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Disproportionation of Silyl Formates, a Novel Strategy for Renewable Methanol Production

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HAL Id: cea-02340728

https://hal-cea.archives-ouvertes.fr/cea-02340728

Submitted on 31 Oct 2019

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Disproportionation of Silyl Formates, a Novel Strategy

for Renewable Methanol Production

Clément Chauvier, Arnaud Imberdis, Pierre Thuéry, Thibault Cantat

To cite this version:

Clément Chauvier, Arnaud Imberdis, Pierre Thuéry, Thibault Cantat. Disproportionation of Silyl

Formates, a Novel Strategy for Renewable Methanol Production. International Conference On

Phos-phorus, Boron and Silicon (PBSi 2018), Dec 2018, Barcelona, Spain. �cea-02340728�

(2)

Disproportionation of Silyl Formates, a Novel Strategy for Renewable Methanol

Production

Clément Chauvier, Arnaud Imberdis, Pierre Thuéry and Thibault Cantat

Methanol (CH3OH) is a useful C1 building block employed in the chemical industry as precursor of important

commodity chemicals such as formaldehyde, acetic acid or light olefins via the methanol-to-olefins (MTO) process. Nevertheless, the current methanol production methods is negatively impacted by the use of fossil resources. The production of CH3OH would therefore strongly benefit from the advent of more sustainable processes like the

six-electron reduction of CO2 by hydrogenation, for example. An alternative strategy has recently emerged to generate

CH3OH from CO2 via the intermediacy of formic acid (FA) as a C–H bond shuttle. At the onset, CO2 is first reduced

into FA by a relatively facile and intensively studied two-electron reduction (e.g. electroreduction). Subsequently, CH3OH is produced by the disproportionation of FA. Under standard conditions, the competitive dehydrogenation

and the targeted disproportionation of FA however display similar energy balances. To overcome this inextricable hurdle, we have thus sought a novel disproportionative route to methanol that suppresses the competing dehydrogenation pathway, while remaining attractive from the viewpoint of renewability. Towards that goal, we present a novel strategy based on the high-yielding catalytic disproportionation of silyl formates (HCO2SiR3) to

methoxysilane (CH3OSiR3) and CO2 followed by the release of free CH3OH and the complete recycling of the

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