Solvent-less method for efficient photocatalytic [small alpha]-Fe2O3 nanoparticles using macromolecular polymeric precursors

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dc.contributor.authorDíaz, Carlos
dc.contributor.authorBarrientos, Lorena
dc.contributor.authorCarrillo, Daniel
dc.contributor.authorValdebenito, Javier
dc.contributor.authorValenzuela, María Luisa
dc.contributor.authorAllende, Patricio
dc.contributor.authorGeaney, Hugh
dc.contributor.authorO'Dwyer, Colm
dc.contributor.funderFondo Nacional de Desarrollo Científico y Tecnológicoen
dc.contributor.funderComisión Nacional de Investigación Científica y Tecnológicaen
dc.date.accessioned2018-05-09T13:27:17Z
dc.date.available2018-05-09T13:27:17Z
dc.date.issued2016-06-06
dc.date.updated2018-05-03T07:31:05Z
dc.description.abstractWe report a method for solvent-less growth of single crystalline hematite Fe2O3 nanoparticles from metal-containing polymeric macromolecular complexes, and demonstrate their efficient photocatalytic degradation of persistent cationic dye pollutants under visible light. Macromolecular complexes such as chitosan·(FeCl2)y, chitosan·(FeCl3)y, PS-co-4-PVP·(FeCl2)y and PS-co-4-PVP·(FeCl3)y with controlled polymer : metal molar ratios of 1 : 1 and 5 : 1 were prepared by single reaction of the respective polymers and iron chloride salts in CH2Cl2. The stable insoluble compounds were characterized by elemental analysis, infra-red spectroscopy, EPR and diffuse reflectance spectroscopy, and confirm Fe salts with degrees of coordination of ∼60–70%. Pyrolysis of these macromolecular precursors under air and at 800 °C forms networked Fe2O3 nanoparticles, whose volumetric density, size and shape is controlled by the metal content and the nature of the macromolecular complex (chitosan or PS-co-4-PVP). For both polymers, the 1 : 1 molar ratio precursor produces nanoparticles ranging from 10–200 nm with a moderate superparamagnetic behavior and optical bandgap marginally larger than bulk Fe2O3. A matrix-incubated formation mechanism involving the carbonization of the organic matter, forming voids within the macromolecular complex wherein the Fe centres coalesce, oxidize and crystallize into nanoparticles is also proposed. The hematite Fe2O3 nanoparticle materials demonstrate very efficient photocatalytic degradation of persistent water pollutants such as the cationic dye methylene blue. The nanoparticulate material obtained from chitosan·(FeCl2)y 1 : 1 under the simulated sunlight (full visible spectrum) irradiation provides high rate degradation of MB by 73% in 60 min and >94% after 150 min, measured at 655 nm.en
dc.description.sponsorshipFondo Nacional de Desarrollo Científico y Tecnológico (Fondecyt Projects 1120179, 1160241 and 1131112); Comisión Nacional de Investigación Científica y Tecnológica (Basal Financing Program CONICYT FB0807 (CEDENNA))en
dc.description.statusPeer revieweden
dc.description.versionAccepted Versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.citationDiaz, C., Barrientos, L., Carrillo, D., Valdebenito, J., Valenzuela, M. L., Allende, P., Geaney, H. and O'Dwyer, C. (2016) 'Solvent-less method for efficient photocatalytic [small alpha]-Fe2O3 nanoparticles using macromolecular polymeric precursors', New Journal of Chemistry, 40(8), pp. 6768-6776. doi: 10.1039/C6NJ00561Fen
dc.identifier.doi10.1039/C6NJ00561F
dc.identifier.endpage6776en
dc.identifier.issn1144-0546
dc.identifier.issued8en
dc.identifier.journaltitleNew Journal Of Chemistryen
dc.identifier.startpage6768en
dc.identifier.urihttps://hdl.handle.net/10468/6049
dc.identifier.volume40en
dc.language.isoenen
dc.publisherRoyal Society of Chemistry (RSC)en
dc.relation.urihttp://pubs.rsc.org/en/content/articlelanding/2016/nj/c6nj00561f#!divAbstract
dc.rights© The Royal Society of Chemistry and the Centre National de la Recherche Scientifique 2016en
dc.subjectDiffuse reflectance spectroscopyen
dc.subjectElectron spin resonanceen
dc.subjectInfrared spectrometryen
dc.subjectIrradiationen
dc.subjectLighten
dc.subjectMacromoleculeen
dc.subjectPhotocatalysisen
dc.subjectPolymerizationen
dc.subjectPrecursoren
dc.subjectPyrolysisen
dc.subjectSunlighten
dc.subjectWater pollutanten
dc.subjectNanoparticleen
dc.titleSolvent-less method for efficient photocatalytic [small alpha]-Fe2O3 nanoparticles using macromolecular polymeric precursorsen
dc.typeArticle (peer-reviewed)en
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