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Issue 22, 2019
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Fast screening of homogeneous catalysis mechanisms using graph-driven searches and approximate quantum chemistry

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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.

Graphical abstract: Fast screening of homogeneous catalysis mechanisms using graph-driven searches and approximate quantum chemistry

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Publication details

The article was received on 23 Jul 2019, accepted on 10 Oct 2019 and first published on 16 Oct 2019


Article type: Paper
DOI: 10.1039/C9CY01997A
Catal. Sci. Technol., 2019,9, 6357-6369

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    Fast screening of homogeneous catalysis mechanisms using graph-driven searches and approximate quantum chemistry

    C. Robertson and S. Habershon, Catal. Sci. Technol., 2019, 9, 6357
    DOI: 10.1039/C9CY01997A

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