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 acceptorles...

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Main Authors: Rahul A. Jagtap, Yuki Nishioka, Stephen M. Geddis, Yu Irie, Tsukasa Takanashi, Rintaro Adachi, Akira Yamakata, Masaaki Fuki, Yasuhiro Kobori, Harunobu Mitsunuma, Motomu Kanai
Format: Article
Language:English
Published: Nature Portfolio 2025-01-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-024-55460-y
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author Rahul A. Jagtap
Yuki Nishioka
Stephen M. Geddis
Yu Irie
Tsukasa Takanashi
Rintaro Adachi
Akira Yamakata
Masaaki Fuki
Yasuhiro Kobori
Harunobu Mitsunuma
Motomu Kanai
author_facet Rahul A. Jagtap
Yuki Nishioka
Stephen M. Geddis
Yu Irie
Tsukasa Takanashi
Rintaro Adachi
Akira Yamakata
Masaaki Fuki
Yasuhiro Kobori
Harunobu Mitsunuma
Motomu Kanai
author_sort Rahul A. Jagtap
collection DOAJ
description 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.
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institution Kabale University
issn 2041-1723
language English
publishDate 2025-01-01
publisher Nature Portfolio
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series Nature Communications
spelling doaj-art-811d5f41ad5d43d1a3246829bf853c6c2025-01-12T12:31:43ZengNature PortfolioNature Communications2041-17232025-01-011611710.1038/s41467-024-55460-yCatalytic acceptorless complete dehydrogenation of cycloalkanesRahul A. Jagtap0Yuki Nishioka1Stephen M. Geddis2Yu Irie3Tsukasa Takanashi4Rintaro Adachi5Akira Yamakata6Masaaki Fuki7Yasuhiro Kobori8Harunobu Mitsunuma9Motomu Kanai10Graduate School of Pharmaceutical Sciences, The University of Tokyo, 7-3-1 Hongo, Bunkyo-kuGraduate School of Pharmaceutical Sciences, The University of Tokyo, 7-3-1 Hongo, Bunkyo-kuGraduate School of Pharmaceutical Sciences, The University of Tokyo, 7-3-1 Hongo, Bunkyo-kuGraduate School of Pharmaceutical Sciences, The University of Tokyo, 7-3-1 Hongo, Bunkyo-kuGraduate School of Natural Science & Technology, Okayama UniversityGraduate School of Natural Science & Technology, Okayama UniversityGraduate School of Natural Science & Technology, Okayama UniversityMolecular Photoscience Research Center, Kobe UniversityMolecular Photoscience Research Center, Kobe UniversityGraduate School of Pharmaceutical Sciences, The University of Tokyo, 7-3-1 Hongo, Bunkyo-kuGraduate School of Pharmaceutical Sciences, The University of Tokyo, 7-3-1 Hongo, Bunkyo-kuAbstract 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.https://doi.org/10.1038/s41467-024-55460-y
spellingShingle Rahul A. Jagtap
Yuki Nishioka
Stephen M. Geddis
Yu Irie
Tsukasa Takanashi
Rintaro Adachi
Akira Yamakata
Masaaki Fuki
Yasuhiro Kobori
Harunobu Mitsunuma
Motomu Kanai
Catalytic acceptorless complete dehydrogenation of cycloalkanes
Nature Communications
title Catalytic acceptorless complete dehydrogenation of cycloalkanes
title_full Catalytic acceptorless complete dehydrogenation of cycloalkanes
title_fullStr Catalytic acceptorless complete dehydrogenation of cycloalkanes
title_full_unstemmed Catalytic acceptorless complete dehydrogenation of cycloalkanes
title_short Catalytic acceptorless complete dehydrogenation of cycloalkanes
title_sort catalytic acceptorless complete dehydrogenation of cycloalkanes
url https://doi.org/10.1038/s41467-024-55460-y
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