Layer-by-layer self-assembly TiO2 and graphene oxide on polyamide reverse osmosis membranes with improved membrane durability

Abstract Improving membrane durability associated with resistance to chlorine and biofouling is critical important for polyamide (PA) reverse osmosis (RO) membrane technology. Here, few-layered TiO2 nanoparticles and graphene oxide (GO) were layer-by-layer self-assembled onto flat PA reverse osmosis membrane surfaces by hydrogen bonding and physical absorption to address this challenge. Contact angle testing proved that the membrane surface hydrophilicity was improved with the increase of bilayers. The modified PA membrane with bilayer number ≤ 6 showed increased water flux. Moreover, XPS results indicated that TiO2 and GO were attached to the membrane surface with good stability in our experimental conditions, and that GO nanoparticles played a part in improving chlorine resistance due to absorbing chlorine radicals. All modified PA membranes showed an anti-fouling effect and had an inhibitory effect on rejection reduction exposed to chlorine solution. For instance, the water flux of pristine membranes varied from 20.3 l/m2 h to 7.5 l/m2 h while the bilayer6-coated membrane dropped from 23.6 to 17.9 l/m2 h after UV light exposure and incubating with microbial cells for 3 d. Meanwhile, for the chlorine resistance, compared with 60% salt rejection of unmodified membrane, the bilayer6-coated membrane was a more effective 75% after 20 h of chlorine exposure.

[1]  Andrew Mills,et al.  An overview of semiconductor photocatalysis , 1997 .

[2]  Vincent G. Gomes,et al.  Hybrid nanostructures based on titanium dioxide for enhanced photocatalysis , 2015 .

[3]  K. R. Reddy,et al.  Enhanced photocatalytic activity of nanostructured titanium dioxide/polyaniline hybrid photocatalysts , 2016 .

[4]  H. Matsuyama,et al.  Biofouling resistance of reverse osmosis membrane modified with polydopamine , 2014 .

[5]  Min Seok Kim,et al.  Analysis of Heavy Metal Toxic Ions by Adsorption onto Amino-functionalized Ordered Mesoporous Silica , 2007 .

[6]  Benny D. Freeman,et al.  Water Purification by Membranes: The Role of Polymer Science , 2010 .

[7]  J. Jegal,et al.  Preparation and characterization of polyamide reverse‐osmosis membranes with good chlorine tolerance , 2011 .

[8]  Yufeng Zhang,et al.  Surface coating on the polyamide TFC RO membrane for chlorine resistance and antifouling performance improvement , 2014 .

[9]  Cong-jie Gao,et al.  Study on hypochlorite degradation of aromatic polyamide reverse osmosis membrane , 2007 .

[10]  A. Gopalan,et al.  Synthesis of metal (Fe or Pd)/alloy (Fe–Pd)‐nanoparticles‐embedded multiwall carbon nanotube/sulfonated polyaniline composites by γ irradiation , 2006 .

[11]  Mahbub Hassan,et al.  Carbon functionalized TiO2 nanofibers for high efficiency photocatalysis , 2014 .

[12]  Jian Jin,et al.  SWCNT-intercalated GO ultrathin films for ultrafast separation of molecules , 2015 .

[13]  Yuan Hu,et al.  Preparation of functionalized graphene oxide/polypropylene nanocomposite with significantly improved thermal stability and studies on the crystallization behavior and mechanical properties , 2014 .

[14]  C. Stafford,et al.  Swelling of ultrathin crosslinked polyamide water desalination membranes , 2013 .

[15]  Z. Shen,et al.  Generic Synthesis of Carbon Nanotube Branches on Metal Oxide Arrays Exhibiting Stable High-Rate and Long-Cycle Sodium-Ion Storage. , 2016, Small.

[16]  E. Haque,et al.  Polymer brush synthesis on surface modified carbon nanotubes via in situ emulsion polymerization , 2016, Colloid and Polymer Science.

[17]  Young-Nam Kwon,et al.  Surface modification of seawater reverse osmosis (SWRO) membrane using methyl methacrylate-hydroxy poly(oxyethylene) methacrylate (MMA-HPOEM) comb-polymer and its performance , 2012 .

[18]  C. M. Patel,et al.  Preparation, characterization and application of GO-TiO2/PVC mixed matrix membranes for improvement in performance , 2017 .

[19]  Jong‐Chan Lee,et al.  High-performance reverse osmosis nanocomposite membranes containing the mixture of carbon nanotubes and graphene oxides , 2015 .

[20]  A. Fujishima,et al.  Facile fabrication and photocatalytic application of Ag nanoparticles-TiO2 nanofiber composites. , 2011, Journal of nanoscience and nanotechnology.

[21]  H. Cachet,et al.  Study by XPS of the chlorination of proteins aggregated onto tin dioxide during electrochemical production of hypochlorous acid , 2007 .

[22]  Jung-Hyun Lee,et al.  Layer-by-layer assembly of graphene oxide nanosheets on polyamide membranes for durable reverse-osmosis applications. , 2013, ACS applied materials & interfaces.

[23]  Youngil Lee,et al.  In situ self-organization of carbon black-polyaniline composites from nanospheres to nanorods: Synthesis, morphology, structure and electrical conductivity , 2009 .

[24]  W. Lu,et al.  Improved synthesis of graphene oxide. , 2010, ACS nano.

[25]  Sang Woo Han,et al.  Adsorption characteristics of 4-dimethylaminobenzoic acid on silver and titania: diffuse reflectance infrared Fourier transform spectroscopy study , 2000 .

[26]  Chuyang Y. Tang,et al.  Degradation of polyamide nanofiltration and reverse osmosis membranes by hypochlorite. , 2012, Environmental science & technology.

[27]  K. R. Reddy,et al.  Compatibility of Thermally Reduced Graphene with Polyesters , 2016 .

[28]  Tai Hyun Park,et al.  Design of TiO2 nanoparticle self-assembled aromatic polyamide thin-film-composite (TFC) membrane as an approach to solve biofouling problem , 2003 .

[29]  Karen K. Gleason,et al.  Surface-modified reverse osmosis membranes applying a copolymer film to reduce adhesion of bacteria as a strategy for biofouling control , 2014 .

[30]  J. Tascón,et al.  Graphene oxide dispersions in organic solvents. , 2008, Langmuir : the ACS journal of surfaces and colloids.

[31]  Raghava Reddy Kakarla,et al.  Advanced electrochemical energy storage supercapacitors based on the flexible carbon fiber fabric-coated with uniform coral-like MnO2 structured electrodes , 2017 .

[32]  I. Pinnau,et al.  Preparation and water desalination properties of POSS-polyamide nanocomposite reverse osmosis membranes , 2015 .

[33]  Jun Chen,et al.  Edge-enriched graphene quantum dots for enhanced photo-luminescence and supercapacitance. , 2014, Nanoscale.

[34]  Qian Zhang,et al.  Graphene oxide modified polyamide reverse osmosis membranes with enhanced chlorine resistance , 2017 .

[35]  Richard B. Kaner,et al.  Low-Fouling Antibacterial Reverse Osmosis Membranes via Surface Grafting of Graphene Oxide. , 2016, ACS applied materials & interfaces.

[36]  Y. Cohen,et al.  An Integrated approach for characterization of polyamide reverse osmosis membrane degradation due to exposure to free chlorine , 2016 .

[37]  Norman C. Billingham,et al.  Carbon nanotubes as polymer antioxidants , 2003 .

[38]  Youngil Lee,et al.  A new one-step synthesis method for coating multi-walled carbon nanotubes with cuprous oxide nanoparticles , 2008 .

[39]  B. Bruggen,et al.  Potential applications of abandoned aromatic polyamide reverse osmosis membrane by hypochlorite degradation , 2016 .

[40]  Greg Leslie,et al.  Assessing the oxidative degradation of polyamide reverse osmosis membrane—Accelerated ageing with hypochlorite exposure , 2010 .

[41]  Bin-bo Jiang,et al.  Influence of wall number and surface functionalization of carbon nanotubes on their antioxidant behavior in high density polyethylene , 2012 .

[42]  Menachem Elimelech,et al.  Thin-Film Composite Polyamide Membranes Functionalized with Biocidal Graphene Oxide Nanosheets , 2014 .