Highly U(VI) immobilization on polyvinyl pyrrolidine intercalated molybdenum disulfide: Experimental and computational studies

Highly U(VI) immobilization on polyvinyl pyrrolidine intercalated molybdenum disulfide: Experimental and computational studies
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聚乙烯吡咯烷插层二硫化钼上的高度 U(VI) 固定化:实验和计算研究

DOI:
10.1016/j.cej.2018.11.016
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发表时间:
2019-03
影响因子:
15.1
通讯作者:
Wang Xiangke
Wang Xiangke
中科院分区:
工程技术1区
文献类型:
--
作者:
Gu Pengcheng;Zhao Chaofeng;Wen Tao;Ai Yuejie;Zhang Sai;Chen Weiqiang;Wang Jian;Hu Baowei;Wang Xiangke

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在这项研究中,聚乙烯吡咯烷插层二硫化钼(PVP/MoS 2)具有良好的互联纳米片成功地制备了一个有效的和通用的一步水热策略。结构表征表明,PVP分子插层到MoS 2中,层间距变宽。所得PVP/MoS 2纳米材料具有良好的吸附性能。在298 K和pH = 4.5条件下,PVP/MoS 2对U(VI)的最大吸附量为117.9 mg/g,明显上级未改性MoS 2的23.7 mg/g,这可能与PVP/MoS 2比表面积增大和官能团增多有关.动力学研究表明,PVP/MoS 2对U(VI)的吸附速度极快,在10 min内即可达到吸附平衡。FT-IR、XPS和DFT计算结果表明,UO 2-S共价键的存在以及UO 2-S与PVP的表面络合是导致U(VI)在PVP/MoS 2上富集的主要原因。这些研究结果对于评价PVP/MoS 2的吸附性能和推进其他聚合物相互作用层状金属硫化物在放射性水处理领域的潜在应用具有重要意义。
In this study, polyvinyl pyrrolidine intercalated molybdenum disulfide (PVP/MoS2) with well-interconnected nanosheets were successfully prepared by an effective and versatile one-step hydrothermal strategy. The structural characterization indicated that the PVP molecules were intercalated into MoS2to produce widened interlayer spacing. The obtained PVP/MoS2nanomaterials exhibited impressive adsorption performance. Specifically, the maximum adsorption capacity of U(VI) on PVP/MoS2(∼117.9 mg/g) was apparently superior than that of pristine MoS2(∼23.7 mg/g) at 298 K and pH = 4.5, which might be related to the enlarged specific surface area and extensive functional groups of PVP/MoS2. The kinetics investigation showed that the uptake of U(VI) with PVP/MoS2was ultrafast and the adsorption equilibrium could be reached within 10 min. The enrichment of U(VI) on PVP/MoS2was caused by the existence of UO2-S covalent bonds and surface complexation with PVP, which was jointly verified by systematic investigation of FT-IR, XPS and DFT calculations. These findings were intriguing for both evaluating the adsorption performance of PVP/MoS2and advancing other polymer interacted layered metal sulfides potential applications in the field of radioactive water treatment.
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