Selective oxidation of alcohols by graphene-like carbon with electrophilic oxygen and integrated pyridinic nitrogen active sites

Author Identifier

Hongqi Sun

ORCID : https://orcid.org/0000-0003-0907-5626

Document Type

Journal Article

Publication Title

Nanoscale

Volume

13

Issue

30

First Page

12979

Last Page

12990

Publisher

Royal Society of Chemistry

School

School of Engineering

RAS ID

39643

Comments

Li, J., Sun, H., Wang, S., Dong, Y., & Liu, S. (2021). Selective oxidation of alcohols by graphene-like carbon with electrophilic oxygen and integrated pyridinic nitrogen active sites. Nanoscale, 13(30), 12979-12990. https://doi.org/10.1039/d1nr03157k

Abstract

The selective oxidations of alcohols into corresponding aldehydes or ketones are essential reactions for organic synthesis. The development of facile, green and cost-effective protocols to accomplish selective oxidation is highly attractive. Here, we present the selective oxidation of alcohols using peroxymonosulfate (PMS) oxidants with N-doped graphene-like carbon (NG) synthesized via a metal-free approach without producing a large amount of hazardous wastes. In the tested selective oxidation reaction, over 96% of benzyl alcohol (BzOH) was converted into benzaldehyde (BzH) with high selectivity under mild conditions. The synthesized NG catalyst contains abundant electrophilic oxygen species, serving as the major active sites for the generation of reactive radicals from PMS to enable the selective oxidation of BzOH in the radical pathway. Besides, non-radical oxidation of BzOH occurs via the electron transfer through the surface coordinated complex, dominantly upon the N species. Particularly, the configuration of integrated pyridinic N is possible to create active domains for BzOH oxidation with activated PMS. This work opens a new avenue to convert metal-free raw materials into effectively functionalized carbon materials, coupled with their potential applications in the selective oxidation of alcohols.

DOI

10.1039/d1nr03157k

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