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Pressure enabled organic reactions via confinement between layers of 2D materials

In Yoon, Seong ; Lee, Joo Song ; Shin, Hyeon Suk and Ghassami, Amirreza LU orcid (2024) In Science Advances 10(45).
Abstract
Confinement of reactants within nanoscale spaces of low-dimensional materials has been shown to provide reorientation of strained reactants or stabilization of unstable reactants for synthesis of molecules and tuning of chemical reactivity. While few studies have reported chemistry within zero-dimensional pores and one-dimensional nanotubes, organic reactions in confined spaces between two-dimensional materials have yet to be explored. Here, we demonstrate that reactants confined between atomically thin sheets of graphene or hexagonal boron nitride experience pressures as high as 7 gigapascal, which allows the propagation of solvent-free organic reactions that ordinarily do not occur under standard conditions. Specifically, we show that... (More)
Confinement of reactants within nanoscale spaces of low-dimensional materials has been shown to provide reorientation of strained reactants or stabilization of unstable reactants for synthesis of molecules and tuning of chemical reactivity. While few studies have reported chemistry within zero-dimensional pores and one-dimensional nanotubes, organic reactions in confined spaces between two-dimensional materials have yet to be explored. Here, we demonstrate that reactants confined between atomically thin sheets of graphene or hexagonal boron nitride experience pressures as high as 7 gigapascal, which allows the propagation of solvent-free organic reactions that ordinarily do not occur under standard conditions. Specifically, we show that cyclodehydrogenation of hexaphenylbenzene without catalysts as a proof of concept and oxidative polymerization of dopamine into sheet-like crystalline structure are enabled by the effective high pressure experienced by the reactants between the graphene layers. Our results demonstrate a facile, general approach for performing high-pressure chemistry based on confinement of reactants within two-dimensional materials. (Less)
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author
; ; and
author collaboration
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Science Advances
volume
10
issue
45
article number
eadp9804
pages
9 pages
publisher
American Association for the Advancement of Science (AAAS)
external identifiers
  • scopus:85209377603
  • pmid:39514661
ISSN
2375-2548
DOI
10.1126/sciadv.adp9804
language
English
LU publication?
yes
id
09e7f891-95be-46ac-b988-d44e22a61f99
date added to LUP
2024-11-27 19:10:04
date last changed
2025-04-04 15:05:17
@article{09e7f891-95be-46ac-b988-d44e22a61f99,
  abstract     = {{Confinement of reactants within nanoscale spaces of low-dimensional materials has been shown to provide reorientation of strained reactants or stabilization of unstable reactants for synthesis of molecules and tuning of chemical reactivity. While few studies have reported chemistry within zero-dimensional pores and one-dimensional nanotubes, organic reactions in confined spaces between two-dimensional materials have yet to be explored. Here, we demonstrate that reactants confined between atomically thin sheets of graphene or hexagonal boron nitride experience pressures as high as 7 gigapascal, which allows the propagation of solvent-free organic reactions that ordinarily do not occur under standard conditions. Specifically, we show that cyclodehydrogenation of hexaphenylbenzene without catalysts as a proof of concept and oxidative polymerization of dopamine into sheet-like crystalline structure are enabled by the effective high pressure experienced by the reactants between the graphene layers. Our results demonstrate a facile, general approach for performing high-pressure chemistry based on confinement of reactants within two-dimensional materials.}},
  author       = {{In Yoon, Seong and Lee, Joo Song and Shin, Hyeon Suk and Ghassami, Amirreza}},
  issn         = {{2375-2548}},
  language     = {{eng}},
  month        = {{11}},
  number       = {{45}},
  publisher    = {{American Association for the Advancement of Science (AAAS)}},
  series       = {{Science Advances}},
  title        = {{Pressure enabled organic reactions via confinement between layers of 2D materials}},
  url          = {{http://dx.doi.org/10.1126/sciadv.adp9804}},
  doi          = {{10.1126/sciadv.adp9804}},
  volume       = {{10}},
  year         = {{2024}},
}