SCI和EI收录∣中国化工学会会刊

Chinese Journal of Chemical Engineering ›› 2023, Vol. 60 ›› Issue (8): 242-252.DOI: 10.1016/j.cjche.2023.02.022

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Tungsten incorporated mobil-type eleven zeolite membranes: Facile synthesis and tuneable wettability for highly efficient separation of oil/water mixtures

Hammad Saulat1, Jianhua Yang1,2, Tao Yan1, Waseem Raza3, Wensen Song1, Gaohong He1,2   

  1. 1. State Key Laboratory of Fine Chemicals, Institute of Adsorption and Inorganic Membrane, Dalian University of Technology, Dalian 116024, China;
    2. Panjin Institute of Industrial Technology, Dalian University of Technology, Panjin 124221, China;
    3. Institute of Advance Study, Shenzhen University, Shenzhen 518060, China
  • Received:2022-12-28 Revised:2023-02-28 Online:2023-10-28 Published:2023-08-28
  • Contact: Jianhua Yang,E-mail:yjianhua@dlut.edu.cn
  • Supported by:
    Financial support from the Science Fund for Creative Research Groups of the National Science Foundation of China (22021005), the National Natural Science Foundation of China (21776032), and the Innovation Team of Dalian University of Technology (DUT2017TB01) are greatly acknowledged.

Tungsten incorporated mobil-type eleven zeolite membranes: Facile synthesis and tuneable wettability for highly efficient separation of oil/water mixtures

Hammad Saulat1, Jianhua Yang1,2, Tao Yan1, Waseem Raza3, Wensen Song1, Gaohong He1,2   

  1. 1. State Key Laboratory of Fine Chemicals, Institute of Adsorption and Inorganic Membrane, Dalian University of Technology, Dalian 116024, China;
    2. Panjin Institute of Industrial Technology, Dalian University of Technology, Panjin 124221, China;
    3. Institute of Advance Study, Shenzhen University, Shenzhen 518060, China
  • 通讯作者: Jianhua Yang,E-mail:yjianhua@dlut.edu.cn
  • 基金资助:
    Financial support from the Science Fund for Creative Research Groups of the National Science Foundation of China (22021005), the National Natural Science Foundation of China (21776032), and the Innovation Team of Dalian University of Technology (DUT2017TB01) are greatly acknowledged.

Abstract: Tungsten (W) incorporated mobil-type eleven (MEL) zeolite membrane (referred to as W-MEL membrane) with high separation performance was firstly explored for the separation of oil/water mixtures under the influence of gravity. W-MEL membranes were grown on stainless steel (SS) meshes through in-situ hydrothermal growth method facilitated with (3-aminopropyl)triethoxysilane (APTES) modification of stainless steel meshes, which promote the heterogeneous nucleation and crystal growth of W-MEL zeolites onto the mesh surface. W-MEL membranes were grown on different mesh size supports to investigate the effect of mesh size on the separation performance of the membrane. The as-synthesized W-MEL membrane supported on 500 mesh (25 μm) (W-MEL-500) exhibit the hydrophilic nature with a water contact angle of 11.8° and delivers the best hexane/water mixture separation with a water flux and separation efficiency of 46247 L·m-2·h-1 and 99.5%, respectively. The wettability of W-MEL membranes was manipulated from hydrophilic to hydrophobic nature by chemically modifying with the fluorine-free compounds (hexadecyltrimethoxysilane (HDTMS) and dodecyltrimethoxysilane (DDTMS)) to achieve efficient oil-permselective separation of heavy oils from water. Among the hydrophobically modified W-MEL membranes, W-MEL-500-HDTMS having a water contact angle of 146.4° delivers the best separation performance for dichloromethane/water mixtures with a constant oil flux and separation efficiency of 61490 L·m-2·h-1 and 99.2%, respectively along with the stability tested up to 20 cycles. Both W-MEL-500-HDTMS and W-MEL-500-DDTMS membranes also exhibit similar separation performances for the separation of heavy oil from sea water along with a 20-fold lower corrosion rate in comparison with the bare stainless-steel mesh, indicating their excellent stability in seawater. Compared to the reported zeolite membranes for oil/water separation, the as-synthesized and hydrophobically modified W-MEL membranes shows competitive separation performances in terms of flux and separation efficiency, demonstrating the good potentiality for oil/water separation.

Key words: Corrosion, Dodecyltrimethoxysilane, Hexadecyltrimethoxysilane, Membranes, Oil/water separation, Zeolite

摘要: Tungsten (W) incorporated mobil-type eleven (MEL) zeolite membrane (referred to as W-MEL membrane) with high separation performance was firstly explored for the separation of oil/water mixtures under the influence of gravity. W-MEL membranes were grown on stainless steel (SS) meshes through in-situ hydrothermal growth method facilitated with (3-aminopropyl)triethoxysilane (APTES) modification of stainless steel meshes, which promote the heterogeneous nucleation and crystal growth of W-MEL zeolites onto the mesh surface. W-MEL membranes were grown on different mesh size supports to investigate the effect of mesh size on the separation performance of the membrane. The as-synthesized W-MEL membrane supported on 500 mesh (25 μm) (W-MEL-500) exhibit the hydrophilic nature with a water contact angle of 11.8° and delivers the best hexane/water mixture separation with a water flux and separation efficiency of 46247 L·m-2·h-1 and 99.5%, respectively. The wettability of W-MEL membranes was manipulated from hydrophilic to hydrophobic nature by chemically modifying with the fluorine-free compounds (hexadecyltrimethoxysilane (HDTMS) and dodecyltrimethoxysilane (DDTMS)) to achieve efficient oil-permselective separation of heavy oils from water. Among the hydrophobically modified W-MEL membranes, W-MEL-500-HDTMS having a water contact angle of 146.4° delivers the best separation performance for dichloromethane/water mixtures with a constant oil flux and separation efficiency of 61490 L·m-2·h-1 and 99.2%, respectively along with the stability tested up to 20 cycles. Both W-MEL-500-HDTMS and W-MEL-500-DDTMS membranes also exhibit similar separation performances for the separation of heavy oil from sea water along with a 20-fold lower corrosion rate in comparison with the bare stainless-steel mesh, indicating their excellent stability in seawater. Compared to the reported zeolite membranes for oil/water separation, the as-synthesized and hydrophobically modified W-MEL membranes shows competitive separation performances in terms of flux and separation efficiency, demonstrating the good potentiality for oil/water separation.

关键词: Corrosion, Dodecyltrimethoxysilane, Hexadecyltrimethoxysilane, Membranes, Oil/water separation, Zeolite