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Volume 29 Issue 3
Mar.  2022
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文章导航 >  矿物冶金与材料学报（英文）  > 2022  >  29(3): 479-489
Yuhui Liu, Meng Tang, Shuang Zhang, Yuling Lin, Yingcai Wang, Youqun Wang, Ying Dai, Xiaohong Cao, Zhibin Zhang, and Yunhai Liu, U(VI) adsorption behavior onto polypyrrole coated 3R-MoS2 nanosheets prepared with the molten salt electrolysis method, Int. J. Miner. Metall. Mater., 29(2022), No. 3, pp. 479-489. https://doi.org/10.1007/s12613-020-2154-5
Cite this article as:
Yuhui Liu, Meng Tang, Shuang Zhang, Yuling Lin, Yingcai Wang, Youqun Wang, Ying Dai, Xiaohong Cao, Zhibin Zhang, and Yunhai Liu, U(VI) adsorption behavior onto polypyrrole coated 3R-MoS2 nanosheets prepared with the molten salt electrolysis method, Int. J. Miner. Metall. Mater., 29(2022), No. 3, pp. 479-489. https://doi.org/10.1007/s12613-020-2154-5
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研究论文

熔盐电解法制备PPy/3R-MoS2纳米片及对U(VI)吸附效果的研究

  • 1)

    东华理工大学核资源与环境国家重点实验室，南昌 330013, 中国

  • 2)

    东华理工大学核科学与工程学院，南昌 330013，中国

  • 通讯作者:

    柳玉辉    E-mail: liuyuhui@ecut.edu.cn

    刘云海    E-mail: walton_liu@163.com

文章亮点

  • (1) 高温电化学方法具有介电弛豫效应，且通过调控界面电势差和温度对MoS2层间范德华力产生快速冲击，有利于不同堆垛方式的形成，解决了传统方法加热时间长和晶格化程度弱等问题。
  • (2) 以聚吡咯通过原位聚合与二硫化钼复合，所形成的复合材料具有更多的活性位点和更高的选择性，在协同作用下，复合材料吸附U(VI)的性能得到了提高。
  • (3) 高温电化学方法具有低成本、高纯度、高效率高量产的特点和优势。
  • 为提高水溶液中铀的分离能力，本文采用熔盐电解法制备3R-MoS2纳米片，并用聚吡咯(PPy)对其进行改性，采用水热法合成了复合纳米吸附剂(PPy/3R-MoS2)。在700 K温度下，以Mo丝为阴极，C棒为阳极，调节恒电流电位仪电流大小为2 A，对KCl–NaCl–Na2MoO4–KSCN熔盐体系进行恒电流电解1 h。待电解产物冷却至室温后，用去离子水洗涤过滤，在60℃下真空干燥2 h，得到3R-MoS2纳米片。将制备的3R-MoS2纳米片(1.0 g)分散在50 mL含PPy(2.34 mL)的去离子水中，加入10 mL(1 mol/L) FeCl3溶液，在10℃下放置24 h。将反应后的样品在5000 r/min下离心20 min，用无水乙醇和去离子水分散两次后，在70°C下真空干燥2 h，得到PPy/3R-MoS2纳米片。通过批次吸附实验，探究了制备的纳米片在不同pH、反应时间、U(VI)初始浓度和温度条件下对U(VI)的吸附效果，并利用SEM、HRTEM、XRD、FTIR和XPS对其进行表征。在不同实验条件下，与3R-MoS2和聚吡咯(PPy)相比，复合纳米吸附剂(PPy/3R-MoS2)对U(VI)的吸附能力增强。当U(VI)初始浓度为80–100 mg/L时， PPy、3R-MoS2和PPy/3R-MoS2的吸附均达到平衡，最大吸附量分别为30.9、58.7和200.4 mg/g。XPS和FTIR分析阐明了其吸附机理：1) 带负电的PPy/3R-MoS2纳米片通过静电吸引捕获UO22+)；2) 裸露的C，N，Mo，S原子通过配位作用与U(VI)络合；3) 络合物中的Mo将吸附的U(VI)部分还原为U(IV)，再生了吸附位点，从而连续吸附U(VI)。具有高吸附容量和化学稳定性的PPy/3R-MoS2复合材料的设计为放射性核素的去除提供了新的方向。
    • Research Article

    U(VI) adsorption behavior onto polypyrrole coated 3R-MoS2 nanosheets prepared with the molten salt electrolysis method

    + Author Affiliations
      Abstract
    • To improve the separation capacity of uranium in aqueous solutions, 3R-MoS2 nanosheets were prepared with molten salt electrolysis and further modified with polypyrrole (PPy) to synthesize a hybrid nanoadsorbent (PPy/3R-MoS2). The preparation conditions of PPy/3R-MoS2 were investigated and the obtained nanosheets were characterized with scanning electron microscope (SEM), high resolution transmission electron microscope (HRTEM), X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS). The results showed that PPy/3R-MoS2 exhibited enhanced adsorption capacity toward U(VI) compared to pure 3R-MoS2 and PPy; the maximum adsorption was 200.4 mg/g. The adsorption mechanism was elucidated with XPS and FTIR: (1) negatively charged PPy/3R-MoS2 nanosheets attracted $ {\rm{UO}}_2^{2 + } $ by an electrostatic interaction; (2) exposed C, N, Mo, and S atoms complexed with U(VI) through coordination; (3) Mo in the complex partly reduced the adsorbed U(VI) to U(IV), which further regenerated the adsorption point and continuously adsorbed U(VI). The design of the PPy/3R-MoS2 composite with a high adsorption capacity and chemical stability provides a new direction for the removal of radionuclide.
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