Abstract
Most transport fuels are derived from fossil fuels, generate greenhouse gases, and consume significant amounts of water in the extraction, purification, and/or burning processes. The generation of hydrogen using solar energy to split water, ideally from abundant water sources such as sea water or other non-potable sources, could potentially provide an unlimited, clean fuel for the future. Solar, electrochemical water splitting typically combines a photoanode at which water oxidation occurs, with a cathode for proton reduction to hydrogen. In recent work, we have found that a bioinspired tetra-manganese cluster catalyzes water oxidation at relatively low overpotentials (0.38 V) when doped into a Nafion proton conduction membrane deposited on a suitable electrode surface, and illuminated with visible light. We report here that this assembly is active in aqueous and organic electrolyte solutions containing a range of different salts in varying concentrations. Similar photocurrents were obtained using electrolytes containing 0.0 - 0.5 M sodium sulfate, sodium Perchlorate or sodium chloride. A slight decline in photocurrent was observed for sodium Perchlorate but only at and above 5.0 M concentration. In acetonitrile and acetone solutions containing 10% water, increasing the electrolyte concentration was found to result in leaching of the catalytic species from the membrane and a decrease in photocurrent. Leaching was not observed when the system was tested in an ionic liquid containing water, however, a lower photocurrent was generated than observed in aqueous electrolyte. We conclude that immersion of the membrane in an aqueous solution containing an electrolyte concentration of 0.05 - 0.5M represent good conditions for operation for the cubium/Nafion catalytic system.
| Original language | English |
|---|---|
| Title of host publication | Proceedings of SPIE - The International Society for Optical Engineering |
| Volume | 7408 |
| DOIs | |
| Publication status | Published - 2009 |
| Event | Solar Hydrogen and Nanotechnology IV - San Diego, CA, United States Duration: Aug 3 2009 → Aug 6 2009 |
Other
| Other | Solar Hydrogen and Nanotechnology IV |
|---|---|
| Country | United States |
| City | San Diego, CA |
| Period | 8/3/09 → 8/6/09 |
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Keywords
- Hydrogen
- Manganese cubane catalyst
- Photocatalysis
- Photosystem ii
- Salt effects
- Water oxidation
ASJC Scopus subject areas
- Applied Mathematics
- Computer Science Applications
- Electrical and Electronic Engineering
- Electronic, Optical and Magnetic Materials
- Condensed Matter Physics
Cite this
A bio-inspired molecular water oxidation catalyst for renewable hydrogen generation : An examination of salt effects. / Brimblecombe, Robin; Rotstein, Miriam; Koo, Annette; Dismukes, G Charles; Swiegers, Gerhard F.; Spiccia, Leone.
Proceedings of SPIE - The International Society for Optical Engineering. Vol. 7408 2009. 74080V.Research output: Chapter in Book/Report/Conference proceeding › Conference contribution
}
TY - GEN
T1 - A bio-inspired molecular water oxidation catalyst for renewable hydrogen generation
T2 - An examination of salt effects
AU - Brimblecombe, Robin
AU - Rotstein, Miriam
AU - Koo, Annette
AU - Dismukes, G Charles
AU - Swiegers, Gerhard F.
AU - Spiccia, Leone
PY - 2009
Y1 - 2009
N2 - Most transport fuels are derived from fossil fuels, generate greenhouse gases, and consume significant amounts of water in the extraction, purification, and/or burning processes. The generation of hydrogen using solar energy to split water, ideally from abundant water sources such as sea water or other non-potable sources, could potentially provide an unlimited, clean fuel for the future. Solar, electrochemical water splitting typically combines a photoanode at which water oxidation occurs, with a cathode for proton reduction to hydrogen. In recent work, we have found that a bioinspired tetra-manganese cluster catalyzes water oxidation at relatively low overpotentials (0.38 V) when doped into a Nafion proton conduction membrane deposited on a suitable electrode surface, and illuminated with visible light. We report here that this assembly is active in aqueous and organic electrolyte solutions containing a range of different salts in varying concentrations. Similar photocurrents were obtained using electrolytes containing 0.0 - 0.5 M sodium sulfate, sodium Perchlorate or sodium chloride. A slight decline in photocurrent was observed for sodium Perchlorate but only at and above 5.0 M concentration. In acetonitrile and acetone solutions containing 10% water, increasing the electrolyte concentration was found to result in leaching of the catalytic species from the membrane and a decrease in photocurrent. Leaching was not observed when the system was tested in an ionic liquid containing water, however, a lower photocurrent was generated than observed in aqueous electrolyte. We conclude that immersion of the membrane in an aqueous solution containing an electrolyte concentration of 0.05 - 0.5M represent good conditions for operation for the cubium/Nafion catalytic system.
AB - Most transport fuels are derived from fossil fuels, generate greenhouse gases, and consume significant amounts of water in the extraction, purification, and/or burning processes. The generation of hydrogen using solar energy to split water, ideally from abundant water sources such as sea water or other non-potable sources, could potentially provide an unlimited, clean fuel for the future. Solar, electrochemical water splitting typically combines a photoanode at which water oxidation occurs, with a cathode for proton reduction to hydrogen. In recent work, we have found that a bioinspired tetra-manganese cluster catalyzes water oxidation at relatively low overpotentials (0.38 V) when doped into a Nafion proton conduction membrane deposited on a suitable electrode surface, and illuminated with visible light. We report here that this assembly is active in aqueous and organic electrolyte solutions containing a range of different salts in varying concentrations. Similar photocurrents were obtained using electrolytes containing 0.0 - 0.5 M sodium sulfate, sodium Perchlorate or sodium chloride. A slight decline in photocurrent was observed for sodium Perchlorate but only at and above 5.0 M concentration. In acetonitrile and acetone solutions containing 10% water, increasing the electrolyte concentration was found to result in leaching of the catalytic species from the membrane and a decrease in photocurrent. Leaching was not observed when the system was tested in an ionic liquid containing water, however, a lower photocurrent was generated than observed in aqueous electrolyte. We conclude that immersion of the membrane in an aqueous solution containing an electrolyte concentration of 0.05 - 0.5M represent good conditions for operation for the cubium/Nafion catalytic system.
KW - Hydrogen
KW - Manganese cubane catalyst
KW - Photocatalysis
KW - Photosystem ii
KW - Salt effects
KW - Water oxidation
UR - http://www.scopus.com/inward/record.url?scp=79959410435&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=79959410435&partnerID=8YFLogxK
U2 - 10.1117/12.824840
DO - 10.1117/12.824840
M3 - Conference contribution
AN - SCOPUS:79959410435
SN - 9780819476982
VL - 7408
BT - Proceedings of SPIE - The International Society for Optical Engineering
ER -