通过电感耦合等离子体光谱(ICP)、热重(TG)等分析方法对黏土矿物的结构成分、加热特性等进行了检测;通过蒸馏冷凝等实验,实现了对吸附后黏土矿物的吸附水、层间水、结构水的分离,检测了氚在黏土矿物结构内外各类型水中的分布;通过红外吸收光谱(IR)等分析方法对氚在黏土矿物结构中的吸附位置及形态进行了检测研究;通过同位素效应等作用对氚在黏土矿物中滞留的动力与途径进行了分析.结果表明,氚在黏土矿物等土壤孔隙介质中产生滞留的主要原因是氚进入黏土矿物的吸附水、层间水、结构水引起的,氚在黏土矿物吸附水、层间水、结构水中的含量占实验中氚总量的质量分数分别为13.65%~38.71%、0.32%~5.96%、1.28%~4.37%,这一比例随黏土矿物种类不同而不同,主要是由于不同黏土矿物有着不同的组成元素及结构;氚在黏土矿物中的主要存在形态为氚羟基(OT)和氚水分子(HTO),氚在黏土矿物的吸附水、层间水中主要以氚水分子形态存在,在黏土矿物的结构水中主要以氚羟基形态存在;氚进入黏土矿物并产生滞留的动力学机制主要是分子扩散作用、电荷吸附作用、同位素交换作用和氚的同位素效应.
To investigate the mechanisms of tritium persistence in clay minerals,three types of clay soils(montmorillonite,kaolinite and illite) and tritiated water were used in this study to conduct the tritium sorption tests and the other related tests.Firstly,the ingredients,metal elements and heat properties of clay minerals were studied with some instrumental analysis methods,such as ICP and TG.Secondly,with a specially designed fractionation and condensation experiment,the adsorbed water,the interlayer water and the structural water in the clay minerals separated from the tritium sorption tests were fractionated for investigating the tritium distributions in the different types of adsorptive waters.Thirdly,the location and configuration of tritium adsorbed into the structure of clay minerals were studied with infrared spectrometry(IR) tests.And finally,the forces and mechanisms for driving tritium into the clay minerals were analyzed on the basis of the isotope effect of tritium and the above tests.Following conclusions have been reached:①The main reason for tritium persistence in clay minerals is the entrance of tritium into the adsorbed water,the interlayer water and the structural water in clay minerals.The percentage of tritium distributed in these three types of adsorptive water are in the range of 13.65%-38.71%,0.32%-5.96%,1.28%-4.37% of the total tritium used in the corresponding test,respectively.The percentages are different for different types of clay minerals.②Tritium adsorbed onto clay minerals are existed in the forms of the tritiated hydroxyl radical(OT) and the tritiated water molecule(HTO).Tritium mainly exists in tritiated water molecule for adsorbed water and interlayer water,and in tritiated hydroxyl radical for structural water.③The forces and effects driving tritium into the clay minerals may include molecular dispersion,electric charge sorption,isotope exchange and tritium isotope effect.