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Chemicals from Lignocellulosic Biomass: a Critical Comparison Between Biochemical, Microwave and Thermochemical Conversion Methods

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Chemicals from Lignocellulosic Biomass: a Critical Comparison Between Biochemical, Microwave and Thermochemical Conversion Methods CRITICAL REVIEWS IN ENVIRONMENTAL SCIENCE AND TECHNOLOGY https://doi.org/10.1080/10643389.2020.1753632 Chemicals from lignocellulosic biomass: A critical comparison between biochemical, microwave and thermochemical conversion methods a,b a,c d d a Iris K. M. Yu à , Huihui Chen Ã, Felix Abeln , Hadiza Auta , Jiajun Fan , Vitaly L. Budarina , James H. Clarka , Sophie Parsonse, Christopher J. Chuckd, Shicheng Zhangc,f , Gang Luoc,f, and Daniel C.W Tsangb aGreen Chemistry Centre of Excellence, University of York, York, UK; bDepartment of Civil and Environmental Engineering, Hong Kong Polytechnic University, Hong Kong, China; cShanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science and Engineering, Fudan University, Shanghai, China; dDepartment of Chemical Engineering, University of Bath, Bath, UK; eDepartment of Mechanical Engineering, University of Bath, Bath, UK; fShanghai Institute of Pollution Control and Ecological Security, Shanghai, China ABSTRACT The past decades have seen an increasing interest in developing pathways to produce bio-based chemicals from lignocellulosic biomass and organic waste as renewable resources. Using bio- mass as a source of chemical building blocks is critical to a future sustainable chemical industry. The successful development of bio-chemicals will also have a profound impact in terms of the innovations of new polymers and materi- als, new solvents, and new bio-active compounds. This article provides a broad review of conventional thermal heating, microwave processing, and biochemical processing for the production of value-added bio-based chemicals. The potentially important but cur- rently little exploited microwave-assisted processes are given particular attention and the microwave-specific, non-thermal effects are explored. The comparative merits of dif- ferent approaches are evaluated from the techno-economic and environmental per- spectives. The opportunities of integrated biorefineries are articulated, with the aim to actualize carbon-efficient valorization of lignocellulosic biomass and organic waste for synthesizing an array of products. Abbreviation: ABE: Acetone-butanol-ethanol; AC: Activated carbon; BTX: Benzene, tolu- ene, and xylene; CAP: Combined Algal Processing; CSHL: Crude waste softwood hydrolysis lignin; FAME: Fatty acid methyl ester; GGE: Gallon gasoline equivalent; GHG: Greenhouse gas; GMO: Genetically modified organism; GVL: c-Valerolactone; HHV: higher heating value; HMF: Hydroxymethylfurfural; HTC: Hydrothermal carbonization; HTG: Hydrothermal gasification; HTL: Hydrothermal liquefaction; HTP: Hydrothermal pro- cess; LA: Levulinic acid; LCA: Life-cycle assessment; LG: Levoglucosan; LGO: CONTACT Jiajun Fan [email protected] Green Chemistry Centre of Excellence, University of York, York, UK; Shicheng Zhang [email protected] Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science and Engineering, Fudan University, Shanghai, China. ÃBoth authors contributed equally to the paper. ß 2020 Taylor & Francis Group, LLC 2 I. K. M. YU ET AL. Levoglucosenone; MIBK: Methyl isobutyl ketone; ROI: Return of investment; SCG: Spentcoffee ground; SSF: Simultaneous saccharification and fermentation; TEA: Techno- economic analysis KEYWORDS Bio-based chemicals; lignocellulosic biomass; sustainable biorefinery 1. Introduction The term “biomass”, according to EU Directive 2003/30/EC, refers to the biodegradable fraction of products, wastes, and residues from agriculture, forestry as well as the biodegradable fraction of industrial and municipal waste. The motivation for seeking renewable biomass for the production of chemical building blocks (platform chemicals) is derived from the expected transition from a fossil fuel-based economy to one based on renewable resources (Tuck et al., 2012). Bio-based platform chemicals, as reported by the US DOE (Werpy et al., 2004) (top bio-based chemicals) and Bozell and Petersen (Bozell & Petersen, 2010) (additional chemicals listed), can be sub- sequently used to produce a wide range of valuable chemicals, pharmaceut- icals, food additives, and biofuels. Biomass can be converted into platform chemicals through different proc- esses, depending on the type, property, and quantity of feedstock and the chemical products required (Cao, Yu, Liu, et al., 2018;Xiongetal.,2019). Three categories of the technologies have been separately reviewed: biochem- ical methods that convert carbohydrates of biomass into sugars and then into products such as ethanol, butanol, and other chemicals via fermentation (Straathof, 2014); conventional thermochemical methods that include pyroly- sis (mainly fast pyrolysis), hydrothermal treatment, and gasification producing bio-oils and synthesis gas (CO, H2)(Gollakotaetal.,2018;Igalavithanaetal., 2020); and microwave processing, an emerging technology potentially superior to conventional heating in terms of higher efficiency and non-thermal effects (Beneroso et al., 2017;Gaudinoetal.,2019). However, limitations exist for each type of the technologies. For instance, biological methods can only use the carbohydrate fractions of biomass. Although thermochemical processes can exploit biomass more, the outputs are often a complex mixture of compounds each at low concentration, and vary with the composition of lignocellulosic biomass, i.e. cellulose, hemicel- lulose, and lignin (Zheng et al., 2017). These components can undergo reactions simultaneously under thermal conditions, which makes it chal- lenging to achieve selective production. Thus, the economic feasibility of obtaining value-added chemicals from biomass is often questioned at pre- sent (Meng et al., 2016). CRITICAL REVIEWS IN ENVIRONMENTAL SCIENCE AND TECHNOLOGY 3 Figure 1. Summary of biomass conversion technologies. A biorefinery, where several primary conversion processes are combined and integrated with separations and downstream upgrading operations, is attractive because it would maximize the feed utilization and the value of the products. It is recommended that a biorefinery is the best solution to maximize economic and environmental benefits, while minimizing waste and pollution. Previous reviews addressed a specific category of conversion technologies (Gaudino et al., 2019; Gollakota et al., 2018) or certain types of feedstocks (Cao, Yu, Liu, et al., 2018; Igalavithana et al., 2020). However, comparison is often missing from the literature among the biological, con- ventional thermochemical, and microwave processes. This review includes a comprehensive summary of the biological and thermochemical (conventional and microwave) technologies for biomass conversion to chemicals. The biochemical technologies have dominated early commercial biorefinery-related processes (Straathof, 2014), whereas the thermochemical routes have received increasing attention recently to pursue cost-effectiveness (Figure 1). In particular, microwave heating has been adopted in novel biorefinery processes, of which the recent research outcomes and mechanistic insights are addressed in this review, fostering further technological advancements. We discuss the possible integrations of technologies for complementary biorefinery, which are often overlooked in the existing reviews, by comparing the merits of different approaches and 4 I. K. M. YU ET AL. Figure 2. Schematic of the chemical reactions for biomass catalytic pyrolysis (Wang, Dai, et al., 2017). recent achievements in research. Techno-economic and environmental con- siderations are also discussed to aid decision making in designing sustain- able biorefinery. 2. Technologies for the production of chemicals from lignocellulosic biomass 2.1. Conventional thermal heating 2.1.1. Conventional pyrolysis Pyrolysis and hydrothermal processes are two promising thermochemical technologies that can convert biomass into chemicals, which are often sepa- rated or undergo secondary conversion (Bu et al., 2011; Lyu et al., 2015). Pyrolysis, which takes place in the absence of oxygen, converts organic materials into solid, liquid, and gaseous products (Mohan et al., 2006). Due to the complexity of the biomass structure and various pyrolysis reaction pathways, hundreds of organic compounds exist in the complex liquid out- puts which are collectively called pyrolysis oil (or bio-oil), and include a low content of value-added chemicals (Wang, Dai, et al., 2017). Adding specific catalysts or other additives under optimal conditions can increase the yields of specific chemicals during selective pyrolysis (Casoni et al., 2016; Kan et al., 2016; Leng et al., 2014). To obtain value-added platform chemicals, selective pyrolysis of biomass to control the pathways has been attractive in recent years, by using cata- lysts such as zeolites, aluminas, silica-aluminas, and metal oxides (Lu et al., 2013). Figure 2 summarizes the major chemical reaction pathways involved CRITICAL REVIEWS IN ENVIRONMENTAL SCIENCE AND TECHNOLOGY 5 in the biomass catalytic pyrolysis, including deoxygenation, cracking, aroma- tization, ketonization, aldol condensation, hydrotreating, and reforming. These reactions may occur selectively depending on the catalysts and reac- tion conditions to significantly promote the formation of target products, while inhibiting other pyrolytic routes. Typical platform chemicals such as levoglucosan and levoglucoseone (Dobele et al., 2005; Meng et al., 2016), aro- matic hydrocarbons (Oh et al., 2013), acetic acid (Leng et al., 2014; Lu,
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