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

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.

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Publication Details

Journal
Science Advances
Published
2024-11-08
DOI
https://doi.org/10.1126/sciadv.adp9804
Citations
5
Primary Topic
Graphene research and applications
Type
article
Field-Weighted Citation Impact
0.59
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Pressure enabled organic reactions via confinement between layers of 2D materials

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

Yeonju Lee, Joo Song Lee, Yoon-jeong Kim, Sunmin Ryu, Seong In Yoon, Seungwoo Son, Hyo Ju Park, Changding Guo, Daeho Han, Seung Kyu Min, Armando Genco, Hyeon Suk Shin, Kyung Yeol, Myeonggi Choe, Seokhoon Ahn, Manish Chhowalla, Jaewoo Shim, Jongyeong Lee, Seonghyun Koo, Yunrui Duan, Sung Wook Moon, Bong Kyun Kang, Amirreza Ghassami, Zonghoon Lee, Sun-Young Park, A. I. Tartakovskii, Ju‐Young Kim, Yu‐Jin Kim, Feng Ding, Young S. Park, Woo Seok Yang, Kyoung-Cheol Kwon
article en
5 citations

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.

Science AdvancesVol. 10(45)
Pohang University of Science and Technology (KR), Korea Atomic Energy Research Institute (KR), Lund University (SE), Samsung (South Korea) (KR), University of Cambridge (GB), Soonchunhyang University (KR), Institute for Basic Science (KR), Korea Electronics Technology Institute (KR), MAX IV Laboratory (SE), Hanyang University (KR), Ulsan National Institute of Science and Technology (KR), Korea Institute of Science and Technology (KR), University at Buffalo, State University of New York (US), Sungkyunkwan University (KR), University of Sheffield (GB)
Openalex Percentile: Top 33%
Graphene research and applications
0.59
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