镧、铈改性介孔氧化铝对氟离子的吸附
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摘要
以La、Ce为改性物负载至其他载体表面作为高效除氟吸附剂已经受到广泛的关注。但是将La和Ce负载到介孔氧化铝(MA)却少见报道。本研究制备了La和Ce改性介孔氧化铝并将其用于氟的去除。采用N2吸脱附等温线、X射线衍射(XRD)、傅里叶红外光谱(FTIR)对该吸附剂的结构性质进行了表征。同时,考察了吸附剂接触时间、初始浓度和溶液pH等吸附条件对氟离子吸附效果的影响。结果表明,反应在150 min时达到吸附平衡,此时La/MA的氟去除率达92. 2%,吸附氟容量大小为La/MA> Ce/MA> MA;氟吸附量随初始浓度的增大而增大;在pH值为5～9时,除氟效果较好;吸附等温线方程均符合Langmuir等温吸附模型; La/MA的氟离子最大吸附容量为27. 9 mg/g;共存阴离子对氟吸附的影响程度为CO32-> SO42-> NO3-> Cl-。最后比较了吸附前后的FTIR,可以看出La/MA对氟离子去除效果最佳。
Nowadays,a kind of highly efficient fluoride adsorbent has that employ La,Ce as the modifier to the surface of certain carriers has aroused wide concerns. However,the loading of La and Ce into mesoporous alumina(MA) is rarely reported. In this study,La and Ce modified mesoporous alumina were prepared they were used for the removal of fluorine. The structural properties of the adsorbent were characterized by N2 desorption isotherm,X-ray diffraction(XRD) and Fourier transform infrared spectroscopy(FTIR). Furthermore,the effects of contact time,initial concentration and pH value on the adsorption of fluoride were investigated. The results showed that the adsorption equilibrium had been achieved at 150 min,with the fluorine removal rate of 92. 2%(La/MA). The order of fluorine adsorption capacity was La/MA > Ce/MA > MA. The fluorine adsorption capacity increased with the increase of initial concentration. Satisfactory fluorine removal effect could be acquired under the pH value of5—9. The adsorption isotherm equation was in accordance with the Langmuir adsorption isotherm model. The La/MA exhibited a maximum adsorption capacity of 27. 9 mg/g. The degree of influence of co-existing anions on fluoride removal followed the order of CO_2-3> SO_2-4> NO-3>Cl-. Finally,by comparing the FTIR before and after adsorption,it could be seen that La/MA exerted the best effect on fluoride removal.
Nowadays,a kind of highly efficient fluoride adsorbent has that employ La,Ce as the modifier to the surface of certain carriers has aroused wide concerns. However,the loading of La and Ce into mesoporous alumina(MA) is rarely reported. In this study,La and Ce modified mesoporous alumina were prepared they were used for the removal of fluorine. The structural properties of the adsorbent were characterized by N2 desorption isotherm,X-ray diffraction(XRD) and Fourier transform infrared spectroscopy(FTIR). Furthermore,the effects of contact time,initial concentration and pH value on the adsorption of fluoride were investigated. The results showed that the adsorption equilibrium had been achieved at 150 min,with the fluorine removal rate of 92. 2%(La/MA). The order of fluorine adsorption capacity was La/MA > Ce/MA > MA. The fluorine adsorption capacity increased with the increase of initial concentration. Satisfactory fluorine removal effect could be acquired under the pH value of5—9. The adsorption isotherm equation was in accordance with the Langmuir adsorption isotherm model. The La/MA exhibited a maximum adsorption capacity of 27. 9 mg/g. The degree of influence of co-existing anions on fluoride removal followed the order of CO_2-3> SO_2-4> NO-3>Cl-. Finally,by comparing the FTIR before and after adsorption,it could be seen that La/MA exerted the best effect on fluoride removal.
引文
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2 Yeung C A.Evidence-based Dentistry,2008,9(2),39.
3 Cai H D.Modern environmental hygiene,People's Medical Publishing House,China,2004(in Chinese).蔡宏道.现代环境卫生学,人民卫生出版社,1994.
4 Mandal S,Mayadevi S.Chemosphere,2008,72(6),995.
5 Das D P,Das J,Parida K.Journal of Colloid&Interface Science,2003,261(2),213.
6 Min Y M,Hashimoto T,Hoshi N,et al.Water Research,1999,33(16),3395.
7 Castel C,Schweizer M,Simonnot M O,et al.Chemical Engineering Science,2000,55(17),3341.
8 Garmes H,Persin F,Sandeaux J,et al.Desalination,2002,145(1),287.
9 Amor Z,Bariou B,Mameri N,et al.Desalination,2001,133(3),215.
10 Hu K,Dickson J M.Journal of Membrane Science,2006,279(1-2),529.
11 Kemer B,Ozdes D,Gundogdu A,et al.Journal of Hazardous Materials,2009,168(2-3),888.
12 Islam M,Patel R K.Journal of Hazardous Materials,2007,143(1-2),303.
13 Meenakshi S,Sundaram C S,Sukumar R.Journal of Hazardous Materials,2008,153(1-2),164.
14 Tor A,Danaoglu N,Arslan G,et al.Journal of Hazardous Materials,2009,164(1),271.
15 Jiménez-Reyes M,Solache-Ríos M.Journal of Hazardous Materials,2010,180(1-3),297.
16 Bhatnagar A,Kumar E,SillanpM.Chemical Engineering Journal,2011,171(3),811.
17 Ghosh A,Chakrabarti S,Biswas K,et al.Applied Surface Science,2014,307,665.
18 Tokunaga S,Haron M J,Wasay S A,et al.International Journal of Environmental Studies,1995,48(1),17.
19 Zhang T,Li Q,Liu Y,et al.Chemical Engineering Journal,2011,168(2),665.
20 Wang J,Xu W H,Chen L,et al.Chemical Engineering Journal,2013,231(17),198.
21 Zhang S Y,Lu Y,Lin X Y,et al.Applied Surface Science,2014,303(5),1.
22 Cheng J M,Meng X G,Jing C Y,et al.Journal of Hazardous Materials,2014,278,343.
23 Yu Y,Wang C H,Guo X,et al.Journal of Colloid&Interface Science,2015,441,113.
24 Sing K S W.Pure&Applied Chemistry,2009,57(4),603.
25 Nazari M,Halladj R.Journal of the Taiwan Institute of Chemical Engineers,2014,45(5),2518.
26 Chen Y,Zhang L,Liu Z,et al.Hans Journal of Chemical Engineering and Technology,2017,7(6),275(in Chinese).陈越,张力,刘铸,等.化学工程与技术,2017,7(6),275.
27 Hou H,Xie Y,Yang Q.Food Research&Development,2005,16(16),741.
28 Chen Y M,Wang M K,Huang P M,et al.Geoderma,2009,152(3-4),296.
29 Viswanathan N,Meenakshi S.Journal of Colloid&Interface Science,2008,322(2),375.
30 Brito A,Borges M E,Garín M,et al.Energy Fuels,2009,23(6),2952.
31 Sundaram C S,Viswanathan N,Meenakshi S.Journal of Hazardous Materials,2009,163(2-3),618.
32 Kang J X,Li B,Song J,et al.Chemical Engineering Journal,2011,166(2),765.
33 Sugi Y,Kubota Y,Komura K,et al.Applied Catalysis A General,2006,299(1),157.
34 Yang L J,Liu X Y,Jiang X,et al.Chinese Journal of Applied Chemistry,2012,29(11),1278(in Chinese).杨丽君,刘雪岩,姜鑫,等.应用化学,2012,29(11),1278.
35 Tang Y L,Guan X H,Su T Z,et al.Colloids&Surfaces A Physicochemical&Engineering Aspects,2009,337(1-3),33.
36 Sun X L,Zeng Q X,Feng C G,et al.Journal of Functional Materials,2009,40(10),1734(in Chinese).孙小莉,曾庆轩,冯长根,等.功能材料,2009,40(10),1734.
37 Pandey N.Removal efficiency of fluoride by La induced Zr-phosphate porous material.Master's thesis,National Institute of Technology,lndia,2012.
38 Hun Z Y,Tang S Y,Wang J,et al.Journal of Henan Chemical Industry,2011,19,36(in Chinese).胡之阳,唐思远,王静,等.河南化工,2011(19),36.
39 Zhang S Y,Lu Y,Lin X Y,et al.Applied Surface Science,2014,303(5),1.
40 Viswanathan N,Meenakshi S.Journal of Colloid&Interface Science,2008,322(2),375.
41 Chen H H,Huang L M,Wu H F,et al.Journal of Environment and Health,2010,27(10),868(in Chinese).陈红红,黄丽玫,毋福海,等.环境与健康杂志,2010,27(10),868.
42 Teutli-Sequeira A,Solache-Ríos M,Martínez-Miranda V,et al.Journal of Colloid&Interface Science,2014,418,254.
43 Kumar E,Bhatnagar A,Kumar U,et al.Journal of Hazardous Materials,2011,186(2-3),1042.
44 Viswanathan N,Meenakshi S.Applied Clay Science,2010,48(4),607.
45 Zhao X L,Wang J M,Wu F C,et al.Journal of Hazardous Materials,2010,173(1-3),102.
46 Bansiwal A,Pillewan P,Biniwale R B,et al.Microporous&Mesoporous Materials,2010,129(1),54.
47 Rao C R N,Karthikeyan J.Water Air&Soil Pollution,2012,223(3),1101.
48 Tripathy S S,Raichur A M.Journal of Hazardous Materials,2008,153(3),1043.