选用活性炭作为吸附剂,研究了新型持久性有机污染物六溴环十二烷( HBCD)在乙腈?水溶液中的吸附行为.结果表明,活性炭的投加量(0.2—2 g·L-1)、HBCD初始浓度(0—60 mg·L-1)及溶液中乙腈的比例(40%—100%)对吸附效果产生显著影响;吸附动力学分析表明活性炭对HBCD的吸附速率受颗粒内扩散过程控制;通过对比Langmuir、Freundlich和Sips模型发现Sips模型更适于描述在0.05 g·L-1的活性炭投加量, HBCD初始浓度为0—60 mg·L-1的条件下,HBCD在乙腈溶液中的吸附过程,且呈现出S型吸附等温线特点,说明在吸附剂表面可能存在较强烈的竞争吸附;通过Sips模型求得的饱和吸附容量为62 mg·g-1;在40%—100%的乙腈比例下,吸附量随着乙腈比例的提高而线性降低.在活性炭投加量为0.05 g·L-1,HBCD初始浓度为5 mg·L-1条件下,获得平衡吸附量随乙腈浓度(40%—100%)变化的回归方程,并且估算乙腈比例为0%情况下,HBCD的平衡吸附量为127.35 mg·g-1.
In this work, activated carbon ( AC ) was selected as the adsorbent to investigate the adsorption behavior of one of the new persistent organic pollutants, hexabromocyclododecane ( HBCD) , in the acetonitrile?water solution. Results showed that the adsorptions were affected significantly by the dosages of AC ( 0. 2 g·L-1—2 g·L-1 ) , initial concentrations of HBCD ( 0—60 mg·L-1 ) and proportions of acetonitrile ( 40%—100%) . The adsorption kinetics analysis showed the rate of adsorption of HBCD was controlled by the inner?sphere diffusion in AC. Langmuir, Freundlich and Sips models were used to fit the adsorption isotherm respectively. In the presence of 0.05 g·L-1 of AC and 0—60 mg·L-1 of initial concentrations of HBCD, the Sips model can better describe the adsorption process in acetonitrile solution which has the S type isotherm and implied the existence of strong competition of adsorption on the surface of AC. The saturated adsorption capacity is 62 mg·g-1 via Sips model. The adsorption capacity decreased linearly as the proportion of acetonitrile over the range of 40% to 100%. The regression equation of equilibrium adsorption capacity that varies with acetonitrile concentrations ( 40—100%) was obtained in the presence of 0?05 g·L-1 of AC and 5 mg·L-1 of initial concentration of HBCD, and the equilibrium adsorption capacity for HBCD was speculated as 127. 35 mg·g-1 under the acetonitrile proportion of 0%. This work provides the basis for removing HBCD from water by AC.
参考文献
[1] | 耿新华;李晓;刘汝锋 等.六溴环十二烷在环境中迁移转化的研究进展[J].环境科学与技术,2012,35(6):144-150. |
[2] | Christopher H. Marvin;Gregg T. Tomy;James M. Arrnitage .Hexabromocyclododecane: Current Understanding of Chemistry, Environmental Fate and Toxicology and Implications for Global Management[J].Environmental Science & Technology: ES&T,2011(20):8613-8623. |
[3] | Zhou D;Wu Y;Feng X et al.Photodegradation of hexabromocyclododecane (HBCD) by Fe(Ⅲ) complexes/H2O2 under simulated sunlight[J].ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH,2014,21(9):6228-6233. |
[4] | Mikael Remberger;John Sternbeck;Anna Palm;Lennart Kaj;Katarina Stroemberg;Eva Brorstroem-Lunden .The environmental occurrence of hexabromocyclododecane in Sweden[J].Chemosphere,2004(1):9-21. |
[5] | 李红华,商红涛,王璞,李英明,张庆华,江桂斌.四川省部分地区土壤中六溴环十二烷的分布特征[J].环境化学,2014(09):1439-1444. |
[6] | Yu ZQ;Chen LG;Maw BX;Wu MH;Sheng GY;Fu J;Peng PA .Diastereoisomer- and enantiomer-specific profiles of hexabromocyclododecane in the atmosphere of an urban city in South China[J].Environmental Science & Technology: ES&T,2008(11):3996-4001. |
[7] | Honghua Li,Hongtao Shang,Pu Wang,Yawei Wang,Haidong Zhang,Qinghua Zhang,Guibin Jiang.Occurrence and distribution of hexabromocyclododecane in sediments from seven major river drainage basins in China[J].环境科学学报(英文版),2013(01):69-76. |
[8] | Tomy G;Halldorson T;Danell R.Hexabromocyclododecane (HBCD) isomers and brominated diphenyl ether (BDE) congeners in fish from Lake Winnipeg, Manitoba (Canada)[A].Toronto,Canada,2004 |
[9] | Stapleton H;Dodder N;Kucklick J et al.Determination of HBCD,PBDEs and MeOBDEs in California sea lion stranded between 1993 and 2003[J].Marine Pollution Bulletin,2006,52(5):522-531. |
[10] | Yu-xin Sun;Xiao-jun Luo;Ling Mo;Ming-jing He;Ojang Zhang;She-jun Chen;Fa-sheng Zou;Bi-xian Mai .Hexabromocyclododecane in terrestrial passerine birds from e-waste, urban and rural locations in the Pearl River Delta, South China: Levels, biomagnification, diastereoisomer- and enantiomer-specific accumulation[J].Environmental Pollution,2012(Dec.):191-198. |
[11] | Johnson-Restrepo, B;Adams, DH;Kannan, K .Tetrabromobisphenol A (TBBPA) and hexabromocyclododecanes (HBCDs) in tissues of humans, dolphins, and sharks from the United States[J].Chemosphere,2008(11):1935-1944. |
[12] | ZHI-XIONG SHI;YONG-NING WU;JING-GUANG LI .Dietary Exposure Assessment of Chinese Adults and Nursing Infants to Tetrabromobisphenol-A and Hexabromocyclododecanes: Occurrence Measurements in Foods and Human Milk[J].Environmental Science & Technology: ES&T,2009(12):4314-4319. |
[13] | Roosens L;Abdallah MA;Harrad .Exposure to hexabromocyclododecanes (HBCDs) via dust ingestion, but not diet, correlates with concentrations in human serum: preliminary results.[J].Environmental health perspectives,2009(11):1707-1712. |
[14] | Wagoner E;Baumberger C;Peverly A et al.Electrochemical reduction of 1,2,5,6,9,10-hexabromocyclododecane at carbon and silver cathodes in dimethylformamide[J].Journal of Electroanalytical Chemistry,2014,713:136-142. |
[15] | Feng A;Chen S;Chen M et al.Hexabromocyclododecane (HBCD) and tetrabromobisphenol A (TBBPA) in riverine and estuarine sediments of the Pearl River Delta in southern China with emphasis on spatial variability indiastereoisomer- and enantiomer-specific distribution of HBCD[J].Marine Pollution Bulletin,2012,64(5):919-925. |
[16] | Hunziker R;Gonsior S;MacGregor J et al.Fate and effect of hexabromocyclododecane in the environment[J].Organohalogen Compounds,2004,66:2300-2305. |
[17] | 吴限,祖国仁,高会,方小丹,王艳洁,姚子伟,张志峰,张春枝,那广水.黄海北部近岸多环境介质中六溴环十二烷的分布特征及生物富集[J].环境化学,2014(01):142-147. |
[18] | 张高生,曲久辉,刘会娟,刘锐平,武荣成.活性炭/铁氧化物磁性复合吸附材料的制备及去除水中酸性橙Ⅱ的研究[J].环境科学学报,2006(11):1763-1768. |
[19] | 徐生盼,陈庆军,梁晓怿.三种活性炭对吲哚和吡啶的吸附性能[J].水处理技术,2009(09):19-21,25. |
[20] | 梅凡民,傅成诚,杨青莉,周亮.活性炭表面酸性含氧官能团对吸附甲醛的影响[J].环境污染与防治,2010(03):18-22. |
[21] | 粉末活性炭粒径对水中菲吸附动力学的影响效应研究[J].环境科学学报,2013(01):67-72. |
[22] | F. Bouhamed;Z. Elouear;J. Bouzid;B. Ouddane .Batch sorption of Pb(Ⅱ) ions from aqueous solutions using activated carbon prepared from date stones: equilibrium, kinetic, and thermodynamic studies[J].Desalination and water treatment: Science and engineering,2014(10/12):2261-2271. |
[23] | S. Vasiliu;I. Bunia;S. Racovita .Adsorption of cefotaxime sodium salt on polymer coated ion exchange resin microparticles: Kinetics, equilibrium and thermodynamic studies[J].Carbohydrate Polymers: Scientific and Technological Aspects of Industrially Important Polysaccharides,2011(2):376-387. |
[24] | 朱步瑶;赵振国.界面化学基础[M].北京:化学工业出版社,1996:247-256. |
[25] | 高强,徐耀,吴东,孙予罕.氨基酸在固体表面的吸附[J].化学进展,2007(06):1016-1025. |
- 下载量()
- 访问量()
- 您的评分:
-
10%
-
20%
-
30%
-
40%
-
50%