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• W2012590987 abstract "Abstract A microscopic model has been developed to describe electron (or hole) diffusion coefficients, D E , in a rigid three-dimensional network as a function of redox species concentration, c . The model takes excluded volume into consideration and is based on simple probability distribution arguments and a random walk. The following conditions are assumed: (1) there is a homogeneous random distribution of hard-sphere redox centers; (2) each step corresponds to an electron transfer across the average nearest neighbor distance between redox centers; and (3) the electron transfer rate constant depends exponentially on edge-to-edge separation between a reacting pair. As the molecular diameter approaches zero, the hard-sphere case approaches the point-molecule case. In general, the point-molecule case affords a simpler relationship between D E and c , but is inadequate for networks with experimentally realistic concentrations. In dilute systems, D E rises sharply with concentration; however, at larger concentrations, the hard sphere D E reaches a limiting value due to packing. Applying the model to rate-distance data in the literature for metalloprotein and steroid-spacer systems yielded semi-empirical D E values as a function of concentration. Hard-sphere D E values for metalloprotein kinetics and a redox molecular diameter of 1.3 nm (corresponding to Ru(bpy) 3 2+ ) are 1.9 × 10 −10 and 5.0 × 10 −9 cm 2 s −1 at 0.10 M and 1.07 M , respectively. At a ferrocene-like diameter (0.6 nm), D E values are 2.8 × 10 −12 and 4.6 × 10 −10 cm 2 s −1 , respectively. The corresponding D E values for the steroid-spacer kinetics are 1.1 × 10 −3 , 3.0 × 10 −2 , 1.7 × 10 −5 , and 2.7 × 10 −3 cm 2 s −1 , respectively. Also derived is a two-dimensional version of the model that may be applied to systems such as Langmuir monolayers. Plots of the two-dimensional hard-sphere electron diffusion coefficient vs. area concentration yield curve shapes and magnitudes that are similar to those of the three-dimensional model." @default.
• W2012590987 created "2016-06-24" @default.
• W2012590987 creator A5027074516 @default.
• W2012590987 creator A5063639826 @default.
• W2012590987 date "1989-05-01" @default.
• W2012590987 modified "2023-10-18" @default.
• W2012590987 title "A microscopic model for diffusion of electrons by successive hopping among redox centers in networks" @default.
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• W2012590987 doi "https://doi.org/10.1016/0022-0728(89)85097-1" @default.
• W2012590987 hasPublicationYear "1989" @default.
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