Autor según el artículo: Fakhrnasova, Dina; Chimentao, Ricardo J.; Medina, Francisco; Urakawa, Atsushi;
Departamento: Enginyeria Química
Autor/es de la URV: CHIMENTON, RICARDO JOSE / Medina Cabello, Francisco
Palabras clave: Urea Transesterification Reaction mechanism Multivariate curve resolution Mixed-metal oxides Kinetics Ethylene glycol Ethylene carbonate Doe Acid-base property
Resumen: This work employs (i) a rational approach to improve the material properties of catalysts for urea transesterification with ethylene glycol (EG) to ethylene carbonate (EC) over metal oxides and (ii) a statistical approach to maximize the desired product. For the rational approach, single- and mixed-metal oxides with different elemental combinations (Zn, Mg, Al, Fe) with a variety of acid−base properties were synthesized and evaluated for the reaction. The roles of acidity and basicity in the identified reaction paths were clarified on the basis of product selectivities and kinetic parameters extracted from the concentration profiles of reactants and products in every reaction path by means of in situ IR monitoring and subsequent multivariate analysis. The paths toward EC are favorably catalyzed by acidic sites, while basic sites catalyze all paths toward undesired products. However, the surface sites are blocked when the acidity is too high and there exists an optimum value for the ratio of total acidic and basic sites to be an efficient catalyst in the targeted reaction. A mixed-metal oxide consisting of Zn and Fe at a 3:1 atomic ratio was found to be the optimum catalyst with a well-balanced acid−base property. Furthermore, a design of experiments (DoE) approach was used to statistically identify critical reaction parameters and optimize them for the best Zn- and Fe-containing catalysts. These approaches successfully gave insights into the determining material factors for the reaction and afforded excellent EC selectivity (up to 99.6%) with high yield.
Áreas temáticas: Química Materiais Interdisciplinar General chemistry Engenharias ii Ciências agrárias i Chemistry, physical Chemistry (miscellaneous) Chemistry (all) Catalysis Astronomia / física
Acceso a la licencia de uso: https://creativecommons.org/licenses/by/3.0/es/
Direcció de correo del autor: francesc.medina@urv.cat
Identificador del autor: 0000-0002-3111-1542
Fecha de alta del registro: 2024-07-20
Versión del articulo depositado: info:eu-repo/semantics/publishedVersion
Enlace a la fuente original: https://pubs.acs.org/doi/10.1021/acscatal.5b01575
URL Documento de licencia: http://repositori.urv.cat/ca/proteccio-de-dades/
Referencia al articulo segun fuente origial: Acs Catalysis. 5 (11): 6284-6295
Referencia de l'ítem segons les normes APA: Fakhrnasova, Dina; Chimentao, Ricardo J.; Medina, Francisco; Urakawa, Atsushi; (2015). Rational and statistical approaches in enhancing yield of ethylene carbonate in urea transesterification with ethylene glycol over metal oxides. Acs Catalysis, 5(11), 6284-6295. DOI: 10.1021/acscatal.5b01575
DOI del artículo: 10.1021/acscatal.5b01575
Entidad: Universitat Rovira i Virgili
Año de publicación de la revista: 2015
Tipo de publicación: Journal Publications
Repositori URV