Lignocellulosic residues as catalysts for CO 2 fixation: complementary experimental and computational approaches
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ORIGINAL RESEARCH
Lignocellulosic residues as catalysts for CO2 fixation: complementary experimental and computational approaches Mohamed Said El Ouahabi . Md Bin Yeamin . Raquel Rivas . Farid El Guemmout . Mar Reguero . Anna M. Masdeu-Bulto´ . Ali Aghmiz
Received: 21 March 2020 / Accepted: 8 October 2020 Ó Springer Nature B.V. 2020
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
Electronic supplementary material The online version of this article (https://doi.org/10.1007/s10570-020-03522-x) contains supplementary material, which is available to authorized users. M. S. El Ouahabi M. B. Yeamin R. Rivas M. Reguero (&) A. M. Masdeu-Bulto´ (&) Department Physical and Inorganic Chemistry, University Rovira i Virgili, Marcellı´ Domingo, s/n, 43007 Tarragona, Spain e-mail: [email protected]
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).
A. M. Masdeu-Bulto´ e-mail: [email protected] M. S. El Ouahabi F. El Guemmout A. Aghmiz (&) De´partement de Chimie, Faculte´ des Sciences, University Abdelmalek Essaadi, M’hannech II, B.P. 2121, 93030 Te´touan, Morocco e-mail: [email protected] Present Address: M. B. Yeamin IUBAT University, Sector-10, Model Town Uttara, Dhaka 1230, Bangladesh
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Cellulose
Graphic abstract
Keywords Carbon dioxide Carbonates Lignocellulosic materials Epoxides DFT calculations
Introduction Biomass is a combination of naturally derived materials originating from plants such as shrubs, trees, algae, crops, as well as all the materials composed of organic matrix. It is a sustainable source of chemicals (Corma et al. 2007) and renewable energy carriers. The use of biomass biofuels avoids the increase in atmospheric carbon dioxide since the plants use it to generate more biomass (Tursi 2019). Biomass has a huge potential as
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