First principles reaction discovery: from the Schrodinger equation to experimental prediction for methane pyrolysis.

ABSTRACT: Our recent success in exploiting graphical processing units (GPUs) to accelerate quantum chemistry computations led to the development of the ab initio nanoreactor, a computational framework for automatic reaction discovery and kinetic model construction. In this work, we apply the ab initio nanoreactor to methane pyrolysis, from automatic reaction discovery to path refinement and kinetic modeling. Elementary reactions occurring during methane pyrolysis are revealed using GPU-accelerated ab initio molecular dynamics simulations. Subsequently, these reaction paths are refined at a higher level of theory with optimized reactant, product, and transition state geometries. Reaction rate coefficients are calculated by transition state theory based on the optimized reaction p

SUBMITTER: Xu R 

PROVIDER: S-EPMC10337770 | biostudies-literature | 2023 Jul

REPOSITORIES: biostudies-literature