Evidence for a chemical clock in oscillatory formation of UiO-66
M.G. Goesten (TU Delft - ChemE/Catalysis Engineering, Eindhoven University of Technology)
MF de Lange (TU Delft - ChemE/Catalysis Engineering)
A.I. Olivos Suarez (TU Delft - ChemE/Catalysis Engineering)
A.V. Bavykina (TU Delft - ChemE/Catalysis Engineering)
P. Serra Crespo (TU Delft - RST/Applied Radiation & Isotopes)
C. Krywka (Helmholtz-Zentrum Geesthacht - Zentrum für Material- und Küstenforschung GmbH, Brookhaven National Laboratory)
F. M. Bickelhaupt (Radboud Universiteit Nijmegen, Vrije Universiteit Amsterdam)
F. Kapteijn (TU Delft - ChemE/Catalysis Engineering)
Jorge Gascon Sabate (TU Delft - ChemE/Catalysis Engineering)
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Abstract
Chemical clocks are often used as exciting classroom experiments, where an induction time is followed by rapidly changing colours that expose oscillating concentration patterns. This type of reaction belongs to a class of nonlinear chemical kinetics also linked to chaos, wave propagation and Turing patterns. Despite its vastness in occurrence and applicability, the clock reaction is only well understood for liquid-state processes. Here we report a chemical clock reaction, in which a solidifying entity, metal-organic framework UiO-66, displays oscillations in crystal dimension and number, as shown by X-ray scattering. In rationalizing this result, we introduce a computational approach, the metal-organic molecular orbital methodology, to pinpoint interaction between the tectonic building blocks that construct the metal-organic framework material. In this way, we show that hydrochloric acid plays the role of autocatalyst, bridging separate processes of condensation and crystallization.
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