低浓度水蒸气/氮气混合气中金属铈的氮化反应

    Nitridation Reaction of Metallic Cerium in Mixed Gas of Low-Concentration Water Vapor and Nitrogen

    • 摘要: 将金属高效转化为氮化物及氧化物是核燃料处理中的关键步骤之一。以金属铈(Ce)为模拟材料,在低浓度水蒸气(分压≤5.0 kPa)和氮气(N2)的混合气氛中实现了金属Ce的氮化反应,并研究了水蒸气分压(0.5、1.0、2.5、5.0 kPa)和反应温度(310、330、350、370 ℃)对金属Ce氮化反应速率的影响。根据反应过程压力变化和X射线衍射(XRD)表征结果,发现金属Ce在低浓度水蒸气存在下与N2发生反应并完全转化为氮化铈(CeN)。提高水蒸气分压和反应温度可以加快金属Ce的氮化反应速率。将液态水替代水蒸气,结果显示:金属Ce仍能发生氮化反应转化为CeN,从而进一步简化了氮化反应工艺。此外,通过XRD、拉曼光谱和X射线光电子能谱表征,证明CeN产物在空气气氛中可快速氧化转化为高纯度的二氧化铈(CeO2)。本工作对金属氮化-氧化反应的研究提供了新的思路。

       

      Abstract: The efficient conversion of metals into nitrides and oxides is one of the key steps in nuclear fuel processing. In this work, metallic cerium(Ce) was used as a surrogate material. The nitridation reaction of metallic Ce was achieved in a mixed atmosphere of low-concentration water vapor(water vapor partial pressure ≤ 5.0 kPa) and nitrogen(N2). The effects of water vapor partial pressure(0.5, 1.0, 2.5 and 5.0 kPa) and reaction temperature(310, 330, 350 and 370 ℃) on the nitridation reaction rate of metallic Ce were investigated. According to the pressure change during the reaction process and the characterization results of X-ray diffraction(XRD), it is found that metallic Ce reacts with N2 in the presence of low-concentration water vapor and is completely converted to cerium nitride(CeN). Increasing the partial pressure of water vapor and the reaction temperature can accelerate the nitridation reaction rate of metallic Ce. When liquid water is used instead of water vapor, metallic Ce can still undergo the nitridation reaction and be converted into CeN, further simplifying the nitridation reaction process. In addition, through the characterization by XRD, Raman spectroscopy and X-ray photoelectron spectroscopy, it is demonstrated that the CeN product is rapidly oxidized and converted into high-purity cerium dioxide(CeO2) in an air atmosphere. This work provides new insights into the mechanisms and processes of metal nitridation-oxidation reactions.

       

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