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oaioai:figshare.com:article/3518132

Reactivity of (Pyridine-Diimine)Fe Alkyl Complexes with Carbon Dioxide

Authors
Publication date
2016
Publisher
Doi

    Abstract

    The reaction of CO<sub>2</sub> with (PDI)­FeMe (<b>1</b>), (PDI)­Fe­(Me)­PMe<sub>3</sub> (<b>1-PMe</b><sub><b>3</b></sub>) and [(PDI)­FeMe]­[BPh<sub>4</sub>] (<b>2</b>, PDI = 2,6-(2,6-<sup><i>i</i></sup>Pr<sub>2</sub>–C<sub>6</sub>H<sub>3</sub>–NCMe)<sub>2</sub>–C<sub>5</sub>H<sub>3</sub>N) generates (PDI)­Fe­OAc (<b>3</b>), (PDI)­Fe­(OAc)­PMe<sub>3</sub> (<b>3-PMe</b><sub><b>3</b></sub>), and [(PDI)­FeOAc]­[BPh<sub>4</sub>] (<b>4</b>), respectively. Kinetic data and solvent effects provide evidence that these reactions occur by precoordination of CO<sub>2</sub> to the Fe center regardless of the charge state and thus favor an insertion mechanism for carboxylation. Carboxylation of <b>1-PMe</b><sub><b>3</b></sub> requires initial dissociation of PMe<sub>3</sub> to generate <b>1</b>, which reacts with CO<sub>2</sub>; <b>1-PMe</b><sub><b>3</b></sub> itself does not react directly with CO<sub>2</sub>. CO<sub>2</sub> reacts 5 times faster with neutral <b>1</b> than with cationic <b>2</b> (at 0 °C), which is ascribed to the higher nucleophilicity of the Fe–Me group in <b>1</b>

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    Last time updated on 12/02/2018

    This paper was published in FigShare.

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