海藻酸钙@Fe_3O_4/生物碳磁性复合材料的制备及其对Co(Ⅱ)的吸附性能和机制
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摘要
利用海藻酸钙(CA)包覆生物碳(BC)、Fe_3O_4制备了一种新型磁性微球(CA@Fe_3O_4/BC),用以吸附水溶液中的Co(Ⅱ)。系统的研究了Co(NO3)2溶液浓度、pH和时间对吸附的影响。CA@Fe_3O_4/BC吸附Co(Ⅱ)等温热力学数据符合Langmuir模型,在pH=6的条件下对Co(Ⅱ)的最大吸附量为16.23 mg/g。研究显示,CA@Fe_3O_4/BC存在显著的协同效应,对Co(Ⅱ)具有更好的吸附性能。由于磁性颗粒的存在,CA@Fe_3O_4/BC吸附Co(Ⅱ)后可以用磁铁吸附快速分离。CA@Fe_3O_4/BC吸附Co(Ⅱ)动力学数据符合准二级动力学模型,研究表明,CA@Fe_3O_4/BC吸附Co(Ⅱ)的机制主要包括形成配合物及Ca(Ⅱ)与Co(Ⅱ)发生离子交换。
A magnetic microspheres(Calcium Alginate@Fe_3O_4/Biochar)was prepared using calcium alginate(CA)encapsulated biochar(BC)and Fe_3O_4 as the green adsorbent for Co(Ⅱ)removal from aqueous solution.The effects of the initial Co(NO3)2 concentration,initial pH value of Co(Ⅱ)solution and equilibrium contact time were investigated on CA@Fe_3O_4/BC.The isothermal thermodynamic datas of the CA@Fe_3O_4/BC conformed to the Langmuir model.The maximum adsorption capacity of the CA@Fe_3O_4/BC from the Langmuir equation is 16.23 mg·g-1 at pH=6.It appears a synergistic effect between biochar and Fe_3O_4 in CA,which enhances the maximum adsorption capacity of Co(Ⅱ)ion.The presence of the magnetic particles in magnetic microsphere allows easy isolation of the material from aqueous solutions by using a magnet.The adsorptions of Co(Ⅱ)by the CA@Fe_3O_4/BC are in good agreement with pseudo-second-order kinetic.The mechanism studies for Co(Ⅱ)removal by the CA@Fe_3O_4/BC show that the nature of Co(Ⅱ)abstraction takes place through the ion exchange between Ca(Ⅱ)and Co(Ⅱ)as well as the formation of coordination complex.
A magnetic microspheres(Calcium Alginate@Fe_3O_4/Biochar)was prepared using calcium alginate(CA)encapsulated biochar(BC)and Fe_3O_4 as the green adsorbent for Co(Ⅱ)removal from aqueous solution.The effects of the initial Co(NO3)2 concentration,initial pH value of Co(Ⅱ)solution and equilibrium contact time were investigated on CA@Fe_3O_4/BC.The isothermal thermodynamic datas of the CA@Fe_3O_4/BC conformed to the Langmuir model.The maximum adsorption capacity of the CA@Fe_3O_4/BC from the Langmuir equation is 16.23 mg·g-1 at pH=6.It appears a synergistic effect between biochar and Fe_3O_4 in CA,which enhances the maximum adsorption capacity of Co(Ⅱ)ion.The presence of the magnetic particles in magnetic microsphere allows easy isolation of the material from aqueous solutions by using a magnet.The adsorptions of Co(Ⅱ)by the CA@Fe_3O_4/BC are in good agreement with pseudo-second-order kinetic.The mechanism studies for Co(Ⅱ)removal by the CA@Fe_3O_4/BC show that the nature of Co(Ⅱ)abstraction takes place through the ion exchange between Ca(Ⅱ)and Co(Ⅱ)as well as the formation of coordination complex.
引文
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[27]YAN L G,YANG K,SHAN R R,et al.Kinetic,isotherm and thermodynamic investigations of phosphate adsorption onto core-shell Fe3O4@ldhs composites with easy magnetic separation assistance[J].Journal of Colloid and Interface Science,2015,448:508-516.
[28]CHEN Y,MU S.Core-shell structured Fe3O4nanoparticles functionalized with rhodamine derived probe for the detection,adsorption and removal of Hg(ii):A sensing system with‘warning’signal[J].Sensors and Actuators B:Chemical,2014,192(192):275-282.
[29]YU C,GENG J,ZHUANG Y,et al.Preparation of the chitosan grafted poly(quaternary ammonium)/Fe3O4nanoparticles and its adsorption performance for food yellow 3[J].Carbohydrate Polymers,2016,152:327-336.
[30]VERMA R,ASTHANA A,SINGH A K,et al.Novel glycine-functionalized magnetic nanoparticles entrapped calcium alginate beads for effective removal of lead[J].Microchemical Journal,2017,130:168-178.
[31]ALGOTHMI W M,BANDARU N M,YU Y,et al.Alginate-graphene oxide hybrid gel beads:An efficient copper adsorbent material[J].Journal of Colloid and Interface Science,2013,397(5):32-38.
[32]ZHANG C J,LIU Y,CUI L,et al.Bio-based calcium alginate nonwoven fabrics:Flame retardant and thermal degradation properties[J].Journal of Analytical and Applied Pyrolysis,2016,122:13-23.
[33]MOUSA N E,SIMONESCU C M,PATESCU R E,et al.Pb2+removal from aqueous synthetic solutions by calcium alginate and chitosan coated calcium alginate[J].Reactive and Functional Polymers,2016,109:137-150.
[34]PLATERO E,FERNANDEZ M E,BONELLI P R,et al.Graphene oxide/alginate beads as adsorbents:Influence of the load and the drying method on their physicochemicalmechanical properties andadsorptive performance[J].Journal of Colloid and Interface Science,2017,491:1-12.
[35]JIANG N,XU Y,DAI Y,et al.Polyaniline nanofibers assembled on alginate microsphere for Cu2+and Pb2+uptake[J].Journal of Hazardous Materials,2012,215-216(4):17-24.
[36]DO X H,LEE B K.Removal of Pb2+using a biochar-alginate capsule in aqueous solution and capsule regeneration[J].Journal of Environmental Management,2013,131:375-382.
[37]TAYYEBI A,OUTOKESH M,MORADI S,et al.Synthesis and characterization of ultrasound assisted“graphene oxide-magnetite”hybrid,and investigation of its adsorption properties for Sr(ii)and Co(ii)ions[J].Applied Surface Science,2015,353(343):350-362.
[38]BOIS L,BONHOMME A,RIBES A,et al.Functionalized silica for heavy metal ions adsorption[J].Colloids and Surfaces A:Physicochemical and Engineering Aspects,2003,221(1-3):221-230.
[39]VILVANATHAN S,SHANTHAKUMAR S.Biosorption of Co(ii)ions from aqueous solution using chrysanthemum indicum:Kinetics equilibrium and thermodynamics[J].Process Safety and Environmental Protection,2015,96:98-110.
[40]KUSHWAHA A K,GUPTA N,CHATTOPADHYAYA M C.Dynamics of adsorption of Ni(ii),Co(ii)and Cu(ii)from aqueous solution onto newly synthesized poly[n-(4-[4-(aminophenyl)methylphenylmethacrylamide])][J].Arabian Journal of Chemistry,2017,10:1645-1653.
[41]GUPTA N,KUSHWAHA A K,CHATTOPADHYAYA M C.Adsorptive removal of Pb2+,Co2+and Ni 2+by hydroxyapatite/chitosan composite from aqueous solution[J].Journal of the Taiwan Institute of Chemical Engineers,2012,43(1):125-131.
[42]EEDEM E,KARAPINAR N,DONAT R.The removal of heavy metal cations by natural zeolites[J].Journal of Colloid and Interface Science,2004,280(2):309-314.
[43]BORDOLOI N,GOSWAMI R,KUMAR M,et al.Biosorption of Co(ii)from aqueous solution using algal biochar:Kinetics and isotherm studies[J].Bioresource Technology,2017,244:1465-1469.
[44]ROH H,YU M R,YAKKALA K,et al.Removal studies of Cd(ii)and explosive compounds using buffalo weed biocharalginate beads[J].Journal of Industrial and Engineering Chemistry,2015,26:226-233.
[45]HASSAN A F,ABDEL MOHSEN A M,ELHADIDY H.Adsorption of arsenic by activated carbon,calcium alginate and their composite beads[J].International Journal of Biological Macromolecules,2014,68(7):125-130.
[46]BAGHERI A R,GHAEDI M,ASFARAM A,et al.Comparative study on ultrasonic assisted adsorption of dyes from single system onto Fe3O4 magnetite nanoparticles loaded on activated carbon:Experimental design methodology[J].Ultrasonics Sonochemistry,2017,34:294-304.
[47]ZHOU B,WANG Z,SHEN D,et al.Low cost earthworm manure-derived carbon material for the adsorption of Cu2+from aqueous solution:Impact of pyrolysis temperature[J].Ecological Engineering,2017,98:189-195.
[48]REN H,GAO Z,WU D,et al.Efficient Pb(II)removal using sodium alginate-carboxymethyl cellulose gel beads:Preparation,characterization,and adsorption mechanism[J].Carbohydr Polym,2016,137:402-409.
[2]KHAN M,YILMAZ E,SOYLAK M.Vortex assisted magnetic solid phase extraction of lead(ii)and cobalt(ii)on silica coated magnetic multiwalled carbon nanotubes impregnated with 1-(2-pyridylazo-2-naphthol)[J].Journal of Molecular Liquids,2016,224:639-647.
[3]MARTIN C B,LECLERCQ S,BARBOUX P,et al.Sorption of nickel and cobalt ions onto cobalt and nickel ferrites[J].Journal of Colloid and Interface Science,2011.360(2):695-700.
[4]AWUAL M R,ISMAEL M,YAITA T.Efficient detection and extraction of cobalt(ii)from lithium ion batteries and wastewater by novel composite adsorbent[J].Sensors and Actuators B:Chemical,2014,191:9-18.
[5]LI M,LIU Q,GUO L,et al.Cu(II)removal from aqueous solution by spartina alterniflora derived biochar[J].Bioresource Technology,2013,141(4):83-88.
[6]MOHAN D,SINGH P,SARSWAT A,et al.Lead sorptive removal using magnetic and nonmagnetic fast pyrolysis energy cane biochars[J].Journal of Colloid and Interface Science,2015,448:238-250.
[7]TRAKAL L,VESELSKA V,SAFARIK I,et al.Lead and cadmium sorption mechanisms on magnetically modified biochars[J].Bioresource Technology,2016,203:318-324.
[8]HAN Z,SANI B,MROZIK W,et al.Magnetite impregnation effects on the sorbent properties of activated carbons and biochars[J].Water Research,2015,70:394-403.
[9]谢水波,罗景阳,刘清,等.羟乙基纤维素/海藻酸钠复合膜对六价铀的吸附性能及吸附机制[J].复合材料学报,2015,32(1):268-275.XIE S B,LUO J Y,LIU Q,et al.Adsorption characteristics and mechanism of hydroxyethyl cellulose/sodium alginate blend film for uranium(Ⅵ)[J].Acta Materiae Compositae Sinica,2015,32(1):268-275(in Chinese).
[10]刘东,赵孔银,宋欢语,等.硅酸钙-海藻酸钙复合水凝胶膜的制备及表征[J].复合材料学报,2017,34(11):2401-2406.LIU Dong,ZHAO Kongyin,SONG Huanyu,et al.Preparation and characterization of calcium silicate-calcium alginate composite hydrogel film[J].Acta Materiae Compositae Sinica,2017,34(11):2401-2406(in Chinese).
[11]TAVAKOLI H,SEPEHRIAN H,CHERAGHALI R.Encapsulation of nanoporous mcm-41in biopolymeric matrix of calcium alginate and its use as effective adsorbent for lead ions:Equilibrium,kinetic and thermodynamic studies[J].Journal of the Taiwan Institute of Chemical Engineers,2013,44(3):343-348.
[12]LI Y,DU Q,LIU T,et al.Methylene blue adsorption on graphene oxide/calcium alginatecomposites[J].Carbohydrate Polymers,2013,95(1):501-507.
[13]SIGDEL A,JUNG W,MIN B,et al.Concurrent removal of cadmium and benzene from aqueous solution by powdered activated carbon impregnated alginate beads[J].Catena,2017,148:101-107.
[14]ZHANG S XU F,WANG Y,et al.Silica modified calcium alginate-xanthan gum hybrid bead composites for the removal and recovery of Pb(II)from aqueous solution[J].Chemical Engineering Journal,2013,234(12):33-42.
[15]蔺洪全,赵孔银,马敬环,等.TiO2-海藻酸钙复合膜的表征、对染料的光催化降解及TiO2回收[J].复合材料学报,2015,32(3):911-917.LIN H Q,ZHAO K Y,MA J H,et al.Characterization and dyes photocatalytic degradation of TiO2-calcium alginate composite films and recycle of TiO2[J].Acta Materiae Compositae Sinica,2015,32(3):911-917(in Chinese).
[16]IDRIS A,ISMAIL N,HASSAN N,et al.Synthesis of magnetic alginate beads based on maghemite nanoparticles for Pb(ii)removal in aqueous solution[J].Journal of Industrial and Engineering Chemistry,2012,18(5):1582-1589.
[17]YANG Y,WEI Z,ZHANG X,et al.Biochar from alternanthera philoxeroides could remove Pb(II)efficiently[J].Bioresource Technology,2014,171(1):227-232.
[18]TALEB M.Adsorption and photocatalytic degradation of 2-cp in wastewater onto CS/CoFe2O4 nanocomposite synthesized using gamma radiation[J].Carbohydrate Polymers,2014,114:65-72.
[19]JUNG K W,JEONG T U,KANG H J,et al.Characteristics of biochar derived from marine macroalgae and fabrication of granular biochar by entrapment in calcium-alginate beads for phosphate removal from aqueous solution[J].Bioresource Technology,2016,211:108-116.
[20]CUI X,DAI X,KHAN K Y,et al.Removal of phosphate from aqueous solution using magnesium-alginate/chitosan modified biochar microspheres derived from thalia dealbata[J].Bioresource Technology,2016,218:1123-1132.
[21]LI J,CHEN C,ZHAO Y,et al.Synthesis of water-dispersible Fe3O4@β-cyclodextrin by plasma-induced grafting technique for pollutant treatment[J].Chemical Engineering Journal,2013,229:296-303.
[22]LI J,ZHANG S,CHEN C,et al.Removal of Cu(ii)and fulvic acid by graphene oxide nanosheets decorated with Fe3O4nanoparticles[J].ACS Applied Materials&Interfaces,2012,4(9):4991-5000.
[23]WU T,MAO L,WANG H.Adsorption of fluoride from aqueous solution by using hybrid adsorbent fabricated with Mg/Fe composite oxide and alginate via a facile method[J].Journal of Fluorine Chemistry,2017,200:8-17.
[24]GUO Y,TANG W,WU J,et al.Mechanism of Cu(II)adsorption inhibition on biochar by its aging process[J].Journal of Environmental Sciences,2014,26(10):2123-2130.
[25]YAN L,LI S,YU H,et al.Facile solvothermal synthesis of Fe3O4/bentonite for efficient removal of heavy metals from aqueous solution[J].Powder Technology,2016,301:632-640.
[26]XU Y,ZHOU Y,LI R.Simultaneous fluorescence response and adsorption of functionalized Fe3O4@SiO2nanoparticles to Cd2+,Zn2+and Cu2+[J].Colloids and Surfaces A:Physicochemical and Engineering Aspects,2014,459(14):240-246.
[27]YAN L G,YANG K,SHAN R R,et al.Kinetic,isotherm and thermodynamic investigations of phosphate adsorption onto core-shell Fe3O4@ldhs composites with easy magnetic separation assistance[J].Journal of Colloid and Interface Science,2015,448:508-516.
[28]CHEN Y,MU S.Core-shell structured Fe3O4nanoparticles functionalized with rhodamine derived probe for the detection,adsorption and removal of Hg(ii):A sensing system with‘warning’signal[J].Sensors and Actuators B:Chemical,2014,192(192):275-282.
[29]YU C,GENG J,ZHUANG Y,et al.Preparation of the chitosan grafted poly(quaternary ammonium)/Fe3O4nanoparticles and its adsorption performance for food yellow 3[J].Carbohydrate Polymers,2016,152:327-336.
[30]VERMA R,ASTHANA A,SINGH A K,et al.Novel glycine-functionalized magnetic nanoparticles entrapped calcium alginate beads for effective removal of lead[J].Microchemical Journal,2017,130:168-178.
[31]ALGOTHMI W M,BANDARU N M,YU Y,et al.Alginate-graphene oxide hybrid gel beads:An efficient copper adsorbent material[J].Journal of Colloid and Interface Science,2013,397(5):32-38.
[32]ZHANG C J,LIU Y,CUI L,et al.Bio-based calcium alginate nonwoven fabrics:Flame retardant and thermal degradation properties[J].Journal of Analytical and Applied Pyrolysis,2016,122:13-23.
[33]MOUSA N E,SIMONESCU C M,PATESCU R E,et al.Pb2+removal from aqueous synthetic solutions by calcium alginate and chitosan coated calcium alginate[J].Reactive and Functional Polymers,2016,109:137-150.
[34]PLATERO E,FERNANDEZ M E,BONELLI P R,et al.Graphene oxide/alginate beads as adsorbents:Influence of the load and the drying method on their physicochemicalmechanical properties andadsorptive performance[J].Journal of Colloid and Interface Science,2017,491:1-12.
[35]JIANG N,XU Y,DAI Y,et al.Polyaniline nanofibers assembled on alginate microsphere for Cu2+and Pb2+uptake[J].Journal of Hazardous Materials,2012,215-216(4):17-24.
[36]DO X H,LEE B K.Removal of Pb2+using a biochar-alginate capsule in aqueous solution and capsule regeneration[J].Journal of Environmental Management,2013,131:375-382.
[37]TAYYEBI A,OUTOKESH M,MORADI S,et al.Synthesis and characterization of ultrasound assisted“graphene oxide-magnetite”hybrid,and investigation of its adsorption properties for Sr(ii)and Co(ii)ions[J].Applied Surface Science,2015,353(343):350-362.
[38]BOIS L,BONHOMME A,RIBES A,et al.Functionalized silica for heavy metal ions adsorption[J].Colloids and Surfaces A:Physicochemical and Engineering Aspects,2003,221(1-3):221-230.
[39]VILVANATHAN S,SHANTHAKUMAR S.Biosorption of Co(ii)ions from aqueous solution using chrysanthemum indicum:Kinetics equilibrium and thermodynamics[J].Process Safety and Environmental Protection,2015,96:98-110.
[40]KUSHWAHA A K,GUPTA N,CHATTOPADHYAYA M C.Dynamics of adsorption of Ni(ii),Co(ii)and Cu(ii)from aqueous solution onto newly synthesized poly[n-(4-[4-(aminophenyl)methylphenylmethacrylamide])][J].Arabian Journal of Chemistry,2017,10:1645-1653.
[41]GUPTA N,KUSHWAHA A K,CHATTOPADHYAYA M C.Adsorptive removal of Pb2+,Co2+and Ni 2+by hydroxyapatite/chitosan composite from aqueous solution[J].Journal of the Taiwan Institute of Chemical Engineers,2012,43(1):125-131.
[42]EEDEM E,KARAPINAR N,DONAT R.The removal of heavy metal cations by natural zeolites[J].Journal of Colloid and Interface Science,2004,280(2):309-314.
[43]BORDOLOI N,GOSWAMI R,KUMAR M,et al.Biosorption of Co(ii)from aqueous solution using algal biochar:Kinetics and isotherm studies[J].Bioresource Technology,2017,244:1465-1469.
[44]ROH H,YU M R,YAKKALA K,et al.Removal studies of Cd(ii)and explosive compounds using buffalo weed biocharalginate beads[J].Journal of Industrial and Engineering Chemistry,2015,26:226-233.
[45]HASSAN A F,ABDEL MOHSEN A M,ELHADIDY H.Adsorption of arsenic by activated carbon,calcium alginate and their composite beads[J].International Journal of Biological Macromolecules,2014,68(7):125-130.
[46]BAGHERI A R,GHAEDI M,ASFARAM A,et al.Comparative study on ultrasonic assisted adsorption of dyes from single system onto Fe3O4 magnetite nanoparticles loaded on activated carbon:Experimental design methodology[J].Ultrasonics Sonochemistry,2017,34:294-304.
[47]ZHOU B,WANG Z,SHEN D,et al.Low cost earthworm manure-derived carbon material for the adsorption of Cu2+from aqueous solution:Impact of pyrolysis temperature[J].Ecological Engineering,2017,98:189-195.
[48]REN H,GAO Z,WU D,et al.Efficient Pb(II)removal using sodium alginate-carboxymethyl cellulose gel beads:Preparation,characterization,and adsorption mechanism[J].Carbohydr Polym,2016,137:402-409.