摘要
通过浮石负载壳聚糖制备了吸附剂壳聚糖/浮石复合物,采用扫描电子显微镜(SEM)、热重分析(TGA)、元素分析、傅里叶红外光谱(FT-IR)、X射线衍射(XRD)和X射线荧光光谱(XRF)等技术手段表征了吸附剂性质,考察了吸附剂量、吸附时间、溶液pH值、离子强度和温度对该吸附剂吸附去除水中丙溴磷的影响,研究了再生吸附剂的吸附性能。结果表明,负载在浮石上的壳聚糖占吸附剂总量的8.69%;在p H值3.0~7.0内,壳聚糖/浮石对丙溴磷的吸附率大于90%;这种吸附剂对丙溴磷的吸附受溶液离子强度影响较小,随温度升高而稍微减小。在溶液温度25℃、pH=7.0、丙溴磷浓度40 mg/L、壳聚糖/浮石剂量为0.7 g/L和吸附平衡时间为90 min条件下,此吸附剂对丙溴磷最大吸附率为93.3%(最大吸附量为53.4 mg/g)。壳聚糖/浮石连续经过3次吸附/再生循环,每次循环对丙溴磷的吸附率下降约12%。可见壳聚糖/浮石通过吸附可有效地去除水中的农药丙溴磷。
An adsorbent named chitosan/pumice has been prepared for adsorptive removal of profenofos from aqueous solutions. The effects of solution p H,adsorbent dosage,contact time,ion strength and temperature on the adsorption of profenofos were investigated by batch experiments. The immobilization of chitosan was characterized by SEM,TGA,elemental analysis,FT-IR,XRD and XRF. The resultsshow that the chitosan loaded on pumice accounts for 8. 69% of the amount of adsorbent; the adsorbent can be employed at p H3. 0 ~ 7. 0 for quantitative adsorption rate( > 90%); the adsorption for profenofos is hardly influenced by ion strength,and slightly decreases with temperature increase. Under the condition of 25 ℃,p H = 7. 0,40 mg/L for the concentration of profenofos and 0. 7 g/L for dose of chitosan/pumice,the adsorption equilibrium time is90 min and the maximum adsorption rate of profenofos is 93. 3%( 53. 4 mg/g for adsorbing capacity). The adsorbent can be reused at least three consecutive times with about 12% decrease on profenofos adsorption efficiency. This method for the adsorptive removal of profenofos from aqueous solution is simple,low cost,rapid and effective.
引文
[1]Abass K,Reponen R,Jalonen J.In Vitro Metabolism and Interaction of Profenofos by Human,Mouse and Rat Liver Preparations[J].Pestic Biochem Physiol,2007,87(3):238-247.
[2]Malghani S,Chatterjee N,Yu H,et al.Isolation and Identification of Profenofos Degrading Bacteria[J].Braz J Microbiol,2009,40(4):893-900.
[3]Costa LG.Current Issues in Organophosphate Toxicology[J].Clin Chim Acta,2006,366:1-13.
[4]Dadson O A,Ellison C A,Singleton S T,et al.Metabolism of Profenofos to 4-Bromo-2-Chlorophenol,A Specific and Sensitive Exposure Biomarker[J].Toxicology,2013,306:35-39.
[5]Jabeen H,Iqbal S,Anwar S,et al.Optimization of Profenofos Degradation by a Novel Bacterial Consortium PBAC Using Response Surface Methodology[J].Int Biodeterior Biodegrad,2015,100:89-97.
[6]Ioannidou O A,Zabaniotou A A,Stavropoulos G G,et al.Preparation of Activated Carbons from Agricultural Residues for Pesticide Adsorption[J].Chemosphere,2010,80(11):1328-1336.
[7]Rojas R,Morillo J,Usero J,et al.Adsorption Study of Low-cost and Locally Available Organic Substances and a Soil to Remove Pesticides from Aqueous Solutions[J].J Hydrol,2015,520:461-472.
[8]Ersoy B,Sariisik A,Dikmen S,et al.Application of Acidic Treated Pumice as an Adsorbent for the Removal of Azo Dye from Aqueous Solutions:Kinetic,Equilibrium and Thermodynamic Studies[J].Powder Technol,2010,197:129-135.
[9]Heibati B,Rodriguez-Couto S,Amrane A,et al.Uptake of Reactive Black 5 by Pumice and Walnut Activated Carbon:Chemistry and Adsorption Mechanisms[J].J Ind Eng Chem,2014,20(5):2939-2947.
[10]Carr D D,Alsobrook A F,Austin G.Industrial Minerals and Rocks,Society for Mining,Metallurgy,and Exploration[M].Inc,Littleton,CO,USA,1994.
[11]Behzad H,Susana R C,Nurdan G T,et al.Removal of Noxious Dye-Acid Orange 7 from Aqueous Solution Using Natural Pumice and Fe-coated Pumice Stone[J].J Ind Eng Chem,2015,31:124-131.
[12]Ozturk B,Yildirim Y.Investigation of Sorption Capacity of Pumice for SO2Capture[J].Process Saf Environ,2008,86(11):31-36.
[13]WU Yaqi,XU Chang,ZHAO Yue,et al.Preparation of Calcium Silicate-chitosan Polymer and the Adsorptive Removal of Heavy Metals in Wastewater[J].Environ Chem,2016,35(3):562-567(in Chinese).吴亚琪,徐畅,赵越,等.硅酸钙-壳聚糖聚合物制备及其对重金属废水的吸附特性[J].环境化学,2016,35(3):562-567.
[14]CHANG Yanhong,DONG Xiaoning.Preparation of Porous Chitosan-graft-poly(ACrylic acid)/Na-montmorillonite Super Absorbent Composite and Its Absorption Performance for Pb2+[J].Chinese J Appl Chem,2015,32(6):623-628(in Chinese).常艳红,董晓宁.多孔壳聚糖接枝聚丙烯酸/钠基蒙脱土复合高吸水凝胶的制备及其对Pb2+的吸附[J].应用化学,2015,32(6):623-628.
[15]WU Liping,ZHANG Zhengpu,GUO Yi,et al.Preparation of Hexanediamine-contained PAMAM Dendrimers Supported on Chitosan Microspheres and Their Application in the Adsorption of Bilirubin[J].Chem J Chinese Univ,2011,32(6):1434-1444(in Chinese).吴丽平,张政朴,郭义,等.壳聚糖微球负载的己二胺型聚酰胺-胺树状大分子的制备及对胆红素的吸附[J].高等学校化学学报,2011,32(6):1434-1444.
[16]Futalan C M,Kan C C,Dalida M L,et al.Comparative and Competitive Adsorption of Copper,Lead,and Nickel Using Chitosan Immobilized on Bentonite[J].Carbohydr Polym,2011,83(2):528-536.
[17]Dalida M L P,Mariano A F V,Futalan C M,et al.Adsorptive Removal of Cu(Ⅱ)from Aqueous Solutions Using Noncrosslinked and Crosslinked Chitosan-coated Bentonite Beads[J].Desalination,2011,275:154-159.
[18]Zou X H,Pan J M,Ou H X,et al.Adsorptive Removal of Cr(Ⅲ)and Fe(Ⅲ)from Aqueous Solution by Chitosan/attapulgite Composites:Equilibrium,Thermodynamics and Kinetics[J].Chem Eng J,2011,167(1):112-121.
[19]Wen Y,Tang Z,Chen Y,et al.Adsorption of Cr(Ⅵ)from Aqueous Solutions Using Chitosan-coated Fly Ash Composite as Biosorbent[J].Chem Eng J,2011,175:110-116.
[20]Sundaram C S,Viswanathan N,Meenakshi S.Defluoridation of Water Using Magnesia/chitosan Composite[J].J Hazard Mater,2009,163:618-624.
[21]Nesic A R,Velickovic S J,Antonovic D G.Characterization of Chitosan/montmorillonite Membranes as Adsorbents for Bezactiv Orange V-3R Dye[J].J Hazard Mater,2012,209/210:256-263.
[22]Chang M Y,Juang R S J.Adsorption of Tannic Acid,Humic Acid,and Dyes from Water Using the Composite of Chitosan and Activated Clay[J].Colloid Interface Sci,2004,278:18-25.
[23]Maghsoodloo S,Noroozi B,Haghi A K,et al.Consequence of Chitosan Treating on the Adsorption of Humic Acid by Granular Activated Carbon[J].J Hazard Mater,2011,191:380-387.
[24]Yavuz M,Gode F,Pehlivan E,et al.An Economic Removal of Cu2+and Cr3+on the New Adsorbents:Pumice and Polyacrylonitrile/pumice Composite[J].Chem Eng J,2008,137(3):435-461.
[25]SHEN Ying,SUN Fusheng,DONG Jie.Determination of Profenofos in Water Using Dispersive Liquid-liquid Microextraction-High Performance Liquid Chromatography[J].Chinese J Anal Chem,2010,38(4):551-554(in Chinese).沈英,孙福生,董杰.分散液相微萃取-高效液相色谱法测定水中丙溴磷农药[J].分析化学,2010,38(4):551-554.
[26]Hina J,Samina I,Samina A,et al.Optimization of Profenofos Degradation by a Novel Bacterial Consortium PBAC Using Response Surface Methodology[J].Int Biodeterior Biodegrad,2015,100:89-97.
[27]Charles P N,Gustave K D,Emmanuel N.Study of the Removal of Paraquat from Aqueous Solution by Biosorption onto Ayous(Triplochiton schleroxylon)Sawdust[J].J Hazard Mater,2010,179(1-3):63-71.
[28]Naseem R,Tahir S S,Kang J H,et al.Equilibrium,Thermodynamics and Kinetics Studies for the Removal of alpha and beta Endosulfan by Adsorption onto Bentonite Clay[J].Chem Eng J,2012,192:369-376.
[29]Tsai W T,Hsien K J,Chang Y M,et al.Removal of Herbicide Paraquat from Aqueous Solution by Adsorption onto Spent and Treated Diatomaceous Earths[J].Bioresour Technol,2005,96(6):657-663.
[30]Mehdi S S,Alireza K,Aydin H,et al.Preparation,Characterization and Application of a CTAB-modified Nanoclay for the Adsorption of an Herbicide from Aqueous Solutions:Kinetic and Equilibrium Studies[J].C R Chim,2015,18(2):204-214.
[31]ZHU Lijun,ZHANG Wei,ZHANG Jinchi,et al.Thermodynamics Adsorption and Its Influencing Factors of Chlorpyrifos and Triazophos on the Bentonite and Humus[J].Environ Sci,2011,31(11):2699-2704(in Chinese).朱丽珺,张维,张金池,等.毒死蜱和三唑磷在膨润土和腐殖质上的热力学吸附及影响因素[J].环境科学,2011,31(11):2699-2704.
[32]Shavisi Y,Sharifnia S,Zendehzaban M,et al.Application of Solar Light for Degradation of Aammonia in Petrochemical Wastewater by a Floating Ti O2/LECA Photocatalyst[J].J Ind Eng Chem,2014,20:2806-2813