摘要
在本研究中,基于碳纳米管(Carbon nanotube, CNT)膜的优异的导电性和分离性能,通过二氧化钛(TiO_2)改性CNT材料,以期提升其渗透性和抗污染性;利用导电性的还原氧化石墨烯(Reducedgrapheneoxide,rGO)作为致密光滑且亲水的膜表面,以期提升复合膜的抗污染性。以真空抽滤的方法制备rGO-CNT/TiO_2复合膜并将其作为电极,将膜分离技术与电化学技术耦合,在电场强化辅助作用下,改善复合膜的抗污染性能。研究结果表明,在外加电场的辅助下,由于静电斥力和阴极膜原位产生具有强氧化性的过氧化氢(H_2O_2)的作用,rGO-CNT/TiO_2复合膜的抗污染性在错流过滤系统中也明显提升。随着负电压的降低而升高,在外加电压为-3 V时,分别提升了复合膜8.9%、15.0%、12.2%的抗污染性能。
In this study, based on the excellent conductivity and separation properties of carbon nanotube(CNT) membranes, CNT was modified by titanium dioxide(TiO_2) in order to improve its permeability and fouling resistance. Conductive reduced graphene oxide(rGO) was used as a smooth and hydrophilic membrane surface in order to improve the anti-fouling performance of the composite membrane. The rGO-CNT/TiO_2 composite membrane was prepared by vacuum suction filtration and used as an electrode. Through membrane separation technology coupled with the electrochemical technology, the anti-fouling performance of the composite membrane was improved by extra electric field. The results showed that the anti-fouling performance of rGO-CNT/TiO_2 composite membrane with extra electric field was also obviously improved in the cross-flow filtration system through the electrostatic repulsion and the in-situ generation of strong oxidizing H_2O_2, which increases with the decrease of the negative voltage. When the applied voltage was-3.0 V, the anti-fouling performance of the composite membranes were enhanced by 8.9 %, 15.0 % and 12.2 %, respectively.
引文
[1]Ying W,Siebdrath N,Uhl W,et al.New insights on early stages of ROmembranes fouling during tertiary wastewater desalination[J].JOURNAL OFMEMBRANE SCIENCE,2014,466:26-35.
[2]Pendergast M M,Hoek E M V.A review of water treatment membrane nanotechnologies[J].ENERGY&ENVIRONMENTAL SCIENCE,2011,4(6):1946-1971.
[3]Karabelas A J,Sioutopoulos D C.New insights into organic gel fouling of reverse osmosis desalination membranes[J].DESALINATION,2015,368(SI):114-126.
[4]Xu W,Zhao Z,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 MEMBRANESCIENCE,2015,491:110-120.
[5]Razmjou A,Mansouri J,Chen V,et al.Titania nanocomposite polyethersulfone ultrafiltration membranes fabricated using a low temperature hydrothermal coating process[J].JOURNAL OF MEMBRANE SCIENCE,2011,380(1-2):98-113.
[6]邵冰,柳丽芬,杨凤林.PVDF/PDA共混膜的制备及其性能研究[J].膜科学与技术,2014,34(01):57-61.
[7]Panizza M,Cerisola G.Direct And Mediated Anodic Oxidation of Organic Pollutants[J].CHEMICAL REVIEWS,2009,109(12):6541-6569.
[8]Martinez-Huitle C A,Brillas E.Electrochemical alternatives for drinking water disinfection[J].ANGEWANDTE CHEMIE-INTERNATIONALEDITION,2008,47(11):1998-2005.
[9]Gao G,Vecitis C D.Electrochemical Carbon Nanotube Filter Oxidative Performance as a Function of Surface Chemistry[J].ENVIRONMENTALSCIENCE&TECHNOLOGY,2011,45(22):9726-9734.
[10]Tettey K E,Yee M Q,Lee D.Photocatalytic and Conductive MWCNT/TiO2 Nanocomposite Thin Films[J].ACS APPLIED MATERIALS&INTERFACES,2010,2(9):2646-2652.
[11]程谦勋.氧化石墨烯改性双面正渗透膜的表征与抗污染研究[D].东华大学,2016.
[12]Zhang J,Yang H,Shen G,et al.Reduction of graphene oxide via L-ascorbic acid[J].CHEMICAL COMMUNICATIONS,2010,46(7):1112-1114.
[13]Wang S,Liang S,Liang P,et al.In-situ combined dual-layer CNT/PVDFmembrane for electrically-enhanced fouling resistance[J].JOURNAL OFMEMBRANE SCIENCE,2015,491:37-44.
[14]Liu Y,Xie J,Ong C N,et al.Electrochemical wastewater treatment with carbon nanotube filters coupled with in situ generated H2O2[J].ENVIRONMENTAL SCIENCE-WATER RESEARCH&TECHNOLOGY,2015,1(6):769-778.
[15]Ishigami T,Amano K,Fujii A,et al.Fouling reduction of reverse osmosis membrane by surface modification via layer-by-layer assembly[J].SEPARATION AND PURIFICATION TECHNOLOGY,2012,99:1-7.
[16]Takizawa Y,Inukai S,Araki T,et al.Antiorganic Fouling and Low-Protein Adhesion on Reverse-Osmosis Membranes Made of Carbon Nanotubes and Polyamide Nanocomposite[J].ACS APPLIED MATERIALS&INTERFACES,2017,9(37):32192-32201.