Wang Guohui, Zhang Qixin, Qin Lailai, Tan Kaixuan, Li Chunguang, Li Lianshun, Yang Tinggui, Liu Xiaojuan
The 404 Company Limited, CNNC, Lanzhou 735100, China; Key Laboratory of Nuclear Fuel Cycle Technology, The 404 Company Limited, Lanzhou 735100, China; Chengdu Nuclear Engineering Design &Research Institute Co., Ltd, 404., CNNC, Chengdu 610000, China.
CPC Affairs and Administration Office, Nanjing University of Aeronautics and Astronautics, Nanjing 211100, China.
Sci Total Environ. 2024 Dec 1;954:176296. doi: 10.1016/j.scitotenv.2024.176296. Epub 2024 Sep 14.
A novel metal-organic framework (MOF) material, MIL-100(Fe)-DMA, was synthesized using the solvothermal method. The structure of the MOF was characterized using scanning electron microscopy-energy dispersive X-ray spectroscopy, N adsorption-desorption isotherms, X-ray diffraction analysis, Fourier-transform infrared spectroscopy, X-ray photoelectron spectroscopy, and Mössbauer spectroscopy. Batch adsorption experiments were performed to investigate the effects of initial Sr and Cs concentrations, adsorption time, pH, and coexisting cations on the adsorption performance of the material. The adsorption mechanism was further elucidated using adsorption kinetics and isotherm models. The results indicated that the adsorption of Sr and Cs does not significantly affect the MOF material structure. As reaction time and initial ion concentration increased, the adsorption capacity of MIL-100(Fe)-DMA for Sr and Cs increased rapidly and then gradually reached equilibrium. Optimal adsorption occurred under alkaline conditions, with maximum adsorption capacity observed at pH = 8. The adsorption process for Sr and Cs was well described by the pseudo-second-order kinetic model, the Weber-Morris model, and the Langmuir adsorption isothermal model. The adsorption process was mainly identified as monolayer chemical adsorption, influenced by multiple factors. Characterization combined with density functional theory calculations revealed that the unsaturated carboxylic acid groups on the surface of the MOFs play a crucial role in the interaction with Sr and Cs.
采用溶剂热法合成了一种新型金属有机框架(MOF)材料MIL-100(Fe)-DMA。利用扫描电子显微镜-能量色散X射线光谱、N吸附-脱附等温线、X射线衍射分析、傅里叶变换红外光谱、X射线光电子能谱和穆斯堡尔光谱对MOF的结构进行了表征。进行了批量吸附实验,以研究初始Sr和Cs浓度、吸附时间、pH值和共存阳离子对该材料吸附性能的影响。利用吸附动力学和等温线模型进一步阐明了吸附机理。结果表明,Sr和Cs的吸附对MOF材料结构没有显著影响。随着反应时间和初始离子浓度的增加,MIL-100(Fe)-DMA对Sr和Cs的吸附容量迅速增加,然后逐渐达到平衡。在碱性条件下发生最佳吸附,在pH = 8时观察到最大吸附容量。Sr和Cs的吸附过程可用准二级动力学模型、韦伯-莫里斯模型和朗缪尔吸附等温模型很好地描述。吸附过程主要被确定为单层化学吸附,受多种因素影响。表征结合密度泛函理论计算表明,MOFs表面的不饱和羧酸基团在与Sr和Cs的相互作用中起关键作用。