无机材料学报 ›› 2020, Vol. 35 ›› Issue (12): 1333-1339.DOI: 10.15541/jim20200182
收稿日期:
2020-04-07
修回日期:
2020-06-12
出版日期:
2020-12-20
发布日期:
2020-07-10
作者简介:
刘金云(1994–), 女, 硕士研究生. E-mail: 1158381254@qq.com
基金资助:
LIU Jinyun(),ZHANG Yuting,HONG Zhou,LIU Hua,WANG Shengxian,GU Xuehong(
)
Received:
2020-04-07
Revised:
2020-06-12
Online:
2020-12-20
Published:
2020-07-10
About author:
LIU Jinyun(1994–), female, Master candidate. E-mail: 1158381254@qq.com
Supported by:
摘要:
中空纤维陶瓷膜具有装填密度高, 传质阻力低, 使用寿命长等优点, 被广泛用于膜分离领域。高度非对称结构的中空纤维膜有利于同时实现高通量与高截留率, 本研究采用共挤出法制备双层中空纤维陶瓷复合膜, 内外层纺丝液分别掺杂平均粒径为1 μm和300 nm的α-Al2O3粉体。系统考察了内层纺丝液TiO2掺杂量、外层纺丝液Al2O3/聚醚砜(PESf)质量比和煅烧温度对膜的结构与性能的影响。结果表明, 在内层纺丝液TiO2掺杂量为2wt%, 外层纺丝液Al2O3/PESf质量比为5.60, 烧结温度为1350 ℃的最优条件下, 中空纤维膜断裂负荷为24 N、平均孔径为0.15 μm、去油率为97.5%。
中图分类号:
刘金云, 张玉亭, 洪周, 刘华, 王圣贤, 顾学红. 共挤出法制备双层中空纤维陶瓷复合膜[J]. 无机材料学报, 2020, 35(12): 1333-1339.
LIU Jinyun, ZHANG Yuting, HONG Zhou, LIU Hua, WANG Shengxian, GU Xuehong. Fabrication of Dual-layer Hollow Fiber Ceramic Composite Membranes by Co-extrusion[J]. Journal of Inorganic Materials, 2020, 35(12): 1333-1339.
Suspension composition | Inner layer | Outer layer |
---|---|---|
Solvent (NMP) | 33.34 | 37.81 |
Al2O3 (1 μm) | 55.35 | / |
Al2O3 (300 nm) | / | 49.15 |
Polymer (PESf) | 9.77 | 11.34 |
Additive (PVP) | 1.54 | 1.70 |
表1 双层中空纤维膜纺丝液组成/wt%
Table 1 Suspension composition of dual-layer hollow fiber membrane/wt%
Suspension composition | Inner layer | Outer layer |
---|---|---|
Solvent (NMP) | 33.34 | 37.81 |
Al2O3 (1 μm) | 55.35 | / |
Al2O3 (300 nm) | / | 49.15 |
Polymer (PESf) | 9.77 | 11.34 |
Additive (PVP) | 1.54 | 1.70 |
图1 双层中空纤维膜和单层中空纤维膜SEM照片
Fig. 1 SEM images of dual-layer hollow fiber and single-layer hollow fiber Cross-section morphologies of (a, b) dual-layer hollow fiber precursor, (c, d) dual-layer hollow fiber, (e, f) 1 μm single-layer hollow fiber; SEM images of the surface morphology: (g) dual-layer hollow fiber, (h) 1 μm single-layer hollow fiber
Property | η/% | Fracture load/N | Pure water flux/(m3?m-2?h-1) | Porosity/% | Average pore size/μm | RTOC/% |
---|---|---|---|---|---|---|
Single-layer (1 μm) | 13.0 | 9 | 3.52 | 51.57 | 0.70 | 95.4 |
Single-layer (300 nm) | 16.9 | 19 | 0.86 | 48.20 | 0.13 | 98.4 |
Dual-layer (1 μm/300 nm) | 14.3 | 12 | 2.30 | 50.89 | 0.24 | 97 |
表2 单层与双层中空纤维膜的性能比较
Table 2 Comparison of properties between single-layer and dual-layer hollow fiber membranes
Property | η/% | Fracture load/N | Pure water flux/(m3?m-2?h-1) | Porosity/% | Average pore size/μm | RTOC/% |
---|---|---|---|---|---|---|
Single-layer (1 μm) | 13.0 | 9 | 3.52 | 51.57 | 0.70 | 95.4 |
Single-layer (300 nm) | 16.9 | 19 | 0.86 | 48.20 | 0.13 | 98.4 |
Dual-layer (1 μm/300 nm) | 14.3 | 12 | 2.30 | 50.89 | 0.24 | 97 |
TiO2 content/wt% | η/% | Fracture load/N | Pure water flux/ (m3?m-2?h-1) | Porosity/% | Average pore size/μm |
---|---|---|---|---|---|
0 | 14.3 | 12 | 2.30 | 50.89 | 0.240 |
2 | 14.9 | 24 | 1.65 | 48.05 | 0.152 |
5 | 14.9 | 22 | 1.32 | 49.97 | 0.147 |
10 | 15.2 | 20 | 1.21 | 46.43 | 0.150 |
15 | 15.3 | 19 | 1.12 | 45.68 | 0.145 |
20 | 16.3 | 17 | 0.91 | 43.90 | 0.141 |
表3 TiO2掺杂量对双层中空纤维膜性能的影响
Table 3 Influence of TiO2 content on properties of dual-layer hollow fiber membranes
TiO2 content/wt% | η/% | Fracture load/N | Pure water flux/ (m3?m-2?h-1) | Porosity/% | Average pore size/μm |
---|---|---|---|---|---|
0 | 14.3 | 12 | 2.30 | 50.89 | 0.240 |
2 | 14.9 | 24 | 1.65 | 48.05 | 0.152 |
5 | 14.9 | 22 | 1.32 | 49.97 | 0.147 |
10 | 15.2 | 20 | 1.21 | 46.43 | 0.150 |
15 | 15.3 | 19 | 1.12 | 45.68 | 0.145 |
20 | 16.3 | 17 | 0.91 | 43.90 | 0.141 |
图3 不同外层纺丝液Al2O3/PESf质量比的双层中空纤维膜SEM照片
Fig. 3 SEM images of dual-layer hollow fiber membranes with different Al2O3/PESf mass ratios in outer suspension (a) 2.75; (b) 4.33; (c) 5.60; (d) 7.50; (e) 13.3
Al2O3/PESf | Outer suspension viscosity/cP | Fracture load/N | Pure water flux/ (m3?m-2?h-1) | Porosity/ % | Mean pore size/μm | RTOC/% |
---|---|---|---|---|---|---|
2.75 | 7320 | 21 | 1.99 | 49.90 | 0.180 | 97.3 |
4.33 | 8580 | 22 | 1.10 | 52.26 | 0.175 | 97.5 |
5.60 | 9720 | 23 | 1.41 | 53.91 | 0.130 | 97.5 |
7.50 | 11020 | 25 | 1.08 | 53.31 | 0.125 | 97.6 |
13.30 | 58300 | 23 | 0.48 | 52.54 | 0.115 | 97.8 |
表4 外层纺丝液Al2O3/PESf质量比对双层中空纤维膜性能的影响
Table 4 Influence of Al2O3/PESf mass ratio in outer suspension on properties of dual-layer hollow fiber membranes
Al2O3/PESf | Outer suspension viscosity/cP | Fracture load/N | Pure water flux/ (m3?m-2?h-1) | Porosity/ % | Mean pore size/μm | RTOC/% |
---|---|---|---|---|---|---|
2.75 | 7320 | 21 | 1.99 | 49.90 | 0.180 | 97.3 |
4.33 | 8580 | 22 | 1.10 | 52.26 | 0.175 | 97.5 |
5.60 | 9720 | 23 | 1.41 | 53.91 | 0.130 | 97.5 |
7.50 | 11020 | 25 | 1.08 | 53.31 | 0.125 | 97.6 |
13.30 | 58300 | 23 | 0.48 | 52.54 | 0.115 | 97.8 |
图4 外层纺丝液Al2O3/PESf质量比对双层中空纤维膜孔径分布的影响
Fig. 4 Influence of Al2O3/PESf mass ratio in outer suspension on pore size distribution of dual-layer hollow fiber membranes
图5 不同温度烧结的双层氧化铝中空纤维膜的SEM照片
Fig. 5 SEM images of dual-layer hollow fiber membrane of alumina sintered at different temperatures (a)1250 ℃, (b)1300 ℃, (c) 1350 ℃, (d)1400 ℃
Temperature/℃ | Fracture load/N | Pure water flux/(m3?m-2?h-1) | Porosity/% | Average pore size/μm | RTOC/% |
---|---|---|---|---|---|
1250 | 11 | 3.23 | 61.97 | 0.235 | 96.7 |
1300 | 15 | 2.34 | 55.62 | 0.199 | 97.4 |
1350 | 24 | 1.20 | 48.88 | 0.150 | 97.5 |
1400 | 37 | 0.26 | 40.33 | 0.126 | 98.3 |
表5 不同烧结温度对双层中空纤维性能的影响
Table 5 Influence of sintering temperature on the properties of dual-layer hollow fiber membranes
Temperature/℃ | Fracture load/N | Pure water flux/(m3?m-2?h-1) | Porosity/% | Average pore size/μm | RTOC/% |
---|---|---|---|---|---|
1250 | 11 | 3.23 | 61.97 | 0.235 | 96.7 |
1300 | 15 | 2.34 | 55.62 | 0.199 | 97.4 |
1350 | 24 | 1.20 | 48.88 | 0.150 | 97.5 |
1400 | 37 | 0.26 | 40.33 | 0.126 | 98.3 |
Membranes | Sintering temperature/℃ | Average pore size/μm | Pure water flux/ (m3?m-2?h-1) | Bending strength/MPa | Fracture load/N | Ref. |
---|---|---|---|---|---|---|
Single-Channel Al2O3 hollow fiber | 1455 | 0.10 | 0.664 | 88.2 | - | [ |
Single-Channel Al2O3 hollow fiber | 1500 | 0.75 | 1.280 | 85.8 | - | [ |
4-Channel Al2O3 hollow fiber | 1500 | 1.20 | 2.710 | - | 22 | [ |
7-Channel Al2O3 hollow fiber | 1350 | 0.183 | 1.070 | - | 14 | [ |
7-Channel YSZ/Al2O3 hollow fiber | 1400 | 230.00 | 1.640 | - | 14 | [ |
4-Channel 1 μm/300 nm Al2O3 hollow fiber | 1350 | 0.15 | 1.260 | - | 24 | This work |
表6 不同中空纤维陶瓷膜性能比较
Table 6 Comparison in properties of different hollow fiber ceramic membranes
Membranes | Sintering temperature/℃ | Average pore size/μm | Pure water flux/ (m3?m-2?h-1) | Bending strength/MPa | Fracture load/N | Ref. |
---|---|---|---|---|---|---|
Single-Channel Al2O3 hollow fiber | 1455 | 0.10 | 0.664 | 88.2 | - | [ |
Single-Channel Al2O3 hollow fiber | 1500 | 0.75 | 1.280 | 85.8 | - | [ |
4-Channel Al2O3 hollow fiber | 1500 | 1.20 | 2.710 | - | 22 | [ |
7-Channel Al2O3 hollow fiber | 1350 | 0.183 | 1.070 | - | 14 | [ |
7-Channel YSZ/Al2O3 hollow fiber | 1400 | 230.00 | 1.640 | - | 14 | [ |
4-Channel 1 μm/300 nm Al2O3 hollow fiber | 1350 | 0.15 | 1.260 | - | 24 | This work |
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