新型杯[4]芳烃衍生物的合成及对U(Ⅵ)吸附性能研究  

Synthesis of novel calix[4]arene derivatives and its adsorption properties towards Uranium(Ⅵ)

作　　者：张康 许玉历 肖方竹[4] 王成[2,3] 罗佳琦 陈方 刘永 彭国文 ZHANG Kang;XU Yu-li;XIAO Fang-zhu;WANG Cheng;LUO Jia-qi;CHEN Fang;LIU Yong;PENG Guo-wen(School of Resource Environment and Safety Engineering;Laboratory of Protein Structure and Function,University of South China;School of Chemistry and Chemical Engineering;School of Public Health,Hengyang 421001,Hunan Province,China)

机构地区：[1]南华大学资源环境与安全工程学院,湖南衡阳421001 [2]南华大学蛋白质结构与功能实验室,湖南衡阳421001 [3]南华大学化学化工学院,湖南衡阳421001 [4]南华大学公共卫生学院,湖南衡阳421001

出　　处：《化学工程》2020年第6期16-22,共7页Chemical Engineering(China)

基　　金：国家自然科学基金资助项目(51574152,11705085);湖南省自然科学基金资助项目(2017JJ2232,2017JJ3262,2017JJ4009);湖南省2017年度中央引导地方科技发展专项资金项目(2017CT5006);湖南省环境保护厅科研项目(湘财建指〔2017〕83号)。

摘　　要：以对叔丁基杯[4]芳烃为原料,用间氨基苯甲酸等化合物对其上沿进行羧基化改性,再利用1,3-二溴丙烷等化合物对其下沿进行功能化修饰,得到一种新型功能化材料间羧基苯偶氮基杯[4]芳烃溴代乙醚衍生物(MCA-BDED),并采用红外光谱、扫描电镜分别对其结构进行表征。考察溶液pH值、吸附时间、铀初始质量浓度、吸附剂投加量等因素对MCA-BDED吸附铀效果的影响,分析吸附过程中的反应动力学和吸附等温线。结果表明:在温度为25℃时,MCA-BDED吸附铀的最佳条件是pH值为4.0,铀初始质量浓度为20 mg/L,吸附剂MCA-BDED投加量为20 mg,吸附平衡时间为4 h。MCA-BDED对U(Ⅵ)的吸附过程符合准二级动力学模型,表明吸附过程为化学吸附。Langmuir、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。使用3种不同的解析剂对MCA-BDED解吸再生3次后,其对铀的吸附率均在60%以上,说明MCA-BDED对铀有良好的再生性能。Using the tert butyl calix[4]arene as raw materials,its upper rim was modified by carboxylation with M-aminobenzoic acid,and its low rim was modified by functional modification with 1,3-dibromopropane.A new type of functional material M-carboxyphenylazo calix[4]arene bromine diethyl ether Derivatives(MCA-BDED)was obtained.The structure of MCA-BDED was characterized by FT-IR and SEM.The effects of pH value of U(Ⅵ)solution,adsorption time,initial uranium mass concentration,temperature,dosage of adsorbent on the adsorption of uranium on MCA-BDED were investigated,finally the reaction kinetics and adsorption isotherm were analyzed.Results show that the best condition of uranium adsorption are as follows,pH value is 4.0,initial mass concentration of uranium is 20 mg/L,dosage of adsorbent is 20 mg,adsorption equilibration time is 4 h at 25℃.The adsorption kinetics of MCA-BDED to uranium was accorded with pseudo-second order model.The adsorption process which is better fitted with Langmuir,and Freundlich sorption isotherm was chemisorption.It suggested that the adsorption system was a model of single-layer coverage combined with multilayer adsorption.In addition,MCA-BDED has good regeneration properties,because the adsorption rate is over 60%after three times of desorption and regeneration with three different desorption agents.

关 键 词：杯[4]芳烃 修饰 等温线 吸附 铀 

分 类 号：O625.1[理学—有机化学] X703.1[理学—化学]