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Dihydrogen attachment and dissociation reactions in Fe(H)2(H2)(PEtPh2)3: a DFT potential-energy scan

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Abstract

A special class of hydrogen-binding metal complexes are complexes able to bind hydrogen molecules at one or more of their ligand positions. One of such complexes, Fe(H)2(H2)(PEtPh2)3, was characterized experimentally and theoretically in previous works. Its specific properties were related to the asymmetry of the non-hydrogen ligands. Following this reasoning, attachment and dissociation of hydrogen molecule to and from the 5-coordinated and 6-coordinated complex were investigated theoretically. Relaxed and partially constrained potential-energy scans were performed and transition-states for these processes were investigated. Non-hydrogen ligand asymmetry seems to reflect on the different barrier energies for approach to and dissociation from the two dihydrogen ligand positions. Steric and environment effects are estimated comparing behavior for partially constrained and gas-phase models. On the basis of these findings, theoretically predicted pathways for single-step dihydrogen binding and dissociation processes are established, and means for experimental verification are proposed.

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Acknowledgements

During this work, the Croatian National Grid (CRO-NGI) computational resources have been used.

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  1. Faculty of Electrical Engineering and Computing, Unska 3, 10 000, Zagreb, Croatia

    Vjeran Gomzi

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Gomzi, V. Dihydrogen attachment and dissociation reactions in Fe(H)2(H2)(PEtPh2)3: a DFT potential-energy scan. Theor Chem Acc 141, 12 (2022). https://doi.org/10.1007/s00214-022-02870-0

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