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

Hu, Haitao; Nie, Yunqing; Tao, Yuewen; Huang, Wenyu; Qi, Long; Nie, Renfeng

doi:10.1126/sciadv.abl9478

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

Journal Article · 28 January 2022 · Science Advances

DOI: https://doi.org/10.1126/sciadv.abl9478 · OSTI ID:1846435

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Zhengzhou University (China); Hubei University, Wuhan (China)
Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States)
Ames Lab., Ames, IA (United States)

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 H₂ 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.

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Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 1846435

Report Number(s):: IS-J-10,707

Journal Information:: Science Advances, Journal Name: Science Advances Journal Issue: 4 Vol. 8; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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