Computer-Generated Kinetics for Coupled Heterogeneous/Homogeneous Systems: A Case Study in Catalytic Combustion of Methane on Platinum

The automatic microkinetic mechanism generator for heterogeneous catalysis, RMG-Cat, has been extensively updated. Density functional theory calculations were performed for 69 adsorbates on Pt(111), and the resulting thermodynamic properties were added to RMG-Cat. The thermo database is significantly more accurate; it includes nitrogen-containing adsorbates for the first time as well as better capabilities for predicting the thermochemistry of novel adsorbates. Additionally, RMG-Cat can now simultaneously pursue a mechanism expansion both on the surface and in the gas phase. This heterogeneous/homogeneously coupled capability is tested on the catalytic combustion of methane on platinum. The results confirm that under some conditions the catalyst is capable of inducing thermal ignition in the gas phase.面向多相催化的自动微观动力学机理生成器RMG-Cat已完成全面更新。研究团队针对Pt(111)晶面上的69种吸附质开展了密度泛函理论（Density Functional Theory）计算，并将所得热力学性质添加至RMG-Cat中。该热力学数据库的精度显著提升，首次纳入含氮吸附质，同时具备更优异的新型吸附质热化学性质预测能力。此外，RMG-Cat如今可同时在表面相与气相中开展机理拓展工作。这种多相-均相耦合功能已通过铂基催化剂上的甲烷催化燃烧实验得到验证。实验结果证实，在部分工况下，该催化剂可引发气相热点火。