Steric or attractive interactions among reactants or between reactants and inert crowders can substantially influence the total rate of a diffusion-influenced reaction in the liquid phase. However, the role of the product species, which has typically different physical properties than the reactant species, has been disregarded so far. Here we study the effects of reactant–product and product–product interactions as well as asymmetric diffusion properties on the rate of diffusion-controlled reactions in the classical Smoluchowski-setup for chemical transformations at a perfect catalytic sphere. For this, we solve the diffusion equation with appropriate boundary conditions coupled by a mean-field approach on the second virial level to account for the particle interactions. We find that all particle spatial distributions and the total rate can change significantly, depending on the diffusion and interaction properties of the accumulated products. Complex competing and self-regulating (homeostatic) or self-amplifying effects are observed for the system, leading to both decrease and increase in the rates, as the presence of interacting products feeds back to the reactant flux and thus the rate with which the products are generated.
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14 February 2018
Research Article|
February 12 2018
Product interactions and feedback in diffusion-controlled reactions
Rafael Roa
;
Rafael Roa
a)
1
Física Aplicada I, Facultad de Ciencias, Universidad de Málaga
, 29071 Málaga, Spain
2
Institut für Weiche Materie und Funktionale Materialien, Helmholtz-Zentrum Berlin für Materialien und Energie
, 14109 Berlin, Germany
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Toni Siegl;
Toni Siegl
2
Institut für Weiche Materie und Funktionale Materialien, Helmholtz-Zentrum Berlin für Materialien und Energie
, 14109 Berlin, Germany
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Won Kyu Kim
;
Won Kyu Kim
2
Institut für Weiche Materie und Funktionale Materialien, Helmholtz-Zentrum Berlin für Materialien und Energie
, 14109 Berlin, Germany
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Joachim Dzubiella
Joachim Dzubiella
b)
2
Institut für Weiche Materie und Funktionale Materialien, Helmholtz-Zentrum Berlin für Materialien und Energie
, 14109 Berlin, Germany
3
Institut für Physik, Humboldt-Universität zu Berlin
, 12489 Berlin, Germany
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J. Chem. Phys. 148, 064705 (2018)
Article history
Received:
November 21 2017
Accepted:
January 26 2018
Citation
Rafael Roa, Toni Siegl, Won Kyu Kim, Joachim Dzubiella; Product interactions and feedback in diffusion-controlled reactions. J. Chem. Phys. 14 February 2018; 148 (6): 064705. https://doi.org/10.1063/1.5016608
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