dorsal/arxiv
View SchemaEfficient, rapid one-electron photooxidation of chemisorbed polyhydroxyl alcohols and carbohydrates by TiO2 nanoparticles in an aqueous solution
| Authors | I. A. Shkrob, M. C. Sauer, Jr., D. Gosztola |
|---|---|
| Categories | |
| ArXiv ID | physics/0401059 |
| URL | https://arxiv.org/abs/physics/0401059 |
Abstract
Time-resolved transient absorption spectroscopy has been used to study nanosecond and sub-microsecond electron dynamics in aqueous anatase nanoparticles in the presence of hole scavengers: chemisorbed polyols and carbohydrates. These polyhydroxylated compounds are rapidly oxidized by the holes; 50-60% of these holes are scavenged within the duration of 355 nm excitation laser pulse. The scavenging efficiency rapidly increases with the number of anchoring hydroxyl groups and varies considerably as a function of the carbohydrate structure. A specific binding site for the polyols and carbohydrates is suggested that involves an octahedral Ti atom chelated by the poly-OH ligand. This mode of binding accounts for the depletion of undercoordinated Ti atoms observed in the XANES spectra of polyol coated nanoparticles. We suggest that these binding sites trap a substantial fraction of holes before the latter descend to surface traps and/or recombine with free electrons. The resulting oxygen hole center rapidly loses a CH proton to the environment, yielding a metastable C-centered radical.
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"abstract": "Time-resolved transient absorption spectroscopy has been used to study\nnanosecond and sub-microsecond electron dynamics in aqueous anatase\nnanoparticles in the presence of hole scavengers: chemisorbed polyols and\ncarbohydrates. These polyhydroxylated compounds are rapidly oxidized by the\nholes; 50-60% of these holes are scavenged within the duration of 355 nm\nexcitation laser pulse. The scavenging efficiency rapidly increases with the\nnumber of anchoring hydroxyl groups and varies considerably as a function of\nthe carbohydrate structure. A specific binding site for the polyols and\ncarbohydrates is suggested that involves an octahedral Ti atom chelated by the\npoly-OH ligand. This mode of binding accounts for the depletion of\nundercoordinated Ti atoms observed in the XANES spectra of polyol coated\nnanoparticles. We suggest that these binding sites trap a substantial fraction\nof holes before the latter descend to surface traps and/or recombine with free\nelectrons. The resulting oxygen hole center rapidly loses a CH proton to the\nenvironment, yielding a metastable C-centered radical.",
"arxiv_id": "physics/0401059",
"authors": [
"I. A. Shkrob",
"M. C. Sauer, Jr.",
"D. Gosztola"
],
"categories": [
"physics.chem-ph"
],
"title": "Efficient, rapid one-electron photooxidation of chemisorbed polyhydroxyl alcohols and carbohydrates by TiO2 nanoparticles in an aqueous solution",
"url": "https://arxiv.org/abs/physics/0401059"
},
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