Abdulsattar Mudar Ahmed
Ministry of Science and Technology, Baghdad, Iraq.
J Mol Model. 2023 Sep 6;29(10):304. doi: 10.1007/s00894-023-05710-5.
Using transition state theory, acetone sensing by pristine and rhodium-doped tin dioxide is discussed. The Evans-Polanyi principle is modified from its original formulation commensurate with the Arrhenius equation to be more suitable for transition state theory. The new formalism for the activation energy replaces enthalpy with Gibbs free energy in the original Evans-Polanyi principle. The new formalism considers reaction entropy, which is not considered previously in Evans-Polanyi principle. Response and response time of interaction of acetone with both pristine and Rh-doped SnO clusters is calculated. Variations of response in terms of acetone concentration and temperature are calculated and compared to the experiment. Acceptable agreement between theory and experiment that calls for more comparisons to demonstrate the modified approach.
The pristine and Rh-doped clusters and their interaction with acetone are simulated using density functional theory at the B3LYP level. 6-311G** and SDD (for heavy atoms) basis sets are used to optimize the structures examined in the present work. Gaussian 09 program and accompanying software performed the current tasks.
运用过渡态理论，探讨了原始二氧化锡和铑掺杂二氧化锡对丙酮的传感作用。埃文斯-波拉尼原理在其原始表述基础上进行了修正，使其与阿仑尼乌斯方程相适配，从而更适用于过渡态理论。活化能的新形式在原始埃文斯-波拉尼原理中用吉布斯自由能取代了焓。新形式考虑了反应熵，而这在之前的埃文斯-波拉尼原理中并未涉及。计算了丙酮与原始二氧化锡和铑掺杂二氧化锡团簇相互作用的响应及响应时间。计算了响应随丙酮浓度和温度的变化，并与实验结果进行比较。理论与实验之间达成了可接受的一致性，这需要更多比较来证明这种修正方法。
在B3LYP水平上使用密度泛函理论模拟原始二氧化锡和铑掺杂团簇及其与丙酮的相互作用。采用6-311G**和SDD（用于重原子）基组来优化本研究中所考察的结构。使用高斯09程序及配套软件执行当前任务。
