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  The effect of temperature on the dynamics of a homogeneous oscillatory system operated in batch and under flow

Nogueira, P. A., Batista, B. C., Faria, R. B., & Varela, H. (2014). The effect of temperature on the dynamics of a homogeneous oscillatory system operated in batch and under flow. RSC Advances, 4(57), 30412-30421. doi:10.1039/c4ra03539a.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-001A-2714-A Version Permalink: http://hdl.handle.net/21.11116/0000-0005-3FF6-0
Genre: Journal Article

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Nogueira, Paulo A.1, Author
Batista, Bruno C.1, Author
Faria, Roberto B.2, Author
Varela, Hamilton1, 3, Author              
Affiliations:
1Institute of Chemistry of São Carlos, University of São Paulo, PO Box 780, São Carlos, Brazil , ou_persistent22              
2Instituto de Química, Universidade Federal do Rio de Janeiro, Av. Athos da Silveira Ramos 149, CT, Bloco A, Rio de Janeiro, Brazil , ou_persistent22              
3Physical Chemistry, Fritz Haber Institute, Max Planck Society, ou_634546              

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 Abstract: The effect of temperature on a network of chemical reactions is not obvious, especially when compared to the effect exerted on elementary steps. There are few reports regarding the estimation of parameters such as activation energies for oscillating chemical systems. Still less investigated is the importance of the relative distance from thermodynamic equilibrium on the way in which temperature influences the oscillators' dynamics – a crucial aspect for the understanding of chemical and bio-chemical oscillating networks. In this paper we use the bromate–oxalic acid–acetone–cerium oscillatory system to study the influence of temperature under close and far-from-equilibrium regimes. The research was carried out under identical conditions for batch and flow (in a continuous flow stirred tank reactor, CSTR) regimes, and the main oscillation features were preserved, so that it was possible to isolate the effect of flow. Overall, increasing the flow results in an increase of the oscillatory frequency. The apparent oscillatory activation energy was found to decrease from 72 ± 6 kJ mol−1, for the system operated in batch, to 50 ± 2 kJ mol−1, under the flow regime. The role of the distance from the thermodynamic equilibrium on the temperature dependence is generalized and discussed in connection with other systems. Numerical simulations using the Brusselator model under batch and flow regimes further helped the discussion of the main experimental results.

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Language(s): eng - English
 Dates: 2014-04-182014-06-172014-06-18
 Publication Status: Published online
 Pages: 10
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 Rev. Type: Peer
 Identifiers: DOI: 10.1039/c4ra03539a
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Title: RSC Advances
  Abbreviation : RSC Adv.
Source Genre: Journal
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Publ. Info: Cambridge, UK : Royal Society of Chemistry
Pages: - Volume / Issue: 4 (57) Sequence Number: - Start / End Page: 30412 - 30421 Identifier: ISSN: 2046-2069
CoNE: https://pure.mpg.de/cone/journals/resource/2046-2069