还原氧化石墨烯/石墨相氮化碳复合膜的制备及其脱盐性能
|
摘要
采用真空抽滤法制备了以氧化石墨烯为基体的rGO/g-C_3N_4复合膜,系统研究了光催化还原时间、GO与g-C_3N_4质量比及GO沉积密度等工艺参数对复合膜脱盐性能的影响,优选出rGO/g-C_3N_4复合膜成膜工艺条件;并基于优选工艺所制备复合膜研究了NaCl溶液浓度对复合膜脱盐性能的影响,为复合膜的制备及应用提供实验依据。研究结果表明:紫外光照射时间为30h,GO与g-C_3N_4的质量比为6∶1,GO沉积密度为477.7mg·m~(-2)时制备的rGO/g-C_3N_4复合膜对NaCl溶液的脱盐性能最佳;复合膜对NaCl截留率和溶液通量均随NaCl溶液浓度降低而升高,对浓度为0.01mol·L~(-1)的NaCl溶液,截留率达到61.1%。
rGO/g-C_3N_4 byhrid membranes based on graphene oxide were prepared by the vacuum filtration in this work.The effects of photocatlytic reduction time,the mass ratio of GO to g-C_3N_4 and the deposition density of GO on the desalination performance of the hybrid membranes were studied and the optimized conditions of preparing rGO/g-C_3N_4 membranes were confirmed.Based on the hybrid membranes prepared under the optimized conditions,the effect of NaCl concentration on the desalination performance of the hybrid membranes was investigated.This work provides experimental clues for the preparation and application of the hybrid membranes.The result indicates that NaCl desalination performance of rGO/gC_3N_4 hybrid membrane is the best when the UV irradiation time is 30 h,mass ratio of GO tog-C_3N_4 is 6∶1,GO deposition density is 477.7 mg·m~(-2).The rejection of NaCl and flux both decrease with the increase of the NaCl concentration and the rejection of NaCl(0.01 mol·L~(-1))reaches 61.1%.
rGO/g-C_3N_4 byhrid membranes based on graphene oxide were prepared by the vacuum filtration in this work.The effects of photocatlytic reduction time,the mass ratio of GO to g-C_3N_4 and the deposition density of GO on the desalination performance of the hybrid membranes were studied and the optimized conditions of preparing rGO/g-C_3N_4 membranes were confirmed.Based on the hybrid membranes prepared under the optimized conditions,the effect of NaCl concentration on the desalination performance of the hybrid membranes was investigated.This work provides experimental clues for the preparation and application of the hybrid membranes.The result indicates that NaCl desalination performance of rGO/gC_3N_4 hybrid membrane is the best when the UV irradiation time is 30 h,mass ratio of GO tog-C_3N_4 is 6∶1,GO deposition density is 477.7 mg·m~(-2).The rejection of NaCl and flux both decrease with the increase of the NaCl concentration and the rejection of NaCl(0.01 mol·L~(-1))reaches 61.1%.
引文
[1]SHANNON M A,BOHN P W,ELIMELECH M,et al.Science and technology for water purification in the coming decades[J].Nature,2008,452(7185):301-310.
[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]HUANG H B,YING Y L,PENG X S.Graphene oxide nanosheet:An emerging star material for novel separation membranes[J].Journal of Materials Chemistry A,2014,2(34):13772-13782.
[4]NAIR R R,WU H A,JAYARAM P N,et al.Unimpeded permeation of water through helium-leaktight graphene-based membranes[J].Science,2012,335(6067):442-444.
[5]JOSHI R K,CARBONE P,WANG F C,et al.Precise and ultrafast molecular sieving throughgraphene oxide membranes[J].Science,2014,343(6172):752-754.
[6]HAN Y,XU Z,GAO C.Ultrathin graphene nanofiltration membrane for water purification[J].Advanced Functional Materials,2013,23(29):3693-3700.
[7]YUAN Y Q,GAO X L,WEI Y,et al.Enhanced desalination performance of carboxyl functionalized grapheme oxide nanofiltration membranes[J].Desalination,2017,405:29-39.
[8]HU M,MI B X.Enabling graphene oxide nanosheets as water separation membranes[J].Environmental Science&Technology,2013,47(8):3715-3723.
[9]MARCANO D C,KOSYNKIN D V,BERLIN J M,et al.Improved synthesis of graphene oxide[J].ACS Nano,2010,4(8):4806-4814.
[10]XIAO J D,XIE Y B,NAWAZ F.Dramatic coupling of visible light with ozone on honeycomb-likeporous g-C3N4towards superior oxidation of water pollutants[J].Applied Catalysis B:Environmental,2016,183:417-425.
[11]邵桂林.氧化石墨烯的制备与表征[D].上海:东华大学,2012.SHAO Guilin.The Preparation and Characterization of Graphene Oxide[D].Shanghai:Donghua University,2012.
[12]DU X R,ZOU G J,WANG Z G,et al.A scalable chemical route to soluble acidified graphitic carbon nitride:An ideal precursor for isolated ultrathin g-C3N4nanosheets[J].Nanoscale,2015,7(19):8701-8706.
[13]XU C,CHEN Z X,FU X Z.Graphene oxide-mediated formation of freestanding thickness controllable metal oxide films[J].Journal of Materials Chemistry,2011,21(34):12889-12893.
[14]LIU H Y,WANG H T,ZHANG X W.Facile fabrication of freestanding ultrathin reduced graphene oxide membranes for water purification[J].Advanced Materials,2015,27(2):249-254.
[15]HU M,ZHENG S X,MI B X.Organic fouling of graphene oxide membranes and its implications for membrane fouling control in engineered osmosis[J].Environmental Science&Technology,2016,50(2):685-693.
[16]HAN Y,JIANG Y Q,GAO C.High-flux graphene oxide nanofiltration membrane intercalated by carbon nanotubes[J].ACS Applied Materials&Interfaces,2015,7(15):8147-8155.
[17]WANG X L,TSURU T,NAKAO S I,et al.The electrostaticand steric-hindrance model for the transport of charged solutes through nanofiltration membranes[J].Journal of Membrane Science,1997,135(1):19-32.
[18]南倩.氧化石墨烯复合膜的制备及其性能研究[D].北京:北京化工大学,2016.NAN Qian.The Study on the Preparation and Performance Grapheme Oxide Based Composite Membrane[D].Beijing:Beijing University of Chemical Technology,2016.
[19]魏怡.自组装氧化石墨烯纳滤膜制备及其脱盐性能研究[D].青岛:中国海洋大学,2015.WEI Yi.Preparation of Self-assembly Graphene Oxide Nanofiltration Membrane and Study of Its Desalination Mechanism[D].Qingdao:Ocean University of China,2015.
[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]HUANG H B,YING Y L,PENG X S.Graphene oxide nanosheet:An emerging star material for novel separation membranes[J].Journal of Materials Chemistry A,2014,2(34):13772-13782.
[4]NAIR R R,WU H A,JAYARAM P N,et al.Unimpeded permeation of water through helium-leaktight graphene-based membranes[J].Science,2012,335(6067):442-444.
[5]JOSHI R K,CARBONE P,WANG F C,et al.Precise and ultrafast molecular sieving throughgraphene oxide membranes[J].Science,2014,343(6172):752-754.
[6]HAN Y,XU Z,GAO C.Ultrathin graphene nanofiltration membrane for water purification[J].Advanced Functional Materials,2013,23(29):3693-3700.
[7]YUAN Y Q,GAO X L,WEI Y,et al.Enhanced desalination performance of carboxyl functionalized grapheme oxide nanofiltration membranes[J].Desalination,2017,405:29-39.
[8]HU M,MI B X.Enabling graphene oxide nanosheets as water separation membranes[J].Environmental Science&Technology,2013,47(8):3715-3723.
[9]MARCANO D C,KOSYNKIN D V,BERLIN J M,et al.Improved synthesis of graphene oxide[J].ACS Nano,2010,4(8):4806-4814.
[10]XIAO J D,XIE Y B,NAWAZ F.Dramatic coupling of visible light with ozone on honeycomb-likeporous g-C3N4towards superior oxidation of water pollutants[J].Applied Catalysis B:Environmental,2016,183:417-425.
[11]邵桂林.氧化石墨烯的制备与表征[D].上海:东华大学,2012.SHAO Guilin.The Preparation and Characterization of Graphene Oxide[D].Shanghai:Donghua University,2012.
[12]DU X R,ZOU G J,WANG Z G,et al.A scalable chemical route to soluble acidified graphitic carbon nitride:An ideal precursor for isolated ultrathin g-C3N4nanosheets[J].Nanoscale,2015,7(19):8701-8706.
[13]XU C,CHEN Z X,FU X Z.Graphene oxide-mediated formation of freestanding thickness controllable metal oxide films[J].Journal of Materials Chemistry,2011,21(34):12889-12893.
[14]LIU H Y,WANG H T,ZHANG X W.Facile fabrication of freestanding ultrathin reduced graphene oxide membranes for water purification[J].Advanced Materials,2015,27(2):249-254.
[15]HU M,ZHENG S X,MI B X.Organic fouling of graphene oxide membranes and its implications for membrane fouling control in engineered osmosis[J].Environmental Science&Technology,2016,50(2):685-693.
[16]HAN Y,JIANG Y Q,GAO C.High-flux graphene oxide nanofiltration membrane intercalated by carbon nanotubes[J].ACS Applied Materials&Interfaces,2015,7(15):8147-8155.
[17]WANG X L,TSURU T,NAKAO S I,et al.The electrostaticand steric-hindrance model for the transport of charged solutes through nanofiltration membranes[J].Journal of Membrane Science,1997,135(1):19-32.
[18]南倩.氧化石墨烯复合膜的制备及其性能研究[D].北京:北京化工大学,2016.NAN Qian.The Study on the Preparation and Performance Grapheme Oxide Based Composite Membrane[D].Beijing:Beijing University of Chemical Technology,2016.
[19]魏怡.自组装氧化石墨烯纳滤膜制备及其脱盐性能研究[D].青岛:中国海洋大学,2015.WEI Yi.Preparation of Self-assembly Graphene Oxide Nanofiltration Membrane and Study of Its Desalination Mechanism[D].Qingdao:Ocean University of China,2015.