Hydrosilylative reduction of carbon dioxide by a homoleptic lanthanum aryloxide catalyst with high activity and selectivity - Archive ouverte HAL
Article Dans Une Revue Dalton Transactions Année : 2021

Hydrosilylative reduction of carbon dioxide by a homoleptic lanthanum aryloxide catalyst with high activity and selectivity

Résumé

An efficient tandem hydrosilylation of CO2, which uses a combination of a simple, homoleptic lanthanum aryloxide and B(C6F5)(3), was performed. Use of a less sterically hindered silane led to an exclusive reduction of CO2 to CH4, with a turnover frequency of up to 6000 h(-1) at room temperature. The catalytic system is robust, and 19 400 turnovers could be achieved with 0.005 mol% loading of lanthanum. The reaction outcome depended highly on the nature of the silane reductant used. Selective production of the formaldehyde equivalent, i.e., bis(silyl)acetal, without over-reduction, was observed when a sterically bulky silane was used. The reaction mechanism was elucidated by stoichiometric reactions and DFT calculations.
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Dates et versions

hal-03717252 , version 1 (08-07-2022)

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Kejian Chang, Iker del Rosal, Xizhou Zheng, Laurent Maron, Xin Xu. Hydrosilylative reduction of carbon dioxide by a homoleptic lanthanum aryloxide catalyst with high activity and selectivity. Dalton Transactions, 2021, 50 (22), pp.7804-7809. ⟨10.1039/d1dt01074c⟩. ⟨hal-03717252⟩
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