秸秆及磁性秸秆吸附剂对废水中亚甲基蓝的去除行为及机理
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摘要
以水稻秸秆(RS)为对象,通过化学沉淀法负载Fe_3O_4以制备秸秆负铁(RS-Fe)复合材料.同时,采用MBET、SEM、FTIR、XRD、XPS、VSM技术对RS、RS-Fe进行表征,研究了秸秆及复合材料对溶液中亚甲基蓝(MB)的去除效果,考察了固液比、溶液初始pH值对亚甲基蓝吸附效果的影响,并结合吸附动力学、吸附等温线、仪器表征及官能团封闭实验探究其作用机理.结果表明,吸附剂投加量为4.0 g·L~(-1)较合适;pH在3.0～11.0内,RS对MB去除率均在90%以上,碱性条件下有利于亚甲基蓝的高效去除.RS和RS-Fe对亚甲基蓝的吸附符合拟二级动力学模型.RS对亚甲基蓝的去除符合Langmuir模型,而RS-Fe对亚甲基蓝的去除更适合用Freundlich模型描述.FTIR、XPS和官能团封闭实验分析表明,秸秆表面官能团能在亚甲基蓝吸附过程中发挥重要作用,其中,羧基和氨基更为重要.秸秆对亚甲基蓝的吸附机理包括静电作用、氢键和π-π作用.Fe_3O_4的引入减少了秸秆官能团数量,降低了对亚甲基蓝的吸附量,但能实现快速固液分离.因此,RS具有作为亚甲基蓝染料废水吸附剂的潜力.负铁RS有利于提升固液分离效果.
Rice straw-Fe_3O_4 composite(RS-Fe) was prepared through chemical precipitation and then characterized by MBET, SEM, FTIR, XRD, VSM, XPS techniques. RS and RS-Fe were used to remove methylene blue(MB) from aqueous solution. The effects of solid-to-liquid ratio and pH on MB removal were investigated. Adsorption kinetic, isotherm, instrumental analysis and functional groups blocking experiment were performed to reveal MB-adsorbing behavior and mechanism. The result indicated that the optimum S/L ratio for MB removal was 4.0 g·L~(-1). MB removal rates of RS and RS-Fe were more than 90% and 60% respectively in the pH range of 3.0～11.0. MB removal was beneficial to alkaline environment. Pseudo-second order kinetic model could well describe the adsorption process of MB by RS and RS-Fe. MB-adsorbing isotherm of RS was fitted to Langmuir. However, Freundlich model could be suitable for MB removal of RS-Fe. FTIR, XPS and functional group blocking analysis indicated that functional groups in RS played an important role in the MB removal process, especially carboxyl and amino groups. The mechanism of MB removal by RS includes electrostatic interaction, hydrogen bond binding and π-π stacking. Introduction of Fe_3O_4 in RS reduced the quantity of functional groups and then theamount of adsorbed MB decreased. Nevertheless, the existence of Fe_3O_4 could realize fast separation of adsorbent and MB solution. Thus, RS has the potential to act as an adsorbent for dye removal and RS-Fe is in favor of solid-liquid separation.
Rice straw-Fe_3O_4 composite(RS-Fe) was prepared through chemical precipitation and then characterized by MBET, SEM, FTIR, XRD, VSM, XPS techniques. RS and RS-Fe were used to remove methylene blue(MB) from aqueous solution. The effects of solid-to-liquid ratio and pH on MB removal were investigated. Adsorption kinetic, isotherm, instrumental analysis and functional groups blocking experiment were performed to reveal MB-adsorbing behavior and mechanism. The result indicated that the optimum S/L ratio for MB removal was 4.0 g·L~(-1). MB removal rates of RS and RS-Fe were more than 90% and 60% respectively in the pH range of 3.0～11.0. MB removal was beneficial to alkaline environment. Pseudo-second order kinetic model could well describe the adsorption process of MB by RS and RS-Fe. MB-adsorbing isotherm of RS was fitted to Langmuir. However, Freundlich model could be suitable for MB removal of RS-Fe. FTIR, XPS and functional group blocking analysis indicated that functional groups in RS played an important role in the MB removal process, especially carboxyl and amino groups. The mechanism of MB removal by RS includes electrostatic interaction, hydrogen bond binding and π-π stacking. Introduction of Fe_3O_4 in RS reduced the quantity of functional groups and then theamount of adsorbed MB decreased. Nevertheless, the existence of Fe_3O_4 could realize fast separation of adsorbent and MB solution. Thus, RS has the potential to act as an adsorbent for dye removal and RS-Fe is in favor of solid-liquid separation.
引文
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Chang Y C,Chen D H.2005.Preparation and adsorption properties of monodisperse chitosan-bound Fe3O4 magnetic nanoparticles for removal of Cu(II) ions[J].Journal of Colloid and Interface Science,283(2):446-497
Chen J P,Yang L.2006.Study of a heavy metal biosorption onto raw and chemically modified Sargassum sp.via spectroscopic and modeling analysis[J].Langmuir: the ACS Journal of Surfaces and Colloids,22:8906-8920
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季雪琴,吕黎,陈芬,等.2016.秸秆生物炭对有机染料的吸附作用及机制[J].环境科学学报,36(5):1648-1654
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Khandanlou R,Ahmad M B,Shameli K,et al.2013.Synthesis and characterization of rice straw/Fe3O4 nanocomposites by a quick precipitation method[J].Molecules,18(6):6597-6607
Konstantinou I K,Albanis T A.2004.TiO2-assisted photocatalytic degradation of azo dyes in aqueous solution: kinetic and mechanistic investigations: a review[J].Applied Catalysis B:Environmental,49(1):1-14
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Liu Q S,Zheng T,Li N,et al.2010.Modification of bamboo-based activated carbon using microwave radiation and its effects on the adsorption of methylene blue[J].Applied Surface Science,256(10):3309-3315
Lyu H,Gao B,He F,et al.2018.Experimental and modeling investigations of ball-milled biochar for the removal of aqueous methylene blue[J].Chemical Engineering Journal,335:110-119
Panneerselvam P,Morad N,Tan K A.2011.Magnetic nanoparticle(Fe3O4) impregnated onto tea waste for the removal of nickel(Ⅱ) from aqueous solution[J].Journal of Hazardous Materials,186(1):160-168
Rafatullah M,Sulaiman O,Hashim R,et al.2010.Adsorption of methylene blue on low-cost adsorbents: a review[J].Journal of Hazardous Materials,177(1/3):70-80
Robinson T,McMullan G,Marchant R,et al.2001.Remediation of dyes in textile effluent: a critical review on current treatment technologies with a proposed alternative[J].Bioresource Technology,77(3):247-255
Rocha C G,Zaia D A M,da Silva Alfaya R V,et al.2009.Use of rice straw as biosorbent for removal of Cu (II),Zn (II),Cd (II) and Hg (II) ions in industrial effluents[J].Journal of Hazardous Materials,166(1):383-388
Safarik I,Baldikova E,Prochazkova J,et al.2018.Magnetically modified agricultural and food waste: preparation and application[J].Journal of Agricultural and Food Chemistry,66(11):2538-2552
Saratale R G,Saratale G D,Chang J S,et al.2011.Bacterial decolorization and degradation of azo dyes: a review[J].Journal of the Taiwan Institute of Chemical Engineers,42(1):138-157
Sud D,Mahajan G,Kaur M P.2008.Agricultural waste material as potential adsorbent for sequestering heavy metal ions from aqueous solutions-a review[J].Bioresource Technology,99(14):6017-6027
Vargas A M M,Cazetta A L,Kunita M H,et al.2011.Adsorption of methylene blue on activated carbon produced from flamboyant pods (Delonix regia): Study of adsorption isotherms and kinetic models[J].Chemical Engineering Journal,168(2):722-730
王章鸿,郭海艳,沈飞,等.2015.蚯蚓粪便制备生物炭及其对罗丹明B吸附的研究[J].环境科学学报,35(10):3170-3177
Weber TW,Chakravorti RK.1974.Pore and solid diffusion models for fixed-bed adsorbers[J].Aiche Journal,20:228-238
吴海露,车晓冬,丁竹红,等.2015.核桃、苔藓和松针基生物质炭对亚甲基蓝及刚果红的吸附性能研究[J].农业环境科学学报,34(8):1575-1581
谢光辉,王晓玉,任兰天.2010.中国作物秸秆资源评估研究现状[J].生物工程学报,26(7):855-863
姚时,张鸣帅,李林璇,等.2018.茶渣负载纳米四氧化三铁复合材料制备及其对亚甲基蓝的吸附机理[J].环境化学,37(1):96-107
曾淦宁,吴勇,柳慧敏,等.2016.铜藻基载铁活性炭的制备及其对亚甲基蓝的吸附特性研究[J].环境科学学报,36(5):1655-1662
Zhang S,Wang Z,Chen H,et al.2018.Polyethylenimine functionalized Fe3O4/steam-exploded rice straw composite as an efficient adsorbent for Cr (VI) removal[J].Applied Surface Science,440:1277-1285
邹雪刚,吕文英,王雅兰,等.2018.介孔铁锰双金属氧化物对Pb2+的吸附及其机理研究[J].环境科学学报,38(3):982-992
Alqadami A A,Naushad M,Alothman Z A,et al.2018.Adsorptive performance of MOF nanocomposite for methylene blue and malachite green dyes: Kinetics,isotherm and mechanism[J].Journal of Environmental Management,223:29-36
Anfar Z,El Haouti R,Lhanafi S,et al.2017.Treated digested residue during anaerobic co-digestion of Agri-food organic waste: Methylene blue adsorption,mechanism and CCD-RSM design[J].Journal of Environmental Chemical Engineering,5(6):5857-5867
Blanchard G,Maunaye M,Martin G.1984.Removal of heavy metals from waters by means of natural zeolites[J].Water Research,18(12):1501-1507
Cao W,Wang Z,Zeng Q,et al.2016.13C NMR and XPS characterization of anion adsorbent with quaternary ammonium groups prepared from rice straw,corn stalk and sugarcane bagasse[J].Applied Surface Science,389:404-410
常春,刘天琪,王瑀婷,等.2017.水热法制备玉米叶基生物炭对亚甲基蓝的吸附性能研究[J].环境科学学报,37(7):2680-2690
Chang Y C,Chen D H.2005.Preparation and adsorption properties of monodisperse chitosan-bound Fe3O4 magnetic nanoparticles for removal of Cu(II) ions[J].Journal of Colloid and Interface Science,283(2):446-497
Chen J P,Yang L.2006.Study of a heavy metal biosorption onto raw and chemically modified Sargassum sp.via spectroscopic and modeling analysis[J].Langmuir: the ACS Journal of Surfaces and Colloids,22:8906-8920
Chen X,Yu J,Zhang Z,et al.2011.Study on structure and thermal stability properties of cellulose fibers from rice straw[J].Carbohydrate polymers,85(1):245-250
Drake L R,Lin S,Rayson G D,et al.2006.Chemical modification and metal binding studies of Datura innoxia[J].Environment Science Technology,40:217-227
Fan S,Wang Y,Li Y,et al.2017.Facile synthesis of tea waste/Fe3O4 nanoparticle composite for hexavalent chromium removal from aqueous solution[J].RSC Advances,7(13):7576-7590
Forgacs E,Cserháti T,Oros G.2004.Removal of synthetic dyes from wastewaters: a review [J].Environment International,30(7):953-1024
Freundlich H.1907.über die adsorption in l?sungen[J].Zeitschrift Fur Physikalische Chemie,57:385-470
Hua M,Zhang S,Pan B,et al.2012.Heavy metal removal from water/wastewater by nanosized metal oxides: a review[J].Journal of Hazardous Materials,211:317-331
季雪琴,吕黎,陈芬,等.2016.秸秆生物炭对有机染料的吸附作用及机制[J].环境科学学报,36(5):1648-1654
Kannan N,Sundaram M M.2001.Kinetics and mechanism of removal of methylene blue by adsorption on various carbons-a comparative study[J].Dyes and Pigments,51(1):25-40
Khandanlou R,Ahmad M B,Shameli K,et al.2013.Synthesis and characterization of rice straw/Fe3O4 nanocomposites by a quick precipitation method[J].Molecules,18(6):6597-6607
Konstantinou I K,Albanis T A.2004.TiO2-assisted photocatalytic degradation of azo dyes in aqueous solution: kinetic and mechanistic investigations: a review[J].Applied Catalysis B:Environmental,49(1):1-14
Lagergren S.1898.About the theory of so-called adsorption of soluble substances[J].Kungliga Svenska Vetenskapsakademiens Handlingar,24:1-39
Langmuir I.1918.The adsorption of gases on plane surfaces of glass,mica and platinum[J].Journal of the American Chemical Society,40(9):1361-1403
Lau W J,Ismail A F.2009.Polymeric nanofiltration membranes for textile dye wastewater treatment:preparation,performance evaluation,transport modelling,and fouling control-a review[J].Desalination,245(1/3):321-348
梁昊,罗朝晖,赵海燕,等.2018.7种改性水稻秸秆对溶液中Cd2+的吸附[J].中国环境科学,38(2):596-607
Liu Q S,Zheng T,Li N,et al.2010.Modification of bamboo-based activated carbon using microwave radiation and its effects on the adsorption of methylene blue[J].Applied Surface Science,256(10):3309-3315
Lyu H,Gao B,He F,et al.2018.Experimental and modeling investigations of ball-milled biochar for the removal of aqueous methylene blue[J].Chemical Engineering Journal,335:110-119
Panneerselvam P,Morad N,Tan K A.2011.Magnetic nanoparticle(Fe3O4) impregnated onto tea waste for the removal of nickel(Ⅱ) from aqueous solution[J].Journal of Hazardous Materials,186(1):160-168
Rafatullah M,Sulaiman O,Hashim R,et al.2010.Adsorption of methylene blue on low-cost adsorbents: a review[J].Journal of Hazardous Materials,177(1/3):70-80
Robinson T,McMullan G,Marchant R,et al.2001.Remediation of dyes in textile effluent: a critical review on current treatment technologies with a proposed alternative[J].Bioresource Technology,77(3):247-255
Rocha C G,Zaia D A M,da Silva Alfaya R V,et al.2009.Use of rice straw as biosorbent for removal of Cu (II),Zn (II),Cd (II) and Hg (II) ions in industrial effluents[J].Journal of Hazardous Materials,166(1):383-388
Safarik I,Baldikova E,Prochazkova J,et al.2018.Magnetically modified agricultural and food waste: preparation and application[J].Journal of Agricultural and Food Chemistry,66(11):2538-2552
Saratale R G,Saratale G D,Chang J S,et al.2011.Bacterial decolorization and degradation of azo dyes: a review[J].Journal of the Taiwan Institute of Chemical Engineers,42(1):138-157
Sud D,Mahajan G,Kaur M P.2008.Agricultural waste material as potential adsorbent for sequestering heavy metal ions from aqueous solutions-a review[J].Bioresource Technology,99(14):6017-6027
Vargas A M M,Cazetta A L,Kunita M H,et al.2011.Adsorption of methylene blue on activated carbon produced from flamboyant pods (Delonix regia): Study of adsorption isotherms and kinetic models[J].Chemical Engineering Journal,168(2):722-730
王章鸿,郭海艳,沈飞,等.2015.蚯蚓粪便制备生物炭及其对罗丹明B吸附的研究[J].环境科学学报,35(10):3170-3177
Weber TW,Chakravorti RK.1974.Pore and solid diffusion models for fixed-bed adsorbers[J].Aiche Journal,20:228-238
吴海露,车晓冬,丁竹红,等.2015.核桃、苔藓和松针基生物质炭对亚甲基蓝及刚果红的吸附性能研究[J].农业环境科学学报,34(8):1575-1581
谢光辉,王晓玉,任兰天.2010.中国作物秸秆资源评估研究现状[J].生物工程学报,26(7):855-863
姚时,张鸣帅,李林璇,等.2018.茶渣负载纳米四氧化三铁复合材料制备及其对亚甲基蓝的吸附机理[J].环境化学,37(1):96-107
曾淦宁,吴勇,柳慧敏,等.2016.铜藻基载铁活性炭的制备及其对亚甲基蓝的吸附特性研究[J].环境科学学报,36(5):1655-1662
Zhang S,Wang Z,Chen H,et al.2018.Polyethylenimine functionalized Fe3O4/steam-exploded rice straw composite as an efficient adsorbent for Cr (VI) removal[J].Applied Surface Science,440:1277-1285
邹雪刚,吕文英,王雅兰,等.2018.介孔铁锰双金属氧化物对Pb2+的吸附及其机理研究[J].环境科学学报,38(3):982-992