Traditional mean-field rate equations of chemical kinetics for spatially uniform systems1−3 and the corresponding reaction−diffusion equations describing spatial heterogeneity4−6 have proved immensely useful in elucidating catalytic processes. However, it is well-recognized that standard mean-field rate expressions neglect spatial correlations in the reactant and/or product distribution. It is less well appreciated that the standard treatment of diffusion is generally applicable only at low concentrations and in unrestricted environments.
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