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Validating a model to predict the chemistry of the fuel used in radioisotope power systems

机译：验证模型以预测放射性同位素动力系统中使用的燃料的化学性质

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U.S. radioisotope power systems convert the decay heat from PuO fuel into electricity using various forms of thermoelectric conversion technology. When placed in an environment that has low oxygen potential and very high temperatures, the fuel can undergo reduction to a sub-stoichiometric form (PuO-x). In order to better understand this system, a model was developed that combines the known relationship between stoichiometry (i.e., x), temperature, and oxygen potential with the chemical thermodynamics of graphite, carbon monoxide, and carbon dioxide. Because of the challenges surrounding PuO experimentation, the model has been benchmarked against a common PuO surrogate: CeO. Samples of CeO were sealed into a reaction tube and allowed to react with graphite using a reaction temperature of 1273 K. When these reaction conditions were used, the model (x = 0.268) and experiment (x = 0.272 + 0.008) found very good agreement. Successful benchmarking of this model suggests that it will be useful in predicting the complex chemical interaction that can occur between the materials inside a radioisotope power system. Kinetic data obtained from these experiments suggests that reaction rates are very slow and that it could take hundreds of hours to reach equilibrium. A change in the rate limiting reaction mechanism is also observed when x > 0.25, but does not appear to impact the thermodynamic equilibrium. In addition to helping inform a Pu based system, this model may also be useful for predicting the chemistry found inside an Am based system, which is currently under development for the European Space Agency.
机译：美国放射性同位素动力系统使用各种形式的热电转换技术将PuO燃料产生的衰变热转换为电能。当放置在氧势低且温度非常高的环境中时，燃料可能会还原为亚化学计量形式（PuO-x）。为了更好地理解该系统，开发了一种模型，该模型将化学计量（即x），温度和氧势之间的已知关系与石墨，一氧化碳和二氧化碳的化学热力学相结合。由于围绕PuO实验的挑战，该模型已针对常见的PuO替代品CeO进行了基准测试。将CeO样品密封到反应管中，并使用1273 K的反应温度使其与石墨反应。使用这些反应条件时，模型（x = 0.268）和实验（x = 0.272 + 0.008）发现很好的一致性。该模型的成功基准测试表明，该模型可用于预测放射性同位素动力系统内部材料之间可能发生的复杂化学相互作用。从这些实验获得的动力学数据表明，反应速度非常慢，可能需要数百小时才能达到平衡。当x> 0.25时，也会观察到限速反应机理的变化，但似乎不会影响热力学平衡。除了帮助告知基于Pu的系统外，该模型还可用于预测基于Am的系统中发现的化学成分，该系统目前正在为欧洲航天局开发。

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