Catalytic acceptorless complete dehydrogenation of cycloalkanes

The advancement of an effective hydrogen liberation technology from liquid organic hydrogen carriers, particularly cycloalkanes such as cyclohexane and methylcyclohexane, holds significance in realizing a hydrogen-centric society. However, the attainment of homogeneous catalytic acceptorless dehydrogenation characterized by elevated selectivity for thorough aromatization under mild conditions remains unrealized. In this study, a catalyst system, facilitated by a double hydrogen atom transfer processes, has been devised for the catalytic acceptorless dehydrogenation of inert cycloalkanes at ambient temperature under visible light irradiation. Through the synergistic utilization of tetrabutylammonium chloride and thiophosphoric acid hydrogen atom transfer catalysts, successful catalytic acceptorless dehydrogenation with comprehensive aromatization has been accomplished with potential liquid organic hydrogen carrier candidates and showcased high functional group tolerance.

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Publication Details

Journal
Nature Communications
Published
2025-01-09
DOI
https://doi.org/10.1038/s41467-024-55460-y
Citations
16
Primary Topic
Metal-Organic Frameworks: Synthesis and Applications
Type
article
Field-Weighted Citation Impact
8.60

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article

Catalytic acceptorless complete dehydrogenation of cycloalkanes

Stephen M. Geddis, Tsukasa Takanashi, Yuki Nishioka, Yasuhiro Kobori et al.
16 citations
Nature Communications
Metal-Organic Frameworks: Synthesis and Applications
8.60
article

Catalytic acceptorless complete dehydrogenation of cycloalkanes

Stephen M. Geddis, Tsukasa Takanashi, Yuki Nishioka, Yasuhiro Kobori, Akira Yamakata, Masaaki Fuki, Harunobu Mitsunuma, Rahul A. Jagtap, Yu Irie, Motomu Kanai, Rintaro Adachi
article en
16 citations

Abstract

The advancement of an effective hydrogen liberation technology from liquid organic hydrogen carriers, particularly cycloalkanes such as cyclohexane and methylcyclohexane, holds significance in realizing a hydrogen-centric society. However, the attainment of homogeneous catalytic acceptorless dehydrogenation characterized by elevated selectivity for thorough aromatization under mild conditions remains unrealized. In this study, a catalyst system, facilitated by a double hydrogen atom transfer processes, has been devised for the catalytic acceptorless dehydrogenation of inert cycloalkanes at ambient temperature under visible light irradiation. Through the synergistic utilization of tetrabutylammonium chloride and thiophosphoric acid hydrogen atom transfer catalysts, successful catalytic acceptorless dehydrogenation with comprehensive aromatization has been accomplished with potential liquid organic hydrogen carrier candidates and showcased high functional group tolerance.

Nature CommunicationsVol. 16(1)
Okayama University (JP), Japan Science and Technology Agency (JP), Kobe University (JP), The University of Tokyo (JP)
University of Tokyo, ENEOS Hydrogen Trust Fund, Japan Society for the Promotion of Science, Core Research for Evolutional Science and Technology, Precursory Research for Embryonic Science and Technology
Openalex Percentile: Top 2%
Metal-Organic Frameworks: Synthesis and Applications
8.60
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