Hydrogenation of CO<sub>2</sub> Promoted by Silicon-Activated H<sub>2</sub>S: Origin and Implications

oleh: Xing Liu

Format: Article
Diterbitkan: MDPI AG 2020-12-01

Deskripsi

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