New lead-free chemistry for in-situ monitoring of advanced nuclear power plant

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Abstract

Nuclear power is essential for sustainable energy infrastructure and economic development, necessitating materials for high-radiation environments that can facilitate visualization and observation. Conventional lead glass is inadequate for future requirements due to radiation-induced darkening, poor mechanical properties, and toxicity. Therefore, there is urgent to find new window materials that offer multi-ionization shielding (particularly against deep-penetrating gamma ray, γ, and neutron, n, radiations), desirable opto-mechanical properties, service stability against darkening, and non-toxicity. In this study, we report a family of transparent rare-earth pyrochlore ceramics LaxGd2−xZr2O7, offering unique chemo-physical properties that are ideal for robust radiation shielding windows. Remarkably, we demonstrated the capability of maintaining high transparency under heavy-dose exposure to 1000 ​kGy 60Co γ radiation. We observed the service stability against radiation darkening can be greatly enhanced with La-rich compositions, while Gd-rich compositions undergo shallow darkening that can be reversibly recovered under visible light. This behavior is attributed to mitigated oxygen migration from 48f to 8a in La-rich compositions, which have high pyrochlore phase stability and well-ordered atomic structures, and reversible oxygen migration between 48f and 8a in Gd-rich compositions, which remain active at room temperature. Our proposal and demonstration unlock ample opportunities in designing functional transparent ceramics as window materials for demanding applications in high-radiation environments.

Abstract Image

用于先进核电站原位监测的新型无铅化学材料
核电对可持续能源基础设施和经济发展至关重要,因此需要可用于高辐射环境的材料,以方便可视化和观察。传统的铅玻璃由于辐射引起的暗化、机械性能差和毒性等问题,已无法满足未来的要求。因此,急需找到能提供多电离屏蔽(特别是针对深穿透伽马射线(γ)和中子辐射(n))、理想的光学机械性能、防变黑的服役稳定性和无毒性的新型窗户材料。在这项研究中,我们报告了一系列透明的稀土热长石陶瓷 LaxGd2-xZr2O7,它们具有独特的化学物理特性,是坚固耐用的辐射屏蔽窗的理想材料。值得注意的是,我们展示了在 1000 kGy 60Co γ 重剂量辐射下保持高透明度的能力。我们观察到,富含 La 的成分可大大提高抗辐射变暗的稳定性,而富含 Gd 的成分则会出现浅度变暗,但在可见光下可逆恢复。这种行为归因于富含 La 的成分中从 48f 到 8a 的氧迁移得到了缓解,La 具有较高的热释电晶体相稳定性和有序的原子结构,而富含 Gd 的成分中从 48f 到 8a 的氧迁移是可逆的,Gd 在室温下保持活跃。我们的建议和演示为设计功能性透明陶瓷提供了大量机会,可将其作为窗口材料,用于高辐射环境中的苛刻应用。
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CiteScore
33.30
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