The unstirred, ferroin (Fe(phen)3(2+)) catalyzed Belousov-Zhabotinsky (BZ) reaction is the prototype oscillatory chemical system. Reaction media with added Br(-) appear red (reduced, low [Fe(phen)3(3+)]) during an induction period of several minutes, followed by the "spontaneous" formation of "pacemaker" sites, which oscillate between a blue, oxidized state (high [Fe(phen)3(3+)]) and the red, reduced state and generate target patterns of concentric, outwardly moving waves of oxidation (blue). Auto-oscillatory behavior is also seen in the Oregonator model of Field, Koros and Noyes (FKN), a robust, reduced model that captures qualitative BZ kinetics in the auto-oscillatory regime. However, the Oregonator model predicts a blue (oxidized) induction phase. Here we develop a generalized Oregonator-like model with no explicit bifurcation parameter that yields the observed transition from a red initial state to oscillatory dynamics, and displays a new bifurcation mechanism not seen in the original Oregonator.
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http://dx.doi.org/10.1021/jp8019073 | DOI Listing |
J Phys Chem B
December 2024
Department of Earth and Planetary Sciences and Origins of Life Initiative, Harvard University, 20 Oxford Street, Cambridge, Massachusetts 02138, United States.
We report the interactions and dynamics of chemically powered soft swimmers that undergo autonomous oscillatory motion. The interaction of autonomous entities is the basis for the development of collective behaviors among biological organisms. Collective behaviors enable organisms to efficiently attain food and coordinate against threats.
View Article and Find Full Text PDFGels
November 2024
Center for Nonlinear Chemistry, Immanuel Kant Baltic Federal University, 14 A. Nevskogo Street, Kaliningrad 236016, Russia.
For the first time, we introduced chemomechanical self-oscillating poly(N-isopropylacrylamide)-based gels containing catalytically active Fe or Ru complexes both as crosslinkers and as pendant groups. All the obtained gels exhibited sustained autonomous oscillations driven by the Belousov-Zhabotinsky reaction within their structure. The Ru complex-based gels also demonstrated pronounced chemomechanical oscillations; they periodically swelled/shrunk when the catalyst was reduced/oxidized.
View Article and Find Full Text PDFACS Macro Lett
November 2024
Department of Materials Engineering, School of Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan.
Developing artificial autonomous materials is crucial for a deeper understanding of the emergence of life-like behavior. In nature, cells achieve autonomy through chemical processing systems incorporated into soft material-based frameworks. Inspired by natural cells, we herein describe a straightforward methodology for constructing artificial autonomous materials consisting of a polymer-based chemical processing system and a hydrogel-based soft framework.
View Article and Find Full Text PDFSci Rep
October 2024
Department of Mathematics, Firat University, 23119, Elazig, Turkey.
In this work, we employed an attractive hybrid integral transform technique known as the natural transform decomposition method (NTDM) to investigate analytical solutions for the Noyes-Field (NF) model of the time-fractional Belousov-Zhabotinsky (TF-BZ) reaction system. The aforementioned time-fractional model is considered within the framework of the Caputo, Caputo-Fabrizio, and Atangana-Baleanu fractional derivatives. The NTDM couples the Adomian decomposition method and the natural transform method to generate rapidly convergent series-type solutions via an elegant iterative approach.
View Article and Find Full Text PDFChaos
September 2024
Polymer Engineering Research Laboratory (PERL), Department of Chemical Engineering, Indian Institute of Technology Gandhinagar, Gujarat 382055, India.
Controlling the dynamics of active stimuli-responsive smart materials is essential to replicate the biomimetic functionalities at different length scales for a variety of biological systems-based applications. Photosensitive Belousov-Zhabotinsky (BZ) gels, powered by a nonlinear chemical oscillator, called a BZ reaction are one of the stimuli-responsive smart materials in demand due to their ability to continuously transduce chemical oscillations into mechanical deformations. The chemical oscillations in a BZ reaction and subsequent mechanical oscillations in photosensitive BZ gels occur due to the redox cycle of photosensitive ruthenium complex-based catalysts.
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