Preparation of PVDF-PFTS/SiO2 membrane and its resistance mixed fouling performance

doi:10.16085/j.issn.1000-6613.2021-1238

Abstract

Abstract:

The PVDF-PFTS/SiO₂superhydrophobic composite membrane was prepared by surface grafting technology. The surface structure and the composition of the membrane before and after contamination were analyzed by scanning electron microscopy (SEM) and infrared spectroscopy (FTIR). The change of the effluent conductivity and membrane flux of the device in direct contact membrane distillation (DCMD) was investigated. The anti-mixed fouling performance and mechanism of the superhydrophobic PVDF-PFTS/SiO₂ superhydrophobic composite membrane were analyzed by XDLVO theory. The results showed that under the combined action of 1H, 1H, 2H, 2H-perfluorooctyltrichlorosilane (PFTS) and SiO₂, a micro-nano composite papillary structure was formed on the surface of the PVDF-PFTS/SiO₂ superhydrophobic composite membrane. The water contact angle (WCA) increased from 99° to 155°. Compared with the PVDF base membrane, the PVDF-PFTS/SiO₂ superhydrophobic composite membrane had a better anti-fouling performance against mixed pollutants. After 10h continuous operation, the membrane flux and rejection rate were maintained at 10.06kg/(m²·h) and 99.80%, respectively. The theoretical analysis of XDLVO showed that the transformation of the force between the surface of the PVDF-PFTS/SiO₂ superhydrophobic composite membrane and the pollutants from gravitational force to repulsive force was one of the main reasons for its enhanced anti-mixed fouling performance.

Key words: PVDF-PFTS/SiO₂ membrane, superhydrophobicity, membrane fouling, membrane preparation, composite material

摘要：

采用表面接枝技术制备了PVDF-PFTS/SiO₂超疏水复合膜，通过扫描电子显微镜（SEM）和红外光谱（FTIR）分析了膜污染前后的表面结构和组成，考察了直接接触式膜蒸馏（DCMD）装置出水电导率和膜通量的变化，利用XDLVO理论分析了PVDF-PFTS/SiO₂超疏水复合膜的抗混合污染性能和机理。结果表明：在1H, 1H, 2H, 2H-全氟辛基三氯硅烷（PFTS）和SiO₂共同作用下，PVDF-PFTS/SiO₂超疏水复合膜表面形成微纳米复合乳突结构，水接触角（WCA）由99°增至155°。与PVDF基膜相比，PVDF-PFTS/SiO₂超疏水复合膜对混合污染物具有较好的抗污染性能；连续运行10h，膜通量和截留率分别保持在10.06kg/(m²·h)和99.80%。XDLVO理论分析表明，PVDF-PFTS/SiO₂超疏水复合膜表面与污染物之间的作用力由引力转变为斥力是其抗混合污染性能增强的主要原因之一。

关键词: PVDF-PFTS/SiO₂膜, 超疏水性, 膜污染, 膜制备, 复合材料

CLC Number:

TQ028.8

LI Zheng, NIU Jingdong, HE Guangze, ZHANG Lanhe, ZHANG Haifeng. Preparation of PVDF-PFTS/SiO₂ membrane and its resistance mixed fouling performance[J]. Chemical Industry and Engineering Progress, 2022, 41(5): 2713-2721.

李正, 牛静东, 何广泽, 张兰河, 张海丰. PVDF-PFTS/SiO₂膜制备及抗混合污染性能[J]. 化工进展, 2022, 41(5): 2713-2721.

Figures/Tables 13

样品	元素含量/%
样品	C	N	F	O	Si	F/C
PVDF基膜	53.81	1.60	42.20	2.39	—	0.78
PVDF-PFTS/SiO₂	32.99	1.46	38.77	17.76	9.02	1.18

样品	膜厚/μm	最大孔径/nm	平均孔径/nm	水接触角/（°）	进水压力/kPa
PVDF基膜	100±1	652	543	99±1	204
PVDF-PFTS/SiO₂膜	101±1	664	561	153±2	235

液体	总表面张力γ/mN·m^-1	非极性表面张力γ^LW/mN·m^-1	电子供体表面张力γ^-/mN·m^-1	电子受体表面张力γ⁺/mN·m^-1
水	72.80	21.80	25.50	25.50
二碘甲烷	50.80	50.80	0.00	0.00
乙二醇	48.00	29.00	47.00	1.90

样品	接触角/（°）			非极性表面张力γ^LW /mN·m^-1	电子供体表面张力γ^-/mN·m^-1	电子受体表面张力γ⁺/mN·m^-1	极性表面张力γ^AB/mN·m^-1	总表面张力γ^TOT/mN·m^-1	zeta电位 /mV
样品	θ_w	θ_D	θ_E	非极性表面张力γ^LW /mN·m^-1	电子供体表面张力γ^-/mN·m^-1	电子受体表面张力γ⁺/mN·m^-1	极性表面张力γ^AB/mN·m^-1	总表面张力γ^TOT/mN·m^-1	zeta电位 /mV
PVDF基膜	98	65	71	22.401	3	0.102	1.106	23.507	-36.787
PVDF-PFTS/SiO₂膜	152	140	136	7.058	6.646	0.003	0.282	7.340	-40.130
BSA+CaCl₂	25	44	30	37.540	63.282	0.017	2.074	39.614	-11.581

膜材料	极性作用能ΔG $m l f A B$ /mJ·m^-2	范德华作用能ΔG $m l f L W$ /mJ·m^-2	静电作用能ΔG $m l f E L$ /mJ·m^-2	总作用能ΔG $m l f T O T$ /mJ·m^-2
PVDF基膜	-5.156	-0.186	2.59×10^-6	-5.342
PVDF-PFTS/SiO₂膜	4.704	5.868	3.55×10^-6	10.572

膜材料	极性作用能ΔG $m l f A B$ /mJ·m^-2	范德华作用能ΔG $m l f L W$ /mJ·m^-2	静电作用能ΔG $m l f E L$ /mJ·m^-2	总作用能ΔG $m l f T O T$ /mJ·m^-2
PVDF基膜	-5.156	-0.186	2.59×10^-6	-5.342
PVDF-PFTS/SiO₂膜	4.704	5.868	3.55×10^-6	10.572

References 38

1	KHAYET M. Membranes and theoretical modeling of membrane distillation: a review[J]. Advances in Colloid and Interface Science, 2011, 164(1/2): 56-88.
2	TIJING L D, WOO Y C, CHOI J S, et al. Fouling and its control in membrane distillation: a review[J]. Journal of Membrane Science, 2015, 475: 215-244.
3	XU W T, ZHAO Z P, LIU M, et al. Morphological and hydrophobic modifications of PVDF flat membrane with silane coupling agent grafting via plasma flow for VMD of ethanol-water mixture[J]. Journal of Membrane Science, 2015, 491: 110-120.
4	王凯, 王德武, 侯得印, 等. 自组装法制备PVDF-SiO₂/PVSQ超疏水复合膜及膜蒸馏抗污染性能[J]. 化工学报, 2019, 70(1): 298-308.
	WANG K, WANG D W, HOU D Y, et al. Fabrication of PVDF-SiO₂/PVSQ superhydrophobic compositemembrane via self-assembly with anti-fouling property for membrane distillation[J]. CIESC Journal, 2019, 70(1): 298-308.
5	REZAEI S, MANOUCHERI I, MORADIAN R, et al. One-step chemical vapor deposition and modification of silica nanoparticles at the lowest possible temperature and superhydrophobic surface fabrication[J]. Chemical Engineering Journal, 2014, 252: 11-16.
6	SONG X Y, ZHAI J, WANG Y L, et al. Self-assembly of amino-functionalized monolayers on silicon surfaces and preparation of superhydrophobic surfaces based on alkanoic acid dual layers and surface roughening[J]. Journal of Colloid and Interface Science, 2006, 298(1): 267-273.
7	KOH E, LEE Y T. Preparation of an omniphobic nanofiber membrane by the self-assembly of hydrophobic nanoparticles for membrane distillation[J]. Separation and Purification Technology, 2021, 259: 118134.
8	NGHIEM L D, CATH T. A scaling mitigation approach during direct contact membrane distillation[J]. Separation and Purification Technology, 2011, 80(2): 315-322.
9	WARSINGER D M, SWAMINATHAN J, GUILLEN-BURRIEZA E, et al. Scaling and fouling in membrane distillation for desalination applications: a review[J]. Desalination, 2015, 356: 294-313.
10	SHIRAZI S, LIN C J, CHEN D. Inorganic fouling of pressure-driven membrane processes: a critical review[J]. Desalination, 2010, 250(1): 236-248.
11	HOU D Y, ZHANG L J, ZHAO C W, et al. Ultrasonic irradiation control of silica fouling during membrane distillation process[J]. Desalination, 2016, 386: 48-57.
12	GRYTA M. Long-term performance of membrane distillation process[J]. Journal of Membrane Science, 2005, 265(1/2): 153-159.
13	HE F, SIRKAR K K, GILRON J. Studies on scaling of membranes in desalination by direct contact membrane distillation: CaCO₃ and mixed CaCO₃/CaSO₄ systems[J]. Chemical Engineering Science, 2009, 64(8): 1844-1859.
14	GRYTA M, TOMASZEWSKA M, GRZECHULSKA J, et al. Membrane distillation of NaCl solution containing natural organic matter[J]. Journal of Membrane Science, 2001, 181(2): 279-287.
15	谢松辰, 文剑平, 庞志广, 等. 膜蒸馏脱盐中膜污染与膜润湿的研究进展[J]. 化工进展, 2021, 40(7): 3942-3956.
	XIE S C, WEN J P, PANG Z G, et al. Research progress of membrane fouling and wetting in membrane distillation process for desalination[J]. Chemical Industry and Engineering Progress, 2021, 40(7): 3942-3956.
16	ZHANG J, SONG Z Y, LI B A, et al. Fabrication and characterization of superhydrophobic poly(vinylidene fluoride) membrane for direct contact membrane distillation[J]. Desalination, 2013, 324: 1-9.
17	HOU D Y, CHRISTIE K S S, WANG K, et al. Biomimetic superhydrophobic membrane for membrane distillation with robust wetting and fouling resistance[J]. Journal of Membrane Science, 2020, 599: 117708.
18	KHAN A A, KHAN I A, SIYAL M I, et al. Optimization of membrane modification using SiO₂ for robust anti-fouling performance with calcium-humic acid feed in membrane distillation[J]. Environmental Research, 2019, 170: 374-382.
19	SONG H, SHI Y F, FU C. Oil adsorption measurements during membrane filtration[J]. Journal of Membrane Science, 2003, 214(1): 93-99.
20	SUN X H, KANANI D M, GHOSH R. Characterization and theoretical analysis of protein fouling of cellulose acetate membrane during constant flux dead-end microfiltration[J]. Journal of Membrane Science, 2008, 320(1/2): 372-380.
21	DENG B, YU M, YANG X X, et al. Antifouling microfiltration membranes prepared from acrylic acid or methacrylic acid grafted poly(vinylidene fluoride) powder synthesized via pre-irradiation induced graft polymerization[J]. Journal of Membrane Science, 2010, 350(1/2): 252-258.
22	FRANKEN A C M, NOLTEN J A M, MULDER M H V, et al. Wetting criteria for the applicability of membrane distillation[J]. Journal of Membrane Science, 1987, 33(3): 315-328.
23	MO H J, TAY K G, NG H Y. Fouling of reverse osmosis membrane by protein (BSA): effects of pH, calcium, magnesium, ionic strength and temperature[J]. Journal of Membrane Science, 2008, 315(1/2): 28-35.
24	HAMZAH N, LEO C P. Fouling prevention in the membrane distillation of phenolic-rich solution using superhydrophobic PVDF membrane incorporated with TiO₂ nanoparticles[J]. Separation and Purification Technology, 2016, 167: 79-87.
25	NAMVAR-MAHBOUB M, PAKIZEH M. Development of a novel thin film composite membrane by interfacial polymerization on polyetherimide/modified SiO₂ support for organic solvent nanofiltration[J]. Separation and Purification Technology, 2013, 119: 35-45.
26	ZHAO Y Y, LI F Y, CARVAJAL M T, et al. Interactions between bovine serum albumin and alginate: an evaluation of alginate as protein carrier[J]. Journal of Colloid and Interface Science, 2009, 332(2): 345-353.
27	LIU C, CHEN L, ZHU L. Fouling mechanism of hydrophobic polytetrafluoroethylene (PTFE) membrane by differently charged organics during direct contact membrane distillation (DCMD) process: an especial interest in the feed properties[J]. Journal of Membrane Science, 2018, 548: 125-135.
28	WANG Q Y, GUO Y F, WANG Z W, et al. Effects of graphene derivatives on polyvinylidene fluoride membrane modification evaluated with XDLVO theory and quartz crystal microbalance with dissipation[J]. Water Environment Research, 2021, 93(3): 360-369.
29	BRANT J A, CHILDRESS A E. Assessing short-range membrane-colloid interactions using surface energetics[J]. Journal of Membrane Science, 2002, 203(1/2): 257-273.
30	寇朝卫, 张干伟, 沈舒苏, 等. 基于XDLVO理论分析物理化学相互作用对纳滤膜有机污染影响[J]. 水处理技术, 2017, 43(8): 32-39.
	KOU C W, ZHANG G W, SHEN S S, et al. Effect of physical and chemical interaction on organic fouling of nanofiltration membrane based on XDLVO theory analysis[J]. Technology of Water Treatment, 2017, 43(8): 32-39.
31	刘永明, 施建宇, 鹿芹芹, 等. 基于杨氏方程的固体表面能计算研究进展[J]. 材料导报, 2013, 27(11): 123-129.
	LIU Y M, SHI J Y, LU Q Q, et al. Research progress on calculation of solid surface tension based on Young’s equation[J]. Materials Review, 2013, 27(11): 123-129.
32	MENG X R, TANG W T, WANG L, et al. Mechanism analysis of membrane fouling behavior by humic acid using atomic force microscopy: effect of solution pH and hydrophilicity of PVDF ultrafiltration membrane interface[J]. Journal of Membrane Science, 2015, 487: 180-188.
33	SUBRAMANI A, HOEK E M V. Direct observation of initial microbial deposition onto reverse osmosis and nanofiltration membranes[J]. Journal of Membrane Science, 2008, 319(1/2): 111-125.
34	BOUCHARD C R, JOLICOEUR J, KOUADIO P, et al. Study of humic acid adsorption on nanofiltration membranes by contact angle measurements[J]. The Canadian Journal of Chemical Engineering, 1997, 75(2): 339-345.
35	WANG X D, ZHOU M, MENG X R, et al. Effect of protein on PVDF ultrafiltration membrane fouling behavior under different pH conditions: interface adhesion force and XDLVO theory analysis[J]. Frontiers of Environmental Science and Engineering, 2016, 10(4): 1-11.
36	WANG H, NEWBY B M Z. Applicability of the extended Derjaguin–Landau–Verwey–Overbeek theory on the adsorption of bovine serum albumin on solid surfaces[J]. Biointerphases, 2014, 9(4): 041006.
37	ZUO G Z, WANG R. Novel membrane surface modification to enhance anti-oil fouling property for membrane distillation application[J]. Journal of Membrane Science, 2013, 447: 26-35.
38	ZHAO Y Q, YU W M, LI R J, et al. Electric field endowing the conductive polyvinylidene fluoride (PVDF)-graphene oxide (GO)-nickel (Ni) membrane with high-efficient performance for dye wastewater treatment[J]. Applied Surface Science, 2019, 483: 1006-1016.

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Preparation of PVDF-PFTS/SiO₂ membrane and its resistance mixed fouling performance

PVDF-PFTS/SiO₂膜制备及抗混合污染性能

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