3.25071×10-15 | 3.08818×10-12 |
1000 | 83.8490566 | 500 | 1250 | 6.12872×10-18 | 3.06436×10-15 | 3.83045×10-12 |
1500 | 100 | 500 | 1750 | 1.42677×10-18 | 7.13386×10-16 | 1.24843×10-12 |
2000 | μ0=5.71396×10-13 | μ1=1.23141×10-10 |
取样编号 | μ0/μm-3 | μ1/μm-2 | ||
---|---|---|---|---|
1 | 5.71396×10-13 | 1.23141×10-10 | 1.18142×10-15 | 0.04116 |
2 | 1.28025×10-12 | 3.51759×10-10 | 1.04789×10-15 | 0.18793 |
3 | 1.90898×10-12 | 5.31568×10-10 | 4.01696×10-15 | 0.14552 |
4 | 4.31916×10-12 | 8.03464×10-10 | 1.57388×10-14 | 0.23945 |
5 | 1.37625×10-11 | 1.55993×10-9 | 4.67263×10-15 | 0.20499 |
6 | 1.656×10-11 | 1.74644×10-9 | 1.09063×10-14 | 0.41233 |
7 | 1.00223×10-11 | 2.07534×10-9 | 1.71882×10-14 | 0.25547 |
8 | 2.03352×10-11 | 2.30801×10-9 | 1.91881×10-14 | 0.62046 |
9 | 3.18481×10-11 | 3.27934×10-9 |
表3 平均成核速率和平均生长速率
取样编号 | μ0/μm-3 | μ1/μm-2 | ||
---|---|---|---|---|
1 | 5.71396×10-13 | 1.23141×10-10 | 1.18142×10-15 | 0.04116 |
2 | 1.28025×10-12 | 3.51759×10-10 | 1.04789×10-15 | 0.18793 |
3 | 1.90898×10-12 | 5.31568×10-10 | 4.01696×10-15 | 0.14552 |
4 | 4.31916×10-12 | 8.03464×10-10 | 1.57388×10-14 | 0.23945 |
5 | 1.37625×10-11 | 1.55993×10-9 | 4.67263×10-15 | 0.20499 |
6 | 1.656×10-11 | 1.74644×10-9 | 1.09063×10-14 | 0.41233 |
7 | 1.00223×10-11 | 2.07534×10-9 | 1.71882×10-14 | 0.25547 |
8 | 2.03352×10-11 | 2.30801×10-9 | 1.91881×10-14 | 0.62046 |
9 | 3.18481×10-11 | 3.27934×10-9 |
杂质种类 | 浓度/mol·L-1 | 成核动力学方程 | 生长动力学方程 |
---|---|---|---|
Mn2+ | 0.001 | ||
0.002 | |||
0.003 | |||
Al3+ | 0.001 | ||
0.002 | |||
0.003 | |||
Fe3+ | 0.001 | ||
0.002 | |||
0.003 | |||
Cr3+ | 0.001 | ||
0.002 | |||
0.003 |
表4 硫酸铵结晶动力学方程
杂质种类 | 浓度/mol·L-1 | 成核动力学方程 | 生长动力学方程 |
---|---|---|---|
Mn2+ | 0.001 | ||
0.002 | |||
0.003 | |||
Al3+ | 0.001 | ||
0.002 | |||
0.003 | |||
Fe3+ | 0.001 | ||
0.002 | |||
0.003 | |||
Cr3+ | 0.001 | ||
0.002 | |||
0.003 |
杂质种类 | 浓度/mol·L-1 | ||
---|---|---|---|
Mn2+ | 0.001 | 1.76419×10-14 | 0.66714 |
0.002 | 1.13867×10-14 | 0.82653 | |
0.003 | 9.17748×10-15 | 0.33817 | |
Al3+ | 0.001 | 7.42176×10-15 | 0.61249 |
0.002 | 6.34097×10-15 | 0.37135 | |
0.003 | 1.76419×10-15 | 0.24965 | |
Fe3+ | 0.001 | 5.25004×10-15 | 0.44396 |
0.002 | 3.54196×10-15 | 0.34471 | |
0.003 | 1.19991×10-15 | 0.14457 | |
Cr3+ | 0.001 | 1.05465×10-14 | 0.74411 |
0.002 | 8.94551×10-15 | 0.37585 | |
0.003 | 5.11125×10-15 | 0.25918 |
表5 不同浓度杂质条件下硫酸铵结晶平均成核速率和平均生长速率
杂质种类 | 浓度/mol·L-1 | ||
---|---|---|---|
Mn2+ | 0.001 | 1.76419×10-14 | 0.66714 |
0.002 | 1.13867×10-14 | 0.82653 | |
0.003 | 9.17748×10-15 | 0.33817 | |
Al3+ | 0.001 | 7.42176×10-15 | 0.61249 |
0.002 | 6.34097×10-15 | 0.37135 | |
0.003 | 1.76419×10-15 | 0.24965 | |
Fe3+ | 0.001 | 5.25004×10-15 | 0.44396 |
0.002 | 3.54196×10-15 | 0.34471 | |
0.003 | 1.19991×10-15 | 0.14457 | |
Cr3+ | 0.001 | 1.05465×10-14 | 0.74411 |
0.002 | 8.94551×10-15 | 0.37585 | |
0.003 | 5.11125×10-15 | 0.25918 |
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