改性硅藻土对水中DDTs的吸附机理

谭凌智; 祁士华; 张家泉; 张小辉; 柯艳萍; 于佳; 陈静; 严春杰

doi:10.3799/dqkx.2012.071

改性硅藻土对水中DDTs的吸附机理

doi: 10.3799/dqkx.2012.071

谭凌智^{1, 2},
祁士华^1, ,,
张家泉¹,
张小辉¹,
柯艳萍¹,
于佳¹,
陈静¹,
严春杰³

1.
生物地质与环境地质教育部重点实验室, 中国地质大学环境学院, 湖北武汉 430074
2.
长江流域水环境监测中心, 湖北武汉 430010
3.
中国地质大学教育部纳米矿物材料及应用工程研究中心, 湖北武汉 430074

基金项目:

国家自然科学基金项目 41073070

生物地质与环境地质教育部实验室开放基金项目 BGEG1012

详细信息

作者简介:
谭凌智(1982-), 男, 博士研究生, 主要从事地球化学相关工作

通讯作者:
祁士华, E-mail: shihuaqi@cug.edu.cn

中图分类号: X142
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- 被引次数: 0
出版历程
- 收稿日期: 2011-07-23
- 网络出版日期: 2021-11-09
- 刊出日期: 2012-05-01

Removal of DDTs from Water by Modified Diatomite

1.
School of Environmental Studies and Key Laboratory of Biogeology and Environmental Geology of Ministry of Education, China University of Geosciences, Wuhan 430074, China
2.
Yangtze Valley Water Environmental Monitoring Center, Wuhan 430010, China
3.
Engineering Research Center of Nano-Geo Materials of Ministry of Education, China University of Geosciences, Wuhan 430074, China

摘要

摘要: 采用阳离子表面活性剂(十六烷基三甲基溴化铵)对硅藻土进行改性, 并以优选的改性方案为基础, 研究了该有机硅藻土对水中有机氯农药DDTs(p, p'-DDT、p, p'-DDE和p, p'-DDD)的吸附过程及增强机理.结果表明, 十六烷基三甲基溴化铵能有效改变硅藻土的Zeta电位、比表面积和表面疏水性质, 从而提高硅藻土吸附有机氯农药的能力.改性硅藻土对水中3种有机氯农药的吸附能力依次为: p, p'-DDT>p, p'-DDE>p, p'-DDD.基于模型的准确性(R²值)考虑, Redlich-Peterson方程能更好地用于拟合DDTs在改性硅藻土上的等温吸附曲线.
- 硅藻土 /
- 有机改性 /
- 吸附 /
- 有机氯农药
Abstract: This study investigates the adsorption behavior of organochlorine pesticides DDTs (p, p'-DDT, p, p'-DDE and p, p'-DDD) onto organo-diatomite (OD), which was modified by Cetyltrimethylammonium Bromide (CTMAB). The strengthen mechanisms and optimization design of the adsorption process are also discussed. The results show that the cationic surfactant could change the Zeta potential, BET surface area and hydrophobic characteristics of diatomite, which lead to the better adsorption efficiency of DDTs. The adsorption efficiency of the three DDTs onto OD follows the order of p, p'-DDT > p, p'-DDE > p, p'-DDD. According to the value of R², it can be concluded that the Redlich-Peterson model fit best for the adsorption data.
- diatomite /
- organic modification /
- adsorption /
- organochlorine pesticides

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图 1 有机硅藻土在吸附过程中Zeta电位的变化

Fig. 1. The variety of Zeta potential while adsorption by organo-diatomite

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图 2 实验所使用硅藻土及改性剂的红外光谱FTIR

Fig. 2. FTIR spectra of diatomite, organo-diatomite and surfactant

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图 3 负载不同浓度改性剂的硅藻土对DDTs的吸附量

Fig. 3. Amount of DDTs adsorbed on differently surfactant loaded diatomite samples

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图 4 改性剂加入量对单位质量吸附量和AI的影响曲线

Fig. 4. The concentration of suspension versus amount of DDTs adsorbed and adsorption index

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表 1 表面活性剂和有机氯农药(DDTs)的相关理化性质

Table 1. The related physicochemical properties of DDTs and surfactants

化合物名称	分子式	摩尔质量(g/mol)	溶解度(mg/L)	辛醇分配系数(logK_ow)
p, p'-DDE	C₁₄H₈Cl₁₄	318.03	0.12^a	5.70^b
p, p'-DDT	C₁₄H₉C₁₅	354.49	0.025^a	6.36^b
p, p'-DDD	C₁₄H₁₀C₁₄	320.05	0.090^a	5.50^b
CTMAB	C₁₆H₃₃(CH₃)₃NBr	364.45	13 000	-0.48
注：a.Howard and Meylan(1997)；b.Schwarzenbach et al.(2003)；T=25±0.5 ℃，pH=7.0.

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表 2 改性硅藻土的表面结构特征

Table 2. Main surface texture characteristics of organo-diatomite

孔参数	DS	DSY	CDSY	CDSY-5
S_BET(m²/g)	0.433 2	0.713 8	0.603 8	0.585 6
V_mi(cm³/g)	0.001 148	0.000 353	0.000 555	0.000 585

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表 3 不同等温曲线的各项指数和相关系数

Table 3. Adjustable parameters and correlation coefficients for various isotherms

Parameters	R²	K	M	β
p, p'-DDD
Linear	0.98	3.92	-9.48
Freundlich	0.95	0.72		1.66
Langmuir	0.90	3.85E-10	7.79E9
Redlich-Peterson	0.99	96.7	0.005 2	3.12
p, p'-DDE
Linear	0.97	3.97	-22.81
Freundlich	0.98	0.74		1.42
Langmuir	0.92	3.41E-9	9.29E8
Redlich-Peterson	0.99	7 720.28	0.000 09	1.43
p, p'-DDT
Linear	0.99	4.01	-27.27
Freundlich	0.98	0.67		1.43
Langmuir	0.93	3.910 9E-10	7.99E9
Redlich-Peterson	0.99	488.95	0.000 61	1.74

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参考文献(22)

Chen, W., Jing, M.M., Bu, J.W., et al., 2011. Organochlorine pesticides in the surface water and sediments from the Peacock River Drainage basin in Xinjiang, China: a study of an arid zone in Central Asia. Environmental Monitoring and Assessment, 177(1-4): 1-21. doi: 10.1007/s10661-010-1613-2
Daković, A., Tomašević-Čanović, M., Rottinghaus, G., et al., 2003. Adsorption of ochratoxin A on octadecyldimethyl benzyl ammonium exchanged-clinoptilolite-heulandite tuff. Colloids and Surfaces, B: Biointerfaces, 30(1-2): 157-165. doi: 10.1016/S0927-7765(03)00067-5
El-Shahawi, M.S., Hamza, A., Bashammakh, A., et al., 2010. An overview on the accumulation, distribution, transformations, toxicity and analytical methods for the monitoring of persistent organic pollutants. Talanta, 80(5): 1587-1597. doi: 10.1016/j.talanta.2009.09.055
Feng, K., Yu, B.Y., Ge, D.M., et al., 2003. Organo-chlorine pesticide (DDT and HCH) residues in the Taihu Lake region and its movement in soil-water system Ⅰ. Field survey of DDT and HCH residues in ecosystem of the region. Chemosphere, 50(6): 683-687. doi: 10.1016/S0045-6535(02)00204-7
Howard, P.H., Meylan, W.M., 1997. Handbook of physical properties of organic chemicals. CRC Press, Lewis Publishers, Boca Raton.
Imo, T.S., Hirosawa, E., Ali, S.M., et al., 2006. Persistent organochlorine pesticides (OCPs) in river waters of southern part of Okinawa Island, Japan. Geochimica et Cosmochimica Acta, 70(18): A276. doi: 10.1016/j.gca.2006.06.560
Lee, S.Y., Kim, S.J., 2002. Adsorption of naphthalene by HDTMA modified kaolinite and halloysite. Appl. Clay Sci. , 22(1-2): 55-63. doi: 10.1016/S0169-1317(02)00113-6
Lemić, J., Kovačević, D., Tomašević-Čanović, M., et al., 2006. Removal of atrazine, lindane and diazinone from water by organo-zeolites. Water Research, 40(5): 1079-1085. doi: 10.1016/j.watres.2006.01.001
Li, K.Q., Zheng, Z., Luo, X.Z., 2010. Adsorption behavior and influence factors of p-nitroaniline on high Surface area activated carbons prepared from plant stems. Environmental Science, 31(8): 1877-1883 (in Chinese with English abstract). http://www.oalib.com/paper/1588579
Li, Z.H., Willms, C.A., Kniola, K., 2003. Removal of anionic contaminants using surfactant-modified palygorskite and sepiolite. Clays and Clay Miner. , 51(4): 445-451. doi: 10.1346/CCMN.2003.0510411
McNeil-Watson, F., Tscharnuter, W., Miller, J., 1998. A new instrument for the measurement of very small electrophoretic mobilities using phase analysis light scattering(PALS). Colloids and Surfaces A: Physicochemical and Engineering Aspects, 140(1-3): 53-57. doi: 10.1016/S0927-7757(97)00267-7
Roy, M.T., Gallardo, M., Estelrich, J., 1998. Influence of size on electrokinetic behavior of phosphatidylserine and phosphatidylethanolamine lipid vesicles. Journal of Colloid and Interface Science, 206(2): 512-517. doi: 10.1016/jcis.1998.5715
Sanchez-Martin, M.J., Rodriguez-Cruz, M.S., Andrades, M.S., et al., 2006. Efficiency of different clay minerals modified with a cationic surfactant in the adsorption of pesticides: influence of clay type and pesticide hydrophobicity. Applied Clay Science, 31(3-4): 216-228. doi: 10.1016/j.clay.2005.07.008
Schwarzenbach, R.P., Gschwend, P.M., Imboden, D.M., 2003. Environmental organic chemistry, 3ed. . Wiley-Interscience, New York.
Wang, P., Keller, A.A., 2008. Partitioning of hydrophobic organic compounds within soil-water-surfactant systems. Water Research, 42(8-9): 2093-2101. doi: 10.1016/j.watres.2007.11.015
Wang, X.H., Wang, W.X., 2005. Uptake, absorption efficiency and elimination of DDT in marine phytoplankton, copepods and fish. Environmental Pollution, 136(3): 453-464. doi: 10.1016/j.envpol.2005.01.004
Xu, Y., Ge, F., Tao, N.G., et al., 2009. Growth inhibition and mechanism of cetyltrimethyl ammonium chloride on Chlorella vulgaris. Environmental Science, 30(6): 1767-1772 (in Chinese with English abstract). http://www.ncbi.nlm.nih.gov/pubmed/19662866
Zhang, C.X., Wang, Y.X., Qi, S.H., et al., 2008. Adsorption mechanisms between dissolved organic matter and endocrine disruptors from Landfill leachate. Earth Science—Journal of China University of Geosciences, 33(3): 399-404 (in Chinese with English abstract). doi: 10.3799/dqkx.2008.053
Zhang, Z.L., Huang, J., Yu, G., et al., 2004. Occurrence of PAHs, PCBs and organochlorine pesticides in the Tonghui River of Beijing, China. Environmental Pollution, 130(2): 249-261. doi: 10.1016/j.envpol.2003.12.002
李坤权, 郑正, 罗兴章, 2010. 高比表面植物基活性炭吸附水中对硝基苯胺的性能及影响因素. 环境科学, 31(8): 1877-1883. https://www.cnki.com.cn/Article/CJFDTOTAL-HJKZ201008029.htm
许银, 葛飞, 陶能国, 等, 2009. 十六烷基三甲基氯化铵抑制小球藻生长的效应及作用机制. 环境科学, 30(6): 1767-1772. https://www.cnki.com.cn/Article/CJFDTOTAL-HJKZ200906037.htm
张彩香, 王焰新, 祁士华, 等, 2008. 垃圾渗滤液中溶解有机质与内分泌干扰物的吸附机理. 地球科学——中国地质大学学报, 33(3): 399-404. https://www.cnki.com.cn/Article/CJFDTOTAL-DQKX200803016.htm