介孔石墨相氮化碳载银聚醚砜膜制备及性能研究
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摘要
膜污染一直是膜分离应用中的主要问题。将不同量的介孔石墨相氮化碳载银(m-g-C_3N_4/Ag)以共混法引入铸膜液中,通过相转化法制备聚醚砜(PES)纳米复合膜,系统研究了m-g-C_3N_4/Ag的添加对纳米复合膜形貌、过滤、抗菌、光催化和抗污染性能的影响。结果表明, m-g-C_3N_4/Ag的添加可以改善纳米复合膜的断面结构及表面亲水性。与纯PES膜相比,纳米复合膜纯水通量随着掺杂量的增加显著提高,各个样品对蛋白质的截留率均在90%以上,表明m-g-C_3N_4/Ag的添加在不影响截留性能的前提下,可以显著提高纳米复合膜的过滤性能。纳米复合膜的抗菌性能随着m-g-C_3N_4/Ag含量的增加而提高,其中对铜绿假单胞菌的抗菌效果明显高于大肠杆菌。纯PES膜在光照下几乎不发生光降解。相比之下,所有添加m-g-C_3N_4/Ag的纳米复合膜在可见光照射下均呈现良好的光催化性能,且光催化活性随着m-g-C_3N_4/Ag的增加而逐渐增强。其中m-g-C_3N_4/Ag添加量最高的纳米复合膜显示出最明显的光催化作用,在120 min内甲基橙的脱色率可达63%。通过四步过滤实验对所有膜的综合抗污染性能进行表征,可知所有纳米复合膜通量恢复率均显著高于纯PES膜。水洗和可见光照射后所有膜的膜通量恢复率皆进一步提高。综上所述,添加m-g-C_3N_4/Ag可以显著提高聚醚砜膜的抗菌性、可见光下光催化降解染料性能,进而改善其综合抗污染性能。
Membrane fouling is still the major problem for the application of membrane separation. In this study,different amounts of silver doped mesoporous graphitic carbon nitride(m-g-C_3N_4/Ag) were introduced into casting solution by blending. The polyethersulfone(PES) nanocomposite membrane was prepared via the phase-inversion method. The impacts of m-g-C_3N_4/Ag addition on the morphology, filtration, antibacterial, photocatalytic, and antifouling properties of nanocomposite membrane were systematically studied. The results showed that the addition of m-g-C_3N_4/Ag can improve the cross-section structure of the nanocomposite membrane as well as its surface hydrophilicity. Compared with pure PES membrane, the pure water flux of the modified nanocomposite membrane increased significantly with the increase of doping amount. The protein rejection rates of all samples were over 90%, indicating that the addition of m-g-C_3N_4/Ag can significantly improve the filtration performance of the nanocomposite membrane without sacrificing the rejection performance. The anti-bacterial activity of the nanocomposite membranes was improved with the increase of m-g-C_3N_4/Ag content in which the anti-bacterial activity to P. aeruginosa was much more significant than that to E. coli. The pure PES membrane almost had not photodegradation under light irradiation. By contrast, all nanocomposite membranes exhibited good photocatalytic properties under visible light irradiation, and the photocatalytic activity improved with increase of m-g-C_3N_4/Ag. The nanocomposite membrane in which the m-g-C_3N_4/Ag content was the highest that showed the optimal photocatalysis, and the decolorization rate of methyl orange reached 63% in 120 min. The comprehensive antifouling performances of all membranes were characterized by four-step filtration experiments. It can be seen that the flux recovery ratio(FRR) of all nanocomposite membranes is much higher than that of PES membrane. The FRR of all membranes was further increased after washing with water and irradiating with visible light. In summary, the addition of m-g-C_3N_4/Ag can endow the PES membrane with the antibacterial and the photocatalytic properties under visible light irradiation, thereby improving its comprehensive antifouling performance.
Membrane fouling is still the major problem for the application of membrane separation. In this study,different amounts of silver doped mesoporous graphitic carbon nitride(m-g-C_3N_4/Ag) were introduced into casting solution by blending. The polyethersulfone(PES) nanocomposite membrane was prepared via the phase-inversion method. The impacts of m-g-C_3N_4/Ag addition on the morphology, filtration, antibacterial, photocatalytic, and antifouling properties of nanocomposite membrane were systematically studied. The results showed that the addition of m-g-C_3N_4/Ag can improve the cross-section structure of the nanocomposite membrane as well as its surface hydrophilicity. Compared with pure PES membrane, the pure water flux of the modified nanocomposite membrane increased significantly with the increase of doping amount. The protein rejection rates of all samples were over 90%, indicating that the addition of m-g-C_3N_4/Ag can significantly improve the filtration performance of the nanocomposite membrane without sacrificing the rejection performance. The anti-bacterial activity of the nanocomposite membranes was improved with the increase of m-g-C_3N_4/Ag content in which the anti-bacterial activity to P. aeruginosa was much more significant than that to E. coli. The pure PES membrane almost had not photodegradation under light irradiation. By contrast, all nanocomposite membranes exhibited good photocatalytic properties under visible light irradiation, and the photocatalytic activity improved with increase of m-g-C_3N_4/Ag. The nanocomposite membrane in which the m-g-C_3N_4/Ag content was the highest that showed the optimal photocatalysis, and the decolorization rate of methyl orange reached 63% in 120 min. The comprehensive antifouling performances of all membranes were characterized by four-step filtration experiments. It can be seen that the flux recovery ratio(FRR) of all nanocomposite membranes is much higher than that of PES membrane. The FRR of all membranes was further increased after washing with water and irradiating with visible light. In summary, the addition of m-g-C_3N_4/Ag can endow the PES membrane with the antibacterial and the photocatalytic properties under visible light irradiation, thereby improving its comprehensive antifouling performance.
引文
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[15]NGUYEN ANH,ZOU LIN-DA,PRIEST CRAIGN.Evaluating the antifouling effects of silver nanoparticles regenerated by TiO2on forward osmosis membrane.Journal of Membrane Science,2014,454(6):264-271.
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[23]LIU SHA-SHA,ZHANG MAN-YING,FANG FANG,et al.Biogenic silver nanocomposite TFC nanofiltration membrane with antifouling properties.Desalination&Water Treatment,2016,57(23):1-12.
[24]ZHANG MAN-YING,ZHANG KAI-SONG,DE GUSSEMEBART,et al.Biogenic silver nanoparticles(bio-Ag0)decrease biofouling of bio-Ag0/PES nanocomposite membranes.Water Research,2012,46(7):2077-2087.
[25]XU ZHI-WEI,WU TENG-FEI,SHI JIE,et al.Photocatalytic antifouling PVDF ultrafiltration membranes based on synergy of graphene oxide and TiO2 for water treatment.Journal of Membrane Science,2016,520:281-293.
[26]MéRICQ J P,MENDRET J,BROSILLON S,et al.High performance PVDF-TiO2 membranes for water treatment.Chemical Engineering Science,2015,123:283-291.
[27]JIN WEN-JIE,HU CHAO-WU,LI LI-HUA,et al,Effect of graphene oxide concentration on morphologies and properties of polysulfone ultrafiltration membranes.Membrane Science and Techology,2015,35:20-24.
[28]LI JIAN-HUA,YAN BANG-FENG,SHAO XI-SHENG,et al.Influence of Ag/TiO2 nanoparticle on the surface hydrophilicity and visible-light response activity of polyvinylidene fluoride membrane.Applied Surface Science,2015,324:82-89.
[29]ZHANG WEI,ZHOU LI,DENG HUI-PING.Ag modified g-C3N4composites with enhanced visible-light photocatalytic activity for diclofenac degradation.Journal of Molecular Catalysis A Chemical,2016,423:270-276.
[30]ZODROW KATHERINE,BRUNET LENA,MAHENDRASHAILY,et al.Polysulfone ultrafiltration membranes impregnated with silver nanoparticles show improved biofouling resistance and virus removal.Water Research,2009,43(3):715-723.
[31]ZHAO HUAN-XIN,CHEN SHUO,QUAN XIE,et al.Integration of microfiltration and visible-light-driven photocatalysis on g-C3N4nanosheet/reduced graphene oxide membrane for enhanced water treatment.Applied Catalysis B Environmental,2016,194:134-140.
[32]MOGHADAM MARYAM TAVAKOL,LESAGE GEOFFROY,MOHAMMADI TORAJ,et al.Improved antifouling properties of TiO2/PVDF nanocomposite membranes in UV-coupled ultrafiltration.Journal of Applied Polymer Science,2015,132(21):41731-41744.
[33]DAMODAR RAHUL A,YOU SHENG-JIE,CHOU HUI-HSIANG.Study the self cleaning,antibacterial and photocatalytic properties of TiO2 entrapped PVDF membranes.Journal of Hazardous Materials,2009,172(2/3):1321-1328.
[34]XU ZHI-WEI,ZHANG JI-GUO,SHAN MING-JING,et al.Organosilane-functionalized graphene oxide for enhanced antifouling and mechanical properties of polyvinylidene fluoride ultrafiltration membranes.Journal of Membrane Science,2014,458(10):1-13.
[35]LIN BO,XUE CHAO,YAN XIAO-QING,et al.Facile fabrication of novel SiO2/g-C3N4 core-shell nanosphere photocatalysts with enhanced visible light activity.Applied Surface Science,2015,357:346-355.
[2]GAO JIE,THONG ZHI-WEI,WANG KAI-YU,et al.Fabrication of loose inner-selective polyethersulfone(PES)hollow fibers by one-step spinning process for nanofiltration(NF)of textile dyes.Journal of Membrane Science,2017,541:413-424.
[3]KANG GUO-DONG,GAO CONG-JIE,CHEN WEI-DONG,et al.Study on hypochlorite degradation of aromatic polyamide reverse osmosis membrane.Journal of Membrane Science,2007,300(1):165-171.
[4]KIM JEONGHWAN,BRUGGEN VAN DER BART.The use of nanoparticles in polymeric and ceramic membrane structures:review of manufacturing procedures and performance improvement for water treatment.Environmental Pollution,2010,158(7):2335-2349.
[5]HUANG JIAN,WANG HUAN-TING,ZHANG KAI-SONG.Modification of PES membrane with Ag-SiO2:reduction of biofouling and improvement of filtration performance.Desalination,2014,336(1):8-17.
[6]SHI HENG,HE YI,PAN YANG,et al.A modified mussel-inspired method to fabricate TiO2 decorated superhydrophilic PVDF membrane for oil/water separation.Journal of Membrane Science,2016,506:60-70.
[7]LI PING,WU WEN-JIAN,LIU JIN-DUN,et al.Investigating the nanostructures and proton transfer properties of Nafion-GO hybrid membranes.Journal of Membrane Science,2018,555:327-336.
[8]KOSEOGLU-IMER DERYA Y,KOSE BORTE,ALTINBASMAHMUT,et al.The production of polysulfone(PS)membrane with silver nanoparticles(AgNP):physical properties,filtration performances,and biofouling resistances of membranes.Journal of Membrane Science,2013,428(12):620-628.
[9]WEN JIU-QING,XIE JUN,CHEN XIAO-BO,et al.A review on g-C3N4-based photocatalysts.Applied Surface Science,2016,391:72-123.
[10]MU?OZ-BATISTA MARIO J,FONTELLES-CARCELLEROLGA,FERRER MANUEL,et al.Disinfection capability of Ag/g-C3N4 composite photocatalysts under UV and visible light illumination.Applied Catalysis B Environmental,2016,183(1):86-95.
[11]XUE JIN-JUAN,MA SHUAI-SHUAI,ZHOU YUMING,et al.Facile photochemical synthesis of Au/Pt/g-C3N4 with plasmonenhanced photocatalytic activity for antibiotic degradation.ACSApplied Materials&Interfaces,2015,7(18):9630-9637.
[12]GONG YU-TONG,ZHANG PENG-FEI,XU XUAN,et al.A novel catalyst Pd@ompg-C3N4 for highly chemoselective hydrogenation of quinoline under mild conditions.Journal of Catalysis,2013,297(1):272-280.
[13]LI YI,LI YA-NAN,MA SHUANG-LONG,et al.Efficient water disinfection with Ag2WO4-doped mesoporous g-C3N4 under visible light.Journal of Hazardous Materials,2017,338:33-46.
[14]BASRI H,ISMAIL A F,AZIZ M.Polyethersulfone(PES)-silver composite UF membrane:effect of silver loading and PVP molecular weight on membrane morphology and antibacterial activity.Desalination,2011,273(1):72-80.
[15]NGUYEN ANH,ZOU LIN-DA,PRIEST CRAIGN.Evaluating the antifouling effects of silver nanoparticles regenerated by TiO2on forward osmosis membrane.Journal of Membrane Science,2014,454(6):264-271.
[16]HOSSEIN RAZZAGHI MOHAMMAD,SAFEKORDI ALIA-KBAR,TAVAKOLMOGHADAM MARYAM,et al.Morphological and separation performance study of PVDF/CA blend membranes.Journal of Membrane Science,2014,470:547-557.
[17]CAO XUE-LIAN,TANG MING,LIU FEI,et al.Immobilization of silver nanoparticles onto sulfonated polyethersulfone membranes as antibacterial materials.Colloids&Surfaces B Biointerfaces,2010,81(2):555-562.
[18]ZHU XIAO-YING,TANG LIN,WEE KIN-HO,et al.Immobilization of silver in polypropylene membrane for anti-biofouling performance.Biofouling,2011,27(7):773-786.
[19]IQBAL WAHEED,DONG CHUN-YANG,XING MINGYANG,et al.Eco-friendly one-pot synthesis of well-adorned mesoporous g-C3N4 with efficiently enhanced visible light photocatalytic activity.Catalysis Science&Technology,2017,7(8):1726-1734.
[20]MENG YA-LI,SHEN JU,CHEN DAN,et al.Photodegradation performance of methylene blue aqueous solution on Ag/g-C3N4catalyst.Rare Metals,2011,30(1):276-279.
[21]ZHANG MAN-YING,LIU ZI-YA,GAO YONG,et al.Ag modified g-C3N4 composite entrapped PES UF membrane with visiblelight-driven photocatalytic antifouling performance.RSC Advances,2017,7(68):42919-42928.
[22]ZHANG MAN-YING,FIELD ROBERT W,ZHANG KAI-SONG.Biogenic silver nanocomposite polyethersulfone UF membranes with antifouling properties.Journal of Membrane Science,2014,471(23):274-284.
[23]LIU SHA-SHA,ZHANG MAN-YING,FANG FANG,et al.Biogenic silver nanocomposite TFC nanofiltration membrane with antifouling properties.Desalination&Water Treatment,2016,57(23):1-12.
[24]ZHANG MAN-YING,ZHANG KAI-SONG,DE GUSSEMEBART,et al.Biogenic silver nanoparticles(bio-Ag0)decrease biofouling of bio-Ag0/PES nanocomposite membranes.Water Research,2012,46(7):2077-2087.
[25]XU ZHI-WEI,WU TENG-FEI,SHI JIE,et al.Photocatalytic antifouling PVDF ultrafiltration membranes based on synergy of graphene oxide and TiO2 for water treatment.Journal of Membrane Science,2016,520:281-293.
[26]MéRICQ J P,MENDRET J,BROSILLON S,et al.High performance PVDF-TiO2 membranes for water treatment.Chemical Engineering Science,2015,123:283-291.
[27]JIN WEN-JIE,HU CHAO-WU,LI LI-HUA,et al,Effect of graphene oxide concentration on morphologies and properties of polysulfone ultrafiltration membranes.Membrane Science and Techology,2015,35:20-24.
[28]LI JIAN-HUA,YAN BANG-FENG,SHAO XI-SHENG,et al.Influence of Ag/TiO2 nanoparticle on the surface hydrophilicity and visible-light response activity of polyvinylidene fluoride membrane.Applied Surface Science,2015,324:82-89.
[29]ZHANG WEI,ZHOU LI,DENG HUI-PING.Ag modified g-C3N4composites with enhanced visible-light photocatalytic activity for diclofenac degradation.Journal of Molecular Catalysis A Chemical,2016,423:270-276.
[30]ZODROW KATHERINE,BRUNET LENA,MAHENDRASHAILY,et al.Polysulfone ultrafiltration membranes impregnated with silver nanoparticles show improved biofouling resistance and virus removal.Water Research,2009,43(3):715-723.
[31]ZHAO HUAN-XIN,CHEN SHUO,QUAN XIE,et al.Integration of microfiltration and visible-light-driven photocatalysis on g-C3N4nanosheet/reduced graphene oxide membrane for enhanced water treatment.Applied Catalysis B Environmental,2016,194:134-140.
[32]MOGHADAM MARYAM TAVAKOL,LESAGE GEOFFROY,MOHAMMADI TORAJ,et al.Improved antifouling properties of TiO2/PVDF nanocomposite membranes in UV-coupled ultrafiltration.Journal of Applied Polymer Science,2015,132(21):41731-41744.
[33]DAMODAR RAHUL A,YOU SHENG-JIE,CHOU HUI-HSIANG.Study the self cleaning,antibacterial and photocatalytic properties of TiO2 entrapped PVDF membranes.Journal of Hazardous Materials,2009,172(2/3):1321-1328.
[34]XU ZHI-WEI,ZHANG JI-GUO,SHAN MING-JING,et al.Organosilane-functionalized graphene oxide for enhanced antifouling and mechanical properties of polyvinylidene fluoride ultrafiltration membranes.Journal of Membrane Science,2014,458(10):1-13.
[35]LIN BO,XUE CHAO,YAN XIAO-QING,et al.Facile fabrication of novel SiO2/g-C3N4 core-shell nanosphere photocatalysts with enhanced visible light activity.Applied Surface Science,2015,357:346-355.