Effects of the Size, the Number, and the Spatial Arrangement of Reactive Patches on a Sphere on Diffusion-Limited Reaction Kinetics: A Comprehensive Study

• Main Author: Changsun Eun
• Format: Article
• Language: English
• Published: MDPI AG 2020-02-01
• Series: International Journal of Molecular Sciences
• Subjects: diffusion-limited reaction; rate constant; diffusion-controlled reaction; curvature; kinetics; finite element method; berg-purcell model; competition
• Online Access: https://www.mdpi.com/1422-0067/21/3/997

We investigate how the size, the number, and the spatial arrangement of identical nonoverlapping reactive patches on a sphere influence the overall reaction kinetics of bimolecular diffusion-limited (or diffusion-controlled) reactions that occur between the patches and the reactants diffusing around the sphere. First, in the arrangement of two patches, it is known that the overall rate constant increases as the two patches become more separated from each other but decreases when they become closer to each other. In this work, we further study the dependence of the patch arrangement on the kinetics with three and four patches using the finite element method (FEM). In addition to the patch arrangement, the kinetics is also dependent on the number and size of the patches. Therefore, we study such dependences by calculating the overall rate constants using the FEM for various cases, especially for large-sized patches, and this study is complementary to the kinetic studies that were performed by Brownian dynamics (BD) simulation methods for small-sized patches. The numerical FEM and BD simulation results are compared with the results from various kinetic theories to evaluate the accuracies of the theories. Remarkably, this comparison indicates that our theory, which was recently developed based on the curvature-dependent kinetic theory, shows good agreement with the FEM and BD numerical results. From this validation, we use our theory to further study the variation of the overall rate constant when the patches are arbitrarily arranged on a sphere. Our theory also confirms that to maximize the overall rate constant, we need to break large-sized patches into smaller-sized patches and arrange them to be maximally separated to reduce their competition.