Catalytic acceptorless complete dehydrogenation of cycloalkanes

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

doi:10.1038/s41467-024-55460-y

Catalytic acceptorless complete dehydrogenation of cycloalkanes

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

^*Corresponding author for this work

Program of Chemistry

Research output: Contribution to journal › Article › peer-review

1 Scopus 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.

Original language	English
Article number	428
Journal	Nature Communications
Volume	16
Issue number	1
DOIs	https://doi.org/10.1038/s41467-024-55460-y
State	Published - 2025/12

ASJC Scopus subject areas

General Chemistry
General Biochemistry, Genetics and Molecular Biology
General Physics and Astronomy

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title = "Catalytic acceptorless complete dehydrogenation of cycloalkanes",

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.",

author = "Jagtap, {Rahul A.} and Yuki Nishioka and Geddis, {Stephen M.} and Yu Irie and Tsukasa Takanashi and Rintaro Adachi and Akira Yamakata and Masaaki Fuki and Yasuhiro Kobori and Harunobu Mitsunuma and Motomu Kanai",

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doi = "10.1038/s41467-024-55460-y",

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T1 - Catalytic acceptorless complete dehydrogenation of cycloalkanes

AU - Jagtap, Rahul A.

AU - Nishioka, Yuki

AU - Geddis, Stephen M.

AU - Irie, Yu

AU - Takanashi, Tsukasa

AU - Adachi, Rintaro

AU - Yamakata, Akira

AU - Fuki, Masaaki

AU - Kobori, Yasuhiro

AU - Mitsunuma, Harunobu

AU - Kanai, Motomu

PY - 2025/12

Y1 - 2025/12

N2 - 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.

AB - 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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Catalytic acceptorless complete dehydrogenation of cycloalkanes

Abstract

ASJC Scopus subject areas

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