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Evolution of chromium, manganese and iron oxidation state during conversion of nuclear waste melter feed to molten glass

机译:核废料料转换期间铬,锰和铁氧化状态的演变熔融玻璃

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摘要

Oxidation state and chemical conversion of three surrogate nuclear high-level waste melter feeds heat treated to temperatures between 500 and 1200 degrees C were studied using X-ray near-edge structure, feed expansion tests, X-ray diffraction, and evolved gas analyses. For the high-chromium feed (3.00 mass% Cr2O3 in glass), the average Cr oxidation state was predominately Cr3+ at the lowest and highest heat-treatment temperatures and Cr6+ at intermediate temperatures while the Fe coordination shifted from octahedral to non-centrosymmetric tetrahedral at higher temperatures with Fe oxidation state unchanged. For the high-manganese-high-iron feed (3.23 mass% MnO and 16.01 mass% Fe2O3 in glass), the average Mn oxidation state decreased from 4 to similar to 2 while the Fe oxidation state shifted towards increasing ferrous content and changed from five-fold coordination to tetrahedral. For the high-alumina feed (24.02 mass% Al2O3 in glass), average Fe coordination did not change, but Fe oxidation state shifted towards higher ferrous content with increasing temperature.
机译:使用X射线近边缘结构,进料膨胀试验,X射线衍射和进化气体分析研究了三种替代核高级废物饲料的氧化状态和化学转化为500和1200℃的温度。对于高铬饲料(3.00质量%CR2O3在玻璃中),平均CR氧化状态主要是在最低和最高的热处理温度和中间温度下的CR6 +处的CR3 +,而FE协调从八面体转移到非亚里索对称四面体Fe氧化状态不变的较高温度。对于高锰 - 高铁进料(3.23质量%MNO和16.01质量%Fe2O3),平均Mn氧化态从4降低到类似于2,而Fe氧化状态朝向增加的黑色含量增加并从五个变化 - 对四面体的协调。对于高氧化铝进料(24.02质量%Al 2 O 3在玻璃中),平均Fe配位不会改变,但Fe氧化状态随温度升高而变化朝向更高的黑色含量。

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