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Liquefaction of Biomass and Upgrading of Bio-Oil: a Review

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Liquefaction of Biomass and Upgrading of Bio-Oil: a Review molecules Review Liquefaction of Biomass and Upgrading of Bio-Oil: A Review Shiqiu Zhang 1,2, Xue Yang 1,2, Haiqing Zhang 1,2, Chunli Chu 1,2, Kui Zheng 3, Meiting Ju 1,2,* and Le Liu 1,2,* 1 College of Environmental Science and Engineering, Nankai University, Jinnan District, Tianjin 300350, China; [email protected] (S.Z.); [email protected] (X.Y.); [email protected] (H.Z.); [email protected] (C.C.) 2 Tianjin Engineering Research Center of Biomass Solid Waste Resources Technology, Nankai University, Jinnan District, Tianjin 300350, China 3 Analytical and Testing Center, Southwest University of Science and Technology, Mianyang 621010, China; [email protected] * Correspondence: [email protected] (M.J.); [email protected] (L.L.); Tel.: +86-138-2098-8813 (M.T.J.); +86-136-7203-1215 (L.L.) Academic Editors: Jalel Labidi and Xabier Erdocia Received: 22 May 2019; Accepted: 14 June 2019; Published: 17 June 2019 Abstract: The liquefaction of biomass is an important technology to converse the biomass into valuable biofuel. The common technologies for liquefaction of biomass are indirect liquefaction and direct liquefaction. The indirect liquefaction refers to the Fischer–Tropsch (F–T) process using the syngas of biomass as the raw material to produce the liquid fuel, including methyl alcohol, ethyl alcohol, and dimethyl ether. The direct liquefaction of biomass refers to the conversion biomass into bio-oil, and the main technologies are hydrolysis fermentation and thermodynamic liquefaction. For thermodynamic liquefaction, it could be divided into fast pyrolysis and hydrothermal liquefaction. In addition, this review provides an overview of the physicochemical properties and common upgrading methods of bio-oil. Keywords: review; biomass; liquefaction; bio-oil; upgrading 1. Introduction Fossil fuels, such as coal, oil, and natural gas, are non-renewable resources. They play a vital role in human life and social progress. Although, the total amount of fossil fuels on the earth would meet the needs of human beings for several decades, these non-renewable fossil fuels would eventually run out [1]. In addition, the excessive emission of greenhouse gases (such as CO, CO2, NOx, SOx, and CH4) into the atmosphere makes the global climate uncontrollable with the consumption of fossil fuels [2]. Hence, the renewable fuels (nuclear energy, solar energy, wind energy, and biomass energy) should be further developed [3,4]. Biomass has a high utilization potential and is one of the most important energy sources of the future. Generally, biomass is usually grouped as follows [5–7]: (1) Agricultural and forestry residues, (2) herbaceous crops, (3) aquatic and marine biomass, and (4) wastes. Biomass waste means the materials generated in the process of production or consumption of biomass, including wood, straw, animal dungs, and household garbage. Lignocellulose is a complex structure (Figure1a), which is composed of a mixture of cellulose (Figure1b), hemicellulose (Figure1c), lignin (Figure1d), and inorganic components. Cellulose and hemicellulose are tightly bound to lignin mainly by hydrogen and covalent bonds. Cellulose is usually represented by (C6H10O5)n, and the polymerization degree of the long polysaccharide chain is approximately 10,000, resulting in a high molecular weight (>500,000). Molecules 2019, 24, 2250; doi:10.3390/molecules24122250 www.mdpi.com/journal/molecules Molecules 2019, 24, 2250 2 of 30 Molecules 2019,, 24,, xx FORFOR PEERPEER REVIEWREVIEW 2 of 29 Cellulose is formed by the β-1,4 glycosidic linkage of D-glucopyranose units. For hemicellulose, the contenthemicellulose, in dry biomass the content is usually in dry about biomass 25%, is andusuall it isy aabout low degree 25%, and of amorphous it is a low degree heteropolysaccharide of amorphous withheteropolysaccharide high degree branching with ofhigh a straight-chain degree branching skeleton. of a The straight-chain basic units in skeleton. hemicellulose The basic are xylan units and in gulucomannan.hemicellulose are Lignin xylan is anand amorphous gulucomannan. aromatic Lignin natural is polymer,an amorph whichous isaromatic linked primarily natural polymer, via ether bondswhich withis linked hydroxyl primarily and methoxyvia ether groups.bonds with The hydroxyl solubility and of lignin methoxy in water groups. is very The low. solubility The main of lignin roles ofin ligninwater inis avery plant low. are asThe follows: main roles Strengthen of lignin their in structure,a plant are regulate as follows: the flow Strengthen of fluids, their protect structure, against microorganisms,regulate the flow andof fluids, store protect energy. against As we know,microorganisms, biomass energy and store is the energy. exclusive As renewablewe know, biomass organic carbonenergy resourceis the exclusive to produce renewable liquid fuels. organic Biomass carbon is the resource renewable to produce organic materials.liquid fuels. While Biomass the biomass is the wasterenewable still belongs organic to materials. the macroscopic While the category biomass of biomass. waste still According belongs toto thethe statistics, macroscopic the total category amount of ofbiomass. biomass According waste could to reachthe statistics, 2 109 tthe/Y. Nevertheless,total amount onlyof biomass about 40% waste of biomasscould reach waste 2 is× used109 t/Y. for × fuel,Nevertheless, building materials,only about feed, 40% and of biomass power generation, waste is us anded for the fuel, residual building parts materials, are treated feed, in an and extensive power mode,generation, for instance and the incineration, residual parts landfill, are treated and centralized in an extensive stacking, mode, resulting for instance in a waste incineration, of resources landfill, and seriousand centralized pollution stacking, of the environment. resulting in a Therefore, waste of resources it is the key and component serious pollution of sustainable of the environment. development forTherefore, biomass it wasteis the key resources. component Recently, of sustainable the mainly development technologies for of biomass the utilization waste ofresources. biomass Recently, resource arethe physical,mainly technologies thermochemical, of the and utilization biological. of Consideringbiomass resource the type are ofphysical, products, thermochemical, it could be divided and intobiological. gasification, Considering liquefaction, the type biorefinery, of products, and combustion.it could be divi Figureded2 showsinto gasification, the current liquefaction, conversion technologiesbiorefinery, and of biomass.combustion. For Figure the dry 2 biomass,shows the the curre primarynt conversion pathways technologi are combustion,es of biomass. gasification, For the anddry liquefaction.biomass, the Moreover,primary pathways the products are ofcombustion, gasification gasification, of biomass couldand liquefaction. also be conversed Moreover, to liquid the products.products of For gasification the wet biomass, of biomass the primarycould also pathways be conversed are hydrolysis to liquid products. fermentation, For the biorefinery, wet biomass, and liquefaction.the primary pathways The products are ofhydrolysis biomass conversionfermentation, are biorefinery, abundant, including and liquefac syngas,tion. bio-oil,The products biodiesel, of methylbiomass alcohol, conversion ethyl are alcohol, abundant, etc. including syngas, bio-oil, biodiesel, methyl alcohol, ethyl alcohol, etc. Figure 1.1. (a(a) )Structure Structure of of plant plant cell cell walls walls [8]; [8]; ( (bb)) structure structure of of cellulose [9]; [9]; ( (c)) basic unitsunits ofof hemicellulose [[9];9]; andand ((dd)) simplesimple structurestructure ofof ligninlignin [[9]9]... Figure 2. Current conversion technologies of biomass. Figure 2. Current conversion technologies of biomass. This review paper aims to provide a solution of the current liquefaction technologies of biomass, including indirect liquefaction and direct liquefaction. In indirect liquefaction, we mainly discuss the Molecules 2019, 24, 2250 3 of 30 This review paper aims to provide a solution of the current liquefaction technologies of biomass, including indirect liquefaction and direct liquefaction. In indirect liquefaction, we mainly discuss the synthesis pathway of ethyl alcohol and summarize the common catalysts. In direct liquefaction, we discuss the hydrolysis fermentation and thermodynamic liquefaction. In the end, the upgrading technologies of bio-oil have been provided. 2. Indirect Liquefaction 2.1. Reaction Process Indirect liquefaction is a promising technology, which is divided into two stages. The first stage is a thermochemical gasification process [10,11]. In this process, the syngas is produced after the raw material reacts with air or steam. In the syngas, the primary substances are CO, CO2,H2, and H2O. The second stage is the well-established Fischer–Tropsch (F–T) process [12]. During the F–T process, the mixture would be used to produce a range of chemicals, including methyl alcohol, dimethyl ether, and ethyl alcohol, while there is little research on the higher alcohols derived from the biomass syngas. The biggest challenges are the design of the novel catalytic reactor for the typically smaller scale of biomass conversion processes and catalysts for specific chemicals according to the molar ratio of H2 to CO. We take the synthesis of ethyl alcohol as an example to introduce the indirect liquefaction process. 2.2. Reaction Mechanism There are two approaches
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