矿物吸附剂结构对水溶液脱泥作用的影响

O. Pushkarov, I. Sevruk, V. Dolin
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引用次数: 0

摘要

介绍。氚在核反应堆中形成,主要排放到水圈中。在乏核燃料后处理过程中,相当一部分氚也会进入环境。目前的问题是开发有效、简单、经济、廉价和低能耗的方法,从大量的低、中水平水溶液中提取氚。回顾以前的出版物。在核电站,它被广泛用于“氢-水”系统中通过同位素交换净化小体积高活性工艺水[专利号:RU 2380144, RU 2060801, RU 2525423, RU 2148426]。目前存在通过低温精馏对НTO进行同位素分馏的方法,这些方法要么需要大量的能量消耗,要么在1.1水平下的同位素效应非常不显著[专利号UA 57558, RU 2010772, RU 2091336]。在世界实践中,矿物吸附剂被广泛使用,但还没有开发出用于净化氚水溶液的技术。我们之前的研究已经阐明了使用层状硅酸盐和沸石从水溶液中提取氚的可能性(专利为UA 103033, UA 103050, UA 113348)。其他矿物从水溶液中吸附氚的能力仍未得到解决。为了解决这一问题,我们参与了从氢氧化物、硫酸盐和链状硅酸盐类矿物的实验研究。这项工作的目的是确定矿物吸附剂的结构特征对从原氚水中去除氚的影响(“НTO”),以及使用更广泛的矿物谱作为这种吸附剂的可能性。从氚化水中提取的氚中,高达39%的氚以表面吸附的形式保留在hisitite中。在边界层中,较重的НTO分子比H2O分子保留更大的优势(α = 1.14)。石膏:由于石膏晶体晶格中的OH基团被矿物结构中的OT基团取代,在部分同位素-氢分馏中吸收的氚溶液中,高达36%是固定的。由于硅灰石中存在缠结的纤维微结构,实验中从氚化水溶液中吸收的氚有很大一部分以表面吸附形式固定(61.3%,分馏系数α = 1.03)。由于重氢同位素与氧形成的共价键比与protium形成的共价键强(α = 1.23),当CaO与氚化水相互作用时,其羟基化反应伴随着НTO分子解离形成的OT基团与钙的主要结合。从水溶液中提取氚的总能力最高的是hibite(38.7%),最低的是硅灰石(34.5%)。本文所获得的新的科学结果与我们以往的研究结果相结合,为更有效地开发水溶液脱硝方法提供了机会。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Influence of the structure of a mineral adsorbent on the detritization of aqueous solutions
Introduction. Formed in a nuclear reactor, tritium is mainly discharged into the hydrosphere. A significant part of tritium also enters the environment during the reprocessing of spent nuclear fuel. Currently, the problem is the development of effective, simple, affordable, inexpensive and low-energy methods for extracting tritium from large volumes of low- and intermediate-level aqueous solutions. Review of previous publications. At nuclear power plants, it is widely used for the purification of small volumes of highly active process waters by isotopic exchange in the "hydrogen-water" system [patents RU 2380144, RU 2060801, RU 2525423, RU 2148426]. There are methods for isotopic fractionation of НTO by low-temperature rectification, which either requires significant energy consumption or occurs with a very insignificant isotopic effect at the level of 1.1 [patents UA 57558, RU 2010772, RU 2091336]. In world practice, mineral adsorbents are widely used, but there are no developments designed to purify aqueous solutions from tritium. Our previous studies have clarified the possibility of using layered silicates and zeolite for the extraction of tritium from aqueous solutions (patents UA 103033, UA 103050, UA 113348). The ability of other minerals to adsorb tritium from aqueous solutions remains unresolved. In order to solve this problem, we involved in experimental research minerals from the classes of hydroxides, sulfates and chain silicates. Purpose. The aim of the work is to determine the influence of the structural features of mineral adsorbents on the removal of tritium from proto-tritium water ("НTO") and the possibility of using a more expanded spectrum of minerals as such adsorbents. Results. Up to 39% of tritium extracted from tritiated water is retained in hibsite in surface adsorbed form. In the boundary layer, heavier НTO molecules are retained with a greater advantage than H2O molecules (α = 1.14). Gypsum: due to the substitution of OH groups of the gypsum crystal lattice by OT groups in the mineral structure, up to 36% of the absorbed tritium solution with partial isotope-hydrogen fractionation is fixed. Due to the presence of tangled fibrous microtexture in wollastonite, a significant part of tritium absorbed during the experiment from a solution of tritiated water is fixed in a surface adsorbed form (61.3%, fractionation coefficient α = 1.03). The reaction of hydroxylation of CaO when it interacts with tritiated water is accompanied by a predominant binding to calcium of OT groups formed by the dissociation of НTO molecules because heavy hydrogen isotopes form a stronger covalent bond with oxygen than with protium (α = 1.23). Conclusions. The highest total ability to extract tritium from aqueous solution was observed in hibsite (38.7%), and the lowest - in wollastonite (34.5%). The obtained new scientific results with the involvement of the results of our previous studies provide an opportunity for more effective development of methods for detritalization of aqueous so-lutions.
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