化工学报 ›› 2021, Vol. 72 ›› Issue (3): 1230-1241.DOI: 10.11949/0438-1157.20200855
唐和礼1(),张冰1(
),黄冬梅1,申渝1,2(
),高旭1,2,时文歆3
收稿日期:
2020-06-30
修回日期:
2020-09-21
出版日期:
2021-03-05
发布日期:
2021-03-05
通讯作者:
张冰,申渝
作者简介:
唐和礼(1998—),男,硕士研究生,基金资助:
TANG Heli1(),ZHANG Bing1(
),HUANG Dongmei1,SHEN Yu1,2(
),GAO Xu1,2,SHI Wenxin3
Received:
2020-06-30
Revised:
2020-09-21
Online:
2021-03-05
Published:
2021-03-05
Contact:
ZHANG Bing,SHEN Yu
摘要:
膜分离过程中存在的膜污染问题严重制约了膜分离技术的大规模应用。扩展的XDLVO(Derjaguin-Landau-Verwey-Overbeek)理论可以为膜污染机理的阐述提供理论支撑,它不仅可以用来解析及预测膜污染,还可为膜污染控制提供理论指导。介绍了XDLVO理论的分析计算方法,综述了XDLVO理论在不同污染物的膜污染行为解析中的应用,讨论了膜面性质及操作条件对膜污染行为的影响以及XDLVO理论对膜污染控制的指导作用,并提出了XDLVO理论在膜污染行为研究中存在的问题以及对未来研究方向的展望。
中图分类号:
唐和礼, 张冰, 黄冬梅, 申渝, 高旭, 时文歆. XDLVO理论在膜污染解析中的应用研究[J]. 化工学报, 2021, 72(3): 1230-1241.
TANG Heli, ZHANG Bing, HUANG Dongmei, SHEN Yu, GAO Xu, SHI Wenxin. Advances in membrane fouling analysis based on XDLVO theory[J]. CIESC Journal, 2021, 72(3): 1230-1241.
图1 2002年以来发表的基于XDLVO理论研究膜污染的文献数量(数据截止于2020年5月24日)
Fig.1 Numbers of publications on membrane fouling based on XDLVO theory since 2002 (data retrieved on May 24, 2020)
污染物-膜材料 | 前期阶段 | 后期阶段 | ||||||||
---|---|---|---|---|---|---|---|---|---|---|
ΔGLW/ (mJ·m-2) | ΔGAB/ (mJ·m-2) | ΔGEL/ (mJ·m-2) | ΔGTOT/ (mJ·m-2) | MFI×10-3 | ΔGLW/ (mJ·m-2) | ΔGAB/(mJ·m-2) | ΔGEL/(mJ·m-2) | ΔGTOT/(mJ·m-2) | MFI×10-3 | |
TiO2-PES | -5.79 | 24.52 | 0.21 | 18.94 | 3.58 | -11.45 | 25.16 | 0.24 | 13.95 | 1.78 |
(2 mg/L HA-TiO2)-PES | -5.81 | 23.75 | 0.21 | 18.15 | 8.23 | -11.52 | 24.31 | 0.25 | 13.04 | 3.48 |
(3 mg/L HA-TiO2)-PES | -5.70 | 22.35 | 0.17 | 16.82 | 11.7 | -11.10 | 21.76 | 0.30 | 10.96 | 3.67 |
(5 mg/L HA-TiO2)-PES | -5.62 | 22.06 | 0.03 | 16.47 | 20.7 | -10.80 | 21.20 | 0.39 | 10.79 | 4.91 |
(10 mg/L HA-TiO2)-PES | -5.61 | 20.13 | -0.02 | 14.50 | 27.6 | -10.75 | 17.32 | 0.41 | 6.98 | 5.86 |
MFI(×10-3)-ΔGTOT线性拟合 | y = -5.49x + 107.6, R2 = 0.93 | y = -0.53x + 9.8, R2 = 0.84 | ||||||||
TiO2-PVDF | -7.02 | -13.14 | 0.05 | 20.11 | 3.53 | -11.45 | 25.16 | 0.24 | 13.95 | 2.37 |
(2 mg/L HA-TiO2) -PVDF | -7.04 | -16.89 | 0.05 | -23.90 | 8.78 | -11.52 | 24.31 | 0.25 | 13.04 | 6.29 |
(3 mg/L HA-TiO2)-PVDF | -6.92 | -19.36 | 0.03 | -26.37 | 12.0 | -11.10 | 21.76 | 0.30 | 10.96 | 6.79 |
(5 mg/L HA-TiO2)-PVDF | -6.82 | -20.29 | -0.09 | -27.47 | 21.2 | -10.80 | 21.20 | 0.39 | 10.79 | 9.51 |
(10 mg/L HA-TiO2)-PVDF | -6.80 | -23.30 | -0.36 | -30.54 | 19.0 | -10.75 | 17.32 | 0.41 | 6.98 | 10.8 |
MFI×10-3 -ΔGTOT线性拟合 | y = 1.68x - 30.3, R2 = 0.82 | y = -1.07x + 19.1, R2 = 0.78 |
表1 膜分离过程中HA-TiO2与膜之间的接触界面自由能及其与MFI的相关关系[32]
Table 1 Adhesion interfacial free energies in different phases of membrane filtration with HA-TiO2 and the correlativity of ΔGTOT and membrane fouling index[32]
污染物-膜材料 | 前期阶段 | 后期阶段 | ||||||||
---|---|---|---|---|---|---|---|---|---|---|
ΔGLW/ (mJ·m-2) | ΔGAB/ (mJ·m-2) | ΔGEL/ (mJ·m-2) | ΔGTOT/ (mJ·m-2) | MFI×10-3 | ΔGLW/ (mJ·m-2) | ΔGAB/(mJ·m-2) | ΔGEL/(mJ·m-2) | ΔGTOT/(mJ·m-2) | MFI×10-3 | |
TiO2-PES | -5.79 | 24.52 | 0.21 | 18.94 | 3.58 | -11.45 | 25.16 | 0.24 | 13.95 | 1.78 |
(2 mg/L HA-TiO2)-PES | -5.81 | 23.75 | 0.21 | 18.15 | 8.23 | -11.52 | 24.31 | 0.25 | 13.04 | 3.48 |
(3 mg/L HA-TiO2)-PES | -5.70 | 22.35 | 0.17 | 16.82 | 11.7 | -11.10 | 21.76 | 0.30 | 10.96 | 3.67 |
(5 mg/L HA-TiO2)-PES | -5.62 | 22.06 | 0.03 | 16.47 | 20.7 | -10.80 | 21.20 | 0.39 | 10.79 | 4.91 |
(10 mg/L HA-TiO2)-PES | -5.61 | 20.13 | -0.02 | 14.50 | 27.6 | -10.75 | 17.32 | 0.41 | 6.98 | 5.86 |
MFI(×10-3)-ΔGTOT线性拟合 | y = -5.49x + 107.6, R2 = 0.93 | y = -0.53x + 9.8, R2 = 0.84 | ||||||||
TiO2-PVDF | -7.02 | -13.14 | 0.05 | 20.11 | 3.53 | -11.45 | 25.16 | 0.24 | 13.95 | 2.37 |
(2 mg/L HA-TiO2) -PVDF | -7.04 | -16.89 | 0.05 | -23.90 | 8.78 | -11.52 | 24.31 | 0.25 | 13.04 | 6.29 |
(3 mg/L HA-TiO2)-PVDF | -6.92 | -19.36 | 0.03 | -26.37 | 12.0 | -11.10 | 21.76 | 0.30 | 10.96 | 6.79 |
(5 mg/L HA-TiO2)-PVDF | -6.82 | -20.29 | -0.09 | -27.47 | 21.2 | -10.80 | 21.20 | 0.39 | 10.79 | 9.51 |
(10 mg/L HA-TiO2)-PVDF | -6.80 | -23.30 | -0.36 | -30.54 | 19.0 | -10.75 | 17.32 | 0.41 | 6.98 | 10.8 |
MFI×10-3 -ΔGTOT线性拟合 | y = 1.68x - 30.3, R2 = 0.82 | y = -1.07x + 19.1, R2 = 0.78 |
污染物-膜材料 | 前期阶段 | 后期阶段 | 文献 | ||||||
---|---|---|---|---|---|---|---|---|---|
ΔGLW/(mJ·m-2) | ΔGAB/ (mJ·m-2) | ΔGEL/(mJ·m-2) | ΔGTOT/ (mJ·m-2) | ΔGLW/(mJ·m-2) | ΔGAB/ (mJ·m-2) | ΔGEL/(mJ·m-2) | ΔGTOT/ (mJ·m-2) | ||
polystyrene-Al2O3 | -3.45 | -32.54 | 1.16×10-6 | -35.99 | -6.56 | -80.82 | 2.55×10-6 | -87.38 | [ |
glass-Al2O3 | -2.16 | 5.55 | 6.27×10-7 | 23.39 | -2.58 | 44.37 | 8.72×10-6 | 41.78 | [ |
SiO2-PAN | -4.66 | -0.589 | 5.67×10-10 | -5.25 | -2.81 | 9.39 | 5.87×10-10 | 6.58 | [ |
TiO2-PES | -5.79 | 24.52 | 0.21 | 18.94 | -11.45 | 25.16 | 0.24 | 13.95 | [ |
TiO2-PVDF | -7.02 | -13.14 | 0.05 | 20.11 | -11.45 | 25.16 | 0.24 | 13.95 | [ |
SA-PVDF | 1.83 | -19.65 | -0.10 | -17.82 | -3.34 | 12.09 | 0.27 | 8.74 | [ |
SA-PES | -3.38 | 17.12 | -0.04 | 13.75 | -3.34 | 12.09 | 0.27 | 8.74 | [ |
BSA-PVDF | 2.03 | -9.31 | 0.08 | -7.21 | -4.13 | 17.60 | 0.09 | 13.56 | [ |
BSA-PES | -4.20 | 21.14 | -0.52 | 16.43 | -4.13 | 17.60 | 0.09 | 13.56 | [ |
HA-PVDF① | 33.17 | 620.21 | 49.47 | 702.85 | -27.35 | 1717.42 | 3.30 | 1693.37 | [ |
HA-PES① | -56.14 | 2512.99 | 101.38 | 2558.23 | -27.35 | 1717.42 | 3.30 | 1693.37 | [ |
(HA+BSA)-PES① | -31.62 | 221.98 | 51.71 | 241.78 | -20.37 | -162.22 | 5.70 | -176.85 | [ |
(SiO2-NOM)-PES① | -97.98 | -362.55 | 87.70 | -372.83 | -42.15 | -141.38 | 5.81 | -177.72 | [ |
污泥絮体-PVDF | -3.80 | -20.44 | 0.16 | -24.08 | -7.47 | -28.56 | 0.12 | -35.92 | [ |
HPO-混合纤维素 | -4.69 | -51.35 | -0.65 | -56.69 | -3.45 | -72.35 | 0.02 | -75.78 | [ |
TPI-混合纤维素 | -5.53 | -38.45 | -0.53 | 44.51 | -4.79 | -39.98 | 0.02 | -44.75 | [ |
C-HPI-混合纤维素 | -3.70 | 32.63 | -0.33 | 28.60 | -2.15 | 35.56 | 0.04 | 33.45 | [ |
N-HPI-混合纤维素 | -4.34 | -47.95 | -0.80 | -53.10 | -2.96 | -60.04 | 0.01 | -62.99 | [ |
酱油-PVDF(0.45②) | -7.64 | 15.72 | -4.83×10-6 | 8.07 | -5.70 | 25.27 | 4.72×10-10 | 19.87 | [ |
酱油-PES(0.45②) | -0.44 | -1.27 | -8.72×10-7 | -1.71 | -5.70 | 25.27 | 4.72×10-10 | 19.87 | [ |
表2 膜分离过程中不同污染物与膜之间的接触界面自由能
Table 2 Adhesion interfacial free energies in different phases of membrane filtration with different foulants
污染物-膜材料 | 前期阶段 | 后期阶段 | 文献 | ||||||
---|---|---|---|---|---|---|---|---|---|
ΔGLW/(mJ·m-2) | ΔGAB/ (mJ·m-2) | ΔGEL/(mJ·m-2) | ΔGTOT/ (mJ·m-2) | ΔGLW/(mJ·m-2) | ΔGAB/ (mJ·m-2) | ΔGEL/(mJ·m-2) | ΔGTOT/ (mJ·m-2) | ||
polystyrene-Al2O3 | -3.45 | -32.54 | 1.16×10-6 | -35.99 | -6.56 | -80.82 | 2.55×10-6 | -87.38 | [ |
glass-Al2O3 | -2.16 | 5.55 | 6.27×10-7 | 23.39 | -2.58 | 44.37 | 8.72×10-6 | 41.78 | [ |
SiO2-PAN | -4.66 | -0.589 | 5.67×10-10 | -5.25 | -2.81 | 9.39 | 5.87×10-10 | 6.58 | [ |
TiO2-PES | -5.79 | 24.52 | 0.21 | 18.94 | -11.45 | 25.16 | 0.24 | 13.95 | [ |
TiO2-PVDF | -7.02 | -13.14 | 0.05 | 20.11 | -11.45 | 25.16 | 0.24 | 13.95 | [ |
SA-PVDF | 1.83 | -19.65 | -0.10 | -17.82 | -3.34 | 12.09 | 0.27 | 8.74 | [ |
SA-PES | -3.38 | 17.12 | -0.04 | 13.75 | -3.34 | 12.09 | 0.27 | 8.74 | [ |
BSA-PVDF | 2.03 | -9.31 | 0.08 | -7.21 | -4.13 | 17.60 | 0.09 | 13.56 | [ |
BSA-PES | -4.20 | 21.14 | -0.52 | 16.43 | -4.13 | 17.60 | 0.09 | 13.56 | [ |
HA-PVDF① | 33.17 | 620.21 | 49.47 | 702.85 | -27.35 | 1717.42 | 3.30 | 1693.37 | [ |
HA-PES① | -56.14 | 2512.99 | 101.38 | 2558.23 | -27.35 | 1717.42 | 3.30 | 1693.37 | [ |
(HA+BSA)-PES① | -31.62 | 221.98 | 51.71 | 241.78 | -20.37 | -162.22 | 5.70 | -176.85 | [ |
(SiO2-NOM)-PES① | -97.98 | -362.55 | 87.70 | -372.83 | -42.15 | -141.38 | 5.81 | -177.72 | [ |
污泥絮体-PVDF | -3.80 | -20.44 | 0.16 | -24.08 | -7.47 | -28.56 | 0.12 | -35.92 | [ |
HPO-混合纤维素 | -4.69 | -51.35 | -0.65 | -56.69 | -3.45 | -72.35 | 0.02 | -75.78 | [ |
TPI-混合纤维素 | -5.53 | -38.45 | -0.53 | 44.51 | -4.79 | -39.98 | 0.02 | -44.75 | [ |
C-HPI-混合纤维素 | -3.70 | 32.63 | -0.33 | 28.60 | -2.15 | 35.56 | 0.04 | 33.45 | [ |
N-HPI-混合纤维素 | -4.34 | -47.95 | -0.80 | -53.10 | -2.96 | -60.04 | 0.01 | -62.99 | [ |
酱油-PVDF(0.45②) | -7.64 | 15.72 | -4.83×10-6 | 8.07 | -5.70 | 25.27 | 4.72×10-10 | 19.87 | [ |
酱油-PES(0.45②) | -0.44 | -1.27 | -8.72×10-7 | -1.71 | -5.70 | 25.27 | 4.72×10-10 | 19.87 | [ |
膜材料名称 | γ- /(mJ·m–2) | ζ /mV | ΔG121 /(mJ·m-2) | 文献 | |||
---|---|---|---|---|---|---|---|
改性膜 | 基膜 | 改性膜 | 基膜 | 改性膜 | 基膜 | ||
PVDF/PES/PVA | 27.58 | 13.91 | -25.0 | -29.35 | 0.51 | -28.32 | [ |
PVDF-HEA | 30.13 | 10.48 | -30.83 | -20.95 | 5.24 | -36.92 | [ |
PES-PVP | 4.23 | 0.47 | — | — | -47.13 | -77.49 | [ |
PES-PVP-GO | 13.39 | 0.47 | — | — | -21.08 | -77.49 | [ |
PAN-PAMAM-ETA/NAOH | 52.70 | 7.67 | — | — | 22.55 | -6.14 | [ |
PVDF@ZnO (100 cycles) | 12.4 | 0.6 | -20.7 | -13.7 | — | — | [ |
PVDF@ZnO (200 cycles) | 46.3 | 0.6 | -27.8 | -13.7 | — | — | [ |
PA/Fe@PVDF-OH | 42.34 | 14.65 | -24.24 | -18.40 | — | — | [ |
PVDF@(TiO2/PSS)7 | 19.6 | 0.53 | -39.4 | -20.3 | — | — | [ |
PES-Ni@TiO2 | 44.188 | 7.098 | -35.74 | -33.8 | — | — | [ |
PANI-DBSA | 48.7 | 19.6 | -55.0 | -40.3 | — | — | [ |
PVDF-GO-Ni | 63.04 | 22.59 | -5.95 | -13.38 | — | — | [ |
表3 改性膜的关键性能参数
Table 3 The key properties of modified membranes
膜材料名称 | γ- /(mJ·m–2) | ζ /mV | ΔG121 /(mJ·m-2) | 文献 | |||
---|---|---|---|---|---|---|---|
改性膜 | 基膜 | 改性膜 | 基膜 | 改性膜 | 基膜 | ||
PVDF/PES/PVA | 27.58 | 13.91 | -25.0 | -29.35 | 0.51 | -28.32 | [ |
PVDF-HEA | 30.13 | 10.48 | -30.83 | -20.95 | 5.24 | -36.92 | [ |
PES-PVP | 4.23 | 0.47 | — | — | -47.13 | -77.49 | [ |
PES-PVP-GO | 13.39 | 0.47 | — | — | -21.08 | -77.49 | [ |
PAN-PAMAM-ETA/NAOH | 52.70 | 7.67 | — | — | 22.55 | -6.14 | [ |
PVDF@ZnO (100 cycles) | 12.4 | 0.6 | -20.7 | -13.7 | — | — | [ |
PVDF@ZnO (200 cycles) | 46.3 | 0.6 | -27.8 | -13.7 | — | — | [ |
PA/Fe@PVDF-OH | 42.34 | 14.65 | -24.24 | -18.40 | — | — | [ |
PVDF@(TiO2/PSS)7 | 19.6 | 0.53 | -39.4 | -20.3 | — | — | [ |
PES-Ni@TiO2 | 44.188 | 7.098 | -35.74 | -33.8 | — | — | [ |
PANI-DBSA | 48.7 | 19.6 | -55.0 | -40.3 | — | — | [ |
PVDF-GO-Ni | 63.04 | 22.59 | -5.95 | -13.38 | — | — | [ |
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