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Electric field-mediated regulation of enzyme orientation for efficient electron transfer at the bioelectrode surface: A molecular dynamics study

Authors
Yoon, TaeyoungPark, WooboumKim, YoonjungNa, Sungsoo
Issue Date
15-1월-2023
Publisher
ELSEVIER
Keywords
Enzymatic bioelectrode; Direct electron transfer; Laccase; Graphene; Electric field; Molecular dynamic
Citation
APPLIED SURFACE SCIENCE, v.608
Indexed
SCOPUS
Journal Title
APPLIED SURFACE SCIENCE
Volume
608
URI
https://scholar.korea.ac.kr/handle/2021.sw.korea/146452
DOI
10.1016/j.apsusc.2022.155124
ISSN
0169-4332
Abstract
Surface immobilization with favorable orientation of biocatalysts is critical for developing bioelectrochemical devices. To improve the performance of electrochemical electrodes, biocatalyst surface modification and engineering has been attempted via expensive and complex fabrication processes. For proper orientation and deposition of biomolecules on the surface, application of external electric field (EF) to small molecules has been suggested. Here, to the best of our knowledge, a unidirectional external EF was applied for the first time to oxygen-reducing enzymes with high catalytic activity and a Laccase-graphene interface was constructed using computational methods. The external EF rotated the active site of laccase, resulting improvement in the electron transfer rate compared to enzymes physically immobilized on graphene. The external EF fabrication process was also evaluated for graphene congeners (graphene oxide (GO) and reduced GO (rGO)). The morphology of the electrode surface was visualized, and computational methods were applied to verify binding conformation, orientations of dipole moment, secondary structure, and binding stability. Graphene was the most promising material compared to GO and rGO by 10 and 5 % for DET rate, respectively. Results suggest that using an external EF to favorably orientate the Laccase-graphene interface may be a simple, economical, and efficient approach for bioelectrode fabrication.
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공과대학 (기계공학부)
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