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基于 LaSr(PO)O 的氧磷灰石磷酸盐主晶相的陶瓷废料的制备、化学和热稳定性研究,用于高放核废物固化。

Fabrication, chemical and thermal stability studies of crystalline ceramic wasteform based on oxyapatite phosphate host LaSr(PO)O for high level nuclear waste immobilization.

机构信息

Department of Chemistry, School of Advanced Sciences, VIT, Vellore- 14, MC & MFCG, Indira Gandhi Centre for Atomic Research (IGCAR), Kalpakkam, 603102, India.

Department of Chemistry, School of Advanced Sciences, VIT, Vellore- 14, MC & MFCG, Indira Gandhi Centre for Atomic Research (IGCAR), Kalpakkam, 603102, India.

出版信息

J Hazard Mater. 2020 Jul 15;394:122552. doi: 10.1016/j.jhazmat.2020.122552. Epub 2020 Mar 16.

Abstract

Reprocessed high-level nuclear waste (HLW) contains range of radioactive components. Crystalline oxyphosphate apatite ceramic of the formula LaSr(PO)O [LSS] was investigated as a host for HLW immobilisation. The systematic study of solid solubility limit of individual rare earth ion substitution leads to the formulation of simulated wasteform of the formula LaPrNdSmGdSr(PO)O (WF1) with the waste loading of 17.95 wt% of rare-earth ions. Both parent and WF1 were synthesized by precipitation method. The thermal stress and groundwater inventory at the repository site can severely affect the wasteform performance, in addition to radiation and mechanical effects. Hence, the fabricated composition with high-level nuclear waste loading must be screened basically for chemical, thermal and radiation resistance. The present study investigated the thermal stability (by TGA), thermal expansion behaviour (by HT-XRD) and chemical durability (MCC-5) of the composition (WF1). The weight loss of WF1 being 2.2% and the average thermal expansion co-efficient (α) of 10.7 ± 1.2 × 10 K in the temperature range (298-973 K) were comparatively lower than the parent phase, LaSr(PO)O. The WF1 showed resistance to leaching of RE and P with only the leaching of Sr ion whose leach rate was of the order 10-10 gmd.

摘要

再处理高放废物(HLW)中含有一系列放射性成分。LaSr(PO)O [LSS] 型结晶氧磷灰石陶瓷被研究作为 HLW 固定化的宿主。对单一稀土离子取代的固溶极限进行系统研究,得出了模拟废物形式的化学式为 LaPrNdSmGdSr(PO)O(WF1),其废物装载量为 17.95wt%的稀土离子。母体和 WF1 均通过沉淀法合成。除辐射和机械效应外,储存库现场的热应力和地下水库存也会严重影响废物形式的性能。因此,必须对高放废物装载量的制造组成进行化学、热和辐射抗性的基本筛选。本研究研究了组成(WF1)的热稳定性(通过 TGA)、热膨胀行为(通过 HT-XRD)和化学耐久性(MCC-5)。WF1 的失重为 2.2%,在 298-973 K 的温度范围内平均热膨胀系数(α)为 10.7 ± 1.2×10-6 K,低于母体相 LaSr(PO)O。WF1 表现出对 RE 和 P 的浸出抗性,仅 Sr 离子浸出,其浸出率为 10-10 gmd 数量级。

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