磺酰基桥联杯[4]芳烃多孔配位笼对海水中U(Ⅵ)的快速吸附  

Calixarene-Based Porous Coordination Cages for Ultrafast Extraction of Uranium From Seawater

作　　者：陈梦伟 刘涛[1] 汤帅 谢祖姬 张若倩 刘胤江 王宁[1] CHEN Meng-wei;LIU Tao;TANG Shuai;XIE Zu-ji;ZHANG Ruo-qian;LIU Yin-jiang;WANG Ning(State Key Laboratory of Marine Resource Utilization in South China Sea,Hainan University,Haikou 570228,China)

机构地区：[1]海南大学南海海洋资源利用国家重点实验室,海南海口570228

出　　处：《核化学与放射化学》2022年第3期276-284,I0005,共10页Journal of Nuclear and Radiochemistry

基　　金：海南省自然科学基金项目(420RC523);海南省重大科技计划项目(ZDKJ2019013);海南大学启动基金项目(KYQD(ZR)1906)。

摘　　要：设计合成具有较强铀酰离子结合能力、较快吸附动力学的多孔框架配合物对于海水中铀吸附具有重大的意义。利用对叔丁基磺酰基桥联杯[4]芳烃(H_(4)TC4A-SO_(2))、六水氯化钴和1,3-二(2H-四氮唑-5-基)苯(H_(2)L)在溶剂热的条件下构筑了一例长方体状杯芳烃基多孔配位笼(Co16),并用于对海水中铀酰离子的吸附。对Co16吸附剂进行U(Ⅵ)吸附实验发现,Co16吸附剂在较宽的pH范围内对U(Ⅵ)具有优异的吸附能力,并在90 min内达到吸附平衡,且符合准二级动力学模型。吸附等温线较好地符合Langmuir模型,表明Co16吸附剂对U(Ⅵ)的吸附属于单层吸附,且对U(Ⅵ)的吸附容量高达547.31 mg/g。热力学实验表明,Co16吸附剂对U(Ⅵ)的吸附属于自发吸热的行为。把该材料置于真实海水中20 d后,其在真实海水中的吸附容量可达4.88 mg/g。以上结果表明,Co16吸附剂在海水铀吸附方面具有巨大的应用潜力。The design and synthesis of porous framework materials with strong affinity and selectivity for uranyl ion are extremely appealing for the efficient extraction of uranium from seawater.Herein,rectangular porous framework cage(denoted as Co16)is prepared by using p-tert-butylsulfonylcalix[4]arene,CoCl_(2)·6H_(2)O and 1,3-bis(2H-tetrazol-5-yl)benzene(H_(2)L)ligands under solvothermal conditions.Further,the Co16 is used for uranium extraction.As the result,the Co16 exhibits short adsorption equilibrium time(≈90 min)and is in accordance with the pseudo-second-order kinetic model.Robust framework and active U(Ⅵ)adsorption in the wide pH range are displayed.Besides,Co16 adsorbents exhibit high U(Ⅵ)uptake capacity(547.31 mg/g)and well fit the Langmuir model.Adsorption thermodynamics research has clearly demonstrated that the adsorption process is endothermic and spontaneous.Furthermore,Co16 achieves a high uranium adsorption capacity(4.88 mg/g)after immersing in real seawater for 20 days.Overall,these advantages of Co16 adsorbents highlight the potential candidate for the selective capture of U(Ⅵ)from seawater.

关 键 词：Co16吸附剂 快速吸附 自发吸热 真实海水 

分 类 号：TL212.5[核科学技术—核燃料循环与材料]