秸秆生物炭对双氯芬酸钠的吸附性能研究
|
摘要
利用廉价的农业废弃物稻草秸秆,通过磷酸氢二铵((NH_4)_2HPO_4)活化制备得到秸秆生物炭(SBC),通过扫描电子显微镜(SEM)、比表面积分析(BET)、红外光谱(FTIR)等手段对其进行表征.研究了SBC对双氯芬酸钠(DCF)的吸附去除,并探讨了吸附时间、SBC投加量、pH值、阴离子浓度对吸附过程的影响.结果表明,当SBC投加量为0.3g/L时,DCF浓度为0.05mmol/L,60min后吸附量达到平衡;pH值范围在5.00～9.00时,SBC对DCF的吸附量去除率随着pH值的增加而减少;Cl~-、SO_4~(2-)和HCO_3~-对吸附过程的影响不大.拟合结果表明,SBC对DCF的吸附过程更符合准二级动力学模型和Freundlich吸附等温线.经Langmuir等温线模型计算理论最大吸附量为277.78mg/g(pH=7.00,T=20℃).热力学参数表明SBC对DCF的吸附是自发吸热过程.同活性炭和碳纳米管相比,SBC对DCF的吸附效果更好.
Straw-biochar(SBC)was prepared by rice straw,a cheap agricultural waste,through activation with ammonium hydrogen phosphate((NH_4)_2HPO_4).SBC was characterized by scanning electron microscopy(SEM),surface area measurements(BET)and Fourier transform infrared spectroscopy(FTIR).The effect of contact time,SBC dosage,initial pH and concentration of anions were investigated.The results indicated that adsorption capacity of SBC reached an equilibrium within 60min with 0.3g/L of SBC and 0.05mmol/L DCF.The removal rate of DCF decreased with pH increasing from 5.00 to 9.00.The addition of Cl~-、SO_4~(2-)and HCO_3~-had a negligible impact on the adsorption of DCF.The adsorption of diclofenac on SBC could be well fitted by the pseudo-second-order kinetics and Freundlich isotherm model.The maximum adsorption capacity of SBC for DCF was calculated to be 277.78mg/g based on Langmuir isotherm model.Thermodynamic parameters illustrated that the adsorption process was spontaneous and endothermic.Compared with activated carbon(AC)and carbon nanotube(CNT),SAC achieved a better performance on the removal of DCF.
Straw-biochar(SBC)was prepared by rice straw,a cheap agricultural waste,through activation with ammonium hydrogen phosphate((NH_4)_2HPO_4).SBC was characterized by scanning electron microscopy(SEM),surface area measurements(BET)and Fourier transform infrared spectroscopy(FTIR).The effect of contact time,SBC dosage,initial pH and concentration of anions were investigated.The results indicated that adsorption capacity of SBC reached an equilibrium within 60min with 0.3g/L of SBC and 0.05mmol/L DCF.The removal rate of DCF decreased with pH increasing from 5.00 to 9.00.The addition of Cl~-、SO_4~(2-)and HCO_3~-had a negligible impact on the adsorption of DCF.The adsorption of diclofenac on SBC could be well fitted by the pseudo-second-order kinetics and Freundlich isotherm model.The maximum adsorption capacity of SBC for DCF was calculated to be 277.78mg/g based on Langmuir isotherm model.Thermodynamic parameters illustrated that the adsorption process was spontaneous and endothermic.Compared with activated carbon(AC)and carbon nanotube(CNT),SAC achieved a better performance on the removal of DCF.
引文
[1]Hu J Y,Shi J C,Chang H,et al.Phenotyping and genotyping of antibiotic-resistant Escherichia coli isolated from a natural river basin[J].Environmental Science&Technology,2008,42(9):3415-3420.
[2]Pei R,Kim S C,Carlson K H,et al.Effect of river landscape on the sediment concentrations of antibiotics and corresponding antibiotic resistance genes(ARG)[J].Water Research,2006,40(12):2427-2435.
[3]Dutta K,Lee M Y,Lai W W,et al.Removal of pharmaceuticals and organic matter from municipal wastewater using two-stage anaerobic fluidized mrmbrane bioreactor[J].Bioresource Technology,2014,165(8):42-49.
[4]Vieno N,Sillanp??M.Fate of diclofenac in municipal wastewater treatment plant-a review[J].Environment International,2014,69(30):28-39.
[5]Acu?a V,Ginebreda A,Mor J R,et al.Balancing the health benefits and environmental risks of pharmaceuticals:Diclofenac as an example[J].Environment International,2015,85(3):327-333.
[6]Bueno M J,Gomez M J,Herrera S,et al.Occurrence and persistence of organic emerging contaminants and priority pollutants in five sewage treatment plants of Spain:two years pilot survey monitoring[J].Environmental Pollution,2012,164:267-273.
[7]Ginebreda A,Mu?oz I,Alda M L D,et al.Environmental risk assessment of pharmaceuticals in rivers:Relationships between hazard indexes and aquatic macroinvertebrate diversity indexes in the Llobregat River(NE Spain)[J].Environment International,2010,36(2):153-162.
[8]Caban M,Lis E,Kumirska J,et al.Determination of pharmaceutical residues in drinking water in Poland using a new SPE-GC-MS(SIM)method based on Speedisk extraction disks and DIMETRISderivatization[J].Science of the Total Environment,2015,538:402-411.
[9]Mehinto A C,Hill E M,Tyler C R.Uptake and biological effects of environmentally relevant concentrations of the nonsteroidal antiinflammatory pharmaceutical diclofenac in rainbow trout(Oncorhynchus mykiss)[J].Environmental Science&Technology,2010,44(6):2176-2182.
[10]Taggart M A,Cuthbert R,Das D,et al.Diclofenac disposition in Indian cow and goat with reference to Gyps vulture population declines[J].Environmental Pollution,2007,147(1):60-65.
[11]Zhang Y J,Gei?en S U,Gal C.Carbamazepine and diclofenac:removal in wastewater treatment plants and occurrence in water bodies[J].Chemosphere,2008,73(8):1151-1161.
[12]Schwaiger J,Ferling H,Mallow U,et al.Toxic effects of the nonsteroidal anti-inflammatory drug diclofenac Part I:histopathological alterations and bioaccumulation in rainbow trout[J].Aquatic Toxicology,2004,68(2):141-150.
[13]Rosal R,Rodríguez A,Perdigón-Melón J A,et al.Occurrence of emerging pollutants in urban wastewater and their removal through biological treatment followed by ozonation[J].Water Research,2010,44(2):578-588.
[14]Sotelo J L,Ovejero G,Rodríguez A,et al.Competitive adsorption studies of caffeine and diclofenac aqueous solutions by activated carbon[J].Chemical Engineering Journal,2014,240(6):443-453.
[15]Aziz K H H,Miessner H,Mueller S,et al.Degradation of pharmaceutical diclofenac and ibuprofen in aqueous solution,a direct comparison of ozonation,photocatalysis,and non-thermal plasma[J].Chemical Engineering Journal,2017,313:1033-1041.
[16]Moreira N F F,Orge C A,Ribeiro A R,et al.Fast mineralization and detoxification of amoxicillin and diclofenac by photocatalytic ozonation and application to an urban wastewater[J].Water Research,2015,87:87-96.
[17]Ravina M,Campanella L,Kiwi J.Accelerated mineralization of the drug Diclofenac via Fenton reactions in a concentric photo-reactor[J].Water Research,2002,36(14):3553-3560.
[18]Coelho A D,Sans C,Agüera A,et al.Effects of ozone pre-treatment on diclofenac:intermediates,biodegradability and toxicity assessment[J].Science of the Total Environment,2009,407(11):3572-3578.
[19]Nam S W,Jung C,Li H,et al.Adsorption characteristics of diclofenac and sulfamethoxazole to graphene oxide in aqueous solution[J].Chemosphere,2015,136:20-26.
[20]Bashir S,Zhu J,Fu Q L,et al.Comparing the adsorption mechanism of Cd by rice straw pristine and KOH-modified biochar[J].Environmental Science&Pollution Research International,2018,25:11875-11883.
[21]Tan G,Wu Y,Liu Y,et al.Removal of Pb(II)ions from aqueous solution by manganese oxide coated rice straw biochar-A low-cost and highly effective sorbent[J].Journal of the Taiwan Institute of Chemical Engineers,2018,84:85-92.
[22]Feng Z J,Zhu L Z.Sorption of phenanthrene to biochar modified by base[J].Frontiers of Environmental Science&Engineering,2018,12(2):1-11.
[23]Dai C M,Geissen S U,Zhang Y L,et al.Selective removal of diclofenac from contaminated water using molecularly imprinted polymer microspheres[J].Environmental Pollution,2011,159(6):1660-1666.
[24]Wei H,Deng S B,Huang Q,et al.Regenerable granular carbon nanotubes/alumina hybrid adsorbents for diclofenac sodium and carbamazepine removal from aqueous solution[J].Water Research,2013,47(12):4139-4147.
[25]Suriyanon N,Punyapalakul P,Ngamcharussrivichai C.Mechanistic study of diclofenac and carbamazepine adsorption on functionalized silica-based porous materials[J].Chemical Engineering Journal,2013,214(1):208-218.
[26]Danmaliki G I,Saleh T A.Influence of conversion parameters of waste tires to activated carbon on adsorption of dibenzothiophene from model fuels[J].Journal of Cleaner Production,2016,117:50-55.
[27]Sotelo J L,Rodríguez A,álvarez S,et al.Removal of caffeine and diclofenac on activated carbon in fixed bed column[J].Chemical Engineering Research&Design,2012,90(7):967-974.
[28]Jodeh S,Abdelwahab F,Jaradat N,et al.Adsorption of diclofenac from aqueous solution using Cyclamen persicum tubers based activated carbon(CTAC)[J].Journal of the Association of Arab Universities for Basic&Applied Sciences,2016,20:32-38.
[29]álvarez S,Ribeiro R S,Gomes H T,et al.Synthesis of carbon xerogels and their application in adsorption studies of caffeine and diclofenac as emerging contaminants[J].Chemical Engineering Research&Design,2015,95:229-238.
[30]Liu T,Xie Z H,Zhang Y,et al.Preparation of cationic polymeric nanoparticles as an effective adsorbent for removing diclofenac sodium from water[J].Rsc Advances,2017,7(61):38279-38286.
[2]Pei R,Kim S C,Carlson K H,et al.Effect of river landscape on the sediment concentrations of antibiotics and corresponding antibiotic resistance genes(ARG)[J].Water Research,2006,40(12):2427-2435.
[3]Dutta K,Lee M Y,Lai W W,et al.Removal of pharmaceuticals and organic matter from municipal wastewater using two-stage anaerobic fluidized mrmbrane bioreactor[J].Bioresource Technology,2014,165(8):42-49.
[4]Vieno N,Sillanp??M.Fate of diclofenac in municipal wastewater treatment plant-a review[J].Environment International,2014,69(30):28-39.
[5]Acu?a V,Ginebreda A,Mor J R,et al.Balancing the health benefits and environmental risks of pharmaceuticals:Diclofenac as an example[J].Environment International,2015,85(3):327-333.
[6]Bueno M J,Gomez M J,Herrera S,et al.Occurrence and persistence of organic emerging contaminants and priority pollutants in five sewage treatment plants of Spain:two years pilot survey monitoring[J].Environmental Pollution,2012,164:267-273.
[7]Ginebreda A,Mu?oz I,Alda M L D,et al.Environmental risk assessment of pharmaceuticals in rivers:Relationships between hazard indexes and aquatic macroinvertebrate diversity indexes in the Llobregat River(NE Spain)[J].Environment International,2010,36(2):153-162.
[8]Caban M,Lis E,Kumirska J,et al.Determination of pharmaceutical residues in drinking water in Poland using a new SPE-GC-MS(SIM)method based on Speedisk extraction disks and DIMETRISderivatization[J].Science of the Total Environment,2015,538:402-411.
[9]Mehinto A C,Hill E M,Tyler C R.Uptake and biological effects of environmentally relevant concentrations of the nonsteroidal antiinflammatory pharmaceutical diclofenac in rainbow trout(Oncorhynchus mykiss)[J].Environmental Science&Technology,2010,44(6):2176-2182.
[10]Taggart M A,Cuthbert R,Das D,et al.Diclofenac disposition in Indian cow and goat with reference to Gyps vulture population declines[J].Environmental Pollution,2007,147(1):60-65.
[11]Zhang Y J,Gei?en S U,Gal C.Carbamazepine and diclofenac:removal in wastewater treatment plants and occurrence in water bodies[J].Chemosphere,2008,73(8):1151-1161.
[12]Schwaiger J,Ferling H,Mallow U,et al.Toxic effects of the nonsteroidal anti-inflammatory drug diclofenac Part I:histopathological alterations and bioaccumulation in rainbow trout[J].Aquatic Toxicology,2004,68(2):141-150.
[13]Rosal R,Rodríguez A,Perdigón-Melón J A,et al.Occurrence of emerging pollutants in urban wastewater and their removal through biological treatment followed by ozonation[J].Water Research,2010,44(2):578-588.
[14]Sotelo J L,Ovejero G,Rodríguez A,et al.Competitive adsorption studies of caffeine and diclofenac aqueous solutions by activated carbon[J].Chemical Engineering Journal,2014,240(6):443-453.
[15]Aziz K H H,Miessner H,Mueller S,et al.Degradation of pharmaceutical diclofenac and ibuprofen in aqueous solution,a direct comparison of ozonation,photocatalysis,and non-thermal plasma[J].Chemical Engineering Journal,2017,313:1033-1041.
[16]Moreira N F F,Orge C A,Ribeiro A R,et al.Fast mineralization and detoxification of amoxicillin and diclofenac by photocatalytic ozonation and application to an urban wastewater[J].Water Research,2015,87:87-96.
[17]Ravina M,Campanella L,Kiwi J.Accelerated mineralization of the drug Diclofenac via Fenton reactions in a concentric photo-reactor[J].Water Research,2002,36(14):3553-3560.
[18]Coelho A D,Sans C,Agüera A,et al.Effects of ozone pre-treatment on diclofenac:intermediates,biodegradability and toxicity assessment[J].Science of the Total Environment,2009,407(11):3572-3578.
[19]Nam S W,Jung C,Li H,et al.Adsorption characteristics of diclofenac and sulfamethoxazole to graphene oxide in aqueous solution[J].Chemosphere,2015,136:20-26.
[20]Bashir S,Zhu J,Fu Q L,et al.Comparing the adsorption mechanism of Cd by rice straw pristine and KOH-modified biochar[J].Environmental Science&Pollution Research International,2018,25:11875-11883.
[21]Tan G,Wu Y,Liu Y,et al.Removal of Pb(II)ions from aqueous solution by manganese oxide coated rice straw biochar-A low-cost and highly effective sorbent[J].Journal of the Taiwan Institute of Chemical Engineers,2018,84:85-92.
[22]Feng Z J,Zhu L Z.Sorption of phenanthrene to biochar modified by base[J].Frontiers of Environmental Science&Engineering,2018,12(2):1-11.
[23]Dai C M,Geissen S U,Zhang Y L,et al.Selective removal of diclofenac from contaminated water using molecularly imprinted polymer microspheres[J].Environmental Pollution,2011,159(6):1660-1666.
[24]Wei H,Deng S B,Huang Q,et al.Regenerable granular carbon nanotubes/alumina hybrid adsorbents for diclofenac sodium and carbamazepine removal from aqueous solution[J].Water Research,2013,47(12):4139-4147.
[25]Suriyanon N,Punyapalakul P,Ngamcharussrivichai C.Mechanistic study of diclofenac and carbamazepine adsorption on functionalized silica-based porous materials[J].Chemical Engineering Journal,2013,214(1):208-218.
[26]Danmaliki G I,Saleh T A.Influence of conversion parameters of waste tires to activated carbon on adsorption of dibenzothiophene from model fuels[J].Journal of Cleaner Production,2016,117:50-55.
[27]Sotelo J L,Rodríguez A,álvarez S,et al.Removal of caffeine and diclofenac on activated carbon in fixed bed column[J].Chemical Engineering Research&Design,2012,90(7):967-974.
[28]Jodeh S,Abdelwahab F,Jaradat N,et al.Adsorption of diclofenac from aqueous solution using Cyclamen persicum tubers based activated carbon(CTAC)[J].Journal of the Association of Arab Universities for Basic&Applied Sciences,2016,20:32-38.
[29]álvarez S,Ribeiro R S,Gomes H T,et al.Synthesis of carbon xerogels and their application in adsorption studies of caffeine and diclofenac as emerging contaminants[J].Chemical Engineering Research&Design,2015,95:229-238.
[30]Liu T,Xie Z H,Zhang Y,et al.Preparation of cationic polymeric nanoparticles as an effective adsorbent for removing diclofenac sodium from water[J].Rsc Advances,2017,7(61):38279-38286.