6533b86efe1ef96bd12cc066
RESEARCH PRODUCT
Visible-light driven oxidation of gaseous aliphatic alcohols to the corresponding carbonyls via TiO2 sensitized by a perylene derivative
Giuseppe CalogeroGaetano Di MarcoVittorio LoddoMario PagliaroFrancesco ParrinoRosaria CiriminnaChiara GuariscoGiovanni Palmisanosubject
Chromatography GasLightHealth Toxicology and MutagenesisInorganic chemistryFormaldehydeElectronsPhotochemistry..ImidesCatalysisCatalysischemistry.chemical_compoundDiimideEnvironmental ChemistryReactivity (chemistry)Partial oxidationVisible light photocatalysisPeryleneTitaniumSettore ING-IND/24 - Principi Di Ingegneria ChimicaMolecular StructureMethanolPerylene-sensitized TiO2General MedicinePollutionAliphatic alcohol oxidationchemistryYield (chemistry)MethanolPerylene-sensitized TiO2 Visible light photocatalysis Aliphatic alcohol oxidationOxidation-ReductionPerylenedescription
Sensitized P25 TiO2 was prepared by wet impregnation with a home-prepared perylene dye, i.e., N,N?-bis(2-(1- piperazino)ethyl)-3,4,9,10-perylene-tetracarboxylic acid diimide dichloride (PZPER). Energy levels of PZPER were found to be compatible with those of TiO2 allowing fast electron transfer. The obtained catalyst has been characterized and used in the gas-phase partial oxidation of aliphatic primary and secondary alcohols, i.e., methanol, ethanol, and 2- propanol. The reaction was carried out under cut-off (?> 400 nm) simulated solar radiation in O2 atmosphere. The perylene derivative allowed a good absorbance of visible radiation thanks to its low optical energy gap (2.6 eV) which was evaluated by cyclic voltammetry. The optimal organic sensitizing amount was found to be 5.6 % w/w in terms of yield in carbonyl derivatives. Moreover, no change in reactivity/selectivity was observed after 10-h irradiation thus confirming the catalyst stability. Yields into formaldehyde, acetaldehyde, and acetone were 67, 70, and 96 %, respectively. No significant amounts of organic byproducts were detected but for methanol oxidation, whereas a minor amount of the substrate degraded to CO2.
year | journal | country | edition | language |
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2013-01-01 |