Abstract
We find that crystallographically resolved Ti17O24(OPri)20 nanoparticles, functionalized by covalent attachment of 4-nitrophenyl-acetylacetonate or coumarin 343 adsorbates, exhibit hole injection into surface states when photoexcited with visible light (λ = 400-680 nm). Our findings are supported by photoelectrochemical measurements, EPR spectroscopy, and quantum dynamics simulations of interfacial charge transfer. The underlying mechanism is consistent with measurements of photocathodic currents generated with visible light for thin layers of functionalized polyoxotitanate nanocrystals deposited on FTO working electrodes. The reported experimental and theoretical analysis demonstrates for the first time the feasibility of p-type sensitization of TiO2 solely based on covalent binding of organic adsorbates.
| Original language | English |
|---|---|
| Pages (from-to) | 16420-16429 |
| Number of pages | 10 |
| Journal | Journal of the American Chemical Society |
| Volume | 136 |
| Issue number | 46 |
| DOIs | |
| Publication status | Published - Nov 19 2014 |
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ASJC Scopus subject areas
- Chemistry(all)
- Catalysis
- Biochemistry
- Colloid and Surface Chemistry
Cite this
Photoelectrochemical hole injection revealed in polyoxotitanate nanocrystals functionalized with organic adsorbates. / Negre, Christian F A; Young, Karin J.; Oviedo, Ma Belén; Allen, Laura J.; Sánchez, Cristián G.; Jarzembska, Katarzyna N.; Benedict, Jason B.; Crabtree, Robert H.; Coppens, Philip; Brudvig, Gary W; Batista, Victor S.
In: Journal of the American Chemical Society, Vol. 136, No. 46, 19.11.2014, p. 16420-16429.Research output: Contribution to journal › Article
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TY - JOUR
T1 - Photoelectrochemical hole injection revealed in polyoxotitanate nanocrystals functionalized with organic adsorbates
AU - Negre, Christian F A
AU - Young, Karin J.
AU - Oviedo, Ma Belén
AU - Allen, Laura J.
AU - Sánchez, Cristián G.
AU - Jarzembska, Katarzyna N.
AU - Benedict, Jason B.
AU - Crabtree, Robert H.
AU - Coppens, Philip
AU - Brudvig, Gary W
AU - Batista, Victor S.
PY - 2014/11/19
Y1 - 2014/11/19
N2 - We find that crystallographically resolved Ti17O24(OPri)20 nanoparticles, functionalized by covalent attachment of 4-nitrophenyl-acetylacetonate or coumarin 343 adsorbates, exhibit hole injection into surface states when photoexcited with visible light (λ = 400-680 nm). Our findings are supported by photoelectrochemical measurements, EPR spectroscopy, and quantum dynamics simulations of interfacial charge transfer. The underlying mechanism is consistent with measurements of photocathodic currents generated with visible light for thin layers of functionalized polyoxotitanate nanocrystals deposited on FTO working electrodes. The reported experimental and theoretical analysis demonstrates for the first time the feasibility of p-type sensitization of TiO2 solely based on covalent binding of organic adsorbates.
AB - We find that crystallographically resolved Ti17O24(OPri)20 nanoparticles, functionalized by covalent attachment of 4-nitrophenyl-acetylacetonate or coumarin 343 adsorbates, exhibit hole injection into surface states when photoexcited with visible light (λ = 400-680 nm). Our findings are supported by photoelectrochemical measurements, EPR spectroscopy, and quantum dynamics simulations of interfacial charge transfer. The underlying mechanism is consistent with measurements of photocathodic currents generated with visible light for thin layers of functionalized polyoxotitanate nanocrystals deposited on FTO working electrodes. The reported experimental and theoretical analysis demonstrates for the first time the feasibility of p-type sensitization of TiO2 solely based on covalent binding of organic adsorbates.
UR - http://www.scopus.com/inward/record.url?scp=84912544502&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=84912544502&partnerID=8YFLogxK
U2 - 10.1021/ja509270f
DO - 10.1021/ja509270f
M3 - Article
AN - SCOPUS:84912544502
VL - 136
SP - 16420
EP - 16429
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
SN - 0002-7863
IS - 46
ER -