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Catalytic Biomass to Renewable Biofuels and Biomaterials

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

Deadline for manuscript submissions: closed (31 December 2019) | Viewed by 47613

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Prof. Dr. Zhen Fang

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Guest Editor

Biomass Group, College of Engineering, Nanjing Agricultural University, 40 Dianjiangtai Road, Nanjing 210031, China
Interests: nanocatalysts; conversion of biomass; thermo-chemical conversion; biomaterials
Special Issues, Collections and Topics in MDPI journals

Dr. Yi-Tong Wang

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Guest Editor

School of Metallurgy and Energy, North China University of Science and Technology, 21 Bohai Avenue, Tangshan, Hebei, China
Interests: acid-base catalysis; biomass conversion; biodiesel; magnetic catalyst

Special Issue Information

Dear Colleagues,

Renewable, clean and environmentally friendly biofuels and biomaterials applications are in line with the healthy development of the world's energy and materials in the future. Biomass as the only renewable carbon source on Earth has been proposed as an ideal alternative to fossil resources and can be catalytically conversed to valuable products, such as hydrolysis of lignocellulosic wastes, synthesis of biodiesel and bioethanol, thermal conversions of biomass and organic wastes and so on. This special issue receives original research papers focused on biomass catalytic conversion to renewable biofuels and biomaterials. Submissions are welcome especially (but not exclusively) in the following areas:

Catalysis;
Bio-catalysis;
Biodiesel;
Nano-cellulose;
Chemicals;
Gaseous and liquid biofuels;
Biogas;
Ethanol;
Butanol;
Green chemistry;

Prof. Zhen Fang
Dr. Yi-Tong Wang
Guest Editors

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Keywords

Hydrolysis and pyrolysis of biomass wastes
Biofuels production
Biomass conversion
Biomaterials synthesis
Novel catalysts synthesis for biomass conversion

Published Papers (12 papers)

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Editorial

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3 pages, 166 KiB

Open AccessEditorial

Catalytic Biomass to Renewable Biofuels and Biomaterials

by Yi-Tong Wang and Zhen Fang

Catalysts 2020, 10(5), 480; https://0-doi-org.brum.beds.ac.uk/10.3390/catal10050480 - 28 Apr 2020

Cited by 2 | Viewed by 2627

Abstract

As the only renewable carbon source, biomass can be converted into biofuels, chemicals, and biomaterials, such as ethanol, butanol, glucose, furfural, biochar, and bio-oils, and is considered as a substitute for fossil oil [...] Full article

(This article belongs to the Special Issue Catalytic Biomass to Renewable Biofuels and Biomaterials)

Research

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16 pages, 2983 KiB

Open AccessArticle

Experimental Design to Improve Cell Growth and Ethanol Production in Syngas Fermentation by Clostridium carboxidivorans

by Carolina Benevenuti, Alanna Botelho, Roberta Ribeiro, Marcelle Branco, Adejanildo Pereira, Anna Carolyna Vieira, Tatiana Ferreira and Priscilla Amaral

Catalysts 2020, 10(1), 59; https://0-doi-org.brum.beds.ac.uk/10.3390/catal10010059 - 01 Jan 2020

Cited by 15 | Viewed by 3505

Abstract

Fermentation of gases from biomass gasification, named syngas, is an important alternative process to obtain biofuels. Sequential experimental designs were used to increase cell growth and ethanol production during syngas fermentation by Clostridium carboxidivorans. Based on ATCC (American Type Culture Collection) 2713 medium composition, it was possible to propose a best medium composition for cell growth, herein called TYA (Tryptone-Yeast extract-Arginine) medium and another one for ethanol production herein called TPYGarg (Tryptone-Peptone-Yeast extract-Glucose-Arginine) medium. In comparison to ATCC^® 2713 medium, TYA increased cell growth by 77%, reducing 47% in cost and TPYGarg increased ethanol production more than four-times, and the cost was reduced by 31%. In 72 h of syngas fermentation in TPYGarg medium, 1.75-g/L of cells, 2.28 g/L of ethanol, and 0.74 g/L of butanol were achieved, increasing productivity for syngas fermentation. Full article

(This article belongs to the Special Issue Catalytic Biomass to Renewable Biofuels and Biomaterials)

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15 pages, 2315 KiB

Open AccessArticle

Glycerol Acetylation Mediated by Thermally Hydrolysed Biosolids-Based Material

by Mattia Bartoli, Chengyong Zhu, Michael Chae and David C. Bressler

Catalysts 2020, 10(1), 5; https://0-doi-org.brum.beds.ac.uk/10.3390/catal10010005 - 18 Dec 2019

Cited by 9 | Viewed by 3257

Abstract

Crude glycerol is the main by-product of many renewable diesel production platforms. However, the process of refining glycerol from this crude by-product stream is very expensive, and thus does not currently compete with alternative processes. The acetylation of glycerol provides an intriguing strategy to recover value-added products that are employable as fuel additives. In this work, the conversion of glycerol to acetyl derivatives was facilitated by a heterogeneous catalyst generated from the thermal hydrolysis of biosolids obtained from a municipal wastewater treatment facility. The reaction was studied using several conditions including temperature, catalyst loading, acetic acid:glycerol molar ratio, and reaction time. The data demonstrate the potential for using two distinct by-product streams to generate fuel additives that can help improve the process economics of renewable diesel production. Full article

(This article belongs to the Special Issue Catalytic Biomass to Renewable Biofuels and Biomaterials)

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20 pages, 3506 KiB

Open AccessArticle

Influence of Base-Catalyzed Organosolv Fractionation of Larch Wood Sawdust on Fraction Yields and Lignin Properties

by Markus Hochegger, Gregor Trimmel, Betty Cottyn-Boitte, Laurent Cézard, Amel Majira, Sigurd Schober and Martin Mittelbach

Catalysts 2019, 9(12), 996; https://0-doi-org.brum.beds.ac.uk/10.3390/catal9120996 - 27 Nov 2019

Cited by 5 | Viewed by 2885

Abstract

Lignocellulose-based biorefineries are considered to play a crucial role in reducing fossil-fuel dependency. As of now, the fractionation is still the most difficult step of the whole process. The objective of this study is to investigate the potential of a base-catalyzed organosolv process as a fractionation technique for European larch sawdust. A solvent system comprising methanol, water, sodium hydroxide as catalyst, and anthraquinone as co-catalyst is tested. The influence of three independent process variables, temperature (443–446 K), catalyst loading (20–30% w/w), and alcohol-to-water ratio (30–70% v/v), is studied. The process conditions were determined using a fractional factorial experiment. One star point (443 K, 30% v/v MeOH, 30% w/w NaOH) resulted in the most promising results, with a cellulose recovery of 89%, delignification efficiency of 91%, pure lignin yield of 82%, residual carbohydrate content of 2.98% w/w, and an ash content of 1.24% w/w. The isolated lignin fractions show promising glass transition temperatures (≥424 K) with high thermal stabilities and preferential O/C and H/C ratios. This, together with high contents of phenolic hydroxyl (≥1.83 mmol/g) and carboxyl groups (≥0.52 mmol/g), indicates a high valorization potential. Additionally, Bjorkman lignin was isolated, and two reference Kraft cooks and a comparison to three acid-catalyzed organosolv fractionations were conducted. Full article

(This article belongs to the Special Issue Catalytic Biomass to Renewable Biofuels and Biomaterials)

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17 pages, 1775 KiB

Open AccessFeature PaperArticle

Ca-based Catalysts for the Production of High-Quality Bio-Oils from the Catalytic Co-Pyrolysis of Grape Seeds and Waste Tyres

by Olga Sanahuja-Parejo, Alberto Veses, José Manuel López, Ramón Murillo, María Soledad Callén and Tomás García

Catalysts 2019, 9(12), 992; https://0-doi-org.brum.beds.ac.uk/10.3390/catal9120992 - 26 Nov 2019

Cited by 26 | Viewed by 3426

Abstract

The catalytic co-pyrolysis of grape seeds and waste tyres for the production of high-quality bio-oils was studied in a pilot-scale Auger reactor using different low-cost Ca-based catalysts. All the products of the process (solid, liquid, and gas) were comprehensively analysed. The results demonstrate that this upgrading strategy is suitable for the production of better-quality bio-oils with major potential for use as drop-in fuels. Although very good results were obtained regardless of the nature of the Ca-based catalyst, the best results were achieved using a high-purity CaO obtained from the calcination of natural limestone at 900 °C. Specifically, by adding 20 wt% waste tyres and using a feedstock to CaO mass ratio of 2:1, a practically deoxygenated bio-oil (0.5 wt% of oxygen content) was obtained with a significant heating value of 41.7 MJ/kg, confirming its potential for use in energy applications. The total basicity of the catalyst and the presence of a pure CaO crystalline phase with marginal impurities seem to be key parameters facilitating the prevalence of aromatisation and hydrodeoxygenation routes over the de-acidification and deoxygenation of the vapours through ketonisation and esterification reactions, leading to a highly aromatic biofuel. In addition, owing to the CO₂-capture effect inherent to these catalysts, a more environmentally friendly gas product was produced, comprising H₂ and CH₄ as the main components. Full article

(This article belongs to the Special Issue Catalytic Biomass to Renewable Biofuels and Biomaterials)

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11 pages, 2209 KiB

Open AccessArticle

Synthesis of Diesel and Jet Fuel Range Cycloalkanes with Cyclopentanone and Furfural

by Wei Wang, Shaoying Sun, Fengan Han, Guangyi Li, Xianzhao Shao and Ning Li

Catalysts 2019, 9(11), 886; https://0-doi-org.brum.beds.ac.uk/10.3390/catal9110886 - 25 Oct 2019

Cited by 16 | Viewed by 4885

Abstract

Diesel and jet fuel range cycloalkanes were obtained in ~84.8% overall carbon yield with cyclopentanone and furfural, which can be produced from hemicellulose. Firstly, 2,5-bis(furan-2-ylmethyl)-cyclopentanone was prepared by the aldol condensation/hydrogenation reaction of cyclopentanone and furfural under solid base and selective hydrogenation catalyst. Over the optimized catalyst (Pd/C-CaO), 98.5% carbon yield of 2,5-bis(furan-2-ylmethyl)-cyclopentanone was acquired at 423 K. Subsequently, the 2,5-bis(furan-2-ylmethyl)-cyclopentanone was further hydrodeoxygenated over the M/H-ZSM-5(Pd, Pt and Ru) catalyst. Overall, 86.1% carbon yield of diesel and jet fuel range cycloalkanes was gained over the Pd/H-ZSM-5 catalyst under solvent-free conditions. The cycloalkane mixture obtained in this work has a high density (0.82 g mL⁻¹) and a low freezing point (241.7 K). Therefore, it can be mixed into diesel and jet fuel to increase their volumetric heat values or payloads. Full article

(This article belongs to the Special Issue Catalytic Biomass to Renewable Biofuels and Biomaterials)

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18 pages, 3752 KiB

Open AccessArticle

Gel-Type and Macroporous Cross-Linked Copolymers Functionalized with Acid Groups for the Hydrolysis of Wheat Straw Pretreated with an Ionic Liquid

by Giulia Lavarda, Silvia Morales-delaRosa, Paolo Centomo, Jose M. Campos-Martin, Marco Zecca and Jose L. G. Fierro

Catalysts 2019, 9(8), 675; https://0-doi-org.brum.beds.ac.uk/10.3390/catal9080675 - 08 Aug 2019

Cited by 13 | Viewed by 2859

Abstract

Several sulfonated cross-linked copolymers functionalized with hydroxyl and carboxylic groups have been synthesized. The amount of the cross-linking monomer was tailored (from 4% up to 40%) to tune the resulting micro- and nano-morphologies, and two types of catalysts, namely, gel-type and macroreticular catalysts, were obtained. These copolymers were employed in the catalytic hydrolysis of wheat straw pretreated in 1-ethyl-3-methylimidazolium acetate to obtain sugars. Remarkably, the presence of additional oxygenated groups enhances the catalytic performances of the polymers by favoring the adsorption of β-(1,4)-glucans and makes these materials significantly more active than an acidic resin bearing only sulfonic groups (i.e., Amberlyst 70). In addition, the structure of the catalyst (gel-type or macroreticular) appears to be a determining factor in the catalytic process. The gel-type structure provides higher glucose concentrations because the morphology in the swollen state is more favorable in terms of the accessibility of the catalytic centers. The observed catalytic behavior suggests that the substrate diffuses within the swollen polymer matrix and indirectly confirms that the pretreatment based on dissolution/precipitation in ionic liquids yields a substantial enhancement of the conversion of lignocellulosic biomass to glucose in the presence of heterogeneous catalysts. Full article

(This article belongs to the Special Issue Catalytic Biomass to Renewable Biofuels and Biomaterials)

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13 pages, 3948 KiB

Open AccessArticle

Role of Humic Acid Chemical Structure Derived from Different Biomass Feedstocks on Fe(III) Bioreduction Activity: Implication for Sustainable Use of Bioresources

by Yuquan Wei, Zimin Wei, Fang Zhang, Xiang Li, Wenbing Tan and Beidou Xi

Catalysts 2019, 9(5), 450; https://0-doi-org.brum.beds.ac.uk/10.3390/catal9050450 - 15 May 2019

Cited by 7 | Viewed by 2399

Abstract

Humic acids (HAs) are redox-active components that play a crucial role in catalyzing relevant redox reactions in various ecosystems. However, it is unclear what role the different compost-derived Has play in the dissimilatory Fe(III) bioreduction and which chemical structures could accelerate Fe reduction. In this study, we compared the effect of eighteen HAs from the mesophilic phase, thermophilic phase and mature phase of protein-, lignocellulose- and lignin-rich composting on catalyzing the bioreduction of Fe(III)-citrate by Shewanella oneidensis MR-1 in temporarily anoxic laboratory systems. The chemical composition and structure of different compost-derived HAs were analyzed by UV–Vis spectroscopy, excitation-emission matrices of the fluorescence spectra, and ¹³C-NMR. The results showed that HAs from lignocellulose- and lignin-rich composting, especially in the thermophilic phase, promoted the bioreduction of Fe(III). They also showed that HA from protein-rich materials suppressed significantly the Fe(II) production, which was mainly affected by the amount and structures of functional groups (e.g., quinone groups) and humification degree of the HAs. This study can aid in searching sustainable HA-rich composts for wide-ranging applications to catalyze redox-mediated reactions of pollutants in soils. Full article

(This article belongs to the Special Issue Catalytic Biomass to Renewable Biofuels and Biomaterials)

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14 pages, 3307 KiB

Open AccessFeature PaperArticle

Selective Production of Terephthalonitrile and Benzonitrile via Pyrolysis of Polyethylene Terephthalate (PET) with Ammonia over Ca(OH)₂/Al₂O₃ Catalysts

by Lujiang Xu, Xin-wen Na, Le-yao Zhang, Qian Dong, Guo-hua Dong, Yi-tong Wang and Zhen Fang

Catalysts 2019, 9(5), 436; https://0-doi-org.brum.beds.ac.uk/10.3390/catal9050436 - 09 May 2019

Cited by 14 | Viewed by 4396

Abstract

A series of Ca(OH)₂/Al₂O₃ catalysts were synthesized for selectively producing N-containing chemicals from polyethylene terephthalate (PET) via catalytic fast pyrolysis with ammonia (CFP-A) process. During the CFP-A process, the carboxyl group in PET plastic was efficiently utilized for the selective production of terephthalonitrile and benzonitrile by controlling the catalysts and pyrolysis parameters (e.g. temperature, residence time, ammonia content). The best conditions were selected as 2% Ca(OH)₂/γ-Al₂O₃ (0.8 g), 500 °C under pure ammonia with 58.3 C% terephthalonitrile yield and 92.3% selectivity in nitriles. In addition, 4% Ca(OH)₂/ Al₂O₃ was suitable for producing benzonitrile. With catalyst dosage of 1.2 g, residence time of 1.87 s, pyrolysis temperature of 650 °C and pure ammonia (160 mL/min carrier gas flow rate), the yield and selectivity of benzonitrile were 30.4 C% and 82.6%, respectively. The catalysts deactivated slightly after 4 cycles. Full article

(This article belongs to the Special Issue Catalytic Biomass to Renewable Biofuels and Biomaterials)

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14 pages, 2596 KiB

Open AccessArticle

Experimental Studies on Co-Combustion of Sludge and Wheat Straw

by Zeyu Xue, Zhaoping Zhong and Bo Zhang

Catalysts 2019, 9(2), 182; https://0-doi-org.brum.beds.ac.uk/10.3390/catal9020182 - 15 Feb 2019

Cited by 13 | Viewed by 2903

Abstract

This work presents studies on the co-combustion of sludge and wheat straw (30 wt % sludge + 70 wt % wheat straw). Prior to the combustion experiment, thermogravimetric analysis was performed to investigate the combustion characteristic of the blended fuel. Results indicated that the blended fuel could remedy the defect of each individual component and also promote the combustion. Co-combustion experiments were conducted in a lab-scale vertical tube furnace and the ash samples were analyzed by Inductively Coupled Plasma Optical Emission Spectrometer (ICP-OES), X-ray Diffraction (XRD), and Scanning Electron Microscope (SEM). Thermodynamic calculations were also made to study the interactions that occurred. Addition of sludge could raise the melting point of wheat straw ash and reduce the slagging tendency. Co-combustion also restrained the release of K and transferred it into aluminosilicate and phosphate. Transfer of Pb and Zn in the co-combustion was also studied. The release and leaching toxicity of the two heavy metals in the co-combustion were weakened effectively by wheat straw. PbCl₂(g) and ZnCl₂(g) could be captured by K₂SiO₃ in wheat straw ash particles and generate silicates. Interactions that possibly occurred between K, Zn, and Pb components were discussed at the end of the paper. Full article

(This article belongs to the Special Issue Catalytic Biomass to Renewable Biofuels and Biomaterials)

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12 pages, 2410 KiB

Open AccessArticle

Carbonate-Catalyzed Room-Temperature Selective Reduction of Biomass-Derived 5-Hydroxymethylfurfural into 2,5-Bis(hydroxymethyl)furan

by Jingxuan Long, Wenfeng Zhao, Yufei Xu, Hu Li and Song Yang

Catalysts 2018, 8(12), 633; https://0-doi-org.brum.beds.ac.uk/10.3390/catal8120633 - 07 Dec 2018

Cited by 19 | Viewed by 4269

Abstract

Catalytic reduction of 5-hydroxymethylfurfural (HMF), deemed as one of the key bio-based platform compounds, is a very promising pathway for the upgrading of biomass to biofuels and value-added chemicals. Conventional hydrogenation of HMF is mainly conducted over precious metal catalysts with high-pressure hydrogen. Here, a highly active, sustainable, and facile catalytic system composed of K₂CO₃, Ph₂SiH₂, and bio-based solvent 2-methyltetrahydrofuran (MTHF) was developed to be efficient for the reduction of HMF. At a low temperature of 25 °C, HMF could be completely converted to 2,5-bis(hydroxymethyl)furan (BHMF) in a good yield of 94% after 2 h. Moreover, a plausible reaction mechanism was speculated, where siloxane in situ formed via hydrosilylation was found to be the key species responsible for the high reactivity. Full article

(This article belongs to the Special Issue Catalytic Biomass to Renewable Biofuels and Biomaterials)

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Review

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37 pages, 2417 KiB

Open AccessReview

Clostridium sp. as Bio-Catalyst for Fuels and Chemicals Production in a Biorefinery Context

by Vanessa Liberato, Carolina Benevenuti, Fabiana Coelho, Alanna Botelho, Priscilla Amaral, Nei Pereira, Jr. and Tatiana Ferreira

Catalysts 2019, 9(11), 962; https://0-doi-org.brum.beds.ac.uk/10.3390/catal9110962 - 15 Nov 2019

Cited by 44 | Viewed by 9383

Abstract

Clostridium sp. is a genus of anaerobic bacteria capable of metabolizing several substrates (monoglycerides, diglycerides, glycerol, carbon monoxide, cellulose, and more), into valuable products. Biofuels, such as ethanol and butanol, and several chemicals, such as acetone, 1,3-propanediol, and butyric acid, can be produced by these organisms through fermentation processes. Among the most well-known species, Clostridium carboxidivorans, C. ragsdalei, and C. ljungdahlii can be highlighted for their ability to use gaseous feedstocks (as syngas), obtained from the gasification or pyrolysis of waste material, to produce ethanol and butanol. C. beijerinckii is an important species for the production of isopropanol and butanol, with the advantage of using hydrolysate lignocellulosic material, which is produced in large amounts by first-generation ethanol industries. High yields of 1,3 propanediol by C. butyricum are reported with the use of another by-product from fuel industries, glycerol. In this context, several Clostridium wild species are good candidates to be used as biocatalysts in biochemical or hybrid processes. In this review, literature data showing the technical viability of these processes are presented, evidencing the opportunity to investigate them in a biorefinery context. Full article

(This article belongs to the Special Issue Catalytic Biomass to Renewable Biofuels and Biomaterials)

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