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Autocatalytic Surface Explosion Chemistry of 2D Metal–Organic Frameworks


Wäckerlin, Christian; Ernst, Karl-Heinz (2021). Autocatalytic Surface Explosion Chemistry of 2D Metal–Organic Frameworks. Journal of Physical Chemistry C, 125(24):13343-13349.

Abstract

Metal–organic frameworks are a combination of inorganic constituents and organic ligands with a high degree of variability which are, as coordination compounds in homogeneous catalysis, potentially highly selective heterogeneous catalysts. The synthesis and thermal stability of monolayer thin Cu-, Ni-, and Fe-squarate 2D MOFs are studied using X-ray photoelectron spectroscopy, scanning tunneling microscopy, and temperature-programmed reaction spectroscopy on a Cu(100) surface in ultrahigh vacuum. Highly ordered 2D squarate MOFs are obtained by mild annealing of squarate multilayers. Upon annealing at higher temperatures, the Ni- and Fe-squarate layers undergo autocatalytic surface explosion chemistry with carbon monoxide as a desorbing product in a very narrow temperature interval. Despite the different stabilities of Ni- and Fe-based MOFs, mixed {Ni + Fe}-MOFs also decompose in a narrow single temperature interval. Such autocatalytic behavior is explained by a numerical model which—unlike rate equation-based kinetics—explicitly considers the chemical nature of nearest neighbors.

Abstract

Metal–organic frameworks are a combination of inorganic constituents and organic ligands with a high degree of variability which are, as coordination compounds in homogeneous catalysis, potentially highly selective heterogeneous catalysts. The synthesis and thermal stability of monolayer thin Cu-, Ni-, and Fe-squarate 2D MOFs are studied using X-ray photoelectron spectroscopy, scanning tunneling microscopy, and temperature-programmed reaction spectroscopy on a Cu(100) surface in ultrahigh vacuum. Highly ordered 2D squarate MOFs are obtained by mild annealing of squarate multilayers. Upon annealing at higher temperatures, the Ni- and Fe-squarate layers undergo autocatalytic surface explosion chemistry with carbon monoxide as a desorbing product in a very narrow temperature interval. Despite the different stabilities of Ni- and Fe-based MOFs, mixed {Ni + Fe}-MOFs also decompose in a narrow single temperature interval. Such autocatalytic behavior is explained by a numerical model which—unlike rate equation-based kinetics—explicitly considers the chemical nature of nearest neighbors.

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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
08 Research Priority Programs > Solar Light to Chemical Energy Conversion
Dewey Decimal Classification:540 Chemistry
Scopus Subject Areas:Physical Sciences > Electronic, Optical and Magnetic Materials
Physical Sciences > General Energy
Physical Sciences > Physical and Theoretical Chemistry
Physical Sciences > Surfaces, Coatings and Films
Uncontrolled Keywords:Surfaces, Coatings and Films, Physical and Theoretical Chemistry, General Energy, Electronic, Optical and Magnetic Materials
Language:English
Date:24 June 2021
Deposited On:16 Feb 2022 15:15
Last Modified:26 Feb 2024 02:47
Publisher:American Chemical Society (ACS)
ISSN:1932-7447
OA Status:Closed
Publisher DOI:https://doi.org/10.1021/acs.jpcc.1c03809
Project Information:
  • : FunderSchweizerischer Nationalfonds zur F??rderung der Wissenschaftlichen Forschung
  • : Grant IDR’Equip, Sinergia
  • : Project Title
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