化学学报 ›› 2021, Vol. 79 ›› Issue (10): 1265-1272.DOI: 10.6023/A21060263 上一篇    下一篇

研究论文

硫化纳米零价铁对水中U(VI)的高效去除研究

白子昂a, 陈瑞兴a, 庞宏伟b, 王祥学b, 宋刚c, 于淑君a,*()   

  1. a 华北电力大学 环境科学与工程学院 资源环境系统优化教育部重点实验室 北京 102206
    b 华北电力大学 环境科学与工程系 燃煤电站烟气多污染物协同控制实验室 保定 071003
    c 广州大学 环境科学与工程学院 广东省放射性核素污染控制与资源化重点实验室 广州 510006
  • 投稿日期:2021-06-09 发布日期:2021-07-20
  • 通讯作者: 于淑君
  • 基金资助:
    国家自然科学基金(21906052); 国家自然科学基金(U2067215); 广东省放射性核素污染控制与资源化重点实验室开放基金(2017B030314182)

Investigation on the Efficient Removal of U(VI) from Water by Sulfide Nanoscale Zero-valent Iron

Ziang Baia, Ruixing Chena, Hongwei Pangb, Xiangxue Wangb, Gang Songc, Shujun Yua()   

  1. a MOE Key Laboratory of Resources and Environmental Systems Optimization, College of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, China
    b Heibei Key Lab of Power Plant Flue Gas Multi-Pollutants Control, Department of Environmental Science and Engineering, North China Electric Power University, Baoding 071003, China
    c Guangdong Provincial Key Laboratory of Radionuclides Pollution Control and Resources, School of Environmental Science and Engineering, Guangzhou University, Guangzhou 510006, China
  • Received:2021-06-09 Published:2021-07-20
  • Contact: Shujun Yu
  • Supported by:
    National Natural Science Foundation of China(21906052); National Natural Science Foundation of China(U2067215); Research Fund Program of Guangdong Provincial Key Laboratory of Radionuclides Pollution Control and Resources(2017B030314182)

近年来, 放射性污染物铀(U(VI))在水环境中的排放对生态环境和生物健康造成严重的威胁. 本研究采用液相还原法制备了硫化纳米零价铁(S-NZVI)材料, 并将其用于水中U(VI)的去除. 首先, 我们采取了一系列的微观表征技术探究了S-NZVI的表面特征及材料特性. 结果表明, 相比于纳米零价铁(NZVI), S-NZVI颗粒不易团聚, 性质更加稳定. 随后, 通过宏观实验探究了反应时间、温度、pH、背景离子浓度等因素对S-NZVI去除U(VI)的影响. 结果表明, S-NZVI对U(VI)的最大去除量高达562.5 mg•g-1, 且在100 min内达到反应平衡. 宏观实验和X射线光电子能谱(XPS)分析表明S-NZVI对U(VI)的去除机理是吸附和氧化还原协同作用的结果. 此外, S-NZVI可以通过外加磁场从水中快速地进行分离, 便于材料再回收与利用. 综上, 本研究构筑了一种制备简单、便于回收且高效的U(VI)净化材料, 未来可能会在放射性核素的处理处置等相关工作中起到重要作用.

关键词: U(VI), 硫化纳米零价铁, 吸附, 氧化还原, 协同作用

In recent years, uranium (U(VI)), a radioactive contaminant, has been widely used in industrial production and military fields. Although the industry has developed, its discharge in water poses a serious threat to the natural environment and biological health. In order to solve this problem, in this study, we prepared sulfide nano zero-valent iron (S-NZVI) material by liquid-phase reduction using NaBH4, FeSO4•7H2O and Na2S2O4 as main materials in N2-filled glove box, and applied them to U(VI) removal from water. First of all, serial microscopic characterization techniques were adopted to explore the surface morphology and physicochemical properties of S-NZVI. The results showed that the S-NZVI particles are less agglomerated and more stable compared to nano zero-valent iron (NZVI). Subsequently, we investigated the effects of reaction time, temperature, pH, and background ion concentration on the removal of U(VI) by S-NZVI through macroscopic batch experiments. The consequence indicated that the maximum removal of U(VI) by S-NZVI at room temperature (20 ℃) could reach 562.5 mg•g-1, and the reaction equilibrium could be received within 100 min. And more importantly, the eliminated process of S-NZVI is consistent with Langmuir single-molecule layer adsorption model, and the conditions for optimal performance were at ambient temperature (20 ℃) and pH=7~8. Combined with the results of macroscopic experiments and X-ray photoelectron spectroscopy (XPS) analysis, the removal mechanism of U(VI) by S-NZVI may be attributed to the synergistic effect of adsorption and redox reaction. In addition, S-NZVI can be separated from water rapidly by external magnetic field due to its magnetic property, which is convenient for material recycle and reutilization. In conclusion, this study has prepared a facile, recyclable, and efficient material for U(VI) decontamination, which may play a significant role in the future of environmental protection, nuclear waste remediation, and other related fields.

Key words: U(VI), sulfide nanoscale zero-valent iron, adsorption, redox, synergistic effect