Reducing CO 2 to Methanol Using Frustrated Lewis Pairs: On the Mechanism of Phosphine–Borane-Mediated Hydroboration of CO 2 - INSA Toulouse - Institut National des Sciences Appliquées de Toulouse Accéder directement au contenu
Article Dans Une Revue Journal of the American Chemical Society Année : 2014

Reducing CO 2 to Methanol Using Frustrated Lewis Pairs: On the Mechanism of Phosphine–Borane-Mediated Hydroboration of CO 2

Résumé

The full mechanism of the hydroboration of CO2 by the highly active ambiphilic organocatalyst 1-Bcat-2-PPh2–C6H4 (Bcat = catecholboryl) was determined using computational and experimental methods. The intramolecular Lewis pair was shown to be involved in every step of the stepwise reduction. In contrast to traditional frustrated Lewis pair systems, the lack of steric hindrance around the Lewis basic fragment allows activation of the reducing agent while moderate Lewis acidity/basicity at the active centers promotes catalysis by releasing the reduction products. Simultaneous activation of both the reducing agent and carbon dioxide is the key to efficient catalysis in every reduction step.
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Dates et versions

hal-01969448 , version 1 (04-01-2019)

Identifiants

  • HAL Id : hal-01969448 , version 1

Citer

Marc-André Courtemanche, Marc-André Légaré, Laurent Maron, Frédéric-Georges Fontaine. Reducing CO 2 to Methanol Using Frustrated Lewis Pairs: On the Mechanism of Phosphine–Borane-Mediated Hydroboration of CO 2. Journal of the American Chemical Society, 2014, 136 (30), pp.10708-10717. ⟨hal-01969448⟩
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