Theoretical understanding of the penetration of O2 in enzymatic redox polymer films: case of unidirectional catalysis and irreversible inactivation in a film of arbitrary thickness - Archive ouverte HAL Access content directly
Journal Articles ChemElectroChem Year : 2021

Theoretical understanding of the penetration of O2 in enzymatic redox polymer films: case of unidirectional catalysis and irreversible inactivation in a film of arbitrary thickness

Abstract

Redox catalysts, including hydrogenases, can be embedded into lms made of redox polymers, whose side chains mediate electrons between the catalyst and an electrode. These lms can be used as bioanodes in H 2-based biofuel cells, because they protect the catalyst from O 2-induced inactivation: self-protection occurs because a fraction of the incoming H 2 is used in the outer region of the lm to catalytically produce electrons that reduce the O 2 molecules that penetrate the lm. Here, we focus on the case of unidirectional catalysis (e.g. H 2 oxidation) by an enzyme that is irreversibly inactivated by O 2 , embedded in a lm of arbitrary thickness. We analytically solve the reaction/di usion system to fully describe the time evolution of the penetration of O 2 and we discuss the amount of H 2 consumed by the protection mechanism. We establish the relation between lm thickness, electron conduction, catalyst use and life time. This provides the theoretical framework required to optimize the design of these systems.
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Dates and versions

hal-03277147 , version 1 (02-07-2021)

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Vincent Fourmond, Christophe Léger. Theoretical understanding of the penetration of O2 in enzymatic redox polymer films: case of unidirectional catalysis and irreversible inactivation in a film of arbitrary thickness. ChemElectroChem, In press, ⟨10.1002/celc.202100586⟩. ⟨hal-03277147⟩

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