Layer-by-layer construction of graphene oxide (GO) framework composite membranes for highly efficient heavy metal removal

Abstract In this study, an ultrathin graphene oxide (GO) framework layer was successfully deposited on a modified Torlon ® hollow fiber support via a layer-by-layer (LbL) approach, enabling the composite membrane with superior nanofiltration (NF) performance. To molecularly design the GO framework, the substrate layer was firstly cross-linked with polyethylenimine (HPEI), followed by repeating the GO and ethylenediamine (EDA) deposition cycles and then an amine-enrichment modification by HPEI. The combination of the GO framework layer and the Torlon ® support can not only effectively seal the defects of the composite membrane with a narrow pore size distribution but also reduce the polymer consumption for the fabrication of traditional integrally skinned NF membranes. The GO/Torlon ® composite membrane has rejections higher than 95% towards Pb 2+ , Ni 2+ , and Zn 2+ with a superior water permeability of 4.7 L m −2  h −1  bar −1 . The membrane also exhibits excellent long-term performance stability during a 150-h NF test. Thus, the newly developed membrane has great potential for heavy metal removal. This study may provide useful insights on the fabrication of new generation 2-dimensional (2D) NF membranes.

[1]  M. Meireles,et al.  A contribution to the translation of retention curves into pore size distributions for sieving membranes , 1990 .

[2]  B. Freeman,et al.  Graphene oxide: a new platform for high-performance gas- and liquid-separation membranes. , 2014, Angewandte Chemie.

[3]  Shiguang Li,et al.  Ultrafiltration Membranes with Structure‐Optimized Graphene‐Oxide Coatings for Antifouling Oil/Water Separation , 2015 .

[4]  R. Mark Bricka,et al.  A review of potentially low-cost sorbents for heavy metals , 1999 .

[5]  Tai‐Shung Chung,et al.  Thin Film Interfacial Cross-Linking Approach To Fabricate a Chitosan Rejecting Layer over Poly(ether sulfone) Support for Heavy Metal Removal , 2015 .

[6]  Yulong Ying,et al.  Graphene oxide nanosheet: an emerging star material for novel separation membranes , 2014 .

[7]  D. R. Paul,et al.  Free-standing graphene oxide thin films assembled by a pressurized ultrafiltration method for dehydration of ethanol , 2014 .

[8]  H. Mahdavi,et al.  Polyurethane TFC nanofiltration membranes based on interfacial polymerization of poly(bis-MPA) and MDI on the polyethersulfone support , 2016 .

[9]  B. Bruggen,et al.  Modern applications in membrane science and technology , 2011 .

[10]  S. Stankovich,et al.  Preparation and characterization of graphene oxide paper , 2007, Nature.

[11]  Tai‐Shung Chung,et al.  Polyethyleneimine (PEI) cross-linked P84 nanofiltration (NF) hollow fiber membranes for Pb2+ removal , 2014 .

[12]  Rong Wang,et al.  Graphene oxide as effective selective barriers on a hollow fiber membrane for water treatment process , 2015 .

[13]  L. Shao,et al.  High flux polyethylene glycol based nanofiltration membranes for water environmental remediation , 2015 .

[14]  Baoxia Mi,et al.  Graphene Oxide Membranes for Ionic and Molecular Sieving , 2014, Science.

[15]  Chao Gao,et al.  Ultrathin Graphene Nanofiltration Membrane for Water Purification , 2013 .

[16]  T. Matsuura,et al.  MEMBRANE CHARACTERIZATION BY SOLUTE TRANSPORT AND ATOMIC FORCE MICROSCOPY , 1998 .

[17]  Ahmad Fauzi Ismail,et al.  Fabrication of polydopamine functionalized halloysite nanotube/polyetherimide membranes for heavy metal removal , 2016 .

[18]  Juin-Yih Lai,et al.  Evolution of polymeric hollow fibers as sustainable technologies: Past, present, and future , 2012 .

[19]  Kang Li,et al.  UV-Enhanced Sacrificial Layer Stabilised Graphene Oxide Hollow Fibre Membranes for Nanofiltration , 2015, Scientific Reports.

[20]  T. A. Hatton,et al.  Hyperbranched polyethyleneimine induced cross-linking of polyamide-imide nanofiltration hollow fiber membranes for effective removal of ciprofloxacin. , 2011, Environmental science & technology.

[21]  Xian-she Feng,et al.  Thin film composite membranes embedded with graphene oxide for water desalination , 2016 .

[22]  Wanqin Jin,et al.  Graphene-based membranes. , 2015, Chemical Society reviews.

[23]  B. Bruggen,et al.  Surface zwitterionic functionalized graphene oxide for a novel loose nanofiltration membrane , 2016 .

[24]  Andre K. Geim,et al.  The rise of graphene. , 2007, Nature materials.

[25]  Yu Zhang,et al.  Nanometric Graphene Oxide Framework Membranes with Enhanced Heavy Metal Removal via Nanofiltration. , 2015, Environmental science & technology.

[26]  R. Viola,et al.  A new technique to fabricate high-performance biologically inspired membranes for water treatment , 2015 .

[27]  P. Sukitpaneenit,et al.  High performance thin-film composite forward osmosis hollow fiber membranes with macrovoid-free and highly porous structure for sustainable water production. , 2012, Environmental science & technology.

[28]  Yu Zhang,et al.  Thin-film composite membranes with modified polyvinylidene fluoride substrate for ethanol dehydration via pervaporation , 2014 .

[29]  Juin-Yih Lai,et al.  Cross-Linking with Diamine Monomers To Prepare Composite Graphene Oxide-Framework Membranes with Varying d-Spacing , 2014 .

[30]  Shi‐Peng Sun,et al.  Green Modification of Outer Selective P84 Nanofiltration (NF) Hollow Fiber Membranes for Cadmium Removal , 2016 .

[31]  A. Mohammadian,et al.  Novel methodology for facile fabrication of nanofiltration membranes based on nucleophilic nature of polydopamine , 2016 .

[32]  Kang Li,et al.  Graphene oxide membranes on ceramic hollow fibers – Microstructural stability and nanofiltration performance , 2015 .

[33]  Juin-Yih Lai,et al.  Pressure-assisted self-assembly technique for fabricating composite membranes consisting of highly ordered selective laminate layers of amphiphilic graphene oxide , 2014 .

[34]  Eric M.V. Hoek,et al.  A review of water treatment membrane nanotechnologies , 2011 .

[35]  Zhanhu Guo,et al.  Nanofiltration membrane achieving dual resistance to fouling and chlorine for "green" separation of antibiotics , 2015 .

[36]  P. McIntyre,et al.  Global threats to human water security and river biodiversity , 2010, Nature.

[37]  Baoxia Mi,et al.  Enabling graphene oxide nanosheets as water separation membranes. , 2013, Environmental science & technology.

[38]  Christopher Bellona,et al.  Factors affecting the rejection of organic solutes during NF/RO treatment--a literature review. , 2004, Water research.

[39]  R. Ruoff,et al.  The chemistry of graphene oxide. , 2010, Chemical Society reviews.

[40]  E. R. Nightingale,et al.  PHENOMENOLOGICAL THEORY OF ION SOLVATION. EFFECTIVE RADII OF HYDRATED IONS , 1959 .

[41]  C Vandecasteele,et al.  Modelling of the retention of uncharged molecules with nanofiltration. , 2002, Water research.

[42]  Zhiping Xu,et al.  Ultrafast viscous water flow through nanostrand-channelled graphene oxide membranes , 2013, Nature Communications.