Bicontinuous porous membranes with micro-nano composite structure using a facile atomization-assisted nonsolvent induced phase separation method

doi:10.1007/s11705-022-2143-5

Front. Chem. Sci. Eng.

2022, Vol. 16

Issue (8) : 1268-1280 https://doi.org/10.1007/s11705-022-2143-5

RESEARCH ARTICLE

Bicontinuous porous membranes with micro-nano composite structure using a facile atomization-assisted nonsolvent induced phase separation method

Jing Wang^1,², Guoyuan Pan², Yu Li^1,², Yang Zhang², Hongwei Shi², Xuanbo Liu², Hao Yu², Muhua Zhao², Yiqun Liu^1,²(

), Changjiang Wu^1,²(

)

¹. College of Materials Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China
². SINOPEC Beijing Research Institute of Chemical Industry, Beijing 100013, China

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Abstract

The micro-nano composite structure can endow separation membranes with special surface properties, but it often has the problems of inefficient preparation process and poor structural stability. In this work, a novel atomization-assisted nonsolvent induced phase separation method, which is also highly efficient and very simple, has been developed. By using this method, a bicontinuous porous microfiltration membrane with robust micro-nano composite structure was obtained via commercially available polymers of polyacrylonitrile and polyvinylpyrrolidone. The formation mechanism of the micro-nano composite structure was proposed. The microphase separation of polyacrylonitrile and polyvinylpyrrolidone components during the atomization pretreatment process and the hydrogen bonding between polyacrylonitrile and polyvinylpyrrolidone molecules should have resulted in the nano-protrusions on the membrane skeleton. The membrane exhibits superhydrophilicity in air and superoleophobicity underwater. The membrane can separate both surfactant-free and surfactant-stabilized oil-in-water emulsions with high separation efficiency and permeation flux. With excellent antifouling property and robust microstructure, the membrane can easily be recycled for long-term separation. Furthermore, the scale-up verification from laboratory preparation to continuous production has been achieved. The simple, efficient, cost-effective preparation method and excellent membrane properties indicate the great potential of the developed membranes in practical applications.

Keywords atomization nonsolvent induced phase separation bicontinuous porous structure micro-nano composite structure oil-water separation

Corresponding Author(s): Yiqun Liu,Changjiang Wu

Online First Date: 10 January 2022 Issue Date: 02 August 2022

Cite this article:

Jing Wang,Guoyuan Pan,Yu Li, et al. Bicontinuous porous membranes with micro-nano composite structure using a facile atomization-assisted nonsolvent induced phase separation method[J]. Front. Chem. Sci. Eng., 2022, 16(8): 1268-1280.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-022-2143-5
https://academic.hep.com.cn/fcse/EN/Y2022/V16/I8/1268

Fig.1 Illustration for the fabrication process of bicontinuous porous membrane by AA-NIPS method.

Fig.2 SEM images of (a) cross-section and (b) top surface of the representative membrane (PAN/PVP-30s) at different magnifications.

Fig.3 (a) SEM image of pure PAN membrane prepared by using AA-NIPS method. (b) SEM images of membrane obtained by VIPS plus NIPS method. (c) SEM images of the PAN/PVP membranes with different exposure time in water mist (I: 0 s; II: 10 s; III: 20 s; IV: 30 s; V: 40 s; VI: 50 s). (d) AFM height image and modulus image of PAN/PVP film prepared by spin coating (DMT: Derjaguin–Müller–Toporov). (e) (I) and (II) AFM height images of PAN/PVP-30s membrane at different magnifications; (III) and (IV) AFM modulus and adhesion images of B.

Fig.4 (a) Photographs of water droplet (stained with methylene blue) and oil droplet (1,2-dichloroethane stained with Sudan red II) spreading on the PAN/PVP-30s membrane in air. The inset is a digital photograph showing the 1,2-dichloroethane droplet on the membrane underwater. (b) Photographs of dynamic measurements of water spreading (top) and underwater oil-adhesion (bottom) on the membrane. Fouling experiments of PAN/PVP-30s membrane with (c) dichloroethane and (d) hexane. Crude oil fouling experiments of glass beakers coated with (e) and without (f) PAN/PVP anti-oil-adhesion layer.

Fig.5 (a) Variation of water CA and underwater oil CA of the membrane with different atomization pretreatment time (The inset images are the corresponding SEM image. Scale bar: 0.5 µm); (b) variation of volume porosity values of the membrane functional layer.

Fig.6 (a) Permeation flux and (b) the corresponding TOC values of the filtrates for various oil-in-water emulsions at a transmembrane pressure of 10 kPa; (c) digital photograph showing the filtration set-up of oil-in-water emulsion separation in cross-flow mode; (d) cycling separation performance of the membrane for SDS/diesel/H₂O emulsion and the corresponding TOC values of the filtrates.

Fig.7 SEM images of the PAN/PVP-30s membrane after (a) soaking in deionized water for one month and (b) ultrasonic treatment in DMF aqueous solution (DMF/water= 1/1, volume ratio) for 30 min. The inset is the image of the underwater oil droplet on the corresponding membrane.

Fig.8 Illustration for the continuous fabrication of bicontinuous porous structure membrane by AA-NIPS method.

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