Abstract
Carbon monoxide (CO) is an indispensable C1 building block. For decades this abundant gas has been employed in hydroformylation and Pausen-Khand catalysis, amongst many related chemistries, where a single, non-coupled CO fragment is delivered to an organic molecule. Despite this, organometallic species which react with CO to yield C1 products remain rare, and are elusive for main group metal complexes. Here, we describe a range of amido-beryllium hydride complexes, and demonstrate their reactivity towards CO, in its mono-insertion into the Be-H bonds of these species. The small radius of the Be2+ ion in conjunction with the non-innocent pendant phosphine moiety of the developed ligands leads to a unique beryllium formyl complex with an ylidic P-COC fragment, whereby the carbon centre, remarkably, datively binds Be. This, alongside reactivity toward carbon dioxide, sheds light on the insertion chemistry of the Be-H bond, complimenting the long-known chemistry of the heavier Alkaline Earth hydrides.
Highlights
Carbon monoxide (CO) is an indispensable C1 building block
In 2015, both the groups of Jones and Hill showed that [(DippNacnac)Mg-μ2-H]2 (DippNacnac = [(DippNCMe)2CH)]−; Dipp = 2,6-iPrC6H3) reacts with CO to yield the ethenediolate moiety through C–C dimerisation of CO, in a similar fashion to fblock and early d-block metals, whilst it was shown by Jones et al that employing the less bulky DepNacnac ligand rather led to CO trimerisation in the formation of a cyclopropanetriolate complex[15,16]
Our studies began with the synthesis of amido-beryllium halide complexes, 1–3, which was readily achieved by the addition of cooled toluene to a mixture of BeBr2·(Et2O)[2] and potassium amides PhiPDippK, PhPhDippK, and iPPhDippK, respectively, at low temperature (Fig. 2)[28]
Summary
Carbon monoxide (CO) is an indispensable C1 building block. For decades this abundant gas has been employed in hydroformylation and Pausen-Khand catalysis, amongst many related chemistries, where a single, non-coupled CO fragment is delivered to an organic molecule. Our studies began with the synthesis of amido-beryllium halide complexes, 1–3, which was readily achieved by the addition of cooled toluene to a mixture of BeBr2·(Et2O)[2] and potassium amides PhiPDippK, PhPhDippK, and iPPhDippK, respectively, at low temperature (Fig. 2)[28].
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