Articles producció científica> Química Física i Inorgànica

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

  • Dades identificatives

    Identificador: imarina:9002817
    Autors:
    El Ouahabi MSYeamin MBRivas REl Guemmout FReguero MMasdeu-Bultó AMAghmiz A
    Resum:
    © 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.]
  • Altres:

    e-ISSN: 1572-882X
    Codi de projecte: CTQ2016-75016-R
    Paraules clau: Propylene-oxide Lignocellulosic materials Epoxides Dft calculations Cycloaddition Cyclic carbonates Conversion Co2 Chemical fixation Carbonates Carbon-dioxide Carbon dioxide Biomass Base catalysts
    Data d'alta del registre: 2024-07-27
    Versió de l'article dipositat: info:eu-repo/semantics/acceptedVersion
    URL Document de llicència: https://repositori.urv.cat/ca/proteccio-de-dades/
    Referència a l'article segons font original: Cellulose. 28 (1): 359-375
    Referència 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
    Acrònim: ECO2VALCAT
    Tipus de publicació: Journal Publications
    Autor segons l'article: El Ouahabi MS; Yeamin MB; Rivas R; El Guemmout F; Reguero M; Masdeu-Bultó AM; Aghmiz A
    Departament: Química Física i Inorgànica
    Autor/s de la URV: Aghmiz, Ali / Masdeu Bultó, Anna Maria / Reguero de la Poza, Maria del Mar / Rivas Del Valle, Raquel / Yeamin, MD Bin
    Resum: © 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.]
    Àrees temàtiques: 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
    Accès a la llicència d'ús: https://creativecommons.org/licenses/by/3.0/es/
    ISSN: 0969-0239
    Adreça de correu electrònic de l'autor: ali.aghmiz@urv.cat raquel.rivas@urv.cat raquel.rivas@urv.cat annamaria.masdeu@urv.cat mar.reguero@urv.cat
    Identificador de l'autor: 0000-0002-2007-7481 0000-0002-2007-7481 0000-0001-7938-3902 0000-0001-9668-8265
    Enllaç font original: https://www.springerprofessional.de/en/lignocellulosic-residues-as-catalysts-for-co2-fixation-complemen/18494140
    Programa de finançament: PROGRAMA ESTATAL DE INVESTIGACIÓN, DESARROLLO E INNOVACIÓN ORIENTADA A LOS RETOS DE LA SOCIEDAD
    DOI de l'article: 10.1007/s10570-020-03522-x
    Entitat: Universitat Rovira i Virgili
    Any de publicació de la revista: 2021
    Acció del programa de finançament: VALORIZACION EFICIENTE DE CO2 A COMBUSTIBLES Y COMPUESTOS DE ALTO VALOR AÑADIDO MEDIANTE CATALISIS HOMOGENEA Y NANO-CATALISIS
  • Paraules clau:

    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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