Natural and technological instances of enzyme catalysis often feature multistep reaction cascades. The throughput and yield of such nanoscale catalytic architectures is limited by the ability to retain reaction intermediates and direct them toward downstream reaction steps. Nature has settled on several approaches to intermediate channelling, including electrostatic attraction, confinement, and surface affinity. This presentation will discuss the limits of such approaches through modeling, from the molecular dynamics to continuum scales. Geometric factors are considered at the continuum scale, where electrostatic interactions are shown to be much more effective than proximity alone. Short range molecular interactions are also significant, however, and molecular dynamics studies will demonstrate structures that we have found to yield high catalytic efficiency. Molecular-scale results can be combined in a Kinetic Monte Carlo model that can be compared directly to experiment.

Quantitative assessment of channeling mechanisms in nanoscale catalytic architectures

256th National Meeting (2018)

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