核化学与放射化学2025，Vol.47Issue(3)：224-234,11.DOI:10.7538/hhx.2025.47.03.0224
氧化石墨烯膜筛分分离强硝酸体系下铀铌锆中铀的性能
Performance of Graphene Oxide Membrane for Separating U From U-Nb-Zr Alloys Under Strong Nitric Acid System
张东平 1黄丽钦 2苏磊 1熊远婷 1赵峰 1陆跃翔2
作者信息
- 1. 中国核动力研究设计院先进核能技术全国重点实验室,四川成都 610213
- 2. 清华大学核能与新能源技术研究院,北京 100084
- 折叠
摘要
Abstract
There are a large amount of uranium,niobium,and niobium elements in the unqualified products generated during the production and manufacturing process of U-Nb-Zr alloy materials,as well as in the wastewater generated during the analysis and characterization process.In order to achieve the recovery and reuse of uranium and reduce the discharge of radioactive waste,this work adopted a membrane separation technology based on graphene oxide membranes(GOMs).By utilizing the size difference between uranyl ions and niobium and zirconium hydrate ions,the separation of uranyl ions from uranium,niobium and zirconium ion solutions under strong nitric acid system was explored.Six groups of GOMs with different graphite particle sizes and oxidation degrees were prepared.The effects of membrane oxidation degree,membrane thickness,solution acidity,and ion concentration on screening and separation efficiency was evaluated.SEM show that the thickness of 1.2 mg GOMs is about 1 μm,and there are obvious wrinkles on the surface of GOMs,provided a channel for the passage of small molecules and ions.XPS and FTIR show that the order of oxidation degree of the six groups of GOMs is 325S2＞200S2＞200S1＞325S1＞100S1＞100S2.The experimental results show that the GOMs products(200Sl)with 200 mesh(particle size is 75 μm)graphite as the raw material and oxidized at 35 ℃ for 2 h have smaller interlayer spacing in 3 mol/L HNO3 solution,and this material can most effectively achieve the separation of uranium from niobium and zirconium.Under the screening separation conditions of 200S1 membrane mass of 1.2 mg,solution acidity of 3 mol/L HNO3,UO22+initial concentration of 3.7 mmol/L,and Nb5+and Zr4+initial concentrations of 1.1 mmol/L,the Nb5+concentration(0.40 mmol/L)and Zr4+concentration(0.38 mmol/L)measured in infiltration side at 48 h are approximately twice the concentration of UO22+(0.21 mmol/L).The permeability of UO22+at 48 h is only 5.32％,while the ion permeability of Nb5+and Zr4+are 36.39％and 34.30％,respectively,approaching osmotic equilibrium.The pseudo-first order separation rate constant of Nb5+(0.008 7 h-1)is approximately 8 times that of UO22+(0.001 1 h-1),while Zr4+(0.0080 h-1)is approximately 7 times that of UO22+(0.0011 h-1).The separation factors ofα(Nb/U)and α(Zr/U)reach 10.2 and 9.3,respectively.In addition,cyclic experiments show that the 200S1 membrane still has screening and separation ability after being reused 5 times.This work provides a new method for the recovery of uranium in U-Nb-Zr materials,and can also provide technical reference for the separation of uranium in high-level radioactive waste.关键词
氧化石墨烯膜/铀/铌/锆/筛分分离Key words
graphene oxide membrane/uranium/niobium/zirconium/sieving分类
核科学引用本文复制引用
张东平,黄丽钦,苏磊,熊远婷,赵峰,陆跃翔..氧化石墨烯膜筛分分离强硝酸体系下铀铌锆中铀的性能[J].核化学与放射化学,2025,47(3):224-234,11.
