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Issue 14, 2014
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Challenges in modelling homogeneous catalysis: new answers from ab initio molecular dynamics to the controversy over the Wacker process

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Abstract

We present here a review of the mechanistic studies of the Wacker process stressing the long controversy about the key reaction steps. We give an overview of the previous experimental and theoretical studies on the topic. Then we describe the importance of the most recent Ab Initio Molecular Dynamics (AIMD) calculations in modelling organometallic reactivity in water. As a prototypical example of homogeneous catalytic reactions, the Wacker process poses serious challenges to modelling. The adequate description of the multiple role of the water solvent is very difficult by using static quantum chemical approaches including cluster and continuum solvent models. In contrast, such reaction systems are suitable for AIMD, and by combining with rare event sampling techniques, the method provides reaction mechanisms and the corresponding free energy profiles. The review also highlights how AIMD has helped to obtain a novel understanding of the mechanism and kinetics of the Wacker process.

Graphical abstract: Challenges in modelling homogeneous catalysis: new answers from ab initio molecular dynamics to the controversy over the Wacker process

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Publication details

The article was received on 20 Dec 2013 and first published on 20 Mar 2014


Article type: Tutorial Review
DOI: 10.1039/C3CS60469A
Citation: Chem. Soc. Rev., 2014,43, 4940-4952
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    Challenges in modelling homogeneous catalysis: new answers from ab initio molecular dynamics to the controversy over the Wacker process

    A. Stirling, N. N. Nair, A. Lledós and G. Ujaque, Chem. Soc. Rev., 2014, 43, 4940
    DOI: 10.1039/C3CS60469A

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