十八烷基三甲基氯化铵/双十八烷基二甲基氯化铵修饰ATP的制备及其吸附重金属的性能
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摘要
使用12 mol/L的盐酸对天然凹凸棒石晶体(ATP)进行粗提处理,再用十八烷基三甲基氯化铵(DOTAC)和双十八烷基二甲基氯化铵(DODMAC)分别对ATP进行接枝改性,得到十八烷基三甲基氯化铵改性凹土(1831-ATP)和双十八烷基二甲基氯化铵改性凹土(D1821-ATP)。通过红外光谱(FT-IR)、X射线衍射(XRD)和比表面积(BET)等表征手段对改性前后凹土的晶体结构变化进行分析比较,并利用扫描电镜(SEM)观察了ATP、1831-ATP和D1821-ATP的形貌变化。对比研究了ATP、1831-ATP和D1821-ATP对常见重金属Pb2+的吸附性能,吸附实验结果表明:吸附平衡时间为4 h;在p H 9时,Pb2+在ATP、1831-ATP和D1821-ATP上的吸附量达到最高,去除率均达到99%以上,去除效果好。动力学和热力学模型拟合结果表明,吸附数据符合准二级动力学方程和Freundlich等温吸附方程。
ATP was prepared by treating natural attapulgite with acid,and then modified by the cationic surfactants octade cyltrimethyl ammonium chloride and dimethyldistearylammonium chloride to prepare 1831-ATP and D1821-ATP,respectively. The effects of varying p H,time and ion concentration on the sorption efficiency of lead( Ⅱ) on attapulgite were investigated in batch experiments and the thermodynamic and dynamic laws of the sorption were studied. The results showed that the sorption was strongly p H-dependent and ion concentration had little impact on sorption. The sorption process can be described by a pseudo-second-order rate model. The Freundlich model fitted the sorption data better than the Langmiur model. Since the adsorption process is not described primarily by monolayer and chemical adsorption,the adsorption of lead( Ⅱ) on 1831-ATP is better than that on ATP from the view point of both capacity and rate.
ATP was prepared by treating natural attapulgite with acid,and then modified by the cationic surfactants octade cyltrimethyl ammonium chloride and dimethyldistearylammonium chloride to prepare 1831-ATP and D1821-ATP,respectively. The effects of varying p H,time and ion concentration on the sorption efficiency of lead( Ⅱ) on attapulgite were investigated in batch experiments and the thermodynamic and dynamic laws of the sorption were studied. The results showed that the sorption was strongly p H-dependent and ion concentration had little impact on sorption. The sorption process can be described by a pseudo-second-order rate model. The Freundlich model fitted the sorption data better than the Langmiur model. Since the adsorption process is not described primarily by monolayer and chemical adsorption,the adsorption of lead( Ⅱ) on 1831-ATP is better than that on ATP from the view point of both capacity and rate.
引文
[1]Feleafel M N,Mirdad Z M.Hazard and effects of pollution by lead on vegetable crops[J].Journal of Agricultural and Environmental Ethics,2013,26(3):547-567.
[2]徐颖,罗玉兰,魏广艳.重金属捕集剂处理含铅废水的试验研究[J].环境科学与技术,2006,29(5):75-76.Xu Y,Luo Y L,Wei G Y.Treatment of lead contained wastewater by heavy metal capturing agent[J].Environmental Science&Technology,2006,29(5):75-76.(in Chinese)
[3]栗帅,查会平,范忠雷.含铅废水处理技术研究现状及展望[J].化工进展,2011,30(增刊1):336-339.Li S,Zha H P,Fan Z L.Research status and prospects in treatment technique for Pb2+-containing wastewater[J].Chemical Industry and Engineering Progress,2011,30(suppl 1):336-339.(in Chinese)
[4]Arab P B,Araújo T P,Pejon O J.Identification of clay minerals in mixtures subjected to differential thermal and thermogravimetry analyses and methylene blue adsorption tests[J].Applied Clay Science,2015,114:133-140.
[5]Bradley W F.The structural scheme of attapulgite[J].American Mineralogist,1940,25(6):405-410.
[6]周杰,刘宁,李云,等.凹凸棒石粘土的显微结构特征[J].硅酸盐通报,1999,18(6):50-55.Zhou J,Liu N,Li Y,et al.Microscopic structure characteristics of attapulgite[J].Bulletin of the Chinese Ceramic Society,1999,18(6):50-55.(in Chinese)
[7]周守勇,薛爱莲,张艳,等.聚丙烯酸改性凹土对Pb2+、Ni2+和Cr3+的选择性吸附[J].化工学报,2015,66(2):618-625.Zhou S Y,Xue A L,Zhang Y,et al.Selective adsorption of Pb2+,Ni2+and Cr3+by polyacrylic acid/attapulgite composite adsorbents[J].CIESC Jorunal,2015,66(2):618-625.(in Chinese)
[8]Chen L F,Liang H W,Lu Y,et al.Synthesis of an attapulgite clay@carbon nanocomposite adsorbent by a hydrothermal carbonization process and their application in the removal of toxic metal ions from water[J].Langmuir,2011,27(14):8998-9004.
[9]Liang X F,Xu Y M,Tan X,et al.Heavy metal adsorbents mercapto and amino functionalized palygorskite:preparation and characterization[J].Colloids&Surfaces A:Physicochemical and Engineering Aspects,2013,426(21):98-105.
[10]Chao H P,Chen S H.Adsorption characteristics of both cationic and oxyanionic metal ions on hexadecyltrimethylammonium bromide-modified Na Y zeolite[J].Chemical Engineering Journal,2012,193/194(25):283-289.
[11]Myriam M,Suárez M,Martín-Pozas J M.Structural and textural modifications of palygorskite and sepiolite under acid treatment[J].Clays and Clay Minerals,1998,46(3):225-231.
[12]国家环境保护局.水质铅的测定双硫腙分光光度法:GB/T 7470—87[S].北京:中国标准出版社,1987:27-30.National Environmental Protection Agency.Determination of lead in water-dithizone spectrophotometric method:GB/T 7470—87[S].Beijing:Standards Press of China,1987:27-30.(in Chinese)
[13]Suárez M,García-Romero E.FTIR spectroscopic study of palygorskite:influence of the composition of the octahedral sheet[J].Applied Clay Science,2006,31(1/2):154-163.
[14]Mckeown D A,Post J E,Etz E S.Vibrational analysis of palygorskite and sepiolite[J].Clays and Clay Minerals,2002,50(5):667-680.
[15]Zhang J P,Chen H,Wang A Q.Study on superabsorbent composite.IV.Effects of organification degree of attapulgite on swelling behaviors of polyacrylamide/organoattapulgite composites[J].European Polymer Journal,2006,42(1):101-108.
[16]Araújo Melo D M,Ruiz J A C,Melo M A F,et al.Preparation and characterization of lanthanum palygorskite clays as acid catalysts[J].Journal of Alloys and Compounds,2002,344(1/2):352-355.
[17]黄健花.凹凸棒土的有机改性及其应用[D].江苏无锡:江南大学,2008.Huang J H.Organo-modification of playgorskite and its application[D].Wuxi,Jiangsu:Jiangnan University,2008.(in Chinese)
[18]Sun S J,Ren N,Zhang J J,et al.Synthesis,crystal structure,and thermal decomposition kinetics of the complex of Ho 2,4-dichlorobenzoic acid and 2,2-bipyridine[J].Journal of Chemical&Engineering Data,2010,55(7):2458-2462.
[19]Li J,Zhang T,Wang L,et al.Characterization and quantification of the nickel resistant microbial community in activated sludge using 16S r DNA and nickel resistance genes[J].Environmental Technology,2011,32(5):533-542.
[20]张娜,张陶娜,蒋京呈,等.叶腊石对水溶液中铀的吸附研究[J].中国科学:化学,2016,46(4):409-416.Zhang N,Zhang T N,Jiang J C,et al.Sorption of uranium from aqueous solution with pyrophyllite[J].Scientia Sinica Chimica,2016,46(4):409-416.(in Chinese)
[2]徐颖,罗玉兰,魏广艳.重金属捕集剂处理含铅废水的试验研究[J].环境科学与技术,2006,29(5):75-76.Xu Y,Luo Y L,Wei G Y.Treatment of lead contained wastewater by heavy metal capturing agent[J].Environmental Science&Technology,2006,29(5):75-76.(in Chinese)
[3]栗帅,查会平,范忠雷.含铅废水处理技术研究现状及展望[J].化工进展,2011,30(增刊1):336-339.Li S,Zha H P,Fan Z L.Research status and prospects in treatment technique for Pb2+-containing wastewater[J].Chemical Industry and Engineering Progress,2011,30(suppl 1):336-339.(in Chinese)
[4]Arab P B,Araújo T P,Pejon O J.Identification of clay minerals in mixtures subjected to differential thermal and thermogravimetry analyses and methylene blue adsorption tests[J].Applied Clay Science,2015,114:133-140.
[5]Bradley W F.The structural scheme of attapulgite[J].American Mineralogist,1940,25(6):405-410.
[6]周杰,刘宁,李云,等.凹凸棒石粘土的显微结构特征[J].硅酸盐通报,1999,18(6):50-55.Zhou J,Liu N,Li Y,et al.Microscopic structure characteristics of attapulgite[J].Bulletin of the Chinese Ceramic Society,1999,18(6):50-55.(in Chinese)
[7]周守勇,薛爱莲,张艳,等.聚丙烯酸改性凹土对Pb2+、Ni2+和Cr3+的选择性吸附[J].化工学报,2015,66(2):618-625.Zhou S Y,Xue A L,Zhang Y,et al.Selective adsorption of Pb2+,Ni2+and Cr3+by polyacrylic acid/attapulgite composite adsorbents[J].CIESC Jorunal,2015,66(2):618-625.(in Chinese)
[8]Chen L F,Liang H W,Lu Y,et al.Synthesis of an attapulgite clay@carbon nanocomposite adsorbent by a hydrothermal carbonization process and their application in the removal of toxic metal ions from water[J].Langmuir,2011,27(14):8998-9004.
[9]Liang X F,Xu Y M,Tan X,et al.Heavy metal adsorbents mercapto and amino functionalized palygorskite:preparation and characterization[J].Colloids&Surfaces A:Physicochemical and Engineering Aspects,2013,426(21):98-105.
[10]Chao H P,Chen S H.Adsorption characteristics of both cationic and oxyanionic metal ions on hexadecyltrimethylammonium bromide-modified Na Y zeolite[J].Chemical Engineering Journal,2012,193/194(25):283-289.
[11]Myriam M,Suárez M,Martín-Pozas J M.Structural and textural modifications of palygorskite and sepiolite under acid treatment[J].Clays and Clay Minerals,1998,46(3):225-231.
[12]国家环境保护局.水质铅的测定双硫腙分光光度法:GB/T 7470—87[S].北京:中国标准出版社,1987:27-30.National Environmental Protection Agency.Determination of lead in water-dithizone spectrophotometric method:GB/T 7470—87[S].Beijing:Standards Press of China,1987:27-30.(in Chinese)
[13]Suárez M,García-Romero E.FTIR spectroscopic study of palygorskite:influence of the composition of the octahedral sheet[J].Applied Clay Science,2006,31(1/2):154-163.
[14]Mckeown D A,Post J E,Etz E S.Vibrational analysis of palygorskite and sepiolite[J].Clays and Clay Minerals,2002,50(5):667-680.
[15]Zhang J P,Chen H,Wang A Q.Study on superabsorbent composite.IV.Effects of organification degree of attapulgite on swelling behaviors of polyacrylamide/organoattapulgite composites[J].European Polymer Journal,2006,42(1):101-108.
[16]Araújo Melo D M,Ruiz J A C,Melo M A F,et al.Preparation and characterization of lanthanum palygorskite clays as acid catalysts[J].Journal of Alloys and Compounds,2002,344(1/2):352-355.
[17]黄健花.凹凸棒土的有机改性及其应用[D].江苏无锡:江南大学,2008.Huang J H.Organo-modification of playgorskite and its application[D].Wuxi,Jiangsu:Jiangnan University,2008.(in Chinese)
[18]Sun S J,Ren N,Zhang J J,et al.Synthesis,crystal structure,and thermal decomposition kinetics of the complex of Ho 2,4-dichlorobenzoic acid and 2,2-bipyridine[J].Journal of Chemical&Engineering Data,2010,55(7):2458-2462.
[19]Li J,Zhang T,Wang L,et al.Characterization and quantification of the nickel resistant microbial community in activated sludge using 16S r DNA and nickel resistance genes[J].Environmental Technology,2011,32(5):533-542.
[20]张娜,张陶娜,蒋京呈,等.叶腊石对水溶液中铀的吸附研究[J].中国科学:化学,2016,46(4):409-416.Zhang N,Zhang T N,Jiang J C,et al.Sorption of uranium from aqueous solution with pyrophyllite[J].Scientia Sinica Chimica,2016,46(4):409-416.(in Chinese)
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