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Heterogenized water oxidation catalysts prepared by immobilizing Klaui-type organometallic precursors
dc.contributor.author | Pastori, Gabriele |
dc.contributor.author | Wahab, Khaja |
dc.contributor.author | Bucci, Alberto |
dc.contributor.author | Bellachioma, Gianfranco |
dc.contributor.author | Zuccaccia, Cristiano |
dc.contributor.author | Llorca Piqué, Jordi |
dc.contributor.author | Idriss, Hicham |
dc.contributor.author | Macchioni, Alceo |
dc.contributor.other | Universitat Politècnica de Catalunya. Departament d'Enginyeria Química |
dc.date.accessioned | 2017-02-15T08:47:20Z |
dc.date.available | 2017-06-27T00:30:40Z |
dc.date.issued | 2016-09-12 |
dc.identifier.citation | Pastori, G., Wahab, K., Bucci, A., Bellachioma, G., Zuccaccia, C., Llorca, J., Idriss, H., Macchioni, A. Heterogenized water oxidation catalysts prepared by immobilizing Klaui-type organometallic precursors. "Chemistry: a european journal", 12 Setembre 2016, vol. 22, núm. 38, p. 13459-13463. |
dc.identifier.issn | 0947-6539 |
dc.identifier.uri | http://hdl.handle.net/2117/101053 |
dc.description.abstract | An efficient heterogenized water oxidation catalyst (2_TiO2) has been synthesized by immobilizing the Kläui-type organometallic precursor [Cp*Ir{P(O)(OH)2}3]Na (2, Cp*=1,2,3,4,5-pentamethylcyclopentadienyl ligand) onto rutile TiO2. Iridium is homogeneously distributed at the molecular and atomic/small cluster level in 2_TiO2 and 2'_TiO2 (solid catalyst recovered after the first catalytic run), respectively, as indicated by STEM-HAADF (scanning transmission electron microscopy - high angle annular dark field) studies. 2'_TiO2 exhibits TOF values up to 23.7 min-1 in the oxidation of water to O2 driven by NaIO4 at nearly neutral pH, and a TON only limited by the amount of NaIO4 used, as indicated by multiple run experiments. Furthermore, while roughly 40¿% leaching is observed during the first catalytic run, 2'_TiO2 does not undergo any further leaching even when in contact with strongly basic solutions and completely maintains its activity for thousands of cycles. NMR studies, in combination with ICP-OES (inductively coupled plasma optical emission spectrometry), indicate that the activation of 2_TiO2 occurs through the initial oxidative dissociation of PO43-, ultimately leading to active centers in which a 1:1 P/Ir ratio is present (derived from the removal of two PO43- units) likely missing the Cp* ligand. |
dc.format.extent | 5 p. |
dc.language.iso | eng |
dc.rights.uri | http://creativecommons.org/licenses/by-nc-nd/3.0/es/ |
dc.subject | Àrees temàtiques de la UPC::Enginyeria química |
dc.subject.lcsh | Renewable energy resources |
dc.subject.other | Iridium |
dc.subject.other | Klaui-type compounds |
dc.subject.other | titanium dioxide |
dc.subject.other | water oxidation |
dc.subject.other | water splitting |
dc.title | Heterogenized water oxidation catalysts prepared by immobilizing Klaui-type organometallic precursors |
dc.type | Article |
dc.subject.lemac | Catàlisi |
dc.subject.lemac | Diòxid de titani |
dc.subject.lemac | Energies renovables |
dc.contributor.group | Universitat Politècnica de Catalunya. NEMEN - Nanoenginyeria de materials aplicats a l'energia |
dc.identifier.doi | 10.1002/chem.201602008 |
dc.description.peerreviewed | Peer Reviewed |
dc.relation.publisherversion | http://onlinelibrary.wiley.com/doi/10.1002/chem.201602008/abstract |
dc.rights.access | Open Access |
local.identifier.drac | 19332518 |
dc.description.version | Postprint (author's final draft) |
local.citation.author | Pastori, G.; Wahab, K.; Bucci, A.; Bellachioma, G.; Zuccaccia, C.; Llorca, J.; Idriss, H.; Macchioni, A. |
local.citation.publicationName | Chemistry: a european journal |
local.citation.volume | 22 |
local.citation.number | 38 |
local.citation.startingPage | 13459 |
local.citation.endingPage | 13463 |
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