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Hydrogenation of CO₂ Promoted by Silicon-Activated H₂S: Origin and Implications.

ABSTRACT: Unlike the usual method of CO_x (x = 1, 2) hydrogenation using H₂ directly, H₂S and HSiSH (silicon-activated H₂S) were selected as alternative hydrogen sources in this study for the CO_x hydrogenation reactions. Our results suggest that it is kinetically infeasible for hydrogen in the form of H₂S to transfer to CO_x at low temperatures. However, when HSiSH is employed instead, the title reaction can be achieved. For this approach, the activation of CO₂ is initiated by its interaction with the HSiSH molecule, a reactive species with both a hydridic H^?- and protonic H^?+. These active hydrogens are responsible for the successive C-end and O-end activations of CO₂ and hence the final product (HCOOH). This finding represents a good example of an indirect hydrogen source used in CO₂ hydrogenation through reactivity tuned by silicon incorporation, and thus the underlying mechanism will be valuable for the design of similar reactions.

SUBMITTER: Liu X

PROVIDER: S-EPMC7796234 | biostudies-literature | 2020 Dec

REPOSITORIES: biostudies-literature

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Hydrogenation of CO2 Promoted by Silicon-Activated H2S: Origin and Implications.

Liu Xing X

Molecules (Basel, Switzerland) 20201224 1

Unlike the usual method of COx (x = 1, 2) hydrogenation using H2 directly, H2S and HSiSH (silicon-activated H2S) were selected as alternative hydrogen sources in this study for the COx hydrogenation reactions. Our results suggest that it is kinetically infeasible for hydrogen in the form of H2S to transfer to COx at low temperatures. However, when HSiSH is employed instead, the title reaction ...[more]

PMID: 33374285

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