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Theoretical Understanding of the Penetration of O 2 in Enzymatic Redox Polymer Films: The Case of Unidirectional Catalysis and Irreversible Inactivation in a Film of Arbitrary Thickness
Author(s) -
Fourmond Vincent,
Léger Christophe
Publication year - 2021
Publication title -
chemelectrochem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.182
H-Index - 59
ISSN - 2196-0216
DOI - 10.1002/celc.202100586
Subject(s) - catalysis , redox , penetration (warfare) , polymer , electron , electrode , thin film , chemistry , electron transport chain , thermal conduction , materials science , chemical engineering , nanotechnology , organic chemistry , physics , composite material , biochemistry , quantum mechanics , operations research , engineering
Abstract Redox catalysts, including hydrogenases, can be embedded into films made of redox polymers, whose side chains mediate electrons between the catalyst and an electrode. These films 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 film to catalytically produce electrons that reduce the O 2 molecules that penetrate the film. 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 film of arbitrary thickness. We analytically solve the reaction/diffusion 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 relations between film thickness, electron conduction, catalyst use and life time. This provides the theoretical framework required to optimize the design of these systems.