Lu Songhua, Zhu Kairuo, Hayat Tasawar, Alharbi Njud S, Chen Changlun, Song Gang, Chen Diyun, Sun Yubing
College of Environmental Science and Engineering, North China Electric Power University, Beijing, 102206, PR China; Key Laboratory of Photovoltaic and Energy Conversation, Institute of Plasma Physics, Chinese Academy of Sciences, P.O. Box 1126, Hefei, 230031, PR China.
Key Laboratory of Photovoltaic and Energy Conversation, Institute of Plasma Physics, Chinese Academy of Sciences, P.O. Box 1126, Hefei, 230031, PR China.
J Hazard Mater. 2019 Feb 15;364:100-107. doi: 10.1016/j.jhazmat.2018.10.035. Epub 2018 Oct 13.
Cubic perovskite (CaTiO) was successfully synthesized by a facile solvothermal method and was utilized to sequestrate U(VI) from aqueous solutions. The batch experiments revealed that carbonate inhibited U(VI) sequestration at pH > 6.0 due to the formation of uranyl-carbonate complexes. The maximum sequestration capacity of U(VI) on perovskite was 119.3 mg/g (pH 5.5). The sequestration mechanism of U(VI) on perovskite were investigated by XPS and EXAFS techniques. According to XPS analysis, the presence of U(IV) and U(VI) oxidation states revealed the photocatalytic reduction of U(VI) by perovskite under UV-vis irradiation. In addition, photocatalytic reduction performance significantly decreased in the presence of carbonate. Based on EXAFS analysis, the occurrence of U-Ti and U-U shells revealed the inner-sphere surface complexation and reductive precipitation of U(VI) on perovskite. These findings herein are crucial for the application of perovskite-based composites in the decontamination of U(VI) in aquatic environmental cleanup.
通过简便的溶剂热法成功合成了立方钙钛矿(CaTiO),并将其用于从水溶液中螯合U(VI)。批量实验表明,由于形成了碳酸铀酰络合物,在pH > 6.0时碳酸盐会抑制U(VI)的螯合。钙钛矿对U(VI)的最大螯合容量为119.3 mg/g(pH 5.5)。采用XPS和EXAFS技术研究了U(VI)在钙钛矿上的螯合机理。根据XPS分析,U(IV)和U(VI)氧化态的存在表明钙钛矿在紫外-可见光照下对U(VI)有光催化还原作用。此外,在有碳酸盐存在的情况下,光催化还原性能显著下降。基于EXAFS分析,U-Ti和U-U壳层的出现表明U(VI)在钙钛矿上发生了内球表面络合和还原沉淀。本文的这些发现对于基于钙钛矿的复合材料在水生环境净化中去除U(VI)的应用至关重要。