碳纳米管/羟基磷灰石复合材料对水体F~-的去除研究
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摘要
以碳纳米管(CNT)和羟基磷灰石(HAP)为原料,通过原位合成法制备碳纳米管/羟基磷灰石(CdH)复合材料.利用XRD、FTIR、SEM与氮气吸附~-脱附等表征其结构形貌,并通过静态吸附实验考察CdH对氟离子(F~-)的吸附性能.结果表明,室温下,CdH对F~-的吸附容量为11.05mg/g,明显高于HAP(5.02mg/g).吸附动力学模型、Weber~-Morris方程、Langmuir和Freundlich方程拟合结果表明, F~-在CdH表面进行Langmuir单分子层吸附,其吸附过程符合准二级动力学方程,并且颗粒内部扩散起主要作用.pH值为6时有利于CdH对F~-的去除.此外,结合反应前后固样XPS分析可知Cd H对F~-的吸附机制主要为离子交换作用.
To improve the removal efficiency of fluoride ion(F~-) in aqueous solution, Carbon nanotubes(CNT)~-doped hydroxyapatite(HAP) composites(CdH) were synthesized via in~-situ synthesis and characterized by XRD, FTIR, SEM and N2 adsorptiondesorption isotherms. The adsorption performance was investigated by static adsorption experiments and analyzed with adsorption kinetic models, Langmuir and Freundlich isotherm adsorption models, and Weber~-Morris equation. The optimal pH value for fluoride removal was 6. The adsorption capacity of CdH reached 11.05mg/g at room temperature, which was much higher than that of HAP(5.02mg/g). The results implied the occurrence of Langmuir monolayer adsorption once F~-contacted the surface of CdH. The adsorption kinetics fitted the pseudo~-second order model, and the internal diffusion of particles played the major role in the adsorption process. Moreover, the XPS results of CdHs before and after fluoride adsorption demonstrated that the mechanism of fluoride removal by CdH is mainly ion exchange.
To improve the removal efficiency of fluoride ion(F~-) in aqueous solution, Carbon nanotubes(CNT)~-doped hydroxyapatite(HAP) composites(CdH) were synthesized via in~-situ synthesis and characterized by XRD, FTIR, SEM and N2 adsorptiondesorption isotherms. The adsorption performance was investigated by static adsorption experiments and analyzed with adsorption kinetic models, Langmuir and Freundlich isotherm adsorption models, and Weber~-Morris equation. The optimal pH value for fluoride removal was 6. The adsorption capacity of CdH reached 11.05mg/g at room temperature, which was much higher than that of HAP(5.02mg/g). The results implied the occurrence of Langmuir monolayer adsorption once F~-contacted the surface of CdH. The adsorption kinetics fitted the pseudo~-second order model, and the internal diffusion of particles played the major role in the adsorption process. Moreover, the XPS results of CdHs before and after fluoride adsorption demonstrated that the mechanism of fluoride removal by CdH is mainly ion exchange.
引文
[1]Organization W H.Guidelines for drinking-water quality-fourth edition[J].World Health Organization,2011.
[2]Zhang L E,Huang D,Yang J,et al.Probabilistic risk assessment of Chinese residents'exposure to fluoride in improved drinking water in endemic fluorosis areas[J].Environmental Pollution,2017,222:118-125.
[3]Amini M,Mueller K,Abbaspour K C,et al.Statistical Modeling of Global Geogenic Fluoride Contamination in Groundwaters[J].Environmental Science&Technology,2008,42(10):3662-3668.
[4]Huang H,Liu J,Zhang P,et al.Investigation on the simultaneous removal of fluoride,ammonia nitrogen and phosphate from semiconductor wastewater using chemical precipitation[J].Chemical Engineering Journal,2016,307:696-706.
[5]Zhang J,Chen N,Li M,et al.Fluoride removal from aqueous solution by Zirconium-Chitosan/Graphene Oxide Membrane[J].Reactive&Functional Polymers,2017,114.
[6]Schaefer C E,Andaya C,Burant A,et al.Electrochemical treatment of perfluorooctanoic acid and perfluorooctane sulfonate:Insights into mechanisms and application to groundwater treatment[J].Chemical Engineering Journal,2017,317:424-432.
[7]Jamhour R M A Q.New inorganic ion-exchange material for the selective removal of fluoride from potable water using ion-selective electrode[J].American Journal of Environmental Sciences,2005,1(1).
[8]Lin K Y,Liu Y T,Chen S Y.Adsorption of fluoride to UiO-66-NH2in water:Stability,kinetic,isotherm and thermodynamic studies[J].Journal of Colloid&Interface Science,2016,461:79-87.
[9]胡家朋,吴代赦,肖丽盈,等.羟基磷灰石的制备及其对水中氟离子的吸附[J].环境工程学报,2015,9(4):1823-1830.Hu J P,Wu D S,Xiao L Y,et al.Fabrication of hydroxyapatite and its absorption property for fluorid ion[J].Chinese Journal of Environmental Engineering,2015,9(4):1823-1830.
[10]Jiménez-Reyes M,Solache-Ríos M.Sorption behavior of fluoride ions from aqueous solutions by hydroxyapatite[J].Journal of Hazardous Materials,2010,180(1-3):297-302.
[11]Prabhu S M,Meenakshi S.Synthesis of surface coated hydroxyapatite powders for fluoride removal from aqueous solution[J].Powder Technology,2014,268(1):306-315.
[12]Li J,Zhang S,Chen C,et al.Removal of Cu(II)and Fulvic Acid by Graphene Oxide Nanosheets Decorated with Fe3O4 Nanoparticles[J].ACS Applied Materials&Interfaces,2012,4(9):4991-5000.
[13]Li S,Gong Y,Yang Y,et al.Recyclable CNTs/Fe3O4,magnetic nanocomposites as adsorbents to remove bisphenol A from water and their regeneration[J].Chemical Engineering Journal,2015,260:231-239.
[14]黄志良,刘羽,王大伟,等.Sol-Gel法合成HAP的结晶特征及其对F~-离子吸附性能研究[J].无机材料学报,2001,16(4):661-666.Huang Z L,Liu Y,Wang D W,et al.Properties of crystallizing and absorbing F-ion of HAP synthesized by Sol-Gel process[J].Journal of Inorganic Materials,2001,16(4):661-666.
[15]Mohamed A,Osman T A,Toprak M S,et al.Visible light photocatalytic reduction of Cr(VI)by surface modified CNT/titanium dioxide composites nanofibers[J].Journal of Molecular Catalysis AChemical,2016,424:45-53.
[16]施周,杨文浩,杨灵芳,等.离子改性CNT/TiO2电极吸附去除水中苯酚的研究[J].中国环境科学,2015,35(9):2664-2669.Shi Z,Yang W h,Yang L F,et al.Electrosorption of phenol in aqueous solution using a plasma-activated CNT/TiO2 electrode[J].China Environmental Science,2015,35(9):2664-2669.
[17]Xu D,Li B,Wei C,et al.Preparation and Characterization of Mn O2/acid-treated CNT Nanocomposites for Energy Storage with Zinc Ions[J].Electrochimica Acta,2014,133(7):254-261.
[18]Begam H,Kundu B,Chanda A,et al.MG63osteoblast cell response on Zn doped hydroxyapatite(HAp)with various surface features[J].Ceramics International,2017,43(4):3752-3760.
[19]Chen L,Zhang K S,He J Y,et al.Enhanced fluoride removal from water by sulfate-doped hydroxyapatite hierarchical hollow microspheres[J].Chemical Engineering Journal,2016:285.
[20]Wang G,Hua Y,Su X,et al.Cr(VI)adsorption by montmorillonite nanocomposites[J].Applied Clay Science,2016,124-125:111-118.
[21]Zhang B,Ma Z,Yang F,et al.Adsorption properties of ion recognition rice straw lignin on PdCl42-:Equilibrium,kinetics and mechanism[J].Colloids&Surfaces A Physicochemical&Engineering Aspects,2017,514:260-268.
[22]蒲生彦,王可心,马慧,等.磁性壳聚糖凝胶微球对水中Pb(Ⅱ)的吸附性能[J].中国环境科学,2018,38(4):1364-1370.Pu S Y,Wang K X,Ma H,et al.Adsorption properties of magneticchitosan hydrogelmicrospheres to Pb(II)from aqueous solutions[J].China Environmental Science,2018,38(4):1364-1370.
[23]Wu F C,Tseng R L,Juang R S,Comparisons of porous and adsorption properties of carbons activated by steam and KOH[J].J Colloid Interface Sci,2005,283(1):49-56.
[24]Michael H J,J?se L V.Kinetic study of liquid-phase adsorptive removal of heavy metal ions by almond tree(Terminalia catappa L.)leaves waste[J].Bulletin of the Chemical Society of Ethiopia,2007,21(3):349-362(14).
[25]Patra B N,Majhi D.Removal of Anionic Dyes from Water by Potash Alum Doped Polyaniline:Investigation of Kinetics and Thermodynamic Parameters of Adsorption[J].Journal of Physical Chemistry B,2015,119(25):8154.
[26]张琴,黄冠燚,赵玲,等.pH值和离子对诺氟沙星在胡敏酸上吸附特征的影响[J].中国环境科学,2011,31(1):78-83.Zhang Q,Huang G Y,Zhao L,et al.Influence of pH and ions on sorption of norfloxacin on humic acid[J].China Environmental Science,2011,31(1):78-83.
[27]He J,Chen K,Cai X,et al.A biocompatible and novelly-defined Al-HAP adsorption membrane for highly effective removal of fluoride from drinking water[J].Journal of Colloid&Interface Science,2016,490:97-107.
[2]Zhang L E,Huang D,Yang J,et al.Probabilistic risk assessment of Chinese residents'exposure to fluoride in improved drinking water in endemic fluorosis areas[J].Environmental Pollution,2017,222:118-125.
[3]Amini M,Mueller K,Abbaspour K C,et al.Statistical Modeling of Global Geogenic Fluoride Contamination in Groundwaters[J].Environmental Science&Technology,2008,42(10):3662-3668.
[4]Huang H,Liu J,Zhang P,et al.Investigation on the simultaneous removal of fluoride,ammonia nitrogen and phosphate from semiconductor wastewater using chemical precipitation[J].Chemical Engineering Journal,2016,307:696-706.
[5]Zhang J,Chen N,Li M,et al.Fluoride removal from aqueous solution by Zirconium-Chitosan/Graphene Oxide Membrane[J].Reactive&Functional Polymers,2017,114.
[6]Schaefer C E,Andaya C,Burant A,et al.Electrochemical treatment of perfluorooctanoic acid and perfluorooctane sulfonate:Insights into mechanisms and application to groundwater treatment[J].Chemical Engineering Journal,2017,317:424-432.
[7]Jamhour R M A Q.New inorganic ion-exchange material for the selective removal of fluoride from potable water using ion-selective electrode[J].American Journal of Environmental Sciences,2005,1(1).
[8]Lin K Y,Liu Y T,Chen S Y.Adsorption of fluoride to UiO-66-NH2in water:Stability,kinetic,isotherm and thermodynamic studies[J].Journal of Colloid&Interface Science,2016,461:79-87.
[9]胡家朋,吴代赦,肖丽盈,等.羟基磷灰石的制备及其对水中氟离子的吸附[J].环境工程学报,2015,9(4):1823-1830.Hu J P,Wu D S,Xiao L Y,et al.Fabrication of hydroxyapatite and its absorption property for fluorid ion[J].Chinese Journal of Environmental Engineering,2015,9(4):1823-1830.
[10]Jiménez-Reyes M,Solache-Ríos M.Sorption behavior of fluoride ions from aqueous solutions by hydroxyapatite[J].Journal of Hazardous Materials,2010,180(1-3):297-302.
[11]Prabhu S M,Meenakshi S.Synthesis of surface coated hydroxyapatite powders for fluoride removal from aqueous solution[J].Powder Technology,2014,268(1):306-315.
[12]Li J,Zhang S,Chen C,et al.Removal of Cu(II)and Fulvic Acid by Graphene Oxide Nanosheets Decorated with Fe3O4 Nanoparticles[J].ACS Applied Materials&Interfaces,2012,4(9):4991-5000.
[13]Li S,Gong Y,Yang Y,et al.Recyclable CNTs/Fe3O4,magnetic nanocomposites as adsorbents to remove bisphenol A from water and their regeneration[J].Chemical Engineering Journal,2015,260:231-239.
[14]黄志良,刘羽,王大伟,等.Sol-Gel法合成HAP的结晶特征及其对F~-离子吸附性能研究[J].无机材料学报,2001,16(4):661-666.Huang Z L,Liu Y,Wang D W,et al.Properties of crystallizing and absorbing F-ion of HAP synthesized by Sol-Gel process[J].Journal of Inorganic Materials,2001,16(4):661-666.
[15]Mohamed A,Osman T A,Toprak M S,et al.Visible light photocatalytic reduction of Cr(VI)by surface modified CNT/titanium dioxide composites nanofibers[J].Journal of Molecular Catalysis AChemical,2016,424:45-53.
[16]施周,杨文浩,杨灵芳,等.离子改性CNT/TiO2电极吸附去除水中苯酚的研究[J].中国环境科学,2015,35(9):2664-2669.Shi Z,Yang W h,Yang L F,et al.Electrosorption of phenol in aqueous solution using a plasma-activated CNT/TiO2 electrode[J].China Environmental Science,2015,35(9):2664-2669.
[17]Xu D,Li B,Wei C,et al.Preparation and Characterization of Mn O2/acid-treated CNT Nanocomposites for Energy Storage with Zinc Ions[J].Electrochimica Acta,2014,133(7):254-261.
[18]Begam H,Kundu B,Chanda A,et al.MG63osteoblast cell response on Zn doped hydroxyapatite(HAp)with various surface features[J].Ceramics International,2017,43(4):3752-3760.
[19]Chen L,Zhang K S,He J Y,et al.Enhanced fluoride removal from water by sulfate-doped hydroxyapatite hierarchical hollow microspheres[J].Chemical Engineering Journal,2016:285.
[20]Wang G,Hua Y,Su X,et al.Cr(VI)adsorption by montmorillonite nanocomposites[J].Applied Clay Science,2016,124-125:111-118.
[21]Zhang B,Ma Z,Yang F,et al.Adsorption properties of ion recognition rice straw lignin on PdCl42-:Equilibrium,kinetics and mechanism[J].Colloids&Surfaces A Physicochemical&Engineering Aspects,2017,514:260-268.
[22]蒲生彦,王可心,马慧,等.磁性壳聚糖凝胶微球对水中Pb(Ⅱ)的吸附性能[J].中国环境科学,2018,38(4):1364-1370.Pu S Y,Wang K X,Ma H,et al.Adsorption properties of magneticchitosan hydrogelmicrospheres to Pb(II)from aqueous solutions[J].China Environmental Science,2018,38(4):1364-1370.
[23]Wu F C,Tseng R L,Juang R S,Comparisons of porous and adsorption properties of carbons activated by steam and KOH[J].J Colloid Interface Sci,2005,283(1):49-56.
[24]Michael H J,J?se L V.Kinetic study of liquid-phase adsorptive removal of heavy metal ions by almond tree(Terminalia catappa L.)leaves waste[J].Bulletin of the Chemical Society of Ethiopia,2007,21(3):349-362(14).
[25]Patra B N,Majhi D.Removal of Anionic Dyes from Water by Potash Alum Doped Polyaniline:Investigation of Kinetics and Thermodynamic Parameters of Adsorption[J].Journal of Physical Chemistry B,2015,119(25):8154.
[26]张琴,黄冠燚,赵玲,等.pH值和离子对诺氟沙星在胡敏酸上吸附特征的影响[J].中国环境科学,2011,31(1):78-83.Zhang Q,Huang G Y,Zhao L,et al.Influence of pH and ions on sorption of norfloxacin on humic acid[J].China Environmental Science,2011,31(1):78-83.
[27]He J,Chen K,Cai X,et al.A biocompatible and novelly-defined Al-HAP adsorption membrane for highly effective removal of fluoride from drinking water[J].Journal of Colloid&Interface Science,2016,490:97-107.