Fast screening of homogeneous catalysis mechanisms using graph-driven searches and approximate quantum chemistry. Issue 22 (21st October 2019)

• Record Type: Journal Article
• Authors: Robertson, Christopher; Habershon, Scott
• Is Part Of: Catalysis science & technology. Volume 9:Issue 22(2019)
• Page Start: 6357
• Page End: 6369
• Publication Date: 2019-10-21
• Subjects: Catalysis -- Periodicals; 541.395
• DOI: 10.1039/c9cy01997a
• Languages: English
• ISSNs: 2044-4753

Abstract

Abstract : Automatic analysis of competing mechanisms. Abstract : Computational methods for predicting multi-step reaction mechanisms, such as those found in homogeneous catalysis by organometallic complexes, are rapidly emerging as powerful tools to support experimental mechanistic insight. We have recently shown how a graph-driven sampling scheme can be successfully used to propose a series of candidate reaction mechanisms for nanoparticle catalysis; however, identifying the most-likely reaction mechanism amongst this candidate set in an efficient scheme remains a challenge. Here, we show how simple descriptors for each reaction path, calculated using quick semi-empirical quantum chemistry, enable identification of the mechanism, but only if one considers both thermodynamic and kinetic parameters of proposed reaction mechanisms. Successful application to cobalt-catalysed alkene hydroformylation is used to benchmark this strategy, and provides insight into remaining algorithmic challenges.