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Acceptorless dehydrogenation of 4-methylpiperidine by supported pincer-ligated iridium catalysts in continuous flow

Chakrabarti, Kaushik LU ; Spangenberg, Alice LU ; Subramaniyan, Vasudevan LU ; Hederstedt, Andreas ; Abdelaziz, Omar Y. LU ; Polukeev, Alexey V. LU ; Wallenberg, Reine LU ; Hulteberg, Christian P. LU orcid and Wendt, Ola F. LU (2023) In Catalysis Science and Technology 13(17). p.5113-5119
Abstract

Finding alternative and sustainable ways to produce, store and convert energy is key for reducing fossil fuel-based CO2 emissions. In this transformation, hydrogen for energy storage and hydrogen-powered fuel cells for energy conversion can play important roles. However, storage of hydrogen itself is difficult and the concept of reversible liquid organic hydrogen carriers (LOHCs) has been proposed given the advantages of using liquid storage materials. A key part in the adaption of LOHCs is the catalyst design for efficient dehydrogenation of these hydrogen-carrying species. In this study, the use of silica- and alumina-supported POCOP-Ir systems for gas phase acceptorless dehydrogenation of 4-methylpiperidine (an LOHC with... (More)

Finding alternative and sustainable ways to produce, store and convert energy is key for reducing fossil fuel-based CO2 emissions. In this transformation, hydrogen for energy storage and hydrogen-powered fuel cells for energy conversion can play important roles. However, storage of hydrogen itself is difficult and the concept of reversible liquid organic hydrogen carriers (LOHCs) has been proposed given the advantages of using liquid storage materials. A key part in the adaption of LOHCs is the catalyst design for efficient dehydrogenation of these hydrogen-carrying species. In this study, the use of silica- and alumina-supported POCOP-Ir systems for gas phase acceptorless dehydrogenation of 4-methylpiperidine (an LOHC with 6.1 wt% hydrogen) is investigated in a continuous-flow system with a high TON. To increase stability and reactivity, a new POCOP-Ir complex with two anchors was designed and found to be highly active in the dehydrogenation of 4-methylpiperidine with ∼91 000 turnovers in 45 h. In addition, this catalyst showed a maintained activity with a TOF of 1684 h−1 after 45 h.

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author
; ; ; ; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Catalysis Science and Technology
volume
13
issue
17
pages
7 pages
publisher
Royal Society of Chemistry
external identifiers
  • scopus:85168824053
ISSN
2044-4753
DOI
10.1039/d3cy00881a
language
English
LU publication?
yes
id
17c83594-b290-4b70-a4c8-0cbd4aa8906a
date added to LUP
2023-09-12 08:29:01
date last changed
2023-12-21 17:45:32
@article{17c83594-b290-4b70-a4c8-0cbd4aa8906a,
  abstract     = {{<p>Finding alternative and sustainable ways to produce, store and convert energy is key for reducing fossil fuel-based CO<sub>2</sub> emissions. In this transformation, hydrogen for energy storage and hydrogen-powered fuel cells for energy conversion can play important roles. However, storage of hydrogen itself is difficult and the concept of reversible liquid organic hydrogen carriers (LOHCs) has been proposed given the advantages of using liquid storage materials. A key part in the adaption of LOHCs is the catalyst design for efficient dehydrogenation of these hydrogen-carrying species. In this study, the use of silica- and alumina-supported POCOP-Ir systems for gas phase acceptorless dehydrogenation of 4-methylpiperidine (an LOHC with 6.1 wt% hydrogen) is investigated in a continuous-flow system with a high TON. To increase stability and reactivity, a new POCOP-Ir complex with two anchors was designed and found to be highly active in the dehydrogenation of 4-methylpiperidine with ∼91 000 turnovers in 45 h. In addition, this catalyst showed a maintained activity with a TOF of 1684 h<sup>−1</sup> after 45 h.</p>}},
  author       = {{Chakrabarti, Kaushik and Spangenberg, Alice and Subramaniyan, Vasudevan and Hederstedt, Andreas and Abdelaziz, Omar Y. and Polukeev, Alexey V. and Wallenberg, Reine and Hulteberg, Christian P. and Wendt, Ola F.}},
  issn         = {{2044-4753}},
  language     = {{eng}},
  number       = {{17}},
  pages        = {{5113--5119}},
  publisher    = {{Royal Society of Chemistry}},
  series       = {{Catalysis Science and Technology}},
  title        = {{Acceptorless dehydrogenation of 4-methylpiperidine by supported pincer-ligated iridium catalysts in continuous flow}},
  url          = {{http://dx.doi.org/10.1039/d3cy00881a}},
  doi          = {{10.1039/d3cy00881a}},
  volume       = {{13}},
  year         = {{2023}},
}