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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Thermochemistry of Ruthenium Oxyhydroxide Species and Their Impact on Volatile Speciations in Severe Nuclear Accident Conditions
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Thermochemistry of Ruthenium Oxyhydroxide Species and Their Impact on Volatile Speciations in Severe Nuclear Accident Conditions

机译：严重核事故条件下羟基氧化钌物种的热化学及其对挥发性物种的影响

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摘要

Literature thermodynamic data of ruthenium oxyhydroxides reveal large uncertainties in some of the standard enthalpies of formation, motivating the use of high-level relativistic correlated quantum chemical methods to reduce the level of discrepancies. Reaction energies leading to the formation of all possible oxyhydroxide species RuOx(OH)(y)(H2O)(z) have been calculated for a series of reactions combining DFT (TPSSh-5%HF) geometries and partition functions, CCSD(T) energies extrapolated to the complete basis set limits. The highly accurate ab initio thermodynamic data were used as input data of thermodynamic equilibrium computations to derive the speciation of gaseous ruthenium species in the temperature, pressure and concentration conditions of severe nuclear accidents occurring in pressurized water reactors. At temperatures lower than 1000 K, gaseous ruthenium tetraoxide is the dominating species, between 1000 and 2000 K ruthenium trioxide becomes preponderant, whereas at higher temperatures gaseous ruthenium oxide, dioxide and even Ru in gaseous phase are formed. Although earlier studies predicted the formation of oxyhydroxides in significant quantities, the use of highly accurate ab initio thermodynamic data for ruthenium gaseous species leads to a more reliable inventory of gaseous ruthenium species in which gaseous oxyhydroxide ruthenium molecules are formed only in negligible amounts.
机译：氢氧化正钌的文献热力学数据显示，在某些标准的生成焓中存在很大的不确定性，这促使人们使用高级相对论相关的量子化学方法来降低差异水平。已针对结合DFT（TPSSh-5％HF）几何形状和分配函数CCSD（T）的一系列反应计算了导致形成所有可能的羟基氧化物RuOx（OH）（y）（H2O）（z）的反应能能量外推到完整的基本设定极限。高精度的从头算起的热力学数据被用作热力学平衡计算的输入数据，以得出在压水反应堆中发生的严重核事故的温度，压力和浓度条件下气态钌物种的形态。在低于1000 K的温度下，气态四氧化钌是主要物质，在1000到2000 K之间的三氧化钌占优势，而在较高的温度下会形成气态氧化钌，二氧化钌甚至气相Ru。尽管较早的研究预测会形成大量的羟基氧化物，但是使用高度准确的从头算起热力学数据来分析钌气态物种会导致更可靠的气态钌物种库存，其中仅以可忽略的量形成气态羟基氧化物钌分子。

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