Evaluación de la actividad fotocatalítica de FexOy/TiO2 obtenido a partir de ilmenita proveniente de residuos mineros para la degradación de cianuro disuelto en agua

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dc.contributor.advisorCarriazo Baños, José Gregoriospa
dc.contributor.advisorMárquez Godoy, Marco Antoniospa
dc.contributor.authorHenao Hoyos, Yuli Marcelaspa
dc.contributor.cvlacHenao Hoyos, Yuli Marcela [0001529361]spa
dc.contributor.orcidHenao-Hoyos, Yuli Marcela [0000000268628668]spa
dc.contributor.researchgateHenao-Hoyos, Yuli Marcelaspa
dc.contributor.researchgroupDiseño y Reactividad de Estructuras Sólidas (Lab DRES)spa
dc.contributor.researchgroupMineralogía aplicada y bioprocesos (GMAB)spa
dc.date.accessioned2024-07-16T20:09:15Z
dc.date.available2024-07-16T20:09:15Z
dc.date.issued2024-07-08
dc.descriptionilustraciones a color, diagramas, fotografíasspa
dc.description.abstractEn el presente trabajo se estudia la síntesis de catalizadores basados en estructuras de Fe(III)-TiO2 (dióxido de titanio dopado con hierro), obtenidos a partir del mineral natural ilmenita extraída de arenas negras que constituyen un tipo de residuo de la industria minera (de explotación de oro) en la región de El Bagre Antioquia-Colombia. La síntesis se desarrolló mediante la extracción ácida controlada de las especies de titanio-hierro, permitiendo la obtención de catalizadores con diferentes contenidos de hierro. Dichos materiales se estudiaron mediante caracterizaciones, estructurales, superficiales, texturales y morfológicas (DRX, XPS, UV-Vis, TEM, EDX, difracción de electrones, isotermas de adsorción de N2, entre otras). Los resultados indican variaciones importantes en los diferentes sólidos, las cuales son marcadamente relacionables con el desempeño catalítico evaluado. Adicionalmente, se caracterizaron también dos sólidos comerciales (anatasa comercial y Degussa P25), con el objetivo de comparar las diferentes propiedades estudiadas. Los resultados indicaron mejores propiedades texturales y de tamaño de partícula (mayor área y menor tamaño) para la mayoría de los sólidos sintetizados y, de acuerdo al estudio estructural, se evidenció una posible substitución de Fe(III) en la estructura de TiO2 tipo anatasa. Los diferentes catalizadores sintetizados se evaluaron en la reacción de degradación fotocatalítica del ion cianuro (CN-) en medio acuoso, tanto en presencia de luz UV como de luz visible. Los resultados se compararon con las evaluaciones fotocatalíticas de los sólidos de referencia (anatasa comercial y Desgussa P25). Aunque los resultados demostraron una actividad comparable de los sólidos sintetizados con la actividad de la anatasa comercial, e inferior a la del TiO2 Degussa, bajo radiación UV, la actividad catalítica de dichos materiales sintetizados fue superior que la de los sólidos de referencia en presencia de luz visible. Además, los estudios cinéticos realizados mostraron excelente ajuste a la cinética de pseudo-primer orden mediante el modelo de Langmuir-Hinshelwood. Finalmente, se realizó la exploración de diferentes especies químicas involucradas en el mecanismo de reacción para la degradación de cianuro. Para ello, se empleó espectroscopía FTIR en modo de reflectancia difusa, mediante ensayos in situ (método transiente). Dichos experimentos permitieron verificar la desaparición progresiva de cianuro, la aparición de especies transitorias como cianato (CNO-), HCONH2 y NH2OH, entre otras. Adicionalmente, este estudio permitió entender mejor el papel del hierro incorporado en la estructura del TiO2, revelando la participación del Fe(III) estructural en la quimiadsorción del cianuro y su transformación en la superficie. Este resultado junto con aquellos obtenidos para la cinética de reacción, sugieren la participación predominante de un mecanismo tipo Langmuir-Hinshelwood. El presente estudio también permitió comprender mejor la función de los grupos -OH superficiales en el desempeño fotocatalítico de los sólidos. (Texto tomado de la fuente)spa
dc.description.abstractThe present study focuses on the synthesis of catalysts based on structures (iron-doped titanium dioxide), derived from the natural mineral ilmenite extracted from black sands, which constitute a type of waste from the gold mining industry in the El Bagre region of Antioquia, Colombia. The synthesis process involved a controlled acid extraction of titanium-iron species, enabling the production of catalysts with different iron contents. These materials were studied by structural, surface, textural, and morphological characterizations (X-ray diffraction, X-ray photoelectron spectroscopy, UV-Visible spectroscopy, transmission electron microscopy, energy-dispersive X-ray spectroscopy, electron diffraction, nitrogen adsorption isotherms, among others). The results revealed significant variations among the different solids, which are closely correlated with the evaluated catalytic performance. Additionally, two commercial solids (commercial anatase and Degussa P25) were also characterized for comparing different properties. The findings indicate superior textural properties (higher surface areas) and lower particle sizes for most of the synthesized solids. Furthermore, based on structural analysis, a potential isomorphic substitution of Fe(III) in the anatase-type TiO2 structure was observed. The synthesized catalysts were assessed in the photocatalytic degradation performance of cyanide (CN-) in aqueous medium, under UV radiation, and also using visible light. The results were compared with the photocatalytic performance of the reference solids (commercial anatase and Degussa P25). The findings demonstrated a comparable photo-activity of the synthesized solids with the commercial anatase and a lower activity than TiO2 Degussa under UV irradiation, but the catalytic photo-activity of these synthesized materials surpassed that of the reference solids under visible light irradiation. On the other hand, the kinetic studies demonstrated an excellent correlation with the Langmuir-Hinshelwood model, using a pseudo-first order approximation. Finally, an exploration of different chemical species involved in the reaction mechanism for cyanide degradation was conducted. For this purpose, diffuse reflectance Fourier-transform infrared (FTIR) spectroscopy was employed by in situ measures (transient method). These experiments allowed the verification of the progressive disappearance of cyanide and the emergence of transient species such as cyanate (CNO-), HCONH2, and NH2OH, among others. Additionally, this study enhanced the understanding of the role of iron incorporated into the TiO2 structure, revealing the participation of structural Fe(III) in the chemisorption and transformation of cyanide on the catalyst surface. This result, and those obtained by the kinetic experiments, suggest the predominant occurrence of the Langmuir-Hinshelwood mechanism. This study also provided a better comprehension on the role of surface -OH groups in the photocatalytic performance of the solids. (Texto tomado de la fuente)eng
dc.description.degreelevelDoctoradospa
dc.description.degreenameDoctor en Ciencias - Químicaspa
dc.description.researchareaFotocatálisis heterogénea con TiO2spa
dc.description.sponsorshipEl Ministerio de Ciencia y Tecnología a través de la convocatoria 785 de 2017 para doctorados nacionalesspa
dc.format.extent220 páginasspa
dc.format.mimetypeapplication/pdfspa
dc.identifier.instnameUniversidad Nacional de Colombiaspa
dc.identifier.reponameRepositorio Institucional Universidad Nacional de Colombiaspa
dc.identifier.repourlhttps://repositorio.unal.edu.co/spa
dc.identifier.urihttps://repositorio.unal.edu.co/handle/unal/86481
dc.language.isospaspa
dc.publisherUniversidad Nacional de Colombiaspa
dc.publisher.branchUniversidad Nacional de Colombia - Sede Bogotáspa
dc.publisher.facultyFacultad de Cienciasspa
dc.publisher.placeBogotá, Colombiaspa
dc.publisher.programBogotá - Ciencias - Doctorado en Ciencias - Químicaspa
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dc.rights.accessrightsinfo:eu-repo/semantics/openAccessspa
dc.rights.licenseAtribución-NoComercial-SinDerivadas 4.0 Internacionalspa
dc.rights.urihttp://creativecommons.org/licenses/by-nc-nd/4.0/spa
dc.subject.ddc540 - Química y ciencias afines::541 - Química físicaspa
dc.subject.ddc540 - Química y ciencias afines::549 - Mineralogíaspa
dc.subject.lembFotocatálisisspa
dc.subject.lembPhotocatalysiseng
dc.subject.lembNanopartículasspa
dc.subject.lembNanoparticleseng
dc.subject.lembCatálisis heterogéneasspa
dc.subject.lembHeterogeneous catalysiseng
dc.subject.lembCianuros -- Análisisspa
dc.subject.lembCyanides -- Analysiseng
dc.subject.lembResiduos de la mineríaspa
dc.subject.lembWaste miningeng
dc.subject.lembEspectrofotometríaspa
dc.subject.lembSpectrophotometryeng
dc.subject.proposalFotocatálisis heterogéneaspa
dc.subject.proposalDióxido de titaniospa
dc.subject.proposalHierrospa
dc.subject.proposalOxidación fotocatalíticaspa
dc.subject.proposalCianurospa
dc.subject.proposalHeterogenous photocatalysiseng
dc.subject.proposalTitanium dioxideeng
dc.subject.proposalIroneng
dc.subject.proposalPhotocatalytic oxidationeng
dc.subject.proposalCyanideeng
dc.subject.wikidataIlmenitaspa
dc.subject.wikidataIlmeniteeng
dc.titleEvaluación de la actividad fotocatalítica de FexOy/TiO2 obtenido a partir de ilmenita proveniente de residuos mineros para la degradación de cianuro disuelto en aguaspa
dc.title.translatedAssessment of the photocatalytic activity of FexOy/TiO2 synthesized from ilmenite sourced from mining wastes for the degradation of cyanide dissolved waterspa
dc.typeTrabajo de grado - Doctoradospa
dc.type.coarhttp://purl.org/coar/resource_type/c_db06spa
dc.type.coarversionhttp://purl.org/coar/version/c_ab4af688f83e57aaspa
dc.type.contentTextspa
dc.type.driverinfo:eu-repo/semantics/doctoralThesisspa
dc.type.redcolhttp://purl.org/redcol/resource_type/TDspa
dc.type.versioninfo:eu-repo/semantics/acceptedVersionspa
dcterms.audience.professionaldevelopmentEstudiantesspa
dcterms.audience.professionaldevelopmentInvestigadoresspa
dcterms.audience.professionaldevelopmentPúblico generalspa
oaire.accessrightshttp://purl.org/coar/access_right/c_abf2spa
oaire.awardtitleEvaluación de la actividad fotocatalítica de FexOy/TiO2 obtenido a partir de ilmenita proveniente de residuos mineros para la degradación de cianuro disuelto en aguaspa
oaire.fundernameMincienciasspa

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