| Özet: | <p>Hydrogen (H<sub>2</sub>) is widely used as a reductant for many hydrogenation reactions; however, it has not been recognized as a catalyst for the acid transformation of active sites on solid surface. Here, we report the H<sub>2</sub>-promoted hydration of alkenes (such as styrenes and cyclic alkenes) and epoxy alkanes over single-atom Co-dispersed nitrogen-doped carbon (Co-NC) via a transformation mechanism of acid–base sites. Specifically, the specific catalytic activity and selectivity of Co-NC are superior to those of classical solid acids (acidic zeolites and resins) per micromole of acid, whereas the hydration catalysis does not take place under a nitrogen atmosphere. Detailed investigations indicate that H<sub>2</sub> can be heterolyzed on the Co–N bond to form H<sup>δ−</sup>–Co–N–H<sup>δ+</sup> and then be converted into OH<sup>δ−</sup>–Co–N–H<sup>δ+</sup> accompanied by H<sub>2</sub> generation via a H<sub>2</sub>O-mediated path, which significantly reduces the activation energy for hydration reactions. This work not only provides a novel catalytic method for hydration reactions but also removes the conceptual barriers between hydrogenation and acid catalysis.</p>
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