Efficiency of carbothermal reduction in treating NORM waste containing Ba(226Ra)SO4

IF 1.6 3区化学 Q3 CHEMISTRY, ANALYTICAL Journal of Radioanalytical and Nuclear Chemistry Pub Date : 2025-01-06 DOI:10.1007/s10967-024-09935-3

Lin Zhang, Zonghui Lu, Zhe Su, Ye Zhang, Hui He

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Abstract

This study delineates the intrinsic composition of naturally occurring radioactive material (NORM) waste and affirms the viability of the carbothermal reduction method for the transformation of Ba(²²⁶Ra)SO₄ into Ba(²²⁶Ra)S. The waste was solubilized using ethylenediaminetetraacetic acid, and its constituents were determined employing X-ray diffraction and inductively coupled plasma-atomic emission spectrometry, identifying barium sulfate (BaSO₄) as the predominant component at a weight percentage of 67.13%. Thermodynamic calculations of the carbothermal reduction process were conducted utilizing the HSC Chemistry software, followed by systematic kinetic validation experiments with BaSO₄ as a proxy for Ba(²²⁶Ra)SO₄. The results demonstrate that carbothermal reduction of BaSO₄ initiates at temperatures surpassing 776 °C. The conversion efficiency of BaSO₄ to BaS is markedly influenced by temperature, with the rate escalating from 47.48% to 89.83% as the temperature is incremented from 850 °C to 950 °C. This method effectively converts the very insoluble NORM waste into readily soluble forms of Ba and Ra.

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碳热还原法处理含 Ba(226Ra)SO4 的核燃料废料的效率

本研究描述了天然放射性物质（NORM）废料的固有组成，并肯定了碳热还原法将Ba(226Ra)SO4转化为Ba(226Ra)S的可行性。采用乙二胺四乙酸对其进行溶解处理，采用x射线衍射和电感耦合等离子体原子发射光谱法对其成分进行测定，发现硫酸钡（BaSO4）为主要成分，质量分数为67.13%。利用HSC化学软件进行了碳热还原过程的热力学计算，然后以BaSO4作为Ba(226Ra)SO4的代理进行了系统的动力学验证实验。结果表明，当温度超过776℃时，BaSO4开始碳热还原。温度对BaSO4转化为BaS的效率有显著影响，温度从850℃升高到950℃，转化率从47.48%上升到89.83%。这种方法有效地将不溶的NORM废物转化为易溶的Ba和Ra。

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来源期刊

Journal of Radioanalytical and Nuclear Chemistry 化学-分析化学

CiteScore

2.80

自引率

18.80%

发文量

504

审稿时长

2.2 months

期刊介绍： An international periodical publishing original papers, letters, review papers and short communications on nuclear chemistry. The subjects covered include: Nuclear chemistry, Radiochemistry, Radiation chemistry, Radiobiological chemistry, Environmental radiochemistry, Production and control of radioisotopes and labelled compounds, Nuclear power plant chemistry, Nuclear fuel chemistry, Radioanalytical chemistry, Radiation detection and measurement, Nuclear instrumentation and automation, etc.