Combustion synthesis of Hf-doped zirconolite-rich composite waste forms and the aqueous durability

Combustion synthesis of Hf-doped zirconolite-rich composite waste forms and the aqueous durability
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铪掺杂富锆石复合废物形态的燃烧合成及其水耐久性

DOI:
10.1007/s40145-019-0339-z
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发表时间:
2019-07
影响因子:
16.9
通讯作者:
Zhang Haibin
Zhang Haibin
中科院分区:
材料科学1区
文献类型:
--
作者:
Zhang Kuibao;Yin Dan;He Zongsheng;Luo Baozhu;Zhang Haibin

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锆英石被公认为是处置高放废物(HLW)最耐用的废物基质之一。本研究采用氧化铪作为四价锕系元素的替代物。以CuO为氧化剂,采用燃烧合成法(CS)快速制备了含Hf的锆英石基复合材料(CaZr 1 − xHfxTi 2 O 7),并引入快速压制(QP)技术获得致密化样品。与固相反应过程相似,CS反应中锆英石中Zr位完全被Hf(x= 1.0)占据。最终产物中保持了原始的2 M锆沸石结构,并产生了少量的钙钛矿杂质相。测试了代表性样品(Cu-Hf-0.6)的水耐久性,其中Ca、Cu和Hf的42天归一化浸出率(LRi)分别为0.25、3.10×10−2和1.11×10− 8 g·m−2·d−1。
Zirconolite is recognized as one of the most durable waste matrices for the disposal of high-level radioactive wastes (HLWs). In this study, HfO2was employed as the surrogate of tetravalent actinides. Hf-bearing zirconolite-based composite waste forms (CaZr1−xHfxTi2O7) were rapidly prepared by combustion synthesis (CS) using CuO as the oxidant, where quick pressing (QP) was introduced to obtain densified samples. Similar as solid state reaction process, the Zr site of zirconolite can be totally occupied by Hf (x= 1.0) under the CS reaction. The original 2M zirconolite structure was maintained and a small amount of perovskite impurity phase was generated in the final products. The aqueous durability of representative sample (Cu-Hf-0.6) was tested, where the 42-day normalized leaching rates (LRi) of Ca, Cu, and Hf are 0.25, 3.10×10−2, and 1.11×10−8g·m−2·d−1.
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