Understanding silver structural rearrangement on zeolite Y for methyl iodide capture in nuclear safety system

IF 12.2 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL
Young-Ho Cho , Keon Ho , Hyun-Chul Lee , Kyung-Min Kim , Dae Woo Kim , Chang-Ha Lee
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Abstract

To enhance nuclear power safety, the adsorptive passive capture of emitted radioactive organic iodine under harsh conditions is essential. Silver states and CH3I reactive adsorption on silver zeolite Y were studied under simulated accident conditions (10 ppm CH3I at 7 bar, 0–80 % RH, and 150 °C). The roles of Ag⁺ ions, silver clusters, and external silver aggregates in silver zeolite Y during CH3I capture were analyzed. Ag⁺ ions enabled near-complete CH3I removal (<0.1 ppm), while silver clusters and external silver aggregates enhanced the overall adsorption capacity. It was also noted that the formation of AgnY+ clusters within sodalite cages could potentially block pores, leading to immediate breakthrough. Pelletized silver zeolite Y adsorbents demonstrated optimal CH3I capture capacity at sufficiently auto-reduced states. Under dry conditions, Ag⁺ ions primarily promoted light hydrocarbon by-products, whereas silver clusters contributed to the formation of heavier hydrocarbons. Humid conditions led to the weakening of adsorption affinity and rate of CH3I, along with oxygenated by-products. The findings, including silver structural rearrangement by auto-reduction, provide critical guidance for understanding the adsorption mechanism and improving the design efficiency of a nuclear containment system.

Abstract Image

了解Y型沸石上银结构重排对核安全系统中碘化甲酯捕获的影响
为了提高核电安全,在恶劣条件下对放射性有机碘进行吸附被动式捕获是十分必要的。在模拟事故条件下(10 ppm CH3I, 7 bar, 0-80% RH, 150°C),研究了银态和CH3I在银沸石Y上的反应吸附。分析了银沸石Y中Ag +离子、银簇和外部银聚集体在CH3I捕获过程中的作用。Ag +离子几乎可以完全去除CH3I (<0.1 ppm),而银团簇和外部银聚集体增强了整体吸附能力。研究人员还指出,在钠石笼中形成的Ag6Y+Ag6Y+团簇可能会堵塞孔隙,从而立即取得突破。颗粒状银沸石Y吸附剂在充分自动还原状态下表现出最佳的CH3I捕获能力。在干燥条件下,Ag +主要促进了轻碳氢化合物的生成,而银团簇则促进了重碳氢化合物的生成。潮湿条件导致CH3I的吸附亲和力和吸附速率减弱,氧化副产物也随之减弱。这些发现,包括银的自动还原结构重排,为理解吸附机制和提高核安全壳系统的设计效率提供了重要的指导。
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来源期刊
Journal of Hazardous Materials
Journal of Hazardous Materials 工程技术-工程:环境
CiteScore
25.40
自引率
5.90%
发文量
3059
审稿时长
58 days
期刊介绍: The Journal of Hazardous Materials serves as a global platform for promoting cutting-edge research in the field of Environmental Science and Engineering. Our publication features a wide range of articles, including full-length research papers, review articles, and perspectives, with the aim of enhancing our understanding of the dangers and risks associated with various materials concerning public health and the environment. It is important to note that the term "environmental contaminants" refers specifically to substances that pose hazardous effects through contamination, while excluding those that do not have such impacts on the environment or human health. Moreover, we emphasize the distinction between wastes and hazardous materials in order to provide further clarity on the scope of the journal. We have a keen interest in exploring specific compounds and microbial agents that have adverse effects on the environment.
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