Direct oxygen and hydrogen production by photo water splitting using a robust bioinspired manganese-oxo oligomer complex/tungsten oxide catalytic system |
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| Authors: | Lien-Yang Chou Rui Liu Wanshu He Ndi Geh Yongjing Lin Emily Y.F. Hou Dunwei Wang Harvey J.M. Hou |
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| Affiliation: | 1. Department of Chemistry and Biochemistry, University of Massachusetts Dartmouth, 285 Old Westport Road, North Dartmouth, MA 02747, USA;2. Chemistry Department, Boston College, 2609 Beacon St., Chestnut Hill, MA 02467, USA;3. Sharon High School, 181 Pond Street, Sharon, MA 02067, USA;4. Department of Physical Sciences, Alabama State University, 915 South Jackson Street, Montgomery, AL 36104, USA |
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| Abstract: | The n-type semiconductor tungsten oxide is readily dissolved in aqueous solution at pH > 4 and may be problematic in water splitting catalysis. We have reported that a tungsten oxide photoanode prepared by atomic layer deposition can be stabilized with a Mn-oxo compound for efficient photo water splitting at pH 4 and pH 7. However the molecular mechanism of water oxidation reaction in this robust catalytic system is not known. In this work, the mechanism for oxygen and hydrogen production by photo water splitting using Mn-oxo complex/tungsten oxide heteronanostructures was examined under different experimental conditions by X-ray photoelectron spectroscopy as well as gas chromatographic analysis, O-18 isotope measurements, and pH dependence of photocurrent. We found that the Mn(II) species plays an important role in the catalytic cycle of water oxidation in the Mn-oxo oligomer complex/tungsten oxide system and propose a working model of the Mn-oxo oligomer complex/tungsten oxide catalytic system in photo water splitting. |
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| Keywords: | Manganese Tungsten oxide Water splitting PS II Catalysis Hydrogen production |
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