Research and Development on C-14 Isotope Separation.

C-14 同位素分离的研究与发展。

基本信息

批准号：
10558078
负责人：
FUJII Yasuhiko
金额：
$ 3.39万
依托单位：
Tokyo Institute of Technology
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (B).
财政年份：
1998
资助国家：
日本
起止时间：
1998 至 2000
项目状态：
已结题

来源：
https://kaken.nii.ac.jp/en/grant/KAKENHI-PROJECT-10558078/
关键词：
Carbon Isotope Separation Carbon Isotope Effect Carbon Monoxide Carbon Oxide Carbamate molecular orbital theory 四配位錯体カルボニル化合物炭素 MO計算

项目摘要

The present work deals with the carbon isotope separation to reduce C-14 contaminated waste generated at the decommissioning of the graphite type reactors. Since the simplest treatment of the graphite is burning, CO and CO_2 were selected as the working materials for the separation. The research activities are divided into following three sub-topics.(1) Theoretical study on carbon isotope effects by molecular orbital theoryThe most appropriate molecular structures and molecular vibrations of CO complexes with Cu (I) and Ag (I) ions and CO_2 complexes with 30 amines were determined by using the computational chemistry program of Gaussian 98 7A.By using computed vibrational frequencies, the reduced partition function ratios of the isotopic molecules were calculated and thus the separation factors (α) of CO and CO_2 complexes were calculated.(2) Experimental study on carbon isotope effects of CO complexesCO is known to form complexes with Ag (I) and Cu (I) ions. In the present work the isotope separation coefficients of CO complexes with Ag (I) in non aqueous solvents and Cu (I) ions in aqueous solutions and amine methanol solutions were determined for the stable isotope pair of ^<12>C and ^<13>C at different temperatures. The maximum value of α observed was 1.03 at-43℃. The results suggest that one can expect the value α=1.06 for the isotope pair ^<12>C and ^<14>C.(3) Study on ion exchange multi-stage enrichmentAs a basic study on the multi-stage isotope enrichment of CO_2 complex systems, chromatographic experiments of Cu (I) and Fe (III) chloride complex were performed using column packed with anion exchange resin. In these experiments, the isotope separations of copper and iron were successfully observed at the boundaries of Cu (I) and Fe(III) ion adsorption bands.

目前的工作涉及碳同位素分离，以减少在石墨型反应器退役时产生的C-14污染废物。由于石墨的最简单处理是燃烧的，因此选择了CO和CO_2作为分离的工作材料。研究活动分为三个亚主题。（1）通过分子轨道理论对碳同位素作用的理论研究，最合适的分子结构和CO复合物的CU（I）和AG（I）和AG（I）和Co_2复合物的CO复合物的分子振动使用Gaussian 98 7A的计算化学量进行了计算率，以确定30胺的CO（I）和CO_2复合物。计算同位素分子，因此计算了CO和CO_2复合物的分离因子（α）。（2）已知CO ComplexESCO的碳同位素效应的实验研究已知与Ag（i）和Cu（i）和Cu（i）离子形成复合物。在目前的工作中，在非水溶液中与Ag（I）的CO复合物的同位素分离系数和水溶液中的Cu（i）离子在不同温度下确定了稳定的同位素对 ^<12> C和 ^<13> C的胺甲醇溶液。观察到的α的最大值为1.03 AT-43℃。结果表明，对于同位素对 ^<12> c和 ^<14> C的值α= 1.06。（3）关于离子交换多阶段多富集的研究，一项关于CO_2复杂系统多阶段同位素富集的基础研究，使用CU（I）和Fe（III）Chorper confection and Conseced Resin进行了cu（i）和Fe（iii）的色谱实验。在这些实验中，在Cu（I）和Fe（III）离子吸附带的边界上成功观察到了铜和铁的同位素分离。