物理化学学报 >> 2025, Vol. 41 >> Issue (9): 100097.doi: 10.1016/j.actphy.2025.100097

所属专题： 电化学分离与资源化

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利用碳纳米管分散的亚铁氰化锌钾电极选择性电吸附高盐放射性废水中的铯(Ⅰ)

项书宏1,2,†, 杨旅3,†, 徐应生1,4,*(), 曹国新3,*(), 周宏建1,*()   

  1. 1 中国科学院合肥物质科学研究院固体物理研究所, 中国科学院材料物理重点实验室, 安徽省纳米材料与纳米技术重点实验室, 安徽 合肥 230031
    2 四川大学高分子科学与工程学院, 四川 成都 610065
    3 美的集团中央研究院, 广东 佛山 528311
    4 湖北师范大学化学化工学院, 污染物分析与资源化技术湖北省重点实验室, 湖北 黄石 435002
  • 收稿日期:2025-02-28 修回日期:2025-04-19 录用日期:2025-04-21 发布日期:2025-07-04
  • 通讯作者: Email: yinsxu@hbnu.edu.cn (徐应生)guoxin.cao@midea.com (曹国新)hjzhou@issp.ac.cn (周宏建)
  • 作者简介:

    †These authors contributed equally to this work.

  • 基金资助:
    国家重点研发计划(2022YFC2904303); 国家自然科学基金(92463309); 国家自然科学基金(52400078); 安徽省重点研发项目(202426j16020001); 湖北省自然科学基金(2024AFB104); 中国科学院合肥物质科学研究院院长基金(YZJJ-GGZX-2022-01)

Selective electrosorption of Cs(Ⅰ) from high-salinity radioactive wastewater using CNT-interspersed potassium zinc ferrocyanide electrodes

Shuhong Xiang1,2, Lv Yang3, Yingsheng Xu1,4,*(), Guoxin Cao3,*(), Hongjian Zhou1,*()   

  1. 1 Key Laboratory of Materials Physics, Anhui Key Laboratory of Nanomaterials and Nanotechnology, Institute of Solid State Physics, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Hefei 230031, Anhui Province, China
    2 College of Polymer Science and Engineering, Sichuan University, Chengdu 610065, Sichuan Province, China
    3 Midea Corporate Research Center, Midea Group, Foshan 528311, Guangdong Province, China
    4 Hubei Key Laboratory of Pollutant Analysis & Reuse Technology, College of Chemistry and Chemical Engineering, Hubei Normal University, Huangshi 435002, Hubei Province, China
  • Received:2025-02-28 Revised:2025-04-19 Accepted:2025-04-21 Published:2025-07-04
  • Contact: Email: yinsxu@hbnu.edu.cn (Yingsheng Xu)guoxin.cao@midea.com (Guoxin Cao)hjzhou@issp.ac.cn (Hongjian Zhou)
  • Supported by:
    the National Key R&D Program of China(2022YFC2904303); the National Natural Science Foundation of China(92463309); the National Natural Science Foundation of China(52400078); the Key Research and Development Projects of Anhui Province, China(202426j16020001); Natural Science Foundation of Hubei Province, China(2024AFB104); the HFIPS Director's Fund, China(YZJJ-GGZX-2022-01)

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摘要：

福岛核事故(FNA)产生的含137Cs放射性废水因其安全处置难题而备受关注。共存Na+离子严重阻碍Cs+的去除，加剧了放射性废水处理成本。近年来，电容去离子(CDI)技术在该领域展现出显著的潜力，但由于缺乏对Cs+具有高选择性的理想电极材料，该技术的实际应用受到了一定限制。本研究开发了一种碳纳米管(CNT)嵌入亚铁氰化锌钾(KZnFC-CNT)的复合材料，通过电化学方法预活化后作为CDI阴极，用于高盐放射性废水中Cs+的选择性电吸附。KZnFC-CNT电极表现出392.75 mg∙g−1的最大电吸附容量和11.21 mg∙g−1∙min−1的最高电吸附速率。在Na+ : Cs+摩尔比为100 : 1时，该电极对Cs+/Na+的选择性系数高达138.2。X射线衍射、电化学分析和理论模拟表明，Cs+的选择性电吸附主要受Cs+与Na+离子交换过程及KZnFC晶格相变的调控。本研究为高盐含铯放射性废水处理提供了有效策略。

关键词: 电容去离子, 选择性铯电吸附, 亚铁氰化锌, 放射性废水, 相变

Abstract:

The management of 137Cs-containing radioactive wastewater from the Fukushima nuclear accident (FNA) has garnered significant attention due to the challenge of its safe disposal. The presence of co-existing Na+ ions severely impedes Cs+ removal, exacerbating the costs associated with radioactive wastewater treatment. Recently, capacitive deionization (CDI) technology has demonstrated significant potential in this field. However, its application is limited by the lack of suitable electrode materials that exhibit high Cs+ selectivity. In this study, we developed a composite of carbon nanotubes (CNT) interspersed potassium zinc ferrocyanide (KZnFC-CNT), which was pre-activated via an electrochemical method, to serve as a CDI cathode for the selective electrosorption of Cs+ ions from saline radioactive wastewater. The KZnFC-CNT electrodes exhibited a maximum electrosorption capacity of 392.75 mg∙g−1, with the highest electrosorption rate of 11.21 mg∙g−1∙min−1. Furthermore, these electrodes exhibited remarkable selectivity, achieving a selectivity factor of 138.2 for Cs+ over Na+ in a Na+ : Cs+ molar ratio of 100 : 1. X-ray diffraction, electrochemical analysis, and theoretical simulations revealed that the selective electrosorption of Cs+ is primarily governed by the ion exchange process between Cs+ and Na+ ions, as well as lattice phase transformations in KZnFC. This study presents an effective approach for the treatment of cesium-containing radioactive wastewater with high salinity.

Key words: Capacitive deionization, Selective cesium electrosorption, Zinc ferrocyanide, Radioactive wastewater, Phase transformation