Cu~(2+)和Pb~(2+)在BS-12两性修饰膨润土上的吸附及其交互作用
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摘要
两性表面修饰可以同时提高黏土矿物对有机物、重金属的吸附性能,研究两性修饰土对多种重金属共存条件下的吸附及交互作用对于其应用具有实际意义.采用红外光谱(FTIR)对膨润土(CK)和150BS-12修饰土(150BS-12)吸附金属离子前后进行表征,通过批处理法研究不同比例BS-12修饰膨润土对Cu~(2+)和Pb~(2+)在单一及Cu-Pb复合体系中的平衡吸附特征和差异,并探讨金属离子在修饰土样上的交互作用机制.结果表明,供试土样在单一及复合体系中对Cu~(2+)和Pb~(2+)的吸附量均呈150BS-12> 100BS-12> 50BS-12> CK的顺序,吸附均符合Freundlich和Langmuir模型; BS-12修饰更有利于Cu~(2+)的吸附,但Pb~(2+)在BS-12修饰土样上的吸附量及选择性系数均大于Cu~(2+); Cu-Pb复合体系中,两种金属离子存在相互拮抗的作用,BS-12修饰在减弱Pb~(2+)对Cu~(2+)的拮抗作用的同时增强了Cu~(2+)对Pb~(2+)的拮抗作用,但Pb~(2+)对Cu~(2+)的拮抗作用仍大于Cu~(2+)对Pb~(2+)的拮抗作用;温度升高、p H升高和离子强度降低均能增加对Cu~(2+)和Pb~(2+)的吸附,但其对两种金属离子的影响程度不同,也导致对金属离子间的交互作用产生影响.
Amphoteric modification can simultaneously improve the adsorption of organic pollutants and heavy metals on clay minerals.Study of the adsorption and interaction of multiple heavy metals on amphoteric modified soils is therefore of practical significance.Here,bentonite-( CK) and 150 BS-12-modified bentonites( 150 BS-12) were characterized both before and after metal ion adsorption using Fourier-transform infrared spectroscopy( FTIR). The equilibrium adsorption characteristics and differences of Cu~(2+)and Pb~(2+)in single and binary systems were studied by batch methods. The interaction mechanism of the metals on modified bentonites is also discussed. The results showed that the adsorption capacity of Cu~(2+)and Pb~(2+)in single and binary systems was ranked,in descending order,as 150 BS-12 > 100 BS-12 > 50 BS-12 > CK,and that the adsorption isotherm could be described by the Langmuir and Freundlich equations. Although the modification of BS-12 was more beneficial for the adsorption of Cu~(2+),the adsorption capacity and selectivity coefficient of Pb~(2+)on BS-12-modified bentonites were larger than for Cu~(2+). Cu~(2+)and Pb~(2+)had a mutually antagonistic effect on each other; modification with BS-12 enhanced the effect of Cu~(2+)on Pb~(2+)and weakened the effect of Pb~(2+)on Cu~(2+),which was always stronger than the effect of Cu~(2+)on Pb~(2+). Increases in temperature and p H,and a reduction in ionic strength,can increase the adsorption of Cu~(2+)and Pb~(2+); however,the influence of these factors varied between the two metals,which also affected the interaction between the metals.
Amphoteric modification can simultaneously improve the adsorption of organic pollutants and heavy metals on clay minerals.Study of the adsorption and interaction of multiple heavy metals on amphoteric modified soils is therefore of practical significance.Here,bentonite-( CK) and 150 BS-12-modified bentonites( 150 BS-12) were characterized both before and after metal ion adsorption using Fourier-transform infrared spectroscopy( FTIR). The equilibrium adsorption characteristics and differences of Cu~(2+)and Pb~(2+)in single and binary systems were studied by batch methods. The interaction mechanism of the metals on modified bentonites is also discussed. The results showed that the adsorption capacity of Cu~(2+)and Pb~(2+)in single and binary systems was ranked,in descending order,as 150 BS-12 > 100 BS-12 > 50 BS-12 > CK,and that the adsorption isotherm could be described by the Langmuir and Freundlich equations. Although the modification of BS-12 was more beneficial for the adsorption of Cu~(2+),the adsorption capacity and selectivity coefficient of Pb~(2+)on BS-12-modified bentonites were larger than for Cu~(2+). Cu~(2+)and Pb~(2+)had a mutually antagonistic effect on each other; modification with BS-12 enhanced the effect of Cu~(2+)on Pb~(2+)and weakened the effect of Pb~(2+)on Cu~(2+),which was always stronger than the effect of Cu~(2+)on Pb~(2+). Increases in temperature and p H,and a reduction in ionic strength,can increase the adsorption of Cu~(2+)and Pb~(2+); however,the influence of these factors varied between the two metals,which also affected the interaction between the metals.
引文
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[11]王建涛,孟昭福,杨亚提,等. SDS对两性修饰膨润土吸附Cd2+的影响[J].环境科学,2014,35(7):2596-2603.Wang J T,Meng Z F,Yang Y T,et al. Effect of SDS on the adsorption of Cd2+onto amphoteric modified bentonites[J].Environmental Science,2014,35(7):2596-2603.
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[17]谢婷,李文斌,孟昭福,等. BS-12+DTAB复配修饰膨润土吸附Cr(Ⅵ)和Cd2+的研究[J].农业环境科学学报,2017,36(9):1778-1786.Xie T,Li W B,Meng Z F,et al. Studies on Cr(Ⅵ)and Cd2+adsorption onto bentonite modified by a BS-12+DTAB complex[J]. Journal of Agro-Environment Science,2017,36(9):1778-1786.
[18]李文斌.两性-阴(阳)离子复配修饰黏土的修饰机制及其对菲、Cr(Ⅵ)的吸附[D].杨凌:西北农林科技大学,2016.50-54.Li W B. Modification mechanism of amphiphilic-cationic and amphiphilic-anionic modified clay and its adsorption to phenanthrene and Cr(Ⅵ)[D]. Yangling:Northwest A&F University,2016. 50-54.
[19]任爽,孟昭福,王腾,等.阳(阴)离子复配修饰两性磁性膨润土的表面特征差异及对苯酚吸附的影响[J].环境科学,2018,39(1):187-194.Ren S,Meng Z F,Wang T,et al. Comparison of amphotericcationic and amphoteric-anionic modified magnetic bentonites:characterization and sorption capacity of Phenol[J].Environmental Science,2018,39(1):187-194.
[20] Zhu K C,Jia H Z,Wang F,et al. Efficient removal of Pb(Ⅱ)from aqueous solution by modified montmorillonite/carbon composite:equilibrium, kinetics, and thermodynamics[J].Journal of Chemical&Engineering Data,2017,62(1):333-340.
[21] Arfaoui S,Frini-Srasra N,Srasra E. Modelling of the adsorption of the chromium ion by modified clays[J]. Desalination,2008,222(1-3):474-481.
[22]孟昭福,李婷,杨淑英,等. BS-12两性修饰膨润土对Cd(Ⅱ)的吸附[A].见:农业环境与生态安全———第五届全国农业环境科学学术研讨会论文集[C].南京:农业部环境保护科研监测所,中国农业生态环境保护协会,2013. 150-157.
[23]刘娟娟,梁东丽,吴小龙,等. Cr(Ⅵ)对两种黏土矿物在单一及复合溶液中Cu(Ⅱ)吸附的影响[J].环境科学,2014,35(1):254-262.Liu J J,Liang D L,Wu X L,et al. Effect of Cr(Ⅵ)anions on the Cu(Ⅱ)adsorption behavior of two kinds of clay minerals in single and binary solution[J]. Environmental Science,2014,35(1):254-262.
[24]孟昭福,张一平.有机修饰改性土对镉离子的吸附及温度效应[J].土壤学报,2005,42(2):238-246.Meng Z F,Zhang Y P. Cd2+adsorption of organic modified soils and its temperature effect[J]. Acta Pedologica Sinica,2005,42(2):238-246.
[25]张雪萍.膨润土的改性及其对部分重金属离子的吸附研究[D].湘潭:湘潭大学,2014. 25-32.Zhang X P. Adsorption of some heavy metal ions from aqueous solution by modified bentonite[D]. Xiangtan:Xiangtan University,2014. 25-32.
[26]刘晶晶. Pb(Ⅱ)、Cu(Ⅱ)、Cd(Ⅱ)在黄土上竞争吸附及解吸特性研究[D].杭州:浙江大学,2014. 88-90.Liu J J. Competitive adsorption and desorption behavior of loess soil towards Pb(Ⅱ),Cu(Ⅱ)and Cd(Ⅱ)[D]. Hangzhou:Zhejiang University,2014. 88-90.
[27] Li Y R,Bai P,Yan Y,et al. Removal of Zn2+,Pb2+,Cd2+,and Cu2+from aqueous solution by synthetic clinoptilolite[J].Microporous and Mesoporous Materials,2019,273:203-211.
[28] Wang X K,Liu X P. Effect of pH and concentration on the diffusion of radiostrontium in compacted bentonite-a capillary experimental study[J]. Applied Radiation and Isotopes,2004,61(6):1413-1418.
[29]徐仁扣,肖双成,蒋新,等. pH对Cu(Ⅱ)和Pb(Ⅱ)在可变电荷土壤表面竞争吸附的影响[J].土壤学报,2006,43(5):871-874.Xu R K,Xiao S C,Jiang X,et al. Effect of pH on competitive adsorption of Cu(Ⅱ)and Pb(II)on variable charge soils[J].Acta Pedologica Sinica,2006,43(5):871-874.
[2] Anna B, Kleopas M, Constantine S, et al. Adsorption of Cd(Ⅱ),Cu(Ⅱ),Ni(Ⅱ)and Pb(Ⅱ)onto natural bentonite:study in mono-and multi-metal systems[J]. Environmental Earth Sciences,2015,73(9):5435-5444.
[3] Du H H,Chen W L,Cai P,et al. Competitive adsorption of Pb and Cd on bacteria-montmorillonite composite[J]. Environmental Pollution,2016,218:168-175.
[4] Sheikhhosseini A,Shirvani M,Shariatmadari H. Competitive sorption of nickel,cadmium,zinc and copper on palygorskite and sepiolite silicate clay minerals[J]. Geoderma,2013,192:249-253.
[5] Liu X F,Hicher P,Muresan B,et al. Heavy metal retention properties of kaolin and bentonite in a wide range of concentration and different pH conditions[J]. Applied Clay Science,2016,119:365-374.
[6]孟昭福,满楠,邓晶,等.几种土壤在单一Zn及Cd Cu共存条件下对Zn的吸附[J].土壤通报,2012,43(2):379-385.Meng Z F,Man N,Deng J,et al. Adsorption of Zn in different soils with single Zn or Zn in combination with Cd and Cu[J].Chinese Journal of Soil Science,2012,43(2):379-385.
[7] He S R,Li Y T,Weng L P,et al. Competitive adsorption of Cd2+, Pb2+, and Ni2+onto Fe3+-modified argillaceous limestone:influence of pH,ionic strength and natural organic matters[J]. Science of the Total Environment,2018,637-638:69-78.
[8] Wang T,Liu W,Xiong L,et al. Influence of p H,ionic strength and humic acid on competitive adsorption of Pb(Ⅱ),Cd(Ⅱ)and Cr(Ⅲ)onto titanate nanotubes[J]. Chemical Engineering Journal,2013,215-216:366-374.
[9] Meng Z F,Zhang Y P,Zhang Z Q. Simultaneous adsorption of phenol and cadmium on amphoteric modified soil[J]. Journal of Hazardous Materials,2008,159(2-3):492-498.
[10] Meng Z F,Zhang Y P,Wang G D. Sorption of heavy metal and organic pollutants on modified soils[J]. Pedosphere,2007,17(2):235-245.
[11]王建涛,孟昭福,杨亚提,等. SDS对两性修饰膨润土吸附Cd2+的影响[J].环境科学,2014,35(7):2596-2603.Wang J T,Meng Z F,Yang Y T,et al. Effect of SDS on the adsorption of Cd2+onto amphoteric modified bentonites[J].Environmental Science,2014,35(7):2596-2603.
[12]李婷.两性修饰膨润土对苯酚和Cd(Ⅱ)的平衡吸附特征[D].杨凌:西北农林科技大学,2012. 5-10.Li T. Equilibrium adsorption characteristics of amphoteric modified bentonites to Cd(Ⅱ)and phenol[D]. Yangling:Northwest A&F University,2012. 5-10.
[13] Ma L Y,Chen Q Z,Zhu J X,et al. Adsorption of phenol and Cu(Ⅱ)onto cationic and zwitterionic surfactant modified montmorillonite in single and binary systems[J]. Chemical Engineering Journal,2016,283:880-888.
[14]张斌.两性修饰膨润土对苯酚、Cd2+复合污染吸附动力学研究[D].杨凌:西北农林科技大学,2012. 52-55.Zhang B. Studies on the adsorption kinetics of phenol and Cd2+in amphoteric modified bentonites[D]. Yangling:Northwest A&F University,2012. 52-55.
[15] Zhu J X,Zhang P,Qing Y H,et al. Novel intercalation mechanism of zwitterionic surfactant modified montmorillonites[J]. Applied Clay Science,2017,141:265-271.
[16] Li W B,Liu Z,Meng Z F,et al. Composite modification mechanism of cationic modifier to amphoteric modified kaolin and its effects on surface characteristics[J]. International Journal of Environmental Science and Technology,2016,13(11):2639-2648.
[17]谢婷,李文斌,孟昭福,等. BS-12+DTAB复配修饰膨润土吸附Cr(Ⅵ)和Cd2+的研究[J].农业环境科学学报,2017,36(9):1778-1786.Xie T,Li W B,Meng Z F,et al. Studies on Cr(Ⅵ)and Cd2+adsorption onto bentonite modified by a BS-12+DTAB complex[J]. Journal of Agro-Environment Science,2017,36(9):1778-1786.
[18]李文斌.两性-阴(阳)离子复配修饰黏土的修饰机制及其对菲、Cr(Ⅵ)的吸附[D].杨凌:西北农林科技大学,2016.50-54.Li W B. Modification mechanism of amphiphilic-cationic and amphiphilic-anionic modified clay and its adsorption to phenanthrene and Cr(Ⅵ)[D]. Yangling:Northwest A&F University,2016. 50-54.
[19]任爽,孟昭福,王腾,等.阳(阴)离子复配修饰两性磁性膨润土的表面特征差异及对苯酚吸附的影响[J].环境科学,2018,39(1):187-194.Ren S,Meng Z F,Wang T,et al. Comparison of amphotericcationic and amphoteric-anionic modified magnetic bentonites:characterization and sorption capacity of Phenol[J].Environmental Science,2018,39(1):187-194.
[20] Zhu K C,Jia H Z,Wang F,et al. Efficient removal of Pb(Ⅱ)from aqueous solution by modified montmorillonite/carbon composite:equilibrium, kinetics, and thermodynamics[J].Journal of Chemical&Engineering Data,2017,62(1):333-340.
[21] Arfaoui S,Frini-Srasra N,Srasra E. Modelling of the adsorption of the chromium ion by modified clays[J]. Desalination,2008,222(1-3):474-481.
[22]孟昭福,李婷,杨淑英,等. BS-12两性修饰膨润土对Cd(Ⅱ)的吸附[A].见:农业环境与生态安全———第五届全国农业环境科学学术研讨会论文集[C].南京:农业部环境保护科研监测所,中国农业生态环境保护协会,2013. 150-157.
[23]刘娟娟,梁东丽,吴小龙,等. Cr(Ⅵ)对两种黏土矿物在单一及复合溶液中Cu(Ⅱ)吸附的影响[J].环境科学,2014,35(1):254-262.Liu J J,Liang D L,Wu X L,et al. Effect of Cr(Ⅵ)anions on the Cu(Ⅱ)adsorption behavior of two kinds of clay minerals in single and binary solution[J]. Environmental Science,2014,35(1):254-262.
[24]孟昭福,张一平.有机修饰改性土对镉离子的吸附及温度效应[J].土壤学报,2005,42(2):238-246.Meng Z F,Zhang Y P. Cd2+adsorption of organic modified soils and its temperature effect[J]. Acta Pedologica Sinica,2005,42(2):238-246.
[25]张雪萍.膨润土的改性及其对部分重金属离子的吸附研究[D].湘潭:湘潭大学,2014. 25-32.Zhang X P. Adsorption of some heavy metal ions from aqueous solution by modified bentonite[D]. Xiangtan:Xiangtan University,2014. 25-32.
[26]刘晶晶. Pb(Ⅱ)、Cu(Ⅱ)、Cd(Ⅱ)在黄土上竞争吸附及解吸特性研究[D].杭州:浙江大学,2014. 88-90.Liu J J. Competitive adsorption and desorption behavior of loess soil towards Pb(Ⅱ),Cu(Ⅱ)and Cd(Ⅱ)[D]. Hangzhou:Zhejiang University,2014. 88-90.
[27] Li Y R,Bai P,Yan Y,et al. Removal of Zn2+,Pb2+,Cd2+,and Cu2+from aqueous solution by synthetic clinoptilolite[J].Microporous and Mesoporous Materials,2019,273:203-211.
[28] Wang X K,Liu X P. Effect of pH and concentration on the diffusion of radiostrontium in compacted bentonite-a capillary experimental study[J]. Applied Radiation and Isotopes,2004,61(6):1413-1418.
[29]徐仁扣,肖双成,蒋新,等. pH对Cu(Ⅱ)和Pb(Ⅱ)在可变电荷土壤表面竞争吸附的影响[J].土壤学报,2006,43(5):871-874.Xu R K,Xiao S C,Jiang X,et al. Effect of pH on competitive adsorption of Cu(Ⅱ)and Pb(II)on variable charge soils[J].Acta Pedologica Sinica,2006,43(5):871-874.
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