Electron-mediated carbohydrate fuel cells: Characterizing the homogeneous viologen-mediated electron transfer rate of carbohydrate oxidation. (January 2020)
- Record Type:
- Journal Article
- Title:
- Electron-mediated carbohydrate fuel cells: Characterizing the homogeneous viologen-mediated electron transfer rate of carbohydrate oxidation. (January 2020)
- Main Title:
- Electron-mediated carbohydrate fuel cells: Characterizing the homogeneous viologen-mediated electron transfer rate of carbohydrate oxidation
- Authors:
- Bingham, Hilary
Oliveira, Dan
Larimer, Cassandra
Hedworth, Hayden
Bahari, Meisam
Watt, Gerald D.
Harb, John N.
Lewis, Randy S. - Abstract:
- Abstract: One area of exploration for renewable energy is the development of fuel cells, including carbohydrate fuel cells that can extract energy from carbohydrates. Viologen electron mediators have been shown to enhance energy extraction and improve carbohydrate conversion efficiencies, although the limiting step appears to be the homogeneous rate at which electrons are first transferred from the carbohydrate to the viologen. In this work, electron transfer rates for various monosaccharides in the presence of methyl viologen were studied in the absence of a fuel cell to isolate the homogeneous rate. Using glucose as the model carbohydrate, a rigorous mechanistic model of the homogeneous electron transfer rate was developed and showed a first-order dependence on OH − concentration, a first-order dependence on carbohydrate concentration, a zero-order dependence when the methyl viologen concentration was ≫ 0.4 mM, and an increasing rate with incubation time when glucose was incubated in a buffer solution prior to exposure to methyl viologen. The incubation effect had a strong dependence on pH and was consistent with interconversion between glucose and fructose. The mechanistic model, which agreed well with experimental data, can be useful for identifying process improvements to carbohydrate fuel cells, especially when the homogenous rate is a limiting step. Highlights: Viologen-mediated carbohydrate electron transfer rates were evaluated. Electron transfer rates generallyAbstract: One area of exploration for renewable energy is the development of fuel cells, including carbohydrate fuel cells that can extract energy from carbohydrates. Viologen electron mediators have been shown to enhance energy extraction and improve carbohydrate conversion efficiencies, although the limiting step appears to be the homogeneous rate at which electrons are first transferred from the carbohydrate to the viologen. In this work, electron transfer rates for various monosaccharides in the presence of methyl viologen were studied in the absence of a fuel cell to isolate the homogeneous rate. Using glucose as the model carbohydrate, a rigorous mechanistic model of the homogeneous electron transfer rate was developed and showed a first-order dependence on OH − concentration, a first-order dependence on carbohydrate concentration, a zero-order dependence when the methyl viologen concentration was ≫ 0.4 mM, and an increasing rate with incubation time when glucose was incubated in a buffer solution prior to exposure to methyl viologen. The incubation effect had a strong dependence on pH and was consistent with interconversion between glucose and fructose. The mechanistic model, which agreed well with experimental data, can be useful for identifying process improvements to carbohydrate fuel cells, especially when the homogenous rate is a limiting step. Highlights: Viologen-mediated carbohydrate electron transfer rates were evaluated. Electron transfer rates generally increased with decreasing number of carbons. A rigorous mechanistic electron transfer model for glucose was developed. Electron transfer model is first order in pH and carbohydrate concentration. Incubation time of glucose increases electron transfer rate and is pH dependent. … (more)
- Is Part Of:
- Renewable energy. Volume 145(2020)
- Journal:
- Renewable energy
- Issue:
- Volume 145(2020)
- Issue Display:
- Volume 145, Issue 2020 (2020)
- Year:
- 2020
- Volume:
- 145
- Issue:
- 2020
- Issue Sort Value:
- 2020-0145-2020-0000
- Page Start:
- 1985
- Page End:
- 1991
- Publication Date:
- 2020-01
- Subjects:
- Fuel cell -- Viologen -- Carbohydrate -- Model -- Homogeneous reaction
Renewable energy sources -- Periodicals
Power resources -- Periodicals
Énergies renouvelables -- Périodiques
Ressources énergétiques -- Périodiques
333.794 - Journal URLs:
- http://www.sciencedirect.com/science/journal/09601481 ↗
http://www.elsevier.com/journals ↗
http://www.journals.elsevier.com/renewable-energy/ ↗ - DOI:
- 10.1016/j.renene.2019.07.079 ↗
- Languages:
- English
- ISSNs:
- 0960-1481
- Deposit Type:
- Legaldeposit
- View Content:
- Available online (eLD content is only available in our Reading Rooms) ↗
- Physical Locations:
- British Library DSC - 7364.187000
British Library DSC - BLDSS-3PM
British Library HMNTS - ELD Digital store - Ingest File:
- 11883.xml