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首页> 外文期刊>Chemistry: A European journal >Solid-State Dynamics of Uranyl Polyoxometalates
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Solid-State Dynamics of Uranyl Polyoxometalates

机译：铀酰多金属氧酸盐的固态动力学

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摘要

Understanding fundamental uranyl polyoxometalate (POM) chemistry in solution and the solid state is the first step to defining its future role in the development of new actinide materials and separation processes that are vital to every step of the nuclear fuel cycle. Many solid-state geometries of uranyl POMs have been described, but we are only beginning to understand their chemical behavior, which thus far includes the role of templates in their self-assembly, and the dynamics of encapsulated species in solution. This study provides unprecedented detail into the exchange dynamics of the encapsulated species in the solid state through Magic Angle Spinning Nuclear Magnetic Resonance (MAS NMR) spectroscopy. Although it was previously recognized that capsule-like molybdate and uranyl POMs exchange encapsulated species when dissolved in water, analogous exchange in the solid state has not been documented, or even considered. Here, we observe the extremely high rate of transport of Li~+ and aqua species across the uranyl shell in the solid state, a process that is affected by both temperature and pore blocking by larger species. These results highlight the untapped potential of emergent f-block element materials and vesicle-like POMs.
机译：了解溶液和固态中的基本铀酰多金属氧酸盐（POM）化学原理是定义其在开发新的materials系元素材料和分离工艺（对核燃料循环的每一步至关重要）的未来作用中的第一步。已经描述了许多铀酰POM的固态几何形状，但我们才刚刚开始了解它们的化学行为，到目前为止，包括模板在其自组装中的作用以及溶液中包封物质的动力学。这项研究通过魔角旋转核磁共振（MAS NMR）光谱为固态封装的物质的交换动力学提供了前所未有的细节。尽管先前已经认识到，胶囊状的钼酸盐和铀酰POM在溶解于水中时会交换被包封的物质，但尚未记录或什至没有考虑固态的类似交换。在这里，我们观察到Li〜+和水族物质在固态状态下穿过铀酰壳的传输速率非常高，该过程受温度和较大物种的孔阻塞的影响。这些结果突出了新兴的f块元素材料和囊泡状POMs的未开发潜力。

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