Role of quinones in electron transfer of PQQ–glucose dehydrogenase anodes—mediation or orientation effect
Abstract
In this study, the influence of two quinones (1,2- and 1,4-benzoquinone) on the operation and mechanism of electron transfer in PQQ-sGDH anodes has been determined. Benzoquinones were experimentally explored as mediators present in the electrolyte. The electrochemical performance of the PQQ–sGDH anodes with and without the mediators was examined and for the first time molecular docking simulations were used to gain a fundamental understanding to explain the role of the mediator molecules in the design and operation of the enzymatic electrodes. It was proposed that the higher performance of the PQQ–sGDH anodes in the presence of 1,2- and 1,4-benzoquinones introduced in the solution is due to the shorter distance between these molecules and PQQ in the enzymatic molecule. It was also hypothesized that when 1,4-benzoquinone is adsorbed on a carbon support, it would play the dual role of a mediator and an orienting agent. At the same time, when 1,2-benzoquinone and ubiquinone are adsorbed on the electrode surface, the enzyme would transfer the electrons directly to the support, and these molecules would primarily play the role of an orienting agent.
- Authors:
-
- Univ. of New Mexico, Albuquerque, NM (United States)
- Univ. of New Mexico, Albuquerque, NM (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Publication Date:
- Research Org.:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1221793
- Report Number(s):
- LA-UR-15-22081
Journal ID: ISSN 0002-7863
- Grant/Contract Number:
- CBET 1158936; W911NF-14-C-0017; AC52-06NA25396
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 137; Journal Issue: 24; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Babanova, Sofia, Matanovic, Ivana, Chavez, Madelaine Seow, and Atanassov, Plamen. Role of quinones in electron transfer of PQQ–glucose dehydrogenase anodes—mediation or orientation effect. United States: N. p., 2015.
Web. doi:10.1021/jacs.5b03053.
Babanova, Sofia, Matanovic, Ivana, Chavez, Madelaine Seow, & Atanassov, Plamen. Role of quinones in electron transfer of PQQ–glucose dehydrogenase anodes—mediation or orientation effect. United States. https://doi.org/10.1021/jacs.5b03053
Babanova, Sofia, Matanovic, Ivana, Chavez, Madelaine Seow, and Atanassov, Plamen. Tue .
"Role of quinones in electron transfer of PQQ–glucose dehydrogenase anodes—mediation or orientation effect". United States. https://doi.org/10.1021/jacs.5b03053. https://www.osti.gov/servlets/purl/1221793.
@article{osti_1221793,
title = {Role of quinones in electron transfer of PQQ–glucose dehydrogenase anodes—mediation or orientation effect},
author = {Babanova, Sofia and Matanovic, Ivana and Chavez, Madelaine Seow and Atanassov, Plamen},
abstractNote = {In this study, the influence of two quinones (1,2- and 1,4-benzoquinone) on the operation and mechanism of electron transfer in PQQ-sGDH anodes has been determined. Benzoquinones were experimentally explored as mediators present in the electrolyte. The electrochemical performance of the PQQ–sGDH anodes with and without the mediators was examined and for the first time molecular docking simulations were used to gain a fundamental understanding to explain the role of the mediator molecules in the design and operation of the enzymatic electrodes. It was proposed that the higher performance of the PQQ–sGDH anodes in the presence of 1,2- and 1,4-benzoquinones introduced in the solution is due to the shorter distance between these molecules and PQQ in the enzymatic molecule. It was also hypothesized that when 1,4-benzoquinone is adsorbed on a carbon support, it would play the dual role of a mediator and an orienting agent. At the same time, when 1,2-benzoquinone and ubiquinone are adsorbed on the electrode surface, the enzyme would transfer the electrons directly to the support, and these molecules would primarily play the role of an orienting agent.},
doi = {10.1021/jacs.5b03053},
journal = {Journal of the American Chemical Society},
number = 24,
volume = 137,
place = {United States},
year = {Tue Jun 16 00:00:00 EDT 2015},
month = {Tue Jun 16 00:00:00 EDT 2015}
}
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