Hydrogen-catalyzed acid transformation for the hydration of alkenes and epoxy alkanes over Co–N frustrated Lewis pair surfaces

Journal article

Hydrogen (H₂) 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 H₂-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 H₂ can be heterolyzed on the Co–N bond to form H^δ−–Co–N–H^δ+ and then be converted into OH^δ−–Co–N–H^δ+ accompanied by H₂ generation via a H₂O-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.

Authors: Deng, Q; Li, X; Gao, R; Wang, J; Zeng, Z

• Publication status: Published
• Peer review status: Peer reviewed
• Publisher: American Chemical Society
• Journal: Journal of the American Chemical Society
• Volume: 143
• Issue: 50
• Pages: 21294-21301
• Publication date: 2021-12-07
• Acceptance date: 2021-12-07
• DOI: 10.1021/jacs.1c08259
• EISSN: 1520-5126
• ISSN: 0002-7863
• Pmid: 34874721
• Language: English
• Keywords: FFR