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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >A theoretical study of the H-abstraction reactions from HOI by moist air radiolytic products (H, OH, and O (3P)) and iodine atoms (2P3/2)
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A theoretical study of the H-abstraction reactions from HOI by moist air radiolytic products (H, OH, and O (3P)) and iodine atoms (2P3/2)

机译：湿空气辐射分解产物（H，OH和O（3P））和碘原子（2P3 / 2）对HOI的H吸收反应的理论研究

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摘要

The rate constants of the reactions of HOI molecules with H, OH, O (3P), and I (2P3/2) atoms have been estimated over the temperature range 300-2500 K using four different levels of theory. Geometry optimizations and vibrational frequency calculations are performed using MP2 methods combined with two basis sets (cc-pVTZ and 6-311G(d,p)). Single-point energy calculations are performed with the highly correlated ab initio coupled cluster method in the space of single, double, and triple (pertubatively) electron excitations CCSD(T) using the cc-pVTZ, cc-pVQZ, 6-311+G(3df,2p), and 6-311++G(3df,3pd) basis sets. Reaction enthalpies at 0 K were calculated at the CCSD(T)/cc-pVnZ//MP2/cc-pVTZ (n = T and Q), CCSD(T)/6-311+G(3df,2p)//MP2/6-311G(d,p), and CCSD(T)/6-311++G(3df,3pd)//MP2/6- 311G(d,p) levels of theory and compared to the experimental values taken from the literature. Canonical transition-state theory with an Eckart tunneling correction is used to predict the rate constants as a function of temperature. The computational procedure has been used to predict rate constants for H-abstraction elementary reactions because there are actually no literature data to which the calculated rate constants can be directly compared. The final objective is to implement kinetics of gaseous reactions in the ASTEC (accident source term evaluation code) program to improve speciation of fission products, which can be transported along the reactor coolant system (RCS) of a pressurized water reactor (PWR) in the case of a severe accident.
机译：HOI分子与H，OH，O（3P）和I（2P3 / 2）原子的反应速率常数已使用四种不同的理论水平在300-2500 K的温度范围内进行了估算。使用MP2方法结合两个基本集（cc-pVTZ和6-311G（d，p））执行几何优化和振动频率计算。单点能量计算是使用cc-pVTZ，cc-pVQZ，6-311 + G在单，双和三（高位）电子激发CCSD（T）的空间中使用高度相关的从头算耦合簇方法进行的（3df，2p）和6-311 ++ G（3df，3pd）基础集。在CCSD（T）/ cc-pVnZ // MP2 / cc-pVTZ（n = T和Q），CCSD（T）/ 6-311 + G（3df，2p）// MP2下计算0 K时的反应焓/ 6-311G（d，p）和CCSD（T）/ 6-311 ++ G（3df，3pd）// MP2 / 6- 311G（d，p）的理论水平，并与从文献。具有Eckart隧道校正的规范过渡态理论可用来预测速率常数与温度的函数关系。由于实际上没有文献数据可以直接比较所计算出的速率常数，因此该计算程序已用于预测H-抽象反应的速率常数。最终目标是在ASTEC（事故源术语评估代码）程序中实施气态反应动力学，以改善裂变产物的形态，这些裂变产物可沿压水反应堆（PWR）的反应堆冷却剂系统（RCS）进行运输。发生严重事故的情况。

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