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Low temperature reaction dynamics for CH3OH + OH collisions on a new full dimensional potential energy surface†
Physical Chemistry Chemical Physics ( IF 3.3 ) Pub Date : 2018-09-28 00:00:00 , DOI: 10.1039/c8cp04970j
Octavio Roncero 1 , Alexandre Zanchet , Alfredo Aguado
Affiliation  

Is the rise of the rate constant measured in laval expansion experiments of OH with organic molecules at low temperatures due to the reaction between the reactants or due to the formation of complexes with the buffer gas? This question has importance for understanding the evolution of prebiotic molecules observed in different astrophysical objects. Among these molecules methanol is one of the most widely observed, and its reaction with OH has been studied by several groups showing a fast increase in the rate constant under 100 K. Transition state theory doesn't reproduce this behavior and here dynamical calculations are performed on a new full dimensional potential energy surface developed for this purpose. The calculated classical reactive cross sections show an increase at low collision energies due to a complex forming mechanism. However, the calculated rate constant at temperatures below 100 K remains lower than the observed one. Quantum effects are likely responsible for the measured behavior at low temperatures.

中文翻译:

新的全维势能表面上 CH3OH + OH 碰撞的低温反应动力学†

在低温下 OH 与有机分子的拉瓦尔膨胀实验中测量到的速率常数的上升是由于反应物之间的反应还是由于与缓冲气体形成络合物?这个问题对于理解在不同天体物理物体中观察到的生命起源前分子的演化具有重要意义。在这些分子中,甲醇是观察最广泛的分子之一,几个小组研究了它与 OH 的反应,结果显示在 100 K 下速率常数快速增加。过渡态理论无法重现这种行为,这里进行了动力学计算在为此目的开发的新的全维势能表面上。计算出的经典反应截面显示,由于复杂的形成机制,低碰撞能量下的反应截面有所增加。然而,在低于 100 K 的温度下计算的速率常数仍然低于观察到的速率常数。量子效应可能是造成低温下测量行为的原因。
更新日期:2018-09-28
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