Metal-free carbocatalyst for room temperature acceptorless dehydrogenation of N-heterocycles

Author:

Hu Haitao12ORCID,Nie Yunqing12,Tao Yuewen12ORCID,Huang Wenyu34ORCID,Qi Long3ORCID,Nie Renfeng12ORCID

Affiliation:

1. School of Chemical Engineering, Zhengzhou University, Zhengzhou 450001, China.

2. School of Chemistry and Chemical Engineering, Hubei University, Wuhan 430062, China.

3. U.S. DOE Ames Laboratory, Ames, IA 50011, USA.

4. Department of Chemistry, Iowa State University, Ames, IA 50011, USA.

Abstract

Catalytic dehydrogenation enables reversible hydrogen storage in liquid organics as a critical technology to achieve carbon neutrality. However, oxidant or base-free catalytic dehydrogenation at mild temperatures remains a challenge. Here, we demonstrate a metal-free carbocatalyst, nitrogen-assembly carbons (NCs), for acceptorless dehydrogenation of N-heterocycles even at ambient temperature, showing greater activity than transition metal–based catalysts. Mechanistic studies indicate that the observed catalytic activity of NCs is because of the unique closely placed graphitic nitrogens (CGNs), formed by the assembly of precursors during the carbonization process. The CGN site catalyzes the activation of C─H bonds in N-heterocycles to form labile C─H bonds on catalyst surface. The subsequent facile recombination of this surface hydrogen to desorb H 2 allows the NCs to work without any H-acceptor. With reverse transfer hydrogenation of various N-heterocycles demonstrated in this work, these NC catalysts, without precious metals, exhibit great potential for completing the cycle of hydrogen storage.

Publisher

American Association for the Advancement of Science (AAAS)

Subject

Multidisciplinary

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