新型硅基焦磷酸锆离子交换剂的制备及其对Cs^(+)的吸附性能研究  

Preparation of Novel Silica-based Zirconium Pyrophosphate Ion-exchanger and Its Adsorption Performance for Cs^(+)DIAO

作　　者：刁新雅 郝乐存 马锋 赵昕[1,2] 靳强 陈宗元[1,2] 郭治军[1,2] 吴王锁[1,2] Xinya;HAO Lecun;MA Feng;ZHAO Xin;JIN Qiang;CHEN Zongyuan;GUO Zhijun;WU Wangsuo(MOE Frontiers Science Center for Rare Isotopes,Lanzhou University,Lanzhou 730000,China;Radiochemistry Laboratory,School of Nuclear Science and Technology,Lanzhou University,Lanzhou 730000,China;Military Civilian Integration Development Research Institute,Xi’an 710122,China)

机构地区：[1]兰州大学教育部稀有同位素前沿科学中心,甘肃兰州730000 [2]兰州大学核科学与技术学院放射化学与核环境研究所,甘肃兰州73000 [3]西北政法大学军民融合发展研究院,陕西西安710122

出　　处：《原子能科学技术》2024年第11期2290-2298,共9页Atomic Energy Science and Technology

基　　金：甘肃省科技重大专项(21ZD8JA006);甘肃省科技计划项目(22JR5RA480);兰州大学中央高校基本科研业务费专项资金(lzujbky-2023-stlt01,lzujbky-2022-sp05,lzujbky-2022-kb01)。

摘　　要：放射性废液中放射性Cs^(+)的高效去除和回收对于降低废物处置成本、促进资源循环利用具有重要意义。本文采用溶胶-凝胶共沉淀和高温处理相结合的新方法,合成了一种成本低廉的新型无机离子交换树脂硅基焦磷酸锆,采用SEM、FT-IR、XRF、XRD等手段对新树脂进行了表征,并通过静态吸附实验及柱实验系统测定了在弱酸性溶液中其对Cs^(+)的吸附性能。结果显示,Cs^(+)在该树脂上的吸附过程符合准二级动力学模型,吸附在6 h内达到平衡。在0.001 mol/L HNO3溶液中,该树脂对Cs^(+)的静态吸附容量可达2.7 mg/g。树脂对Cs^(+)的吸附具有良好的选择性,Cs^(+)与高放废液中其他共存金属离子的分离因子均大于1.5。此外,柱实验结果显示树脂颗粒柱负载的Cs^(+)可以被2.0 mol/L NH4NO3有效洗脱回收。Efficient removal and recovery of radioactive Cs^(+)from high-level liquid waste(HLLW)is of great significance for reducing disposal cost and promoting nuclear resource recycling.Due to the significant selectivity for Cs^(+),zirconium pyrophosphate possesses great potential to uptake Cs^(+)from HLLW,whereas the micro-crystalline structure and fine powder morphology limits its industrial application with column separation.In this study,a new method combining sol-gel and high-temperature treatment was developed,and a novel silica-based zirconium pyrophosphate resin was prepared by this method.The prepared resin was characterized using scanning electron microscopy(SEM),Fourier transform infrared(FT-IR)spectra,X-ray fluorescence(XRF),X-ray diffraction(XRD),N2 adsorption/desorption isotherms and the universal testing machine,and its adsorption performance for Cs^(+)in weakly acidic solution was determined using both batch-type and dynamic column experiments in terms of the kinetics,equilibrium capacity and selectivity.The characterization results indicate the successful fabrication of silica-based zirconium pyrophosphate resin with excellent physical and chemical stability.Batch-type experiments demonstrate that Cs^(+)adsorption on the resin is equilibrated within 6 h,and the adsorption kinetics could be described by a pseudo-second-order model.Due to the competing adsorption of H+,the adsorption rate of Cs^(+)exhibits a decrease as the concentration of HNO3 increasing from 0.001 mol/L to 2.0 mol/L.The adsorption capacity of Cs^(+)increases significantly with the increase of initial Cs^(+)concentration,and the adsorption of Cs^(+)on the resin can be well fitted with Langmuir model.This implies that the adsorption process of Cs^(+)by the resin is a homogeneous single-layer adsorption process.The maximum adsorption capacity of silica-based zirconium pyrophosphate resin for Cs^(+)is determined to be 2.7 mg/g with batch-type experiment in 0.001 mol/L HNO3.More importantly,the resin exhibits high selectivity for Cs^(+)upta

关 键 词：Cs^(+) 焦磷酸锆 二氧化硅 无机离子交换剂 吸附 

分 类 号：TL99[核科学技术—核技术及应用] O647.32[理学—物理化学]