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Hydrogen-Catalyzed Acid Transformation for the Hydration of Alkenes and Epoxy Alkanes over Co-N Frustrated Lewis Pair Surfaces

Authors :
Deng, Q
Li, X
Gao, R
Wang, J
Zeng, Z
Zou, J-J
Deng, S
Tsang, SCE
Source :
Journal of the American Chemical Society. 143(50)
Publication Year :
2021

Abstract

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 H2can be heterolyzed on the Co–N bond to form Hδ−–Co–N–Hδ+and then be converted into OHδ−–Co–N–Hδ+accompanied by H2generation 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.

Details

ISSN :
15205126
Volume :
143
Issue :
50
Database :
OpenAIRE
Journal :
Journal of the American Chemical Society
Accession number :
edsair.doi.dedup.....a6a7c7778579e5f281b7f0ff130990f3