功能化杯[4]芳烃对称硫醚衍生物的制备及其对铀的吸附行为
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摘要
以1,3-二溴丙烷对对叔丁基杯[4]芳烃的下沿进行修饰,再利用Na_2S·9H_2O合成制备一种新型的吸附材料杯[4]芳烃对称硫醚衍生物,并研究其吸附铀的主要影响因素,即U(Ⅵ)溶液pH值、吸附剂投入量、铀初始浓度及反应时间,分析其吸附过程的反应动力学和等温吸附规律。结果表明:当温度为25℃时,杯[4]芳烃对称硫醚衍生物吸附铀的最佳条件是pH值为4.0,铀初始浓度为20mg/L,杯[4]芳烃对称硫醚衍生物加入量为20mg以及吸附平衡时间为6h。杯[4]芳烃对称硫醚衍生物对铀的吸附动力学符合准二级动力学模型,吸附过程为化学吸附,相关系数为0.9998;Langmuir、D-R和Freundlich等温线均可较好地拟合吸附过程,说明该吸附体系是一个单层覆盖与多层吸附相结合的模式。红外谱图表明,杯[4]芳烃对称硫醚衍生物吸附一定质量的铀后,在817.82cm~(-1)和810.10 cm~(-1)处出现了铀酰离子的伸缩振动峰,且未发生主要的结构形态变化。
By modifying the lower edge of tert butyl calix [4] arene with 1,3-dibromopropane, and then utilizing Na_2 S·9 H_2 O to prepare a new type of absorption material, that is calix [4] arene symmetric sulfide derivatives. The main influence factors of the uranium adsorption, such as pH value of U(Ⅵ) solution, input of adsorbent, initial concentration of uranium and reaction time, were explored, finally the reaction kinetics and adsorption isothermal law of adsorption process were analyzed. The results show that, the best condition of uranium adsorption are as follows: pH value of 4.0,initial concentration of uranium of 20 mg/L, addition adsorbent of 20 mg, adsorption equilibration time of 6 h at 25 ℃.The adsorption kinetics of calix [4] arene symmetric sulfide derivatives to uranium is accorded with pseudo-second order model. The adsorption process which is better fitted by Langmuir, D-R and Freundlich sorption isotherm is chemisorption and its correlation is 0.9998. The adsorption system is a single layer covering combined with multilayer adsorption model.And the infrared spectrum shows that, after adsorbing, a certain quality of uranium by calix [4] arene symmetric sulfide derivatives. In 817.82 cm~(-1 )and 810.10 cm~(-1), the stretching vibrations of uranyl ion peak appears and the main structure morphology does not change.
By modifying the lower edge of tert butyl calix [4] arene with 1,3-dibromopropane, and then utilizing Na_2 S·9 H_2 O to prepare a new type of absorption material, that is calix [4] arene symmetric sulfide derivatives. The main influence factors of the uranium adsorption, such as pH value of U(Ⅵ) solution, input of adsorbent, initial concentration of uranium and reaction time, were explored, finally the reaction kinetics and adsorption isothermal law of adsorption process were analyzed. The results show that, the best condition of uranium adsorption are as follows: pH value of 4.0,initial concentration of uranium of 20 mg/L, addition adsorbent of 20 mg, adsorption equilibration time of 6 h at 25 ℃.The adsorption kinetics of calix [4] arene symmetric sulfide derivatives to uranium is accorded with pseudo-second order model. The adsorption process which is better fitted by Langmuir, D-R and Freundlich sorption isotherm is chemisorption and its correlation is 0.9998. The adsorption system is a single layer covering combined with multilayer adsorption model.And the infrared spectrum shows that, after adsorbing, a certain quality of uranium by calix [4] arene symmetric sulfide derivatives. In 817.82 cm~(-1 )and 810.10 cm~(-1), the stretching vibrations of uranyl ion peak appears and the main structure morphology does not change.
引文
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[16]彭国文,丁德馨,胡南,杨雨山,王晓亮.纳米Fe3O4负载啤酒酵母菌对铀的吸附性能与机理[J].中国有色金属学报,2012,22(2):604-610.PENG Guo-wen,DING De-xin,HU Nan,YANG Yu-shan,WANG Xiao-liang.Adsorption properties and mechanism of saccharomyces cerevisiae loaded by Nano-Fe3O4 on uranium[J].The Chinese Journal of Nonferrous Metals,2012,22(2):604-610.
[17]GUTSCHE C D,IQBAL M.P-tert-butylcalix[4]arene[J].Organic Syntheses,1986,68:243-244.
[2]PENG Guo-wen,DING De-xin,XIAO Fang-zhu,WANGXiao-liang,HU Nan,WANG Yong-dong,DAI Yi-min,CAOZheng.Adsorption of uranium ions from aqueous solution by amine group functionalized magnetic Fe3O4nanoparticle[J].J Radioanal Nucl Chem,2014,301:781-788.
[3]XIAO Fang-zhu,PENG Guo-wen,DING De-xin,DAI Yi-min.Preparation of a novel biosorbent ISCB and its adsorption and desorption properties of uranium ions in aqueous solution[J].JRadioanal Nucl Chem,2015,306:349-356.
[4]WANG Xiao-liang,PENG Guo-wen,YANG Yan,WANGYang-fei,HE Ting-ting.Uranium adsorption by dry and wet immobilized Saccharomyces cerevisiae[J].J Radioanal Nucl Chem,2012,291:825-830.
[5]RAHMAN R O,IBRAHIUM H A,HUNG Y T.Liquid radioactive wastes treatment:A review[J].Water,2011,3(2):551-565.
[6]WANG Jing-song,BAO Zheng-lei,CHEN Si-guang,YANGJin-hui.Removal of Uranium from aqueous solution by chitosan and ferrous ions[J].Journal of Engineering for Gas Turbines and Power-Transactions of The Asme,2011,133(8):084502.
[7]SHINKAI S.Calixarenes-the third generation of supramolecules[J].Tetrahdron,1993,49(40):8933-8968.
[8]BOHMER V.Calixarenes macrocycles with(almost)unlimited possibilities[J].Angewandte Chemie-International Edition,1995,34(2):713-745.
[9]IKEDA A.ASHINKAL S.Novel cavity design using calix[n]arene skeletons:toward molecular recognition and metal binding[J].Chemical Review,1997,97(5):1713-1734.
[10]GUTSCHE C D,IQBAL M,NAM K S,SEE K,ALAM I.Conformational and complexational characteristics of calixarenes[J].Pure and Applied Chemistry,1988,60(4):483-488.
[11]OZCAN F,BAYRAKAL M,ERTUL?.Synthesis and characterization of novel nanofiber based calixarene and its binding efficiency towards chromium and uranium ions[J].Journal of Inclusion Phenomena and Macrocyclic Chemistry,2016,85(1/2):49-58.
[12]OZCAN F,BAYRAKAL M,ERTUL?.Synthesis and preparation of novel magnetite nanoparticles containing calix[4]arenes with different chelating group towards uranium anions[J].Journal of Macromolecular Science,Part A:Pure and Applied Chemistry,2015,52(8):599-608.
[13]SALMN L,THUERY P,EPHRITIKHINE M.Uranium(Ⅳ)complexes of calix[n]arenes(n=4,6 and 8)[J].Chemical Communications,2006(8):856-858.
[14]SHRINER R L,STRUCK H C,JORISON W J.The preparation and properties of certain sulfoxides and sulfones[J].Journal of the American Chemical Society,1930,52(5):2060-2069.
[15]TARBELL D SWEAVER C.The condensation of sulfoxides with P-toluenesulfonamide and substituted acetamides[J].Journal of the American Chemical Society,1941,63(11):2939-2942.
[16]彭国文,丁德馨,胡南,杨雨山,王晓亮.纳米Fe3O4负载啤酒酵母菌对铀的吸附性能与机理[J].中国有色金属学报,2012,22(2):604-610.PENG Guo-wen,DING De-xin,HU Nan,YANG Yu-shan,WANG Xiao-liang.Adsorption properties and mechanism of saccharomyces cerevisiae loaded by Nano-Fe3O4 on uranium[J].The Chinese Journal of Nonferrous Metals,2012,22(2):604-610.
[17]GUTSCHE C D,IQBAL M.P-tert-butylcalix[4]arene[J].Organic Syntheses,1986,68:243-244.