Our disquisition examines the role of connectivity in site ensembles and in reaction networks in kinetic descriptions of reactions catalyzed by surfaces.<br/><br/>The first part of this presentation will describe why canonical descriptions of unidirectional rates (e.g., forward and reverse rates), prescribed for elementary step and for single-path reaction networks, are inapplicable to interconnected reaction networks. We show that nodes in interconnected reaction networks alter functional forms of both the forward and reverse rates but do so without changing the functional form of the effective reversibility and we outline a strategy for writing kinetic expressions for unidirectional rates in interconnected reaction networks.<br/><br/>The second part of this presentation will describe the utility of an analytical formalism that describes propensity of disparate elementary step rates and catalytic-site-size requirements to engender clustering of slowly consumed ensembles and partitioning of rapidly consumed ensembles. This description of coverages and chemical dynamics of multi-site ensembles proffers kinetic detail inaccessible in the mean-field Langmuir Hinshelwood kinetic formalism.

Catalytic site ensembles and catalytic reaction networks: Hic sunt leones

ACS Spring 2022

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