交互作用对有机-矿质复合体吸附四环素的影响
The impact of interaction on organic-mineral complexes adsorb tetracycline
-
摘要: 为探究有机质与矿物质间交互作用对有机-矿质复合体吸附典型药物的影响,并明确其与有机质含量、制备时间之间的关系,以腐殖酸和高岭土分别代表有机质和矿物质、以四环素(TC)为模式药物进行吸附续批实验研究.结果表明,有机-矿质复合体对TC的吸附符合Langmuir和Freundlich等温线.交互作用对于复合体吸附TC具有显著的抑制作用,且抑制作用的强弱与腐殖酸含量和复合体制备时间有关.当腐殖酸含量从0.5%增至1.0%时,负载于高岭土表面的腐殖酸使复合体表面不光滑,交互作用对复合体吸附TC的抑制强度减弱;当腐殖酸含量从1.0%增至2.0%时,其与TC之间出现竞争吸附,交互作用对复合体吸附TC的抑制强度增强;当腐殖酸含量从2.0%增至5.0%时,腐殖酸的强吸附能力抵消了其对高岭土吸附TC的竞争抑制作用,交互作用对复合体吸附TC的抑制强度减弱.制备时间不同时,交互作用通常会抑制复合体对TC的吸附,并且随制备时间增长呈现先增强后减弱的趋势.Abstract: In order to explore the effect of interaction between organic matter and mineral on the adsorption of typical pharmaceuticals by organic-mineral complex, and to clarify the relationship between the interaction and the content of organic matter and the preparation time, the adsorption batch experiment was carried out with humic acid and kaolin representing organic matter and mineral respectively, and tetracycline (TC) as model drug. The results showed that the adsorption of TC by organic-mineral complex conforms to the Langmuir and Freundlich isotherms. The interaction had a significant inhibitory effect on the adsorption of the TC by the complex, and the degree of inhibition was related to the content of humic acid and the preparation time of the composite. When the content of humic acid increased from 0.5% to 1.0%, the humic acid loaded on the surface of kaolin made the surface of the complex not smooth, and the inhibition intensity of interaction on the adsorption of TC was weakened. When the content of humic acid increased from 1.0% to 2.0%, there may be competitive adsorption between humic acid and TC, and the inhibition intensity of interaction on TC adsorption was enhanced. When the content of humic increased from 2.0% to 5.0%, strong adsorption capacity of humic acid counteracted its competitive inhibition on the adsorption of TC by kaolin, and the inhibition of interaction on the adsorption of TC by the complex was weakened. When the preparation time is different, the interaction between humic acid and kaolin generally suppressed the adsorption of the TC by the complex, and increased at first and then decreased with the increase in preparation time.
-
Key words:
- interaction /
- adsorption /
- humic acid /
- kaolin /
- tetracycline
-
-
[1] KVMMERER K. Antibiotics in the aquatic environment-A review-Part Ⅰ[J]. Chemosphere, 2009, 75(4):417-434. [2] KVMMERER K. Antibiotics in the aquatic environment-A review-Part Ⅱ[J]. Chemosphere, 2009, 75(4):435-441. [3] LI Z, SCHULZ L, ACKLEY C, et al. Adsorption of tetracycline on kaolinite with pH-dependent surface charges[J]. Journal of Colloid and Interface Science, 2010, 351(1):254-260. [4] KIM K R, OWENS G, KWON S I, et al. Occurrence and environmental fate of veterinary antibiotics in the terrestrial environment[J]. Water, Air, & Soil Pollution, 2011, 214:163-174. [5] BOUND J, VOULVOULIS N. Pharmaceuticals in the aquatic environment-a comparison of risk assessment strategies[J]. Chemosphere, 2004, 56(11):1143-1155. [6] BOXALL A, KOLPIN D, HALLING-S B, JOHANNES T, et al. Peer reviewed:Are veterinary medicines causing environmental risks?[J]. Environmental Science & Technology, 2003, 37(15):286-294. [7] ZHAO Y, GU X, GAO S, et al. Adsorption of tetracycline (TC) onto montmorillonite:Cations and humic acid effects[J]. Geoderma, 2012, 183/184:12-18. [8] DAUGHTON C G, TERNES T A. Pharmaceuticals and personal care products in the environment:Agents of subtle change?[J]. Environmental Health Perspectives, 1999, 107(6):907-938. [9] 张俊, 杨晓洪, 葛峰, 等. 长期施用四环素残留猪粪对土壤中耐药菌及抗性基因形成的影响[J]. 环境科学, 2014, 35(6):2374-2380. ZHANG J, YANG X H, GE F, et al. Effects of long-term application of pig manure containing residual tetracycline on the formation of drug-resistant bacteria and resistance genes[J]. Environment Science, 2014, 35(6):2374-2380(in Chinese).
[10] 张婷. 四环素类抗生素在土壤中的吸附/解吸行为研究[D]. 阜新:辽宁工程技术大学, 2015. ZHANG T. Adsorption/desorption behavior of tetracycline antibiotic in soils[D]. Fuxing:Liaoning Technical University,2015(in Chinese). [11] 鲍艳宇. 四环素类抗生素在土壤中的环境行为及生态毒性研究[D]. 天津:南开大学, 2008. BAO Y Y. Environmental behavior and ecotoxicity of tetracycline antibiotics in soils[D]. Tianjin:Nankai University, 2008(in Chinese). [12] GU C, KARTHIKEYAN K G, SIBLEY S D, et al. Complexation of the antibiotic tetracycline with humic acid[J]. Chemosphere, 2007, 66(8):1494-1501. [13] 吴敏, 宁平, 刘书言. 土壤有机质对诺氟沙星的吸附特征[J]. 环境化学, 2013, 32(1):112-117. WU M, NING P, LIU S Y. Adsorption characteristics of norfloxacin in soil organic matter fractions[J]. Environmental Chemistry, 2013,32(1):112-117(in Chinese).
[14] YOON T H, JOHNSON S B, BROWN G E. Adsorption of organic matter at mineral/water interfaces. IV. adsorption of humic substances at boehmite/water interfaces and impact on boehmite dissolution[J]. Langmuir, 2005, 21(11):5002-5012. [15] KRETZSCHMAR R, STICHER H, HESTERBERG D. Effects of adsorbed humic acid on surface charge and flocculation of kaolinite[J]. Soil Science Society of America Journal, 1997, 61(1):101-108. [16] WANG K, XING B. Structural and sorption characteristics of adsorbed humic acid on clay minerals[J]. Journal of Environmental Quality, 2005, 34(1):342-349. [17] HUI L, SHENG G, TEPPEN B J, et al. Sorption and desorption of pesticides by clay minerals and humic acid-clay complexes[J]. Soil Science Society of America Journal, 2003, 67(1):122-131. [18] GUA C, KARTHIKEYAN K G. Sorption of the antibiotic tetracycline to humic-mineral complexes[J]. Journal of Environmental Quality, 2008, 37(2):704-711. [19] 王超, 王迎亚, 陈宁华, 等. 磁性膨润土对四环素的吸附特性[J]. 精细化工, 2017, 34(10):1185-1193. WANG C, WANG Y Y, CHEN N H, et al. Adsorption of tetracycline by magnetic bentonite[J]. Fine Chemicals,2017, 34(10):1185-1193(in Chinese).
[20] PILS J R V, LAIRD D A. Sorption of tetracycline and chlortetracycline on K-and Ca-saturated soil clays, humic substances, and clay-Humic complexes[J]. Environmental Science & Technology, 2007, 41(6):1928-1933. [21] 彭流月. C/M值对不同环境中有机-矿质复合体形成机制影响[D]. 北京:中国地质大学(北京), 2019. PENG L Y. Formation mechanism of organic-mineral complexes affected by various values of C/M in conditions of different temperature and pressure[D]. Beijing:China University of Geosciences (Beijing), 2019(in Chinese). [22] REN X, WANG F, ZHANG P, et.al. Aging effect of minerals on biochar properties and sorption capacities for atrazine and phenanthrene[J]. Chemosphere, 2018, 206:51-58. [23] 王磊, 孙成, 郭会琴. 土壤有机质对疏水性有机污染物的非线性吸附及其影响因素[J]. 土壤, 2012, 44(3):366-373. WANG L, SUN C, GUO H Q. Non-linear adsorption of soil organic matter to hydrophobic organic pollutants and its influencing factors[J]. Soils, 2012, 44(3):366-373(in Chinese).
[24] 许中坚, 刘广深, 刘维屏. 土壤中溶解性有机质的环境特性与行为[J]. 环境化学, 2003, 22(5):427-433. XU Z J,LIU G S,LIU W P. Environmental characteristic and behavior of dissolved organic matter in soils[J]. Environmental Chemistry, 2003, 22(5):427-433(in Chinese).
[25] POLLARD S J T, SOLLARS C J, R P. A low cost adsorbent from spent bleaching earth. I-the selection of an activation procedure[J]. Journal of Chemical Technology & Biotechnology, 1991, 50(2):265-275. [26] 朱晓婧, 何江涛, 苏思慧. 腐殖酸-高岭土复合体形成机制及对三氯乙烯的吸附[J]. 环境科学, 2015, 36(1):227-236. ZHU X J, HE J T, SU S H. Forming mechanism of humic Acid-Kaolin complexs and the adsorption of trichloroethylene[J]. Environment Science, 2015, 36(1):227-236(in Chinese).
[27] 周玲棣, 郭九皋, 袁汉珍, 等. 碱性长石29Si,27Al核磁共振谱研究[J]. 中国科学(B辑化学生命科学地学), 1994, 24(4):434-440. ZHOU L L,GUO J G, YUAN H Z, et al. Study on NMR spectrum of alkaline feldspar 29Si, 27Al[J]. Science In China (series B), 1994, 24(4):434-440(in Chinese). [28] 李小红, 江向平, 陈超, 等. 几种不同产地高岭土的漫反射傅里叶红外光谱分析[J]. 光谱学与光谱分析, 2011, 31(1):114-118. LI X H, JIANG X P, CHEN C, et al. Fourier transform infrared spectroscopic analysis of kaolin clay from several origins[J]. Spectroscopy and Spectral Analysis, 2011, 31(1):114-118(in Chinese).
[29] 顾志忙, 王晓蓉, 顾雪元, 等. 傅里叶变换红外光谱和核磁共振法对土壤中腐殖酸的表征[J]. 分析化学, 2000, 28(3):314-317. GU Z M, WANG X R, GU X Y, et al. Characterization of humic acid in soil by fourier transform infrared spectroscopy and nuclear magnetic resonance[J]. Chinese Journal of Analytical Chemistry, 2000, 28(3):314-317(in Chinese).
[30] 苏思慧, 何江涛, 石钰婷, 等. 模拟有机-矿质体中不同吸附域对TCE的吸附影响[J]. 中国环境科学, 2013, 33(2):234-242. SU S H, HE J T, SHI Y T, et al. The effects on the trichloroethylene sorption behaviors caused by the interactions between different sorption domains in model organic-mineral complexes[J]. China Environmental Science, 2013, 33(2):234-242(in Chinese).
[31] SPARKS D L, CHEN C. The role of mineral complexation and metal redox coupling in carbon cycling and stabilization functions of natural organic matter in changing environment[M]. Germany:Springer, Dordrecht, 2013:7-12. [32] 张小亮, 何江涛, 石钰婷, 等. C/M及TCE初始浓度对有机-矿物质复合体中有机质的吸附行为影响[J]. 岩石矿物学杂志, 2013, 32(6):809-817. ZHANG X L, HE J T, SHI Y T, et al. The influence of C/M and TCE initial concentrations on the organic adsorption behavior in simulated organo-mineral complexes[J]. ACTA Petrolgica Et Mineralogica, 2013, 32(6):809-817(in Chinese).
[33] KAAHWA Y, D'UJANGA F M. Dependence of kaolinite content on particle size distribution in Ugandan kaolin clay[J]. British Ceramic Transactions, 2004, 103(3):143-144. [34] SOUZA S O, SILVA M D M, SANTOS J C C, et.al. Evaluation of different fractions of the organic matter of peat on tetracycline retention in environmental conditions:in vitro studies[J]. Journal of Soils and Sediments, 2016, 16(6):1764-1775. [35] ILLÉS E, TOMBÁCZ E. The effect of humic acid adsorption on pH-dependent surface charging and aggregation of magnetite nanoparticles[J]. Journal of Colloid & Interface Science, 2006, 295(1):115-1123. [36] BARRIUSO E, BAER U, CALVET R. Dissolved organic matter and adsorption-desorption of dimefuron, atrazine, and carbetamide by soils[J]. Journal of Environmental Quality, 1992, 21(3):359-367. [37] 吴沙沙. 可溶性腐殖酸对典型粘土矿物吸附诺氟沙星的影响研究[D]. 北京:中国地质大学(北京), 2014. WU S S. Effests of dissolved humic acid on sorption of norfloxacin onto typical clay minerals[D]. Beijing:China University of Geosciences (Beijing), 2014(in Chinese). [38] 乔肖翠. 有机质及pH对卡马西平吸附及迁移影响研究[D]. 北京:中国地质大学(北京), 2015. QIAO X C. Influences of DOM and pH on adsorption and migrations of carbamazepine[D]. Beijing:China University of Geosciences (Beijing), 2015(in Chinese). [39] 李爱民, 朱燕, 代静玉. 胡敏酸在高岭土上的吸附行为[J]. 岩石矿物学杂志, 2005, 24(2):145-150. LI A M, ZHU Y, DAI J Y. The adsorption behavior of humic acid on kaolin[J]. ACTA Petrolgica Et Mineralogica, 2005, 24(2):145-150(in Chinese).
[40] 吴宏海, 张秋云, 卢平, 等. 土壤和水体环境中矿物-腐殖质交互作用的研究进展[J]. 岩石矿物学杂志, 2003, (4):429-432. WU H H, ZHANG Q Y, LU P, et al. Advances in the study of mineral humus interactions in soils and waters[J]. ACTA Petrolgica Et Mineralogica, 2003 ,22(4):429-432(in Chinese).
-

计量
- 文章访问数: 1756
- HTML全文浏览数: 1756
- PDF下载数: 36
- 施引文献: 0