UiO-66/UiO-66-PYDC的制备及其对UO_2~(2+)吸附性研究
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摘要
通过水热法合成了两种锆基有机骨架材料,采用XRD、SEM、IR、TG、EDS、BET等技术对材料的结构和形貌进行了表征,并通过静态吸附实验在不同条件下测试所制材料对UO2+2的吸附性能,考察了时间、温度、初始铀浓度、pH、CO2-3对吸附的影响.结果表明:Ui O-66体系对铀酰离子的吸附以化学吸附为主,通过表面的羧基官能团与铀酰离子结合从而达到吸附的目的.此外,本实验中材料的比表面积对吸附的影响不明显.在初始最佳pH为10.5的条件下,通过热力学模型拟合发现,低浓度下Ui O-66拥有更大的吸附量.随着溶液中初始铀酰离子浓度的升高,Ui O-66-PYDC展现出更好的吸附效果.
Various zirconium-based organic-framework materials were synthesized with hydrothermal method. The structure and morphology of materials were analyzed by using XRD,SEM,IR,TG,EDS and BET. The absorption properties of UO2+2 were tested in static absorption experiments. The effects of time,temperature,initial concentration of uranyl ions,p H and CO2-3 ions on the uranyl ions absorption were studied. The results show that the Ui O-66 system absorbs the UO2+2 mainly based on chemisorption,through combining uranyl ions and carboxylate group. Besides,the specific surface area of the material has little effect on adsorption. It can be found that Ui O-66 has greater absorption capacity at low concentration by the thermodynamic model under the optimum pH of 10.5. With the increase of uranyl ion concentration,Ui O-66-PYDC shows the better absorption performance.
Various zirconium-based organic-framework materials were synthesized with hydrothermal method. The structure and morphology of materials were analyzed by using XRD,SEM,IR,TG,EDS and BET. The absorption properties of UO2+2 were tested in static absorption experiments. The effects of time,temperature,initial concentration of uranyl ions,p H and CO2-3 ions on the uranyl ions absorption were studied. The results show that the Ui O-66 system absorbs the UO2+2 mainly based on chemisorption,through combining uranyl ions and carboxylate group. Besides,the specific surface area of the material has little effect on adsorption. It can be found that Ui O-66 has greater absorption capacity at low concentration by the thermodynamic model under the optimum pH of 10.5. With the increase of uranyl ion concentration,Ui O-66-PYDC shows the better absorption performance.
引文
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Cassidy C S,Lin J,Frey P A.1997.A new concept for the mechanism of action of chymotrypsin: The role of the low-barrier hydrogen bond[J].Biochemistry,36(15):4576-4584
Chu X Z,Liu S S,Zhou S Y,et al.2016.Adsorption and separation of carbon dioxide and methane in new zeolites using the Grand Canonical Monte Carlo method[J].Adsorption-journal of the International Adsorption Society,22(7):1-9
Condon J B.2005.Mesopore measurement by physical adsorption utilizing chi theory[J].Microporous & Mesoporous Materials,84(1/3):105-115
杜静静.2015.功能化金属有机框架材料的设计、合成与性质研究[D].长春:吉林大学
Ealy J B,Hermanson J.2006.Molecular images in organic chemistry: Assessment of understanding in aromaticity,symmetry,spectroscopy,and shielding[J].Journal of Science Education & Technology,15(1):59
Guo Q,Chen C,Zhou L,et al.2018.Design of ZIF-8/ion copolymer hierarchically porous material: Coordination effect on the adsorption and diffusion for carbon dioxide[J].Microporous & Mesoporous Materials,261:79-87
Ivanov D,Kolikov K.2013.Short-range action and long-range action of the electrostatic forces within atomic nuclei[J].Natural Science,5(4):508-513
Lang X,Fan S,Wang Y.2010.Intensification of methane and hydrogen storage in clathrate hydrate and future prospect[J].Journal of Energy Chemistry, 19(3):203-209
Li P Y, Tezel F H. 2007.Adsorption separation of N2,O2,CO2 and CH4 gases by β-zeolite[J].Microporous & Mesoporous Materials,98(1):94-101
Lin J Q,Lin H,Yang W L,et al.2013.Effect of different particle size of nano-zinc oxide on the surface binding energy in polyimide/zinc oxide composites[J].Advanced Materials Research,785-786:556-560
刘晨,陈元涛,张炜,等.2017.KH-550改性埃洛石对水中铀酰离子吸附性能的研究[J].环境科学学报,37(1):243-248
Mujoo K,Hunt C R,Horikoshi N,et al.2017.A multifaceted role for MOF histone modifying factor in genome maintenance[J].Mechanisms of Ageing & Development,161(Pt A):177-180
Ning J F,Zhao G P.2016.A fractal study of sound propagation characteristics in roughened porous materials[J].Wave Motion,68:190-201
Parafiniuk J,Dobrzycki ,Woc niak.Slavikite—Revision of chemical composition and crystal structure[J].American Mineralogist,95(1):11-18Rao C N R.1999. Porous materials: A case study of supramolecular organization in materials design[J].Bulletin of Materials Science,22(3):141-151
Ren G,Wei Z,Wang X,et al.2015.Research and implementation of the monitor for in situ radioactivity measurements in the marine environment[J].Instrumentation,2:33-40
孙玉坤,李冬云,邹杰,等.2016.我国磁性材料领域标准现状分析[J].磁性材料及器件,47(1):67-71
王晓彧,郑新艳,沈扬皓,等.2017.酵母菌对低浓度铀的吸附机理及动力学研究[J].环境科学学报,37(1):169-177
Wang L,Wang R,Wu J,et al.2005.Research on the chemical adsorption precursor state of CaCl2-NH3 for adsorption refrigeration[J].Science in China,48(1):70-82
王平华,王志刚,刘春华,等.2010.基于π-π相互作用合成星型聚丙烯腈-石墨烯复合材料[J].功能高分子学报,23(4):391-395
王一浒. 2017.核能开发和应用指引人类未来生活[J].黑龙江科学, 8(4):128-129
Wang Z,Huang Y,Yang J,et al.2017.The water-based synthesis of chemically stable Zr-based MOFs using pyridine-containing ligands and their exceptionally high adsorption capacity for iodine.[J].Dalton Transactions,46(23):7412
魏广芝,徐乐昌.2007.低浓度含铀废水的处理技术及其研究进展[J].铀矿冶,26(2):90-95
Zhang J,Gong C,Zeng X,et al.2016.Continuous flow chemistry: New strategies for preparative inorganic chemistry[J].Coordination Chemistry Reviews,324:39-53
邹照华,何素芳,韩彩芸,等.2010.吸附法处理重金属废水研究进展[J].环境保护科学,36(3):22-24