硅藻土原位生长Nb_2O_5纳米棒及表面Cr(Ⅵ)吸附转化行为研究
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摘要
以活化铌酸为铌源,草酸铵为沉积剂,十二烷基苯磺酸钠为模板剂,采用水热法在硅藻土表面原位生长Nb_2O_5纳米棒。采用SEM、TEM、XRD、BET、FT-IR和XPS等分析方法对样品进行表征,反应14 h后,Nb_2O_5纳米棒长度为500~700 nm,直径为25~35 nm;硅藻土原位生长Nb_2O_5纳米棒样品比表面积为157 m~2/g。研究了样品对Cr(Ⅵ)的吸附与光还原行为,可见光条件下对Cr(Ⅵ)吸附量可达220 mg/g;紫外光条件下,可将表面吸附的Cr(Ⅵ)转变为Cr(Ⅲ),样品经过5次循环使用后,对Cr(Ⅵ)(100 mg/L)降解率仍能保持在93%左右。样品可对重金属污染废水中Cr(Ⅵ)进行吸附与毒性降解一体化去除。
Nb_2O_5 nanorods decorated diatomite were synthesized via a hydrothermal method by using niobic acid,ammonium oxalate and sodium dodecyl benzene sulfonate(SDBS).The as-prepared samples were characterized by SEM,TEM,XRD,BET,and FT-IR techniques.The Nb_2O_5 nanorod was obtained with length of 500~700 nm and diameter of 25~35 nm.BET test showed that specific surface area of Nb_2O_5 nanorods decorated diatomite reached 157 m~2/g which show a high adsorbance tendence.Under visible light irradiation,the adsorption capacity for Cr(Ⅵ) could be 220 mg/g.With the assistance of UV-light photoreduction,the maximum removal capacity for Cr(Ⅵ) could be 340 mg/g,and the absorbed Cr(Ⅵ) was transformed to Cr(Ⅲ).After photodegradation for five times,the degradation rate of Cr(Ⅵ)(100 mg/L) were still at about 93%.Nb_2O_5 nanorods/diatomite could adsorb Cr(Ⅵ) from sewage effectively and in the meantime accomplish the toxicity degradation,showing a promising treatment of Cr(Ⅵ) containing waste water.
Nb_2O_5 nanorods decorated diatomite were synthesized via a hydrothermal method by using niobic acid,ammonium oxalate and sodium dodecyl benzene sulfonate(SDBS).The as-prepared samples were characterized by SEM,TEM,XRD,BET,and FT-IR techniques.The Nb_2O_5 nanorod was obtained with length of 500~700 nm and diameter of 25~35 nm.BET test showed that specific surface area of Nb_2O_5 nanorods decorated diatomite reached 157 m~2/g which show a high adsorbance tendence.Under visible light irradiation,the adsorption capacity for Cr(Ⅵ) could be 220 mg/g.With the assistance of UV-light photoreduction,the maximum removal capacity for Cr(Ⅵ) could be 340 mg/g,and the absorbed Cr(Ⅵ) was transformed to Cr(Ⅲ).After photodegradation for five times,the degradation rate of Cr(Ⅵ)(100 mg/L) were still at about 93%.Nb_2O_5 nanorods/diatomite could adsorb Cr(Ⅵ) from sewage effectively and in the meantime accomplish the toxicity degradation,showing a promising treatment of Cr(Ⅵ) containing waste water.
引文
[1]METIN G,DUYGU V,AYSE M.Removal of trivalent chromium from water using low-cost natural diatomite.J.Hazard.Mater.,2008,160(2/3):318–323.
[2]JIANG BO,XIN SHUAI-SHUAI,GAO LI,et al.Dramatically enhanced aerobic Cr(VI)reduction with scrap zero-valent aluminum induced by oxalate.Chemical Engineering Journal,2016,308:588–596.
[3]HANS R,SENANAYAKE G,DHARMASIRI L C S,et al.A preliminary batch study of sorption kinetics of Cr(VI)ions from aqueous solutions by a magnetic ion exchange(MIEX?;)resin and determination of film/pore diffusivity.Hydrometallurgy,2016,164:208–218.
[4]FU XIAO-FEI,YANG HAN-PEI,LU GUANG-HUA,et al.Improved performance of surface functionalized Ti O2/activated carbon for adsorption-photocatalytic reduction of Cr(VI)in aqueous solution.Materials Science in Semiconductor Processing,2015,39:362–370.
[5]DINDA D,KUMAR S S.Sulfuric acid doped poly diaminopyridine/graphene composite to remove high concentration of toxic Cr(VI).Journal of Hazardous Materials,2015,291:93–101.
[6]GUAN XIAO-HONG,DU JUAN-SHAN,MENG XIAO-GUANG,et al.Application of titanium dioxide in arsenic removal from water:a review.Journal of Hazardous Materials,2012,215–216(10):1–16.
[7]LI HUI,LI WEI,ZHANG YAN-JUN,et al.Chrysanthemum-like a-Fe OOH microspheres produced by a simple green method and their outstanding ability in heavy metal ion removal.J.Mater.Chem.,2011,21:7878–7881.
[8]MISHRA S,BHARAGAVA R N.Toxic and genotoxic effects of hexavalent chromium in environment and its bioremediation strategies.Journal of Environmental Science&Health Part C Environmental Carcinogenesis&Ecotoxicology Reviews,2016,34(1):1–32.
[9]YAO HUA,GUO LAN,JIANG BING-HUA,et al.Oxidative stress and chromium(VI)carcinogenesis.Journal of Environmental Pathology Toxicology&Oncology Official Organ of the International Society for Environmental Toxicology&Cancer,2008,27(2):77–88.
[10]WISE S S,HOLMES A L,SR J P W.Particulate and soluble hexavalent chromium are cytotoxic and genotoxic to human lung epithelial cells.Mutation Research/genetic Toxicology&Environmental Mutagenesis,2006,610(1/2):2–7.
[11]MYROSLAV SPRYNSKYY.The separation of uranium ions by natural and modified diatomite from aqueous solution.Hazard.Mater.,2010,181:700–707.
[12]LI CONG-JU,LI YONG-JIAN,WANG JIAO-NA,et al.PA6@FexOy nanofibrous membrane preparation and its strong Cr(VI)-removal performance.Chemical Engineering Journal,2013,220:294–301.
[13]LOPES O F,PARIS E C,RIBERIRO C.Synthesis of Nb2O5,nanoparticles through the oxidant peroxide method applied to organic pollutant photodegradation:a mechanistic study.Applied Catalysis B Environmental,2014,144(2):800–808.
[14]ZHAO YUN,ELEY CLIVE,HU JING-PING,et al.Shape-dependent acidity and photocatalytic activity of Nb2O5 nanocrystals with an active TT(001)surface.Angew.Chem.Int.Ed.,2012,51(16):3846–3849.
[15]GAO BAO-JIAO,JIANG PENG-FEI,AN FU-QIANG,et al.Studies on the surface modification of diatomite with polyethyleneimine and trapping effect of the modified diatomite for phenol.Applied Surface Science,2005,250(1–4):273–279.
[16]ONOZATO T,KATASE T,YAMAMOTO A,et al.Optoelectronic properties of valence-state-controlled amorphous niobium oxide.Journal of Physics Condensed Matter An Institute of Physics Journal,2016,28(25):1–8.
[17]HUO QI-SHENG,MARGOLESE DAVID I,CIESLA U LRIKE,et al.Organization of organic molecules with inorganic molecular species into nanocomposite biphase arrays.Chemistry of Materials,1994,6(8):1176–1191.
[18]YAN CHENG-LIN,XUE DONG-FENG.Formation of Nb2O5nanotube arrays through phase transformation.Advanced Materials,2010,20(5):1055–1058.
[19]DU YU-CHENG,YAN JING,MENG QI,et al.Fabrication and excellent conductive performance of antimony-doped tin oxidecoated diatomite with porous structure.Materials Chemistry&Physics,2012,133(2/3):907–912.
[20]SHENG GUO-DONG,WANG SUO-WEI,HU JUN,et al.Adsorption of Pb(II)on diatomite as affected via aqueous solution chemistry and temperature.Colloids and Surfaces A:Physicochemical and Engineering Aspects,2009,339(1/2/3):159–166.
[21]KHRAISHEH M A,AL-GHOUTI M A,ALLEN S J,et al.Effect of OH and silanol groups in the removal of dyes from aqueous solution using diatomite.Water Research,2005,39(5):922–932.
[22]HADJAR H,HAMDI B,JABER M,et al.Elaboration and characterization of new mesoporous materials from diatomite and charcoal.Microporous and Mesoporous Materials,2007,107(3):219–226.
[23]CHENG YUE-HONG,JIANG HENG,GONG HONG,et al.Synthesis and characterization of niobic acid.Industrial Catalysis,2011,19(1):50–52.
[24]JULIEN C M,MASSOT M.Spectroscopic studies of the structural transitions in positive electrodes for lithium batteries.Physical Chemistry Chemical Physics,2002,4(17):4226–4235.
[2]JIANG BO,XIN SHUAI-SHUAI,GAO LI,et al.Dramatically enhanced aerobic Cr(VI)reduction with scrap zero-valent aluminum induced by oxalate.Chemical Engineering Journal,2016,308:588–596.
[3]HANS R,SENANAYAKE G,DHARMASIRI L C S,et al.A preliminary batch study of sorption kinetics of Cr(VI)ions from aqueous solutions by a magnetic ion exchange(MIEX?;)resin and determination of film/pore diffusivity.Hydrometallurgy,2016,164:208–218.
[4]FU XIAO-FEI,YANG HAN-PEI,LU GUANG-HUA,et al.Improved performance of surface functionalized Ti O2/activated carbon for adsorption-photocatalytic reduction of Cr(VI)in aqueous solution.Materials Science in Semiconductor Processing,2015,39:362–370.
[5]DINDA D,KUMAR S S.Sulfuric acid doped poly diaminopyridine/graphene composite to remove high concentration of toxic Cr(VI).Journal of Hazardous Materials,2015,291:93–101.
[6]GUAN XIAO-HONG,DU JUAN-SHAN,MENG XIAO-GUANG,et al.Application of titanium dioxide in arsenic removal from water:a review.Journal of Hazardous Materials,2012,215–216(10):1–16.
[7]LI HUI,LI WEI,ZHANG YAN-JUN,et al.Chrysanthemum-like a-Fe OOH microspheres produced by a simple green method and their outstanding ability in heavy metal ion removal.J.Mater.Chem.,2011,21:7878–7881.
[8]MISHRA S,BHARAGAVA R N.Toxic and genotoxic effects of hexavalent chromium in environment and its bioremediation strategies.Journal of Environmental Science&Health Part C Environmental Carcinogenesis&Ecotoxicology Reviews,2016,34(1):1–32.
[9]YAO HUA,GUO LAN,JIANG BING-HUA,et al.Oxidative stress and chromium(VI)carcinogenesis.Journal of Environmental Pathology Toxicology&Oncology Official Organ of the International Society for Environmental Toxicology&Cancer,2008,27(2):77–88.
[10]WISE S S,HOLMES A L,SR J P W.Particulate and soluble hexavalent chromium are cytotoxic and genotoxic to human lung epithelial cells.Mutation Research/genetic Toxicology&Environmental Mutagenesis,2006,610(1/2):2–7.
[11]MYROSLAV SPRYNSKYY.The separation of uranium ions by natural and modified diatomite from aqueous solution.Hazard.Mater.,2010,181:700–707.
[12]LI CONG-JU,LI YONG-JIAN,WANG JIAO-NA,et al.PA6@FexOy nanofibrous membrane preparation and its strong Cr(VI)-removal performance.Chemical Engineering Journal,2013,220:294–301.
[13]LOPES O F,PARIS E C,RIBERIRO C.Synthesis of Nb2O5,nanoparticles through the oxidant peroxide method applied to organic pollutant photodegradation:a mechanistic study.Applied Catalysis B Environmental,2014,144(2):800–808.
[14]ZHAO YUN,ELEY CLIVE,HU JING-PING,et al.Shape-dependent acidity and photocatalytic activity of Nb2O5 nanocrystals with an active TT(001)surface.Angew.Chem.Int.Ed.,2012,51(16):3846–3849.
[15]GAO BAO-JIAO,JIANG PENG-FEI,AN FU-QIANG,et al.Studies on the surface modification of diatomite with polyethyleneimine and trapping effect of the modified diatomite for phenol.Applied Surface Science,2005,250(1–4):273–279.
[16]ONOZATO T,KATASE T,YAMAMOTO A,et al.Optoelectronic properties of valence-state-controlled amorphous niobium oxide.Journal of Physics Condensed Matter An Institute of Physics Journal,2016,28(25):1–8.
[17]HUO QI-SHENG,MARGOLESE DAVID I,CIESLA U LRIKE,et al.Organization of organic molecules with inorganic molecular species into nanocomposite biphase arrays.Chemistry of Materials,1994,6(8):1176–1191.
[18]YAN CHENG-LIN,XUE DONG-FENG.Formation of Nb2O5nanotube arrays through phase transformation.Advanced Materials,2010,20(5):1055–1058.
[19]DU YU-CHENG,YAN JING,MENG QI,et al.Fabrication and excellent conductive performance of antimony-doped tin oxidecoated diatomite with porous structure.Materials Chemistry&Physics,2012,133(2/3):907–912.
[20]SHENG GUO-DONG,WANG SUO-WEI,HU JUN,et al.Adsorption of Pb(II)on diatomite as affected via aqueous solution chemistry and temperature.Colloids and Surfaces A:Physicochemical and Engineering Aspects,2009,339(1/2/3):159–166.
[21]KHRAISHEH M A,AL-GHOUTI M A,ALLEN S J,et al.Effect of OH and silanol groups in the removal of dyes from aqueous solution using diatomite.Water Research,2005,39(5):922–932.
[22]HADJAR H,HAMDI B,JABER M,et al.Elaboration and characterization of new mesoporous materials from diatomite and charcoal.Microporous and Mesoporous Materials,2007,107(3):219–226.
[23]CHENG YUE-HONG,JIANG HENG,GONG HONG,et al.Synthesis and characterization of niobic acid.Industrial Catalysis,2011,19(1):50–52.
[24]JULIEN C M,MASSOT M.Spectroscopic studies of the structural transitions in positive electrodes for lithium batteries.Physical Chemistry Chemical Physics,2002,4(17):4226–4235.