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通过光谱研究研究三维石墨烯基宏观结构对 Eu(III)和 Th(IV)的吸附。

Adsorption of Eu(III) and Th(IV) on three-dimensional graphene-based macrostructure studied by spectroscopic investigation.

机构信息

Radiochemistry Laboratory, School of Nuclear Science and Technology, Lanzhou University, 730000, Lanzhou, China; Laboratory of Nuclear Energy Chemistry, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100049, China.

Laboratory of Nuclear Energy Chemistry, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100049, China.

出版信息

Environ Pollut. 2019 May;248:82-89. doi: 10.1016/j.envpol.2019.01.050. Epub 2019 Feb 4.

Abstract

One of the most important reasons for the controversy over the development of nuclear energy is the proper disposal of spent fuel. Separation of actinide and lanthanide ions is an important part of safe long-term storage of radioactive waste. Herein, a three-dimensional (3D) graphene-based macrostructure (GOCS) was utilized to remove actinide thorium and lanthanide europium ions from aqueous solutions. The adsorption of Eu(III) and Th(IV) on the GOCS was evaluated as a function of adsorption time, solution pH, initial ion concentrations, and ionic strength. The experimentally determined maximum adsorption capacities of this GOCS for Eu(III) (pH 6.0) and Th(IV) (pH 3.0) are as high as 150 and 220 mg/g, respectively. By using Fourier transformation infrared (FT-IR), X-ray photoelectron (XPS), and extended X-ray absorption fine structure (EXAFS) spectroscopy, we concluded that the Eu(III) and Th(IV) adsorption was predominantly attributed to the inner-sphere coordination with various oxygen- and nitrogen-containing functional groups on GOCS surfaces. Our selective adsorption results demonstrate that the actinide and lanthanide ions can be effectively separated from transition metal ions. This study provides new clues to the overall recycling of actinide and lanthanide ions in radioactive environmental pollution treatments.

摘要

核能发展争议的最重要原因之一是乏燃料的妥善处理。锕系元素和镧系元素离子的分离是放射性废物安全长期储存的重要组成部分。在此,利用基于三维(3D)石墨烯的宏观结构(GOCS)从水溶液中去除锕系元素钍和镧系元素铕离子。评估了 GOCS 对 Eu(III)和 Th(IV)的吸附作为吸附时间、溶液 pH 值、初始离子浓度和离子强度的函数。该 GOCS 对 Eu(III)(pH 6.0)和 Th(IV)(pH 3.0)的实验确定的最大吸附容量分别高达 150 和 220 mg/g。通过使用傅里叶变换红外(FT-IR)、X 射线光电子能谱(XPS)和扩展 X 射线吸收精细结构(EXAFS)光谱,我们得出结论,Eu(III)和 Th(IV)的吸附主要归因于与 GOCS 表面各种含氧和含氮官能团的内球配位。我们的选择性吸附结果表明,可以有效地将锕系元素和镧系元素离子与过渡金属离子分离。这项研究为放射性环境污染处理中锕系元素和镧系元素离子的整体回收提供了新线索。

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