Special Issue "Sustainable Catalytic Conversion of Biomass for the Production of Biofuels and Bioproducts"

A special issue of Catalysts (ISSN 2073-4344). This special issue belongs to the section "Biomass Catalysis".

Deadline for manuscript submissions: 31 December 2019.

Special Issue Editors

Guest Editor
Dr. Gabriel Morales Website E-Mail
Chemical and Environmental Engineering Group, Universidad Rey Juan Carlos, Mostoles, Spain
Interests: catalysis; bioproducts; biofuels; biomass conversion
Guest Editor
Dr. Jose Iglesias Website E-Mail
Chemical and Environmental Engineering Group, Universidad Rey Juan Carlos, Mostoles, Spain
Interests: catalysis; bioproducts; biofuels; biomass conversion
Guest Editor
Prof. Juan A. Melero Website E-Mail
Chemical and Environmental Engineering Group, Universidad Rey Juan Carlos, Mostoles, Spain
Interests: catalysis, bioproducts, biofuels, biomass conversion

Special Issue Information

Dear Colleagues,

Biomass is widely considered a potential alternative to dwindling fossil fuel reserves. There is a large variety of biomass sources (oleaginous, lignocellulosic, algae, etc.), with many possible conversion routes and products, and currently it is, not just viewed as a source of biofuels, but also as an interesting feedstock for the production of bio-based chemicals that could largely replace petrochemicals. In this context, the search for new sustainable and efficient alternatives to fossil sources is gaining increasing relevance within the chemical industry, wherein the role of catalysis is often critical for the development of clean and sustainable processes, aiming to the production of commodity chemicals or liquid fuels with a high efficiency and atom economy. 

This Special Issue embraces original research papers, reviews and commentaries focused on the current challenges in the catalytic valorization and conversion of biomass sources. Submissions are welcome especially, though not exclusively, in the following areas: 

  • Fundamentals and applied catalysis in the context of biorefineries.
  • Catalytic routes for direct polysaccharides, lignin, and raw biomass transformation.
  • Catalytic transformation of lignocellulosic platform chemicals.
  • Catalytic transformation of vegetable oils, fats, algae and oleaginous chemicals.
  • Catalytic upgrading technologies for bio-oils.
  • Modeling aspects of the processes and mechanistic studies.
  • Molecular insights in processing of biomass.
  • Development of analytic tools, in situ characterization techniques.

Dr. Gabriel Morales
Dr. Jose Iglesias
Prof. Juan A. Melero
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All papers will be peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Catalysts is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 1600 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • Biomass conversion
  • Catalysis
  • Lignocellulose
  • Platform molecules
  • Vegetable oils
  • Biofuels
  • Bioproducts
  • Biorefinery processes

Published Papers (4 papers)

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Research

Open AccessFeature PaperArticle
C-O Bond Hydrogenolysis of Aqueous Mixtures of Sugar Polyols and Sugars over ReOx-Rh/ZrO2 Catalyst: Application to an Hemicelluloses Extracted Liquor
Catalysts 2019, 9(9), 740; https://doi.org/10.3390/catal9090740 - 31 Aug 2019
Abstract
The recovery and upgrade of hemicelluloses, a family of heteropolysaccharides in wood, is a key step to making lignocellulosic biomass conversion a cost-effective sustainable process in biorefinery. The comparative selective catalytic C-O bond hydrogenolysis of C5-C6 polyols, sugars, and their mixtures for the [...] Read more.
The recovery and upgrade of hemicelluloses, a family of heteropolysaccharides in wood, is a key step to making lignocellulosic biomass conversion a cost-effective sustainable process in biorefinery. The comparative selective catalytic C-O bond hydrogenolysis of C5-C6 polyols, sugars, and their mixtures for the production of valuable C6 and C5 deoxygenated products was studied at 200 °C under 80 bar H2 over ReOx-Rh/ZrO2 catalysts. The sugars were rapidly converted to the polyols or converted into their hydrogenolysis products. Regardless of the reactants, C-O bond cleavage occurred significantly via multiple consecutive deoxygenation steps and led to the formation of linear deoxygenated C6 or C5 polyols. The distribution of products depended on the nature of the substrate and C-C bond scission was more important from monosaccharides. In addition, we demonstrated effective hydrogenolysis of a hemicellulose-extracted liquor from delignified maritime pine containing monosaccharides and low MW oligomers. Compared with the sugar-derived polyols, the mono- and oligosaccharides in the liquor were more rapidly converted to hexanediols or pentanediols. C-O bond scission was significant, giving a yield of desired deoxygenated products as high as 65%, higher than in the reaction of the synthetic mixture of glucose/xylose of the same C6/C5 sugar ratio (yield of 30%). Full article
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Open AccessArticle
Waste Seashells as a Highly Active Catalyst for Cyclopentanone Self-Aldol Condensation
Catalysts 2019, 9(8), 661; https://doi.org/10.3390/catal9080661 - 01 Aug 2019
Abstract
For the first time, waste-seashell-derived CaO catalysts were used as high-performance solid base catalysts for cyclopentanone self-condensation, which is an important reaction in bio-jet fuel or perfume precursor synthesis. Among the investigated seashell-derived catalysts, Scapharca Broughtonii-derived CaO catalyst (S-shell-750) exhibited the highest [...] Read more.
For the first time, waste-seashell-derived CaO catalysts were used as high-performance solid base catalysts for cyclopentanone self-condensation, which is an important reaction in bio-jet fuel or perfume precursor synthesis. Among the investigated seashell-derived catalysts, Scapharca Broughtonii-derived CaO catalyst (S-shell-750) exhibited the highest dimer yield (92.1%), which was comparable with commercial CaO (88.2%). The activity sequence of different catalysts was consistent with the CaO purity sequence and contact angle sequence. X-ray diffraction (XRD) results showed that CaCO3 in waste shell were completely converted to CaO after calcination at 750 °C or above for 4 h. CO2 temperature-programmed desorption (CO2-TPD) results indicate that both the amount and strength of base sites increase significantly when the calcination temperature climbs to 750 °C. Therefore, we can attribute the excellent performance of S-shell-750/850/950 catalysts to the higher CaO content, relatively low hydrophilicity, and stronger acidity and basicity of this catalyst. This study developed a new route for waste shell utilization in bio-derived ketone aldol condensation. Full article
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Open AccessArticle
Evaluation on the Methane Production Potential of Wood Waste Pretreated with NaOH and Co-Digested with Pig Manure
Catalysts 2019, 9(6), 539; https://doi.org/10.3390/catal9060539 - 17 Jun 2019
Abstract
Wood waste generated during the tree felling and processing is a rich, green, and renewable lignocellulosic biomass. However, an effective method to apply wood waste in anaerobic digestion is lacking. The high carbon to nitrogen (C/N) ratio and rich lignin content of wood [...] Read more.
Wood waste generated during the tree felling and processing is a rich, green, and renewable lignocellulosic biomass. However, an effective method to apply wood waste in anaerobic digestion is lacking. The high carbon to nitrogen (C/N) ratio and rich lignin content of wood waste are the major limiting factors for high biogas production. NaOH pre-treatment for lignocellulosic biomass is a promising approach to weaken the adverse effect of complex crystalline cellulosic structure on biogas production in anaerobic digestion, and the synergistic integration of lignocellulosic biomass with low C/N ratio biomass in anaerobic digestion is a logical option to balance the excessive C/N ratio. Here, we assessed the improvement of methane production of wood waste in anaerobic digestion by NaOH pretreatment, co-digestion technique, and their combination. The results showed that the methane yield of the single digestion of wood waste was increased by 38.5% after NaOH pretreatment compared with the untreated wood waste. The methane production of the co-digestion of wood waste and pig manure was higher than that of the single digestion of wood waste and had nonsignificant difference with the single-digestion of pig manure. The methane yield of the co-digestion of wood waste pretreated with NaOH and pig manure was increased by 75.8% than that of the untreated wood waste. The findings indicated that wood waste as a sustainable biomass source has considerable potential to achieve high biogas production in anaerobic digestion. Full article
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Open AccessArticle
Effect of Dilute Acid and Alkali Pretreatments on the Catalytic Performance of Bamboo-Derived Carbonaceous Magnetic Solid Acid
Catalysts 2019, 9(3), 245; https://doi.org/10.3390/catal9030245 - 07 Mar 2019
Abstract
Lignocellulose is a widely used renewable energy source on the Earth that is rich in carbon skeletons. The catalytic hydrolysis of lignocellulose over magnetic solid acid is an efficient pathway for the conversion of biomass into fuels and chemicals. In this study, a [...] Read more.
Lignocellulose is a widely used renewable energy source on the Earth that is rich in carbon skeletons. The catalytic hydrolysis of lignocellulose over magnetic solid acid is an efficient pathway for the conversion of biomass into fuels and chemicals. In this study, a bamboo-derived carbonaceous magnetic solid acid catalyst was synthesized by FeCl3 impregnation, followed by carbonization and –SO3H group functionalization. The prepared catalyst was further subjected as the solid acid catalyst for the catalytic conversion of corncob polysaccharides into reducing sugars. The results showed that the as-prepared magnetic solid acid contained –SO3H, –COOH, and polycyclic aromatic, and presented good catalytic performance for the hydrolysis of corncob in the aqueous phase. The concentration of H+ was in the range of 0.6487 to 2.3204 mmol/g. Dilute acid and alkali pretreatments of raw material can greatly improve the catalytic activity of bamboo-derived carbonaceous magnetic solid acid. Using the catalyst prepared by 0.25% H2SO4-pretreated bamboo, 6417.5 mg/L of reducing sugars corresponding to 37.17% carbohydrates conversion could be obtained under the reaction conditions of 120 °C for 30 min. Full article
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Planned Papers

The below list represents only planned manuscripts. Some of these manuscripts have not been received by the Editorial Office yet. Papers submitted to MDPI journals are subject to peer-review.

Title: 5-Chloromethylfurfural production from glucose: A pioneer kinetic model development exploring the mechanism 
Authors: Amal J. Chennattussery, Ajit Haridas, Churchil A. Antonyraj*
Affiliation: CSIR-National Institute for Interdisciplinary Science and Technology. Thiruvananthapuram PIN: 695019
E-mail: [email protected]
Abstract: Conversion of glucose to 5-chloromethylfurfural (CMF) is one of the well-known high yield unit processes for the ligno-cellulosic biomass valorization. Owing to the complexity in quantification of CMF, an experimental kinetic modeling study has to understand the mechanism never been reported for this reaction. Herein we have been successful in developing a rapid, sensitive, specific, reverse phase HPLC method to quantify generated CMF (range: 10 µg/mL - 650 µg/mL) in the dichloroethane (DCE) solvent. The Box-Behnken design of experiment (DOE) approach was used for the statistical optimization and kinetic model was developed based on the homogeneous first-order kinetics and the results are in good agreement with the experiment data. The mechanism of CMF formation glucose and HCl were modeled first time using a serial parallel reaction mechanism. The apparent activation energy (Ea) for glucose decomposition and CMF formation are 86 and 17 kJ/mol respectively.

Title: C-O hydrogenolysis of sugar polyols and sugars using ReOx-Rh/ZrO2 catalyst. Application to mixtures and to a hemicellulose extraction liquor
Authors: Michèle Besson [email protected]; Noemie Perret [email protected]; Catherine Pinel <[email protected]>
Abstract: Appropriate utilization of abundant hemicelluloses to prepare valuable chemicals is a key step in order to make lignocellulosic biomass conversion a cost effective process in a biorefinery. Catalytic hydrogenolysis of aqueous solutions of C5-C6 sugar polyols and sugars, alone or in different compositions, to linear deoxygenated polyols were compared over ReOx-Rh/ZrO2. The hydrogenolysis of an hemicellulose liquor extracted from maritime pine was then performed.

Title: "Mini-review of in situ methods of catalyst characterisation relevant to biomass transformations"
Description: This paper focused on in-situ methods of acid and base characterisation that move beyond conventional NH3 and CO2 titration.

Tentative title: Sulfonated hydrothermal carbons as catalysts for glycerol ketalization
Authors: Pablo Fernándeza, José M. Fraileb, Enrique García-Bordejéc, Raúl Grimaa, Elísabet Pires*a,b
Affiliations: a Departamento de Química Orgánica. Facultad de Ciencias. Universidad de Zaragoza. C/ Pedro Cerbuna, 12. E-50009 Zaragoza, Spain
b Instituto de Síntesis Química y Catálisis Homogénea (ISQCH). CSIC-Universidad de Zaragoza. C/ Pedro Cerbuna, 12. E-50009 Zaragoza, Spain
c Instituto de Carboquímica (ICB-CSIC). C/ Miguel Luesma Castán 4. E-50018 Zaragoza, Spain
Abstract: The substitution of conventional solvents in industrial processes and different applications is a relevant topic nowadays in order to overcome some of their main drawbacks, such as their (eco)toxicity, volatility or flammability. Among the different proposals, the use of glycerol and its derivatives as renewable solvents has attracted a great attention in the last decade1,2 and in particular glycerol carbonate3 and solketal4 can be considered the most popular glycerol derived solvents up to now.

In order to envisage the possibility of producing large amounts of solketal, a sustainable synthetic methodology must be developed and thus many works have been published so far related to the study of different catalytic systems for the reaction of glycerol with acetone.5

text

Scheme 1: Synthesis of solketal

Many efforts have been devoted in searching efficient heterogeneous catalysts for this reaction, as the use of homogeneous acid catalysts implies a work-up of the reaction that derives in a large transfer of the ketal to the aqueous phase, and thus a seriously lowering of the global isolated ketal yield.
Over the different catalytic systems, sulfonic solids such as Amberlyst 156 or SBA-157 have been described as effective catalysts for solketal production. An interesting point when developing sustainable processes is the possibility of using heterogeneous catalysts coming also from renewable raw materials. This is the case of carbons. Thus sulfonated activated carbon8 and hydrothermal carbon prepared from glycerine as biodiesel waste9 have been proposed as catalysts in the reaction of glycerol and acetone.
In this work, we present the study of the synthesis of solketal catalyzed by sulfonated hydrothermal carbons. Hydrothermal carbons from glucose and cellulose have been prepared with different textural properties depending on the hydrothermal treatment conditions.10 Sulfonation of these carbons provides active catalysts for the synthesis of solketal, Thus, up to nine different sulfonated carbons have been tested, their activity has been compared with sulfonic resins such as Amberlyst 15, Dowex 50W×2 or SAC13.
The study of the recoverability of the solids will be also presented. In this case, an influence of the preparation parameters of the catalyst on the activity of the solids upon reuse has been observed.

Title: Clean up and Conversion of Biomass Liquefaction Aqueous Phase to Olefins over ZnxZryOz Catalyst
Authors: Robert A Dagle [email protected], Stephen D Davidson [email protected]
Abstract: The viability of using a previously studied ZnxZryOz catalyst for the direct production of olefins from aqueous phase bio-oil feedstocks was explored. In this work, we looked at three different bio-mass derived aqueous phases: hydrothermal liquefaction of cornstover (PNNL), fluidized bed fast pyrolysis of horse litter (USDA), and screw pyrolysis of wood pellets (KIT). While overall composition varied for each feedstock, the main components for each were the carboxylic acids: acetic acid and propionic acid. Expanding on a previously reported clean-up process, a continuous liquid-liquid extraction process was developed instead of a batch process. Complete conversion of the carboxylic acids over the ZnxZryOz catalyst was achieved for all feedstocks. The main product for all feedstocks was isobutene, followed by CO2. The effect of gas environment was also studied. By changing the carrier gas from N2 to H2, the selectivity to propene was increased while selectivity to isobutene decreased.

Tentative title: Kinetics of enzymatic esterification of mammalian fat for acidity reduction

Authors: António A. Martins, Soraia Andrade, Daniela Correia, Elisabete Matos, Nídia S. Caetano, Teresa M. Mata

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