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231225s2017 xx |||||o 00| ||eng c |
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|a 10.1021/acs.langmuir.7b01117
|2 doi
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|a pubmed24n0913.xml
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|a (DE-627)NLM27398344X
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|a (NLM)28723093
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|a DE-627
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|c DE-627
|e rakwb
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|a eng
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| 100 |
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|a DeSario, Paul A
|e verfasserin
|4 aut
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| 245 |
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|a Plasmonic Aerogels as a Three-Dimensional Nanoscale Platform for Solar Fuel Photocatalysis
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|c 2017
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|a Text
|b txt
|2 rdacontent
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|a ƒaComputermedien
|b c
|2 rdamedia
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|a ƒa Online-Ressource
|b cr
|2 rdacarrier
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|a Date Completed 23.07.2018
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|a Date Revised 23.07.2018
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|a published: Print-Electronic
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|a Citation Status PubMed-not-MEDLINE
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|a We use plasmonic Au-TiO2 aerogels as a platform in which to marry synthetically thickened particle-particle junctions in TiO2 aerogel networks to Au∥TiO2 interfaces and then investigate their cooperative influence on photocatalytic hydrogen (H2) generation under both broadband (i.e., UV + visible light) and visible-only excitation. In doing so, we elucidate the dual functions that incorporated Au can play as a water reduction cocatalyst and as a plasmonic sensitizer. We also photodeposit non-plasmonic Pt cocatalyst nanoparticles into our composite aerogels in order to leverage the catalytic water-reducing abilities of Pt. This Au-TiO2/Pt arrangement in three dimensions effectively utilizes conduction-band electrons injected into the TiO2 aerogel network upon exciting the Au SPR at the Au∥TiO2 interface. The extensive nanostructured high surface-area oxide network in the aerogel provides a matrix that spatially separates yet electrochemically connects plasmonic nanoparticle sensitizers and metal nanoparticle catalysts, further enhancing solar-fuels photochemistry. We compare the photocatalytic rates of H2 generation with and without Pt cocatalysts added to Au-TiO2 aerogels and demonstrate electrochemical linkage of the SPR-generated carriers at the Au∥TiO2 interfaces to downfield Pt nanoparticle cocatalysts. Finally, we investigate visible light-stimulated generation of conduction band electrons in Au-TiO2 and TiO2 aerogels using ultrafast visible pump/IR probe spectroscopy. Substantially more electrons are produced at Au-TiO2 aerogels due to the incorporated SPR-active Au nanoparticle, whereas the smaller population of electrons generated at Au-free TiO2 aerogels likely originate at shallow traps in the high surface-area mesoporous aerogel
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|a Journal Article
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|a Research Support, U.S. Gov't, Non-P.H.S.
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|a Pietron, Jeremy J
|e verfasserin
|4 aut
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|a Dunkelberger, Adam
|e verfasserin
|4 aut
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|a Brintlinger, Todd H
|e verfasserin
|4 aut
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|a Baturina, Olga
|e verfasserin
|4 aut
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|a Stroud, Rhonda M
|e verfasserin
|4 aut
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| 700 |
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|a Owrutsky, Jeffrey C
|e verfasserin
|4 aut
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| 700 |
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|a Rolison, Debra R
|e verfasserin
|4 aut
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| 773 |
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|i Enthalten in
|t Langmuir : the ACS journal of surfaces and colloids
|d 1992
|g 33(2017), 37 vom: 19. Sept., Seite 9444-9454
|w (DE-627)NLM098181009
|x 1520-5827
|7 nnns
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| 773 |
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|g volume:33
|g year:2017
|g number:37
|g day:19
|g month:09
|g pages:9444-9454
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|u http://dx.doi.org/10.1021/acs.langmuir.7b01117
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