Articles producció científica> Química Física i Inorgànica

Lignocellulosic residues as catalysts for CO2 fixation: complementary experimental and computational approaches

  • Datos identificativos

    Identificador: imarina:9002817
    Autores:
    El Ouahabi MSYeamin MBRivas REl Guemmout FReguero MMasdeu-Bultó AMAghmiz A
    Resumen:
    © 2020, Springer Nature B.V. Abstract: Lignocellulosic wastes obtained from vegetal residues in combination with nucleophiles were used as catalysts for carbon dioxide fixation in epoxides to form cyclic carbonates. An adequate combination of the residue and the nucleophile was essential to obtain active catalytic systems. The best binary systems were formed by olive bones, grape waste, date pit and corn leaves husk residues with tetrabutylammonium bromide (TBAB). High conversions in the cycloaddition of CO2 to propylene oxide (76–84%) and 1,2-epoxyhexane (68–79%) were achieved at very low nucleophile loading (0.47 mol % respect to the substrate) under mild conditions (95 °C and 10 atm of CO2). The vegetal wastes were stable under catalytic conditions and could be recycled after adequately supporting the nucleophile TBAB in silica gel. The mechanistic computational study carried out with Density Functional Theory calculations on model catalysts describes the contribution of individual lignin and cellulosic components to the experimental substrate conversion into cyclic carbonate. The energy barriers obtained and the experimental data suggest that the contribution of lignin to the total catalytic activity (barrier energy of 9.9 kcal/mol) may be more important than the contribution of cellulose (energy barrier 11.9 kcal/mol). Graphic abstract: [Figure not available: see fulltext.]
  • Otros:

    e-ISSN: 1572-882X
    Código de proyecto: CTQ2016-75016-R
    Palabras clave: Propylene-oxide Lignocellulosic materials Epoxides Dft calculations Cycloaddition Cyclic carbonates Conversion Co2 Chemical fixation Carbonates Carbon-dioxide Carbon dioxide Biomass Base catalysts
    Fecha de alta del registro: 2024-07-27
    Versión del articulo depositado: info:eu-repo/semantics/acceptedVersion
    URL Documento de licencia: https://repositori.urv.cat/ca/proteccio-de-dades/
    Referencia al articulo segun fuente origial: Cellulose. 28 (1): 359-375
    Referencia de l'ítem segons les normes APA: El Ouahabi MS; Yeamin MB; Rivas R; El Guemmout F; Reguero M; Masdeu-Bultó AM; Aghmiz A (2021). Lignocellulosic residues as catalysts for CO2 fixation: complementary experimental and computational approaches. Cellulose, 28(1), 359-375. DOI: 10.1007/s10570-020-03522-x
    Acrónimo: ECO2VALCAT
    Tipo de publicación: Journal Publications
    Autor según el artículo: El Ouahabi MS; Yeamin MB; Rivas R; El Guemmout F; Reguero M; Masdeu-Bultó AM; Aghmiz A
    Departamento: Química Física i Inorgànica
    Autor/es de la URV: Aghmiz, Ali / Masdeu Bultó, Anna Maria / Reguero de la Poza, Maria del Mar / Rivas Del Valle, Raquel / Yeamin, MD Bin
    Resumen: © 2020, Springer Nature B.V. Abstract: Lignocellulosic wastes obtained from vegetal residues in combination with nucleophiles were used as catalysts for carbon dioxide fixation in epoxides to form cyclic carbonates. An adequate combination of the residue and the nucleophile was essential to obtain active catalytic systems. The best binary systems were formed by olive bones, grape waste, date pit and corn leaves husk residues with tetrabutylammonium bromide (TBAB). High conversions in the cycloaddition of CO2 to propylene oxide (76–84%) and 1,2-epoxyhexane (68–79%) were achieved at very low nucleophile loading (0.47 mol % respect to the substrate) under mild conditions (95 °C and 10 atm of CO2). The vegetal wastes were stable under catalytic conditions and could be recycled after adequately supporting the nucleophile TBAB in silica gel. The mechanistic computational study carried out with Density Functional Theory calculations on model catalysts describes the contribution of individual lignin and cellulosic components to the experimental substrate conversion into cyclic carbonate. The energy barriers obtained and the experimental data suggest that the contribution of lignin to the total catalytic activity (barrier energy of 9.9 kcal/mol) may be more important than the contribution of cellulose (energy barrier 11.9 kcal/mol). Graphic abstract: [Figure not available: see fulltext.]
    Áreas temáticas: Zootecnia / recursos pesqueiros Química Polymers and plastics Polymer science Odontología Medicina ii Materials science, textiles Materials science, paper & wood Materiais Interdisciplinar Farmacia Engenharias iv Engenharias iii Engenharias ii Engenharias i Ciências biológicas ii Ciências biológicas i Ciências ambientais Ciências agrárias i Ciência de alimentos Biotecnología Biodiversidade Astronomia / física
    Acceso a la licencia de uso: https://creativecommons.org/licenses/by/3.0/es/
    ISSN: 0969-0239
    Direcció de correo del autor: ali.aghmiz@urv.cat raquel.rivas@urv.cat raquel.rivas@urv.cat annamaria.masdeu@urv.cat mar.reguero@urv.cat
    Identificador del autor: 0000-0002-2007-7481 0000-0002-2007-7481 0000-0001-7938-3902 0000-0001-9668-8265
    Enlace a la fuente original: https://www.springerprofessional.de/en/lignocellulosic-residues-as-catalysts-for-co2-fixation-complemen/18494140
    Programa de financiación: PROGRAMA ESTATAL DE INVESTIGACIÓN, DESARROLLO E INNOVACIÓN ORIENTADA A LOS RETOS DE LA SOCIEDAD
    DOI del artículo: 10.1007/s10570-020-03522-x
    Entidad: Universitat Rovira i Virgili
    Año de publicación de la revista: 2021
    Acción del progama de financiación: VALORIZACION EFICIENTE DE CO2 A COMBUSTIBLES Y COMPUESTOS DE ALTO VALOR AÑADIDO MEDIANTE CATALISIS HOMOGENEA Y NANO-CATALISIS
  • Palabras clave:

    Materials Science, Paper & Wood,Materials Science, Textiles,Polymer Science,Polymers and Plastics
    Propylene-oxide
    Lignocellulosic materials
    Epoxides
    Dft calculations
    Cycloaddition
    Cyclic carbonates
    Conversion
    Co2
    Chemical fixation
    Carbonates
    Carbon-dioxide
    Carbon dioxide
    Biomass
    Base catalysts
    Zootecnia / recursos pesqueiros
    Química
    Polymers and plastics
    Polymer science
    Odontología
    Medicina ii
    Materials science, textiles
    Materials science, paper & wood
    Materiais
    Interdisciplinar
    Farmacia
    Engenharias iv
    Engenharias iii
    Engenharias ii
    Engenharias i
    Ciências biológicas ii
    Ciências biológicas i
    Ciências ambientais
    Ciências agrárias i
    Ciência de alimentos
    Biotecnología
    Biodiversidade
    Astronomia / física
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