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Contents lists available at ScienceDirect Renewable and Sustainable Energy Reviews journal homepage: www.elsevier.com/locate/rser A review on hydrothermal liquefaction of biomass A.R.K. Gollakota a , Nanda Kishore b, , Sai Gu a, a Department of Chemical and Processing Engineering, University of Surrey, Guildford GU2 7XH, United Kingdom b Department of Chemical Engineering, Indian Institute of Technology Guwahati, Assam 781039, India ARTICLE INFO Keywords: Wet biomass Dry biomass Hydrothermal liquefaction HTL mechanism Value-added chemicals Energy eciency ABSTRACT The rapid depletion of conventional fossil fuels and day-by-day growth of environmental pollution due to extensive use of fossil fuels have raised concerns over the use of the fossil fuels; and thus search for alternate renewable and sustainable sources for fuels has started in the last few decades. In this context biomass derived fuels seems to be the promising path; and various routes are available for the biomass processing such as pyrolysis, transesterication, hydrothermal liquefaction, steam reforming, etc.; and the hydrothermal liquefac- tion (HTL) of wet biomass seems to be the promising route. Therefore, this article briey enlightened a few concepts of HTL such as the elemental composition of bio-crude obtained by HTL, dierent types of feedstock adopted for HTL, mechanism of HTL processes, possible process ow diagrams for HTL of both wet and dry biomass and energy eciency of the process. In addition, this article also enlisted possible future research scope for concerned researchers and a few of them are setting up HTL plant suitable for both wet and dry biomass feedstock; analyzing inuence of parameters such as temperature, pressure, residence time, catalytic eects, etc.; deriving optimized pathways for better conversion; and development of theoretical models representing the process to the best possible accuracy depending on nature of feedstock. 1. Introduction The rapid increase in energy demand and the lack in the supply to cater the needs, enables to nd the alternatives to meet the current demands of the society which is of primary concern in terms of socio economics of the globe. The rapid growth rate of urbanization in the past decades, water quality degradation became a public health threat. Eutrophication associated with nutrient content of wastewater and treatment plant euents have become a serious concern to water environment. Combining these two critical environmental and social causes an alternate source for the conventional fossil fuels which has to be sustainable, energy secured, and reduce global warming is highly desirable. This lead several researchers to focus in search of alternate source for commercialization from several decades and came up with one source which is nothing other than the biomass. Biomass sources include wood wastes, energy crops, aquatic plants, agricultural crops, and their waste products and municipal and animal wastes; and are considered as potential sources of fuels and chemical feedstock's. The choice of biomass and its derivatives generate high expectations for the production of fuels, raw materials for synthesis in the petrochemical industry and ne chemicals. Biomass, in addition to the production of the rst generation biofuels (bioethanol and biodiesel), is also of interest for the production of bio oil due to its perspectives for production by pyrolysis of lignocellulose biomass. Several statistics related to production and consumption of biomass as an alternated source of energy is listed by several authors. As of 2010, world biofuel production has been largely focused on rst generation bio fuels producing ethanol and biodiesel from starch, sugars, and vegetable oils. Advanced bio fuels or biofuels produced from lignocellulose materials such as wood waste and straw made up to only 0.2% of total biofuel production. In recent years, research on using biomass for liquid fuels has been robust, ranging from studies of pyrolysis and hydrothermal liquefaction (HTL) of lignocellulose material, gasication and biomass to liquid technologies to the upgrading processes. Secondly, converting biomass from its natural solid form to liquid fuels is not a spontaneous process. The liquid fuels that humans have harnessed on a large scale as fossil fuel took thousands of years of geochemical processing to convert biomass to crude oil and gas. In recent years, several conversion technologies have been developed to obtain liquid products from dierent kinds of biomass for use as fuels and chemicals. Biomass conversion technologies are broadly classied into two categories namely, biochemical and thermo- chemical con- version. In general, the unprocessed bio-oil derived from the biomass has low energy density, high moisture content, and its physical form is not free owing that creates a problem as a feedstock for reciprocating engines. Thermochemical conversions compared to biochemical con- http://dx.doi.org/10.1016/j.rser.2017.05.178 Received 14 August 2016; Received in revised form 26 April 2017; Accepted 20 May 2017 Corresponding author. E-mail addresses: [email protected] (N. Kishore), [email protected] (S. Gu). Renewable and Sustainable Energy Reviews 81 (2018) 1378–1392 Available online 08 June 2017 1364-0321/ © 2017 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY license (http://creativecommons.org/licenses/BY/4.0/). MARK

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Page 1: Renewable and Sustainable Energy Reviewsepubs.surrey.ac.uk/841479/3/A Review on Hydrothermal Liquefaction... · A review on hydrothermal liquefaction of biomass ... interest for the

Contents lists available at ScienceDirect

Renewable and Sustainable Energy Reviews

journal homepage: www.elsevier.com/locate/rser

A review on hydrothermal liquefaction of biomass

A.R.K. Gollakotaa, Nanda Kishoreb,⁎, Sai Gua,⁎

a Department of Chemical and Processing Engineering, University of Surrey, Guildford GU2 7XH, United Kingdomb Department of Chemical Engineering, Indian Institute of Technology Guwahati, Assam 781039, India

A R T I C L E I N F O

Keywords:Wet biomassDry biomassHydrothermal liquefactionHTL mechanismValue-added chemicalsEnergy efficiency

A B S T R A C T

The rapid depletion of conventional fossil fuels and day-by-day growth of environmental pollution due toextensive use of fossil fuels have raised concerns over the use of the fossil fuels; and thus search for alternaterenewable and sustainable sources for fuels has started in the last few decades. In this context biomass derivedfuels seems to be the promising path; and various routes are available for the biomass processing such aspyrolysis, transesterification, hydrothermal liquefaction, steam reforming, etc.; and the hydrothermal liquefac-tion (HTL) of wet biomass seems to be the promising route. Therefore, this article briefly enlightened a fewconcepts of HTL such as the elemental composition of bio-crude obtained by HTL, different types of feedstockadopted for HTL, mechanism of HTL processes, possible process flow diagrams for HTL of both wet and drybiomass and energy efficiency of the process. In addition, this article also enlisted possible future research scopefor concerned researchers and a few of them are setting up HTL plant suitable for both wet and dry biomassfeedstock; analyzing influence of parameters such as temperature, pressure, residence time, catalytic effects,etc.; deriving optimized pathways for better conversion; and development of theoretical models representing theprocess to the best possible accuracy depending on nature of feedstock.

1. Introduction

The rapid increase in energy demand and the lack in the supply tocater the needs, enables to find the alternatives to meet the currentdemands of the society which is of primary concern in terms of socioeconomics of the globe. The rapid growth rate of urbanization in thepast decades, water quality degradation became a public health threat.Eutrophication associated with nutrient content of wastewater andtreatment plant effluents have become a serious concern to waterenvironment. Combining these two critical environmental and socialcauses an alternate source for the conventional fossil fuels which has tobe sustainable, energy secured, and reduce global warming is highlydesirable. This lead several researchers to focus in search of alternatesource for commercialization from several decades and came up withone source which is nothing other than the biomass. Biomass sourcesinclude wood wastes, energy crops, aquatic plants, agricultural crops,and their waste products and municipal and animal wastes; and areconsidered as potential sources of fuels and chemical feedstock's. Thechoice of biomass and its derivatives generate high expectations for theproduction of fuels, raw materials for synthesis in the petrochemicalindustry and fine chemicals. Biomass, in addition to the production ofthe first generation biofuels (bioethanol and biodiesel), is also ofinterest for the production of bio oil due to its perspectives for

production by pyrolysis of lignocellulose biomass. Several statisticsrelated to production and consumption of biomass as an alternatedsource of energy is listed by several authors. As of 2010, world biofuelproduction has been largely focused on first generation bio fuelsproducing ethanol and biodiesel from starch, sugars, and vegetableoils. Advanced bio fuels or biofuels produced from lignocellulosematerials such as wood waste and straw made up to only 0.2% of totalbiofuel production. In recent years, research on using biomass forliquid fuels has been robust, ranging from studies of pyrolysis andhydrothermal liquefaction (HTL) of lignocellulose material, gasificationand biomass to liquid technologies to the upgrading processes.

Secondly, converting biomass from its natural solid form to liquidfuels is not a spontaneous process. The liquid fuels that humans haveharnessed on a large scale as fossil fuel took thousands of years ofgeochemical processing to convert biomass to crude oil and gas. Inrecent years, several conversion technologies have been developed toobtain liquid products from different kinds of biomass for use as fuelsand chemicals. Biomass conversion technologies are broadly classifiedinto two categories namely, biochemical and thermo- chemical con-version. In general, the unprocessed bio-oil derived from the biomasshas low energy density, high moisture content, and its physical form isnot free flowing that creates a problem as a feedstock for reciprocatingengines. Thermochemical conversions compared to biochemical con-

http://dx.doi.org/10.1016/j.rser.2017.05.178Received 14 August 2016; Received in revised form 26 April 2017; Accepted 20 May 2017

⁎ Corresponding author.E-mail addresses: [email protected] (N. Kishore), [email protected] (S. Gu).

Renewable and Sustainable Energy Reviews 81 (2018) 1378–1392

Available online 08 June 20171364-0321/ © 2017 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY license (http://creativecommons.org/licenses/BY/4.0/).

MARK

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versions are processed at several higher degrees of temperature in thepresence of appropriate catalysts to obtain liquid products fromdifferent sources. In general, thermochemical conversions are muchrapid than the biochemical conversions. Thermochemical conversionconversions generally implied to upgrade biomass by heating underpressurized and oxygen deprived enclosure. It can be further classifiedinto combustion, gasification, pyrolysis, and direct liquefaction. Amongwhich direct liquefaction or hydrothermal liquefaction is one of thepromising routes that drawn attention in the recent past. This processis synonym of hydrous pyrolysis, but compared to pyrolysis HTL iscarried at lower temperatures and heating rates. In other words,hydrothermal liquefaction of biomass is the thermochemical conver-sion of biomass into liquid fuels by processing in a hot, pressurizedwater environment for sufficient time to break down the solid biopolymeric structure to mainly liquid components. Typical hydrother-mal processing conditions are 523–647 K of temperature and operat-ing pressures from 4 to 22 MPa. The low operating temperature, highenergy efficiency and low tar yield compared to pyrolysis is the keyparameter that drives the attention of researchers on the liquefactionprocess.

Till date all the paradigm research on the production of biofuel isrested on the solid dry wood but liquid bio-waste has a better edge overthe solid manure which is the critical processing parameter for thehydrothermal liquefaction process. Among several possibilities of wetbiomass, microalgae is considered to be an excellent source of biofuelproduction because of their advantages such as high photosyntheticefficiency, maximum biomass production, fast growth rate and lack ofarable soil requirements. A very little attention on the HTL of wetbiomass process is available as of now and very few attempts of pilotplants globally, for instance, Pittsburgh Energy Research centre of U.SBureau of Mines took place in 1990s but stopped later on due toeconomic crisis. Hence, an attempt has been made to bridge the gap inthe literature and create a possibility to take the research on HTL ofbiomass to next level by selecting the best available feedstock and theoperating conditions. Further research on tuning of the criticaloperating parameters like temperature and pressure for better yieldis still under progress. Thus, this article tries to enlighten the existingknowledge and research gaps available pertained to biomass andhydrothermal liquefaction. However, before presenting thorough lit-erature review along with HTL mechanisms, energy efficiency andadvantages/disadvantages of this process, a few details of elementalcomposition; and wet and dry biomass feedstock suitable for HTL arepresented below.

1.1. Elemental composition of biomass

Any biomass consists of elemental carbon (C), hydrogen (H),nitrogen (N), sulphur (S) and oxygen (O); and a few details of themare presented below.

1.1.1. Carbon (C)It is obviously the most important constituent of the biomass. It

comes from the atmospheric CO2 that become a part of the plantmatter during photosynthesis. Carbon represents the major contribu-tion to the overall heating value. During combustion, it is principallyremodelled into CO2 that is discharged within the atmosphere [1]. Inany combustion application an area of carbon is not combusted utterlyand ends up in emissions of change state gases, usually carbon-monoxide gas or PAH's [2]. Generally, the carbon content of the fuelis estimated via the composition of lignin, hemicellulose and cellulose.Similarly, the char content is majorly depended on the amount of thelignin i.e., for herbaceous biomass yields lower carbon content ascompared to wood biomass. Fuels rich in lignin, such as olive kernel,have carbon contents higher than 50% (by wt) on dry basis [3].

1.1.2. Hydrogen (H)It is another major constituent of biomass, as can be expected from

the chemical structure of the carbohydrate and phenolic polymers.During combustion, hydrogen is converted to H2O, significantlycontributing to the overall heating value [4]. The weight content ofhydrogen, on a dry basis, is usually slightly lower in herbaceousbiomass (5.5–6%) than in woody biomass (6–8%) [3].

1.1.3. Nitrogen (N)It constitutes the vital nutrient form for plants. For instance, the

nitrogen is applied as a fertilizer to soil that enhances the growth andyield of the plants. By the continual application of the nitrogen in themodern day agricultural era, the nitrogen content of herbaceousbiomass species acquires a greater amount of nitrogen ranging between(0.4–1.0% wt dry basis) compared to woody biomass [5]. Further, thepresence of nitrogen significantly contributes the degradation inbiochemical processes like digestion or fermentation. On the otherhand, nitrogen during combustion process doesn’t oxidize and there-fore its contribution to the overall heating values [3].

1.1.4. Sulphur (S)This is considered to be the other important nutrient hindered in

structures of amino acids, proteins and enzymes for substantial plantgrowth similar to nitrogen. The high growth rate of most herbaceouscrops means that the sulphur concentration in plant biomass istypically higher than those in woody biomass. The concentration ofsulphur in wood can be as low as 0% (which means below the detectionlimit of most laboratory devices) and reaches up to 0.1% on a dry basisin exceptional cases, herbaceous biomasses have a sulphur contentranging from 0% to 0.2% or even higher [6]. In waste fractions, valuesup to approximately 1% have been reported. However, it's mostimportant impact relates to gaseous emissions, syngas cleaning ingasification processes and corrosion [3].

1.1.5. Oxygen (O)Oxygen constitutes the vital element in the chemical composition of

the biomass which is evident from the nature through photosyntheticprocess. The composition of the oxygen content controls the heatingvalue of the bio crude that is obtained via any processing technique [7];and majority of the bio crudes are limited their utilization just becauseof the excess content of the oxygen. It is evident that the oxygen contentin the phenolic compound structure are very complex to break (or toremove) it in the form of water so that to enhance the heating values. Itshould be noted that oxygen is not measured directly – its weightconcentration is estimated by subtracting from 100 the concentrationsof all other elements (C, H, N, S) and of the ash content in the dry fuel[3]. In the context of HTL of biomass, the elemental composition ofbio-crude obtained by the hydrothermal liquefaction of both wet anddry biomass is given in Table 1.

1.2. Biomass Feedstock

1.2.1. Dry feedstockThe tangled biomass properties lead to the braid chemical reactions

during the hydrothermal liquefaction procedure. Woody biomass/lignocellulose built is embedded with hemicellulose, cellulose and thelignin compounds; and hence the rigid crystallinity of the structuremakes it rigid and tougher to process. Further, accommodating acontinuous flow framework again involves the complexity of theprocedure that leads to the solubility criteria in the solvents due tothe hindered resistance to the structure of biomass. Thus the entireframework of the process is penalized economically. Despite, theintrinsic source of hydrogen and carbon, the processing of thelignocellulose biomass is limited due to the substantial amount of theoxygen. The detailed explanation of the individual fractions of ligno-cellulose is presented below.

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Table 1Elemental composition of the bio crude obtained through hydrothermal liquefaction of biomass (both wet and dry).

S.No Feedstock Elemental composition of product species after HTL References

C (%) H (%) N (%) O (%) S (%) Ash (%) Moisture (%) HHV % Yield

1 Spirulina algae 68.9 8.9 6.5 14.9 0.86 – – 33.2 32.6 Vardon et al. [8]2 Swine manure 71.2 9.5 3.7 15.6 0.12 – – 34.7 30.23 Anaerobic sludge 66.6 9.2 4.3 18.9 0.97 – – 32.0 9.44 Arthrospira platensis 74.5 10.2 6.8 7.5 1.0 – – 38.65 30 Lavanya et al. [9]5 Tetraselmis 71.4 9.5 5.7 12.3 1.1 – – 35.58 296 Nannochloropsis gaditana 76.1 10.3 4.5 8.8 0.4 – – 38.00 Barriero et al. [10]7 Scenedesmus almeriensis 74.9 9.1 5.9 9.6 0.7 – – 36.208 Nannochloropsis Sp 77.2 9.9 4.7 8.2 0.5 – – 399 Almeriansis 73.2 9.3 5.1 0.8 11.7 35.8 20.0 – 42.610 Gaditana 74.2 9.3 4.0 0.6 11.8 36.2 12.4 – 50.811 Nannochloropsis Oceana 77.6 4.9 3.4 – 0.3 – – 37.70 54.2 Caporgno et al. [11]12 Derbesia 73 7.5 6.5 10.6 0.7 – – 33.2 Neveux et al. [12]13 Ulva 72.6 8.2 5.8 11.0 0.4 – – 33.814 Chaetomorpha 70.9 7.7 6.8 11.4 0.1 – – 32.515 Cladophora 71.6 8.0 7.1 10.6 0.9 – – 33.316 Oedogonium 72.1 8.1 6.3 10.4 1.3 – – 33.717 Cladophora FW 71.1 8.3 6.8 10.6 1.3 – – 33.518 Aspen wood 75.2 8.2 0.5 15.8 0.3 0.48 3.8 34.3 Pedersen et al. [13]19 Scenedesmus 72.6 9.0 6.5 10.5 1.35 – – 35.5 Vardon et al. [14]20 Defatted scene 72.2 8.9 7.8 10.5 0.90 – – 35.321 Spirulina 72.2 9.1 8.1 9.2 1.41 – – 35.822 Nutrient depleted Oedogonium 65.8 8.5 1.5 18.3 – – – He et al. [15]23 Spent coffee grounds 71.2 7.1 3.0 18.7 – – – 31.00 Yang et al. [16]24 Pinus 60.1 6.0 1.2 32.7 0.1 – – 23.1 Cao et al. [17]25 Cupressus funebris 62.0 6.6 1.6 29.8 0.1 – – 25.126 Platanus 70.0 6.3 0.7 23.0 0.01 – – 28.627 Cinnamomum Camphora 74.0 8.4 1.5 16.1 0.01 – – 34.228 Pittosporum tobira 71.0 8.5 1.5 19.0 0.01 – – 32.929 Distylium racemosum 64.1 6.8 0.7 28.4 0.01 – – 26.330 Viburnum odoratissimum 71.7 8.1 1.2 19.0 0.01 – – 32.531 Salix alba 73.7 9.2 3.1 14.1 0.01 – – 35.632 Algal waste of Indiana polis 71.4 8.36 4.92 15.4 – – – 33.3 Chen et al. [18]33 Swine manure 71 8.9 4.1 0.21 14.2 35 – – 61 Toor et al. [19]34 Garbage 73.6 9.1 4.6 12.7 36 – – 2135 Indonesian biomass residue 67–80 6–8 0–2 11–23 30 – – 21–3636 Sawdust, rice husk, lignin – – – 837 Beech wood 76.7 7.1 0.1 16.1 34.9 – – 2838 Phytomass 76.6 7.6 2.1 0.1 13.6 – – –

39 Algae Dunaliella tertiolecta 63.55 7.66 3.71 25.8 30.7 – – 25.840 Porphyridium 66–83 5–11 0–12 0–1 8–27 22.8–36.9 – – 5–2541 Nannochloropsis 51 7 9 0.6 28.8 3 – 46 Valdez et al. [20]42 Acid mine drainage 68.8 7.9 7.1 – – 29.70 Raikova et al. [21]43 Cyanobacteria sp. 76.02 9.10 6.29 7.44 1.15 – – 36.51 Huang et al. [22]44 Bacillariophyta sp. 76.09 9.11 5.60 8.28 0.92 – – 36.4545 Seaweed 75.54 9.16 3.65 11.66 0.62 – – 35.97 Bach et al. [23]46 L.digitata 70.5 7.8 4.0 17 0.7 – – 32 17.6 Anastasakis and Ross [24]47 L.hyperbore 72.8 7.7 3.7 14.9 0.8 – – 33 9.848 L.saccharina 74.5 7.9 3.0 14.0 0.6 – – 33.9 1349 A.esculenta 73.8 8 3.8 14 0.8 – – 33.8 17.850 L.Saccharina 31.3 3.7 2.4 26.3 0.7 24.2 9.2 1251 Taihu cyanophyta 77.30 12.08 1.10 9.01 – – 41.73 Guo et al. [25]52 Coffee Husk 43.13 5.02 1.55 32.78 0.67 7.4 8.44 16.79 Braz et al. [26]53 Tucuma Seed 48.83 6.12 0.88 32.20 – 5.97 6.08 20.7754 Sugarcane 45.05 5.57 0.25 37.91 – 3.21 6.95 20.7755 Peanut shell 41.52 7.43 2.12 27.96 0.60 12.80 7.98 16.5256 Rice husk 31.47 6.67 1.04 23.03 0.50 29.53 8.19 15.3957 Pine sawdust 45.95 7.47 0.32 34.32 0.57 4.71 6.90 17.0358 Pond water algae biomass 46.09 6.22 9.70 37.35 0.64 Nautiyal et al. [27]59 Spirulina 48.10 6.97 10.14 34.13 0.6660 Chlorella 51.33 7.90 9.80 30.38 0.5961 Pond water algae oil 59.94 11.57 0.11 28.37 0.3162 Spirulina oil 66.73 12.40 0.50 20.21 0.1663 Cladophora glomerata 26.8 3.53 2.14 20.48 0.22 36.5 9.1 10.29 Plis et al. [28]64 Posidonia Oceanica 35.5 3.60 0.27 28.85 0.18 26.1 5.5 12.8265 Nannochloropsis gaditana 40.3 5.97 6.30 14.49 0.37 28.3 4.1 18.5366 Microcystis 42.26 6.27 7.88 43.07 0.52 6.14 9.59 16.2 Hu et al. [29]67 Almeriensis 41.78 6.81 7.94 42.93 0.55 14.5 17.6 Diaz-Rey et al. [30]68 S.japonica 34.7 5.5 1 41.6 0.3 18.3 7.4 12.1 Choi et al. [31]69 S.pallidum 22.64 4.90 2.96 21.34 1.42 36.44 10.30 9.63 Li et al. [32]70 P.elongata 35.81 5.93 6.86 51.40 27.45 11.55 12.54 Ceylan et al. [33]71 Sargassum sp 26.70 4.23 1.35 67.53 36.82 9.34 10.1072 U.fasciata 25.64 5.75 3.13 5.52 16 19.86 Trivedi et al. [34]

(continued on next page)

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1.2.1.1 CelluloseThe chemical formula of the cellulose is denoted by (C6H10O5)n

which is a long chain polysaccharide, high molecular weight, and withhigh degree of polymerization. Cellulose is a non-polar compound atambient temperature, but tends to soluble with the increase in thetemperature [54]. Monomers of glucose are stiffly bonded possessingthe formation of strong intramolecular and intermolecular interactionsamongst hydrogen bonds that originates the glucose monomers [55].

1.2.1.2 HemicelluloseIt is a branched structure hetero polymer with amorphous structure

embracing pentose and hexose as a polymer. The composition of thehemicelluloses varies significantly for woody biomass and the grassybiomass which comprises xylan in the earlier and mannan, glucan andgalactan in the later [56]. Further, hemicellulose in comparison to thecellulose possess the weaker structure and less resistant to intramole-cular hydrogen bonding allows the easier disintegration of the mole-cules [57]. Hence, the conducive nature to hydrolysis of hemicelluloseis severe and prone to easy miscibility characteristic [58].

1.2.1.3 LigninThe other fraction of the lignocellulose biomass is lignin which is

treated as a natural polymer can be referred as an aromatic compoundin which phenyl-propane with hydroxyl and ethoxy groups are linkedvia ether bonds [59]. Lignin possess similar morphological character-istic of amorphous form as hemicellulose, less solubility similar tocellulose and the peculiar behaviour of hydrophobic nature. Also itpossesses the binding capacity of stem cells or fibrous contents ofplants fibrous contents of the plant to strengthen cell wall structure,improves the sublimation capacity of micro-organisms and to store theenergy [60]. In contrast to other bioorganic compounds the decay rateof lignin is very low, in other words, it is resistant to biologicaldegradation. The significant feature of lignin encompasses the higherenergy content compared to the other two compounds that leads tohigher heating value to the product and considered to be the mostvaluable phenol compound [61].

1.2.2 Wet biomass feedstock

1.2.2.1 Lipids/FatsThese are majorly non-polar compounds otherwise immiscible/

hydrophobic in nature that resembles the similarities with the aliphaticcompounds and particularly referred to triglycerides (TAG's) nothingother than triesters of fatty acids and glycerol [62]. At normaltemperatures, the fats are generally insoluble in solvents and graduallytends to be polar with the change in temperature. The similarphenomenon on the effect of the temperature on the solubility of thefats can be seen in the case of cellulose. The dielectric constant of thesolvent in particular water at sub-critical conditions allows the greatermiscibility [57]. This leads to the stability in the structure of the TGA'sfurther leading to the formation of the glycerol a major by-product ofthe bio-diesel production which is a combination of fatty acids,methanol and salts. During HTL, glycerol is not converted to any oilyphase rather it turns to be a water-soluble compound [63]. Furtherdegradation of glycerol leads to the product stream of acetaldehydes,propionaldehyde, acrolein, allyl alcohol, ethanol, formaldehyde, CO,CO2, and H2 [62].

1.2.2.2 Proteins/Amino acidsOne of the major constituent of microbial or algal biomass is

protein consisting several chains of peptide reduces to polymers ofamino acids. They are the building blocks of proteins and highlyheterogeneous and hence the complexity in degrading the amino acidsis challenging. The strong peptide chain of proteins undergoes dec-arboxylation, and deamination reaction upon hydrothermal liquefac-tion leads to the formation of hydrocarbons, amines, aldehydes andacids [19]. Further degradation resulting carboxylic acids, acetic acid,propionic acid, n-butyric acid, and iso-butyric acids.

2. Evolution of HTL process over decades

Environmental issues, sustainability, declining fossil fuels, andenergy security concerns have led the world to explore alternate, clean,

Table 1 (continued)

S.No Feedstock Elemental composition of product species after HTL References

C (%) H (%) N (%) O (%) S (%) Ash (%) Moisture (%) HHV % Yield

73 Xuzhou SS 47.4 7.9 8.2 35.2 1.3 56.8 5.6 Huang et al. [35]74 S.patens C.Agardh 17.7 14.38 15.47 Li et al. [36]75 E.grandis 47.19 5.77 0.21 46.59 0.24 0.09 18.07 Louw et al. [37]76 T.suesica 43.32 7.27 5.75 40.55 3.11 12.20 7.88 Zainan et al. [38]77 Dunaliella tertiolecta 53.3 5.2 9.8 31.7 – 19.8 Minowa et al. [39]78 Chlorella vulgaris 52.6 7.1 8.2 32.2 0.5 23.2 Biller and Ross [40]79 Nannochloropsis oculata 57.8 8.0 8.6 25.7 – 17.980 Botryococcus braunii 77.04 12.40 1.23 9.86 0.18 35.6 Liu et al. [41]81 Fucus vesiculosus 32.88 4.77 2.53 35.63 2.44 11.8 15.0 Ross et al. [42]82 Chorda filum 39.14 4.69 1.42 37.23 1.62 9.9 15.5583 Laminaria digitata 31.59 4.85 0.90 34.16 2.44 10 17.6084 Fucus Serratus 33.5 4.78 2.39 34.44 1.31 18.6 16.6685 Laminaria hyperborea 34.97 5.31 1.12 35.09 2.06 11.2 16.5486 Macrocystis pyrifera 27.3 4.08 2.03 34.8 1.89 18.5 16.087 Miscanthus 46.32 5.58 0.56 41.79 0.2 2.1 19.0888 Nannochloropsis Salina 55.16 6.87 2.73 33.97 1.27 2.48 4.95 25.40 Toor et al. [43]89 Mougeotia 41.51 5.59 5.40 27.03 0.51 19.96 5.14 16.63 Sharara et al. [44]90 Cladophora 33.79 4.73 6.35 21.27 1.57 32.29 5.09 14.5391 Seaweed meal 43.99 5.95 5.21 36.13 1.02 7.7 7.92 18.35 Lorenzo et al. [45]92 Synechococcus/Anabaena 42.78 7.74 7.91 38.1 7.4 9.61 Wagner et al. [46]93 Synechocystis 46.12 7.98 3.52 11.2 4.5 15.3794 A.azuera 40.82 5.56 0.63 52.99 10.61 6.03 52.99 Aysu et al. [47]95 Chlorella.sp 47.54 7.1 6.73 38.63 5.93 6.8 18.59 Phukan et al. [48]96 E.prolifera 35.20 5.20 2.10 32.98 15.91 8.61 13.4 Yang et al. [49]97 Datura Stramonium L 43.55 5.98 0.77 49.70 6.38 3.73 14.39 Aysu and Durak [50]98 E.Spectabilis 39.27 6.54 1.28 52.91 4.6 5.6 13.17 Aysu et al. [51]99 Brewers spent grain 46.6 6.85 3.54 42.26 0.74 4.5 8 20.39 Mahmood et al. [52]100 Laurel algae 48.97 6.38 3.02 41.63 10.53 9.95 19.77 Ertas and Alma [53]

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cheap and renewable energy sources. Though biomass is one of theprominent option for renewable and sustainable energy, choosing thereliable and efficient conversion methodology is a big challenge. Overthe decades of research lightened different thermo-chemical conversiontechnologies and each of them has their own advantages and dis-advantages. In this regard, HTL is found to be the suitable processavailable to tackle the wet feed stock conversion to fuel energy.Research on HTL can date back to the 1930s and there is considerableamount of literature available worldwide pertaining the wet biomassconversion. The pioneering work on the HTL process on a commercialscale of cellulose biomass to heavy oil was initiated at PittsburghEnergy Research Centre in 1970. This process of HTL was takenfurther by Schaleger et al. [64] at Lawrence Berkeley Laboratory,Thigpen [65] at Albany Biomass Liquefaction Experimental Facility.Further details of studies of the HTL process by several researchers arebriefly described below.

Beckman and Elliott [66] performed comparison studies on yieldsand properties of oil obtained from direct thermochemical biomassliquefaction process. The authors developed correlations for the keyparameters such as temperature, pressure, time, catalyst and con-cluded that the changes in the governing parameters has a significantimpact on the product output. White and Wolf [67] developed a uniquemethod of pumping concentrated viscous biomass slurries throughliquefaction system. The authors introduced the extruder – feedersystem to pump the high viscous liquids for the liquefaction process.One of the pioneering works of the HTL of microalgae with high lipidcontent was done by Dote et al. [68]. In the years that followed severalresearchers had begun to explore this technology and verified theproperties of algae bio-oil in comparison with the petroleum Minowaet al. [39]. Itoh et al. [69] developed a scale up of HTL of sewage sludgeoperating at temperature of 300 °C and pressure of 10 MPa. Sawayamaet al. [70] studied energy consumption for the HTL process of variousalgae and presented the energy consumption ratio for the HTL couldproduce net energy with low energy consumption. Also HTL opens upnew possibilities for combined fuel production and waste watertreatment in densely populated areas where large amounts of wetwaste materials are available. Behrendt et al. [71] reviewed the directliquefaction especially for lignocellulose biomass through sub criticaland super critical solvents. Since 2009, the study gradually grabbed theattention of some reputed international research laboratories exploringthe liquefaction reaction parameters that includes residence time,reaction temperature, catalyst selection and loading. Peterson et al.[57] provided a comprehensive overview on the hydrothermal liquefac-tion of bio-oil from biomass using sub and super critical water orsolvent extraction technique. Further the products of HTL processcomprises a wide range of value added chemical compounds whichinclude branched aliphatic compounds, aromatics and phenolic deri-vatives, carboxylic acids, esters, and nitrogenous ring structures Xiuet al. [72]. Savage [73] published a brief but insightful overview on thehydrothermal liquefaction of microalgae. This was supported by theseveral other researches of Alba et al. [74], Minowa et al. [39], Rosset al. [75], Vardon et al. [14], Zou et al. [76]. Researchers have recentlyposted a renewable algal biorefinery based on HTL of algae Jena et al.[77], Alba et al. [74,78]. Recently the prominence of algae as thefeedstock for HTL is addressed by Barreiro et al. [10] and Chow et al.[79]. Latest review of Elliott et al. [80] and Jindal and Jha [81]enlightened some of the previous and current research works onhydrothermal liquefaction of biomass (both solid and liquid) whichincluded studies of Appell et al. [82], Kaufman et al. [83], Inoue et al.[84], Chornet and Overend [85], Ocfemia et al. [86], Heilmann et al.[87], Elliott [7], Akhtar and Amin [88], Xu et al. [89] and Tekin et al.[90].

Further literature pertaining to the reaction mechanisms of HTL iscritical in understanding the process so as to better design the reactorsand control the process. At present, understanding of HTL mechanismsis largely qualitative and indicative although efforts have been made

through years by many researchers Balat [91], Demirbas [92,93],Minowa et al. [94], Yuan et al. [95]. Generally, biomass is first brokenup into fragments by hydrolysis, and then degraded into smallercompounds by dehydration, dehydrogenation, deoxygenation anddecarboxylation. At the end, some complex chemicals may be synthe-sized by repolymerization. Biocrude product generated in the repoly-merization process usually contains acids, alcohols, aldehydes, esters,ketones, phenols and other aromatic compounds Chornet and Overend[85]. Hietala et al. [95] introduced new dimensions of kinetic model forfast hydrothermal liquefaction of biomass with good yield of 41% at400 0C and short residence time. However, the exact mechanisms orpathways of the HTL still remain unclear mainly due to the complexityof the feedstock and HTL products, as well as the seemingly-infinitepossible intermediate reactions. Hydrothermal liquefaction now is inthe transient state from lab-pilot scale to pilot-industrial scale, whichmakes the mechanisms study more important and urgent. With thesupport of mechanisms work, development of large-scale units could bemore reasonable and high-grade products may be produced, adding asolution to current environmental and energy problems.

Recently, immense amount of the work pertaining to hydrothermalliquefaction of wet and dry biomass through different techniques hasbeen carried out by many researchers. For instance, Alhassan et al. [96]presented glimpses of HTL process on dry biomass and obtained bio-oil with properties equivalent to pyrolysis oil. Costanzo et al. [97]obtained bio-oil derived from wet biomass and reported that thecomposition of the bio-oil is equivalent to conventional gasoline.Further, to obtain higher percentages of yield Lavanya et al. [9]introduced the blending of algal crude to petro crude that is turnedto diesel fraction. Pedersen et al. [13] obtained aspen wood derivedbio-oil characteristics equivalent to gasoline which supports theresearch work of Costanzo et al. [97]. Zhu et al. [98] reported thathydrothermal liquefaction of wet and dry biomass results in the higheryields of phenolics at the conventional operating temperatures ratherthan desired aromatics. Maddi et al. [99] made an attempt to obtainvalue added chemicals through hydrothermal liquefaction of bio-oiland succeeded in obtaining the same. Another important aspect of thisHTL process is the introduction of continuous flow reactor which yieldsa significant amount of heating values which was reported by Pedersenet al. [13]. Recent review of Elliot et al. [80] also stressed theimportance of introducing the continuous flow reactors rather thanconventional batch process for the higher yields of HTL products.

Several other explorations on the critical parameters such as energyconsumption economics by Sawayama et al. [70]; reaction mechan-isms/pathways [91–94,100]; algal biomass as feedstock [97,74,78];generation of value added chemicals by Xiu et al. [72]; temperature,pressure, reaction residence time and catalyst loading effects byAnastasakis and Ross [101] and more insights by several researchers[36,40,75,76,82,84–89,102–104] are praiseworthy. Finally, Table 2presents the comprehensive details of aforementioned and some moreliterature in tabular form pertained to various aspects of hydrothermalliquefaction over the years.

In the past decade, there were also several review papers on variousaspects of HTL. For instance, Peterson et al. [57] presented sub- andsupercritical water technologies available for thermochemical biofuelproduction from various types of biomass. Toor et al. [134] reviewedthe subcritical water technologies for production of biocrude frombiomass; and they summarized that the chemical properties of bio-crude are highly dependent of the biomass composition. Akhtar andAmin [88] reviewed the literature pertaining to HTL of biomass withthe aim to report process conditions such as final liquefactiontemperature, residence times, rate of biomass heating, size of biomassparticles, types of solvents, etc. for optimum bio-oil yield. They havealso included brief discussion on decomposition mechanisms duringhydrothermal liquefaction. Tekin et al. [90] explained the physico-chemical properties of water under subcritical and supercritical condi-tions on HTL and interactions of water with biomass during HTL

A.R.K. Gollakota et al. Renewable and Sustainable Energy Reviews 81 (2018) 1378–1392

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Table

2Su

mmaryof

literature

pertained

tohyd

rothermal

liqu

efaction

ofbiom

ass(bothwet

anddry).

S.No

Auth

or

Desc

ription

Feed

Pro

cess

conditions

Pro

ducts

1Alhassanet

al.[96]

Hyd

rothermal

liqu

efaction

ofde-oiledJa

trop

hacu

rcas

cake

usingdeep

eutectic

solven

ts(D

ESs)as

catalyst

andco

solven

tsDe-oiledJa

trop

hacu

rcas

cake

Tem

p:25

0°C

HHV

values

oftheHTLbiooilis

25.01MJ/kg

.Pressure:4.5MPa

Reactor:Batch

2Anastasakisan

dRoss

[24]

Hyd

rothermal

liqu

efaction

offourbrow

nmacro

alga

ecommon

lyfound

ontheUK

coasts:Anen

ergetican

alysis

oftheprocess

andcomparison

withbio-ch

emical

conversionmethod

s

Digitata,

hyp

erbo

rea,

saccharina,

escu

lenta

Tem

p:35

0°C

Highnitrogencontentis

observed

from

thebiooilob

tained

indicatingthenecessity

forupgrad

ation.

Pressure:

Reactor:Batch

3Bachet

al.[23]

Fasthyd

rothermal

liqu

efaction

ofNorwegianalga

-Screeningtests

Lam

inaria

saccharina

Tem

p:35

0°C

Highestyieldof

79%

bio-oilis

obtained

with35

.97MJ/kg

HHV.

Pressure:16

.5ba

rReactor:Muffle

furn

ace

4Barrieroet

al.[10]

Hyd

rothermal

liqu

efaction

ofmicroalga

e:Effecton

theproduct

yieldsof

thead

ditionof

anorga

nic

solven

tto

separatetheaq

ueo

usphasean

dthe

biocrudeoil

Nan

nochloropsisga

ditan

a,Sc

ened

esmusalmeriensis

Tem

p:35

0°C

Organ

icsolven

tdichloromethan

eincreasestheyieldof

biocrudeat

higher

oxyg

enan

dnitrogencontents.

Pressure:2MPa

Reactor:Micro

autoclav

e5

Cap

orgn

oet

al.[11]

Hyd

rothermal

liqu

efaction

ofNan

nochloropsisOcean

icain

different

solven

tsNan

nochloropsisOcean

ica

Tem

p:24

0–30

0°C

Alcoh

olco

solven

tsyieldhighbiooil~60

%.

Pressure:32

43ba

rReactor:Batch

6Chan

etal.[105

]Effectof

process

param

eterson

hyd

rothermal

liqu

efaction

ofoilpalm

biom

assforbio-oilproductionan

ditslife

cycleassessmen

tRaw

fruitbu

nch

,palm

Mesocarp

fibrean

dpalm

kern

elsh

ell

Tem

p:33

0–39

0°C

Optimum

biooilyieldis

obtained

at39

0°C

and25

MPa

Pressure:25

35MPa

Reactor:Batch

7Chen

etal.[18]

Hyd

rothermal

liqu

efaction

ofmixed

culture

alga

lbiom

assfrom

waste

water

treatm

entsystem

into

bio-crudeoil

Feedstockfrom

Onewater

INC.

Indianap

olis

Tem

p:26

0–32

0°C

HHVva

lues

of33

.3MJ/Kgisviab

lewithhyd

rocarbon

s,fattyacids,

cyclic

amines.

Pressure:1MPa

Reactor:Batch

8Costanzo

etal.[97]

Effectof

low

temperature

hyd

rothermal

liqu

efaction

oncatalytic

hyd

roden

itrogenationof

alga

ebiocrudean

dmod

elmacromolecules

Sorokiniana,

minutissim

a,bijuga

Tem

p:22

5°C

Bio

oilwithsimilar

compositionto

gasoilob

tained

viaHTL/H

DO

process

usingRu/C

catalyst.

Pressure:20

.7ba

rReactor:Batch

9Dav

idet

al.[106

]Review

andexperim

entalstudyon

pyrolysis

andhyd

rothermal

liqu

efaction

ofmicroalga

eforbiofuel

production.

Nan

nochloropsis

Tem

p:25

0°C

Algal

HTLis

very

han

dywhen

compared

topyrolysis

interm

sof

yield.

Pressure:10

25MPa

Reactor:

Con

tinuou

s10

Ebo

ibiet

al.[107

]Hyd

rothermal

liqu

efaction

ofmicroalga

eforbiocrudeproduction:

improvingthebiocrudeproperties

withva

cuum

distillation

Tetraselm

is,Sp

irulina

Tem

p:30

0–35

0°C

ThehighestHHVof

40MJ/kg

was

obtained

aftertheprocess

for

thesp

ecified

feed

stock.

Pressure:30

bar

Reactor:Batch

11Guoet

al.[25]

Areview

ofbio-oilproductionfrom

hyd

rothermal

liqu

efaction

ofalga

eAlgal

feed

stock

Tem

p:43

0–53

0°C

Freefattyacids,

phen

olsan

darom

atic

compou

nds.

Pressure:24

34MPa

Reactor:Batch

12Guoet

al.[108

]Hyd

rothermal

liqu

efaction

ofcyan

ophyta:

Evo

lution

ofpoten

tial

bio-

crudeoilproductionan

dcompon

entan

alysis

Cyanop

hyta

Tem

p:37

0°C

Hightemperaturesfavo

uredphen

ols,

benzenes,alka

nes

andfatty

acidsan

dlow

temperaturesfavo

uredalka

nes

andheterocyclic

compou

nds.

Pressure:1.5P

siReactor:Batch

13Haa

rlem

mer

etal.

[109

]Analysis

andcomparison

ofbiooils

obtained

from

hyd

rothermal

liqu

efaction

andfast

pyrolysis

ofbe

achwoo

dBeech

woo

dTem

p:30

0°C

Highiodineva

luebiooilis

obtained

Pressure:1MPa

Reactor:Batch

14Had

hou

met

al.[110

]Hyd

rothermal

liqu

efaction

ofmillwaste

water

forbio-oilproductionin

subc

riticalconditions

Oilmillwaste

water

Tem

p:20

0–30

0°C

Amax

imum

yieldof

58wt%

was

achievedhav

ingmajoritycontent

ofphen

olics.

Pressure:19

0ba

rReactor:Batch

15Heet

al.[15]

Con

tinuou

shyd

rothermal

liqu

efaction

ofmacro

alga

ein

thepresence

oforga

nic

co-solvents

Oed

ogon

ium

Tem

p:30

0–35

0°C

Presence

ofco

solven

thas

minor

effect

ontheproduct

yield.

Pressure:10

bar

Reactor:Batch

16Hietala

etal.[95]

Aqu

antitative

kinetic

mod

elforthefast

andisothermal

hyd

rothermal

liqu

efaction

ofNan

nochlorosisSp

Nan

nochlorosisSp

Tem

p:10

0–40

0°C

Bio

crudeyieldas

highas

46%

isachieva

bleat

400°C

and1min

residen

cetime.

Pressure:40

0ba

r(con

tinued

onnextpage)

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Table

2(con

tinued

)

S.No

Auth

or

Desc

ription

Feed

Pro

cess

conditions

Pro

ducts

Reactor:Batch

17Hog

non

etal.[111

]Com

parison

ofpyrolysis

andhyd

rothermal

liqu

efaction

ofChlamyd

omon

asreinhardtii.Growth

studieson

therecovered

hyd

rothermal

aqueo

usphases

c.reinhardtii

Tem

p:22

0–31

0°C

Yield

ofbio-oilishigher

inpyrolysisan

den

ergy

ratios

arehigher

inHTL.

Pressure:10

MPa

Reactor:Batch

18Gao

etal.[17]

Bio-oilproductionfrom

eigh

tselected

greenlandscap

ingwastesthrough

hyd

rothermal

liqu

efaction

Lan

dscap

ewaste

leav

esTem

p:30

0°C

Thepresence

ofva

lue-ad

ded

chem

icals,

phen

olics,

ketones,esters,

acids,

andalcohols,

inbio-oils

areconfirm

edPressure:2MPa

Reactor:Batch

19Lav

anya

etal.[9]

Hyd

rothermal

liqu

efaction

offreshwater

andmarinealga

lbiom

ass.

Arthrosp

iraPlatensis,

tetraselmis

spTem

p:20

0–35

0°C

Introd

ucedaprocedure

toblen

dalga

lcrudeto

petrocrudean

dyielding18

%dieselfraction

.Pressure:18

0ba

rReactor:Batch

20Lyu

etal.[112

]Twostag

enan

ofiltrationprocess

forhigh-valuech

emical

production

from

hyd

rolysatesof

lign

ocellulose

biom

assthrough

hyd

rothermal

liqu

efaction

Ricestraw

Tem

p:30

0°C

TNSF

hyd

rolysatesinto

threeparts:su

garconcentrates,mon

ophen

ols,

cyclop

entanon

es,acid

acids.

Pressure:12

MPa

Reactor:Batch

21Mad

diet

al.[99]

Quan

titative

characterization

oftheaq

ueo

usfraction

from

hyd

rothermal

liqu

efaction

ofalga

eChlorella,

Scen

edesmusob

liqu

es,

Tetraselm

isTem

p:35

0°C

Aceticacid,propan

icacid,pyridine,

aceton

e,ethan

olan

dother

orga

nic

chem

ical

compou

ndsarequ

antified

.Pressure:20

.7MPa

Reactor:

Con

tinuou

s22

Meryemog

luet

al.

[113

]Biofuel

productionby

liqu

efaction

ofKen

afbiom

ass

Ken

afan

dwheatstraw

biom

ass

Tem

p:20

0–35

0°C

Higher

yieldsareseen

at30

0°C

andreducedthereafter.

Pressure:5MPa

Reactor:Batch

23Nazariet

al.[114

]Hyd

rothermal

liqu

efaction

ofwoo

dybiom

assin

hot

compressed

water:

catalyst

screen

ingan

dcomprehen

sive

characterization

ofbio-crudeoils

Birch

woo

dsaw

dust

Tem

p:30

0°C

Occurence

ofphen

olic

derivatives

andaliphatic

compou

nds

increasedsign

ifican

tlyin

thepresence

ofcatalyst

than

withou

tcatalyst.

Pressure:90

bar

Reactor:Stirred

reactor

24Neveu

xet

al.[12]

Bio

crudeyieldan

dproductivityfrom

thehyd

rothermal

liqu

efaction

ofmarinean

dfreshwater

greenmicroalga

eOed

ogon

ium,Derbe

sia,

Ulva

Tem

p:35

0°C

Derbe

sia

>Ulva

>Oed

ogon

ium.This

isthesequ

ence

ofthe

higher

biocrudeproduced

Pressure:25

0ba

rReactor:Batch

25Patilet

al.[115

]Hyd

rothermal

liqu

efaction

ofwheatstraw

inhot

compressed

water

and

subc

riticalwater-alcoh

olmixtures

Wheatstraw

Tem

p:35

0°C

Amax

imum

of28

MJ/kg

HHV

isob

tained

.Pressure:20

0ba

rReactor:Tubu

lar

26Ped

ersenan

dRosen

dah

l[116

]Productionof

fuel

range

oxyg

enates

bysu

percritical

hyd

rothermal

liqu

efaction

oflign

ocellulosicsystem

sAsp

enwoo

dTem

p:40

0°C

Themajoritygrou

psob

tained

arecyclop

entanon

esan

dox

ygen

ated

arom

atics.

Pressure:30

0ba

rReactor:Batch

micro

27Ped

ersenet

al.[13]

Con

tinuou

shyd

rothermal

co-liquefaction

ofaspen

woo

dan

dglycerol

withwater

phaserecirculation

Asp

enwoo

dan

dglycerol

mixture

Tem

p:40

0°C

Bio

crudewithhighqu

alityof

34.3

MJ/kg

HHVva

lue,an

dva

luab

lech

emicalsin

therange

ofC6-C

12similar

toga

soline.

Pressure:30

0ba

rReactor:

Con

tinuou

s28

Raiko

vaet

al.[21]

Assessinghyd

rothermal

liqu

efaction

fortheproductionof

bio-oilan

den

han

cedmetal

recovery

from

microalga

ecu

ltivated

onacid

mine

drainag

e

Arthrosp

iraplatensis,

Chlamyd

omon

assp

Tem

p:31

0–35

0°C

HTLproducedbio-oilforupgrad

ingprocess

from

theacid

mine

drainag

ealso

theprevention

ofAMD.

Pressure:12

0ba

rReactor:Batch

29Red

dyet

al.[117

]Tem

perature

effect

onhyd

rothermal

liqu

efaction

ofNan

nochloropsis

gaditan

aan

dChlorellasp

Nan

nochloropsisga

ditan

aan

dChlorellasp

Tem

p:30

0°C

Higher

yieldsof

HHVof

39MJ/kg

ispossiblewiththefeed

stock.

Pressure:20

0Psi

Reactor:Batch

30Sh

akya

etal.[118

]Effectof

temperature

andNa 2CO3catalyst

onhyd

rothermal

liqu

efaction

ofalga

eNan

nochloropsis,

Pav

lova

,Isochrysis

Tem

p:25

0–35

0°C

Bio

oilwithheatingva

lueof

37MJ/kg

isob

tained

whichis

equivalen

tto

heavy

crudeoil.

Pressure:35

Psi

Reactor:Batch

31Singh

etal.[119

]Catalytic

hyd

rothermal

liqu

efaction

ofwater

hyacinth

Water

hyacinth

Tem

p:25

0–30

0°C

Max

imum

bio-oilyieldof

23%

isob

tained

usingcatalyst

KOH

and

K2CO3withless

oxyg

en.

Pressure:13

00Psi

Reactor:Batch

32Singh

etal.[120

]Hyd

rothermal

liqu

efaction

ofrice

straw:Effectof

reaction

environmen

tRicestraw

Tem

p:28

0–32

0°C

Bio

oilyieldof

17%

and78

%conversionwithether

solublebio-oil

under

O2en

vironmen

t.Pressure:6–9MPa

(con

tinued

onnextpage)

A.R.K. Gollakota et al. Renewable and Sustainable Energy Reviews 81 (2018) 1378–1392

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Table

2(con

tinued

)

S.No

Auth

or

Desc

ription

Feed

Pro

cess

conditions

Pro

ducts

Reactor:Autoclav

e33

Sudasingh

eet

al.

[121

]Hyd

rothermal

liqu

efaction

oilan

dhyd

rotreatedproduct

from

pine

feed

stockch

aracterizedby

heteronucleartw

odim

ension

alNMR

spectroscopyan

dFT-ICR

masssp

ectrom

etry

Pine

Tem

p:40

0°C

Fusion

ofFT-ICR

further

simplified

iniden

tification

ofthe

compou

ndspresentin

thebio-oilob

tain

through

HTLprocess.

Pressure:30

00Psi

Reactor:

Con

tinuou

s34

Tek

inet

al.[122

]Hyd

rothermal

liqu

efaction

ofbe

achwoo

dusinganaturalcalcium

borate

mineral

Beach

woo

dTem

p:25

0–35

0°C

Mostof

theproduct

stream

isof

phen

ols,withan

optimum

HHVof

23.81M

J/kg

Pressure:4–

16.5

MPa

Reactor:Batch

35Tianet

al.[123

]Hyd

rothermal

liqu

efaction

ofharvested

high–ashlowlipid

alga

lbiomass

from

Dianch

ilake

:Effects

ofop

erational

param

etersan

drelation

sof

products

Algal

bloo

msof

Dianch

ilake

Tem

p:26

0–34

0°C

18.4%

yieldof

biocrudewithhighestcontentof

ash41

.6%

isob

tained

through

thefeed

stock.

Pressure:3MPa

Reactor:Batch

36Tran[124

]Fasthyd

rothermal

liqu

efaction

forproductionof

chem

icalsan

dbiofuels

from

wet

biom

assusingaplugflow

reactor

Wet

slurryfeed

Tem

p:37

4°C

Possiblech

allengesan

dcu

rren

tstatusof

possiblesolution

sto

the

challenges,

focu

singon

theneedof

develop

ingasp

ecialplug-flow

reactorforscalingupof

theHTLprocess

Pressure:22

.1MPa

Reactor:Plugflow

reactor

37Valdez

etal.[20]

Hyd

rothermal

liqu

efaction

ofnan

nochlorpsissp

:Sy

stem

atic

studyof

process

variab

lesan

dan

alysis

oftheproduct

fraction

sNan

nochlorpsissp

:Tem

p:25

0–40

0°C

Pressure:30

000P

siReactor:Batch

38Vardon

etal.[14]

Thermochem

ical

conversionof

raw

anddefattedalga

lbiom

assvia

hyd

rothermal

liqu

efaction

andslow

pyrolysis

Scen

edesmus,

Spirulina

Tem

p:30

0–45

0°C

Wet

alga

lbiomassfavo

urs

theHTLprocess

that

yieldshigher

HHV

values

of35

–37

MJ/kg

Pressure:10

12MPa

Reactor:ba

tch

39Wan

get

al.[125

]Hyd

rothermal

liqu

efaction

ofLitseaCube

baseed

toproduce

bio-oil

LitseaCube

baTem

p:29

0°C

Theliqu

efiedbio-oilwas

characterizedin

higher

C,H

,contentan

dmuch

lower

Ncontent.

Pressure:–

Reactor:Batch

40Wan

get

al.[126

]Hyd

rothermal

liqu

efaction

oflign

ite,

wheatstraw

andplastic

waste

insu

bcritical

water

foroil:product

distribution

Lignite,

wheatstraw

Tem

p:26

0–32

0°C

Addingtourm

alineduringHTLincreasestheoilyield,higher

conversionrates.

Pressure:2–5MPa

Reactor:Batch

41Xuan

dEtcheverry

[127

]Hyd

roliqu

efaction

ofwoo

dybiom

assin

suban

dsu

per

critical

ethan

olwithiron

basedcatalysts

Jack

pinewoo

dTem

p:47

3–62

3K

Highyieldbio-oilof

63%

withFeS

O4catalyst

withdom

inan

tphen

olic

compou

nds.

Pressure:2–

10MPa

Reactor:Batch

42Xuet

al.[89]

Hyd

rothermal

liqu

efaction

ofChlorellapyren

oidosaforbio-oil

productionov

erCe/HZSM

-5Chlorellapyren

oidosa

Tem

p:30

0°C

Zeo

lite

Ce/HZSM

-5exhibitsgo

odpoten

tial

forpreparationof

bio-

oilfrom

microalga

ewithhighefficien

cyPressure:

Reactor:Autoclav

e43

Yan

etal.[128

]Com

positionof

thebio-oilfrom

thehyd

rothermal

liqu

efaction

ofduck

weedan

dtheinfluen

ceof

theextraction

solven

tsDuckweed

Tem

p:35

0°C

Extractionsolven

tswithhighpolarityyieldshigher

%of

biooilof

26%.

Pressure:5kP

aReactor:Batch

44Yan

get

al.[16]

Hyd

rothermal

liqu

efaction

ofsp

entcoffee

grou

ndsin

water

med

ium

for

bio-oilproduction

Spen

tcoffee

grou

nd

Tem

p:20

0–30

0°C

Amax

imum

of31

MJ/kg

HHV

valueof

biooilis

form

edPressure:0.5–

2MPa

Reactor:Autoclav

e45

Yim

etal.[129

]Metal

oxidecatalysedhyd

rothermal

liqu

efaction

ofMalaysian

oilpalm

biom

assto

bio-oilunder

super

critical

conditions.

Malaysian

oilpalm

Tem

p:39

0°C

Thepresence

ofphen

ols,

ketones,arom

atic

carbox

ylic

acidsare

confirm

ed.

Pressure:25

MPa

Reactor:Batch

46Zhan

get

al.[130

]Hyd

rothermal

liqu

efaction

ofChlorellapyren

oidosain

Ethan

ol-w

ater

for

biocrudeproduction

Chlorellapyren

oidosa

Tem

p:28

0°C

Ethan

olwater

solution

has

best

yieldof

57.3

wt%

biocrude.

Pressure:1MPa

Reactor:Batch

47Zhan

get

al.[131

]Thermograv

imetrican

dkinetic

analysis

ofbiocrudefrom

hyd

rothermal

liqu

efaction

ofEnteromorphaprolifera

Enteromorphaprolifera

Tem

p:57

3K

Atw

ostep

mechan

ism

willb

eabe

tter

persp

ective

inop

timizingthe

kineticsof

HTLprocess.

Pressure:1MPa

Reactor:Batch

48Zhen

get

al.[132

]Alkalinehyd

rothermal

liqu

efaction

ofsw

inecarcassesto

bio-oil

Swinecarcasses

Tem

p:25

0°C

62.2

wt%

ofbio-oilan

d22

wt%

solidresidueis

obtained

Pressure:–

Reactor:Batch

(con

tinued

onnextpage)

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process. Tian et al. [156] presented review on HTL from algalprospective for algal biorefinery including the factors such as feedstockpreparation, scale-up of algae HTL and process integration. Guo et al.[25] also presented the details of research works pertaining toproduction of bio-oil from HTL of algae and reported that the proper-ties of resulting bio-oil from HTL are affected by temperature, reactiontime, algae species, algae concentration, reaction atmosphere, catalystsand sub and supercritical water reaction conditions. Elliott et al. [80]presented the review of research papers of HTL with aim to describeevolution of HTL processes from batch to continuous state. Furtherthey described the mass and energy balances from the existing processmodels which are used for process costs calculations with the aim toprovide optimum way for commercial likelihood of technology. Jindaland Jha [81] reviewed effects of process variables such as biomasscomposition, temperature, residence time, pressure, biomass heatingrate, particle size, catalysts, etc. on the yield and quality of bio oil.Dimitriadis and Bezergianni [147] presented review on HTL of variousfeedstock such as woody biomass, wastes, plastics and microalgae forbio-crude production through HTL. On the other hand, this articlebriefly reviewed the elemental composition of bio-crude obtained byHTL, different types of feedstock adopted for HTL, mechanism of HTLprocesses, possible process flow diagrams for HTL of both wet and drybiomass and energy efficiency of the process. In addition, this articlealso enlisted a possible future research scope for concerned research-ers.

3. HTL process mechanism

The mechanism of the hydrothermal liquefaction has not beenelucidated much in the literature. The pathway of HTL comprises threemajor steps, depolymerisation followed by decomposition and recom-bination [19]. The details of these are explained in the further sections.Briefly, biomass is decomposed and depolymerized in to small com-pounds. These compounds may be highly reactive, thus polymerizingand forming bio crude, gas and solid compounds is essential. Furtherthe critical process parameters such as temperature, residence time,the process of repolymerization, condensation and decomposition ofthe components from the different phases may vary accordingly. Sincebiomass is a complex mixture of carbohydrates, lignin, proteins, andlipids, the reaction chemistry and mechanisms of biomass liquefactionare consequently also complex [135,136]. Fig. 1 presents the schematicoverview of the reaction pathway and the details of the steps areenlisted [137].

3.1. Depolymerisation of the biomass

Depolymerisation of biomass is a sequential dissolving of macro-molecules through utilization of their physical and chemical properties.The intrinsic hemicellulose and cellulose biopolymers contributespositively towards the thermal stability of the biofuel [138].Depolymerisation process overcomes the difficulties and obstinateproperties of lignocellulose biomass that mimics the natural geologicalprocesses of producing fossil fuels. The decisive parameters tempera-ture and pressure changes the structure of the long chain polymersconsisting of hydrogen, oxygen, and carbon to shorter chain hydro-carbons [139]. Further, the energy contents of the organic materials arerecycled in the presence of water.

3.2. Decomposition of the biomass monomers by cleavage,dehydration, decarboxylation and deamination

This step involves the loss of water molecule (dehydration), loss ofCO2 molecule (decarboxylation) and removal of amino acid content(deamination) [140]. The dehydration and decarboxylation facilitatethe removal of oxygen from the biomass in the form of H2O and CO2

respectively. Biomass comprising macromolecules are hydrolysed toTable

2(con

tinued

)

S.No

Auth

or

Desc

ription

Feed

Pro

cess

conditions

Pro

ducts

49Zhuet

al.[98]

Hyd

rothermal

liqu

efaction

ofba

rley

straw

tobio-crudeoil.Effects

ofreaction

temperature

andaq

ueo

usphaserecirculation

'sBarleystraw

Tem

p:28

0–40

0°C

Thecrudebio-oilcompositionis

adjusted

byreducingtheam

ount

ofphen

olsan

dacids

Pressure:35

0ba

rReactor:Batch

50Zhuet

al.[133

]Influen

ceof

alka

licatalyst

onproduct

yieldan

dproperties

via

hyd

rothermal

liqu

efaction

ofba

rley

straw

Barleystraw

Tem

p:30

0°C

Morephen

olic,less

carbox

ylic

compou

ndswithcatalyticactivity

andhighcarbon

anden

ergy

recovery

withou

tan

ycatalyst

isob

served

.Pressure:90

112ba

rReactor:Autoclav

e

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form polar oligomers and monomers [141]. Water at high tempera-tures and pressure breaks down the hydrogen bonded structure ofcellulose and causes the formation of glucose monomers. Becausefructose is more reactive than glucose, it rapidly degrades in plethora ofproducts by the different types of reactions, including isomerization,hydrolysis, dehydration, reverse-aldol defragmentation, rearrangementand recombination reactions [142]. The majority of the degradationproducts such as polar organic molecules, furfurals, glycoaldehydes,phenols and organic acids are highly soluble in water.

3.3. Recombination and repolymerization of reactive fragments

This is the third step in which the reverse to the initial processingsteps are happening due to the unavailability of the hydrogen com-pound [19]. If hydrogen is freely available in the organic matrix for theliquefaction process the free radicals will be capped yielding the stablemolecular weight species. At conditions the unavailability of thehydrogen or the concentration of the free radicals are excessively large,the fragments are recombined or repolymerized to form high molecularweight char compounds otherwise noted as coke formation [143].

3.4. Hydrothermal liquefaction process

Hydrothermal liquefaction is a biomass to bio-liquid conversionroute carried out in water at moderate temperature of 280–370 °C and

high pressures (10–25 MPa) that has a liquid bio crude as mainproduct along with the gaseous, aqueous and solid phase byproducts[144]. The product stream of this process have high energy content andunique feature of enhanced heat recovery in comparison to otherprocesses [145]. Many complex reactions take place during thetransformation of biomass into crude oil like products [146]. In thisregard, the process mechanism is classified for two types of feedstocknamely lignocellulose biomass (dry feedstock) and algal biomass (wetfeedstock). The sub classification or the major fractions of the dry/lignocellulose biomass is hemicellulose, cellulose and lignin [147]. Onthe other hand, the wet feed stock composition comprises of lipids,proteins, carbohydrates and algaenans. The description of HTL of thedry and wet feedstock of biomass are presented herein.

3.4.1. HTL of lignocellulose biomassThe reactor design in the hydrothermal processing can be either

batch or continuous. Continuous reactors require feeding system thatoperate under pressure and include either slurry based pump or lockand hopper systems for large particles. The detailed pathway of thebiomass to bio-crude through hydrothermal liquefaction of lignocellu-lose biomass was shown in Fig. 2 adopted from Biller and Ross [148].The feedstock requires pre-treatment especially the woody biomass forthe reasons of reducing the particle size, removing the contaminants,and alkaline treatment to obtain a stable slurry for easy pumping. Thefeedstock is then processed via HTL at temperature of around 350 °C

Fig. 1. Reaction pathway of the hydrothermal liquefaction.

Biomass/Wet Waste Pre-treatment Hydrothermal

LiquefactionPhase

Separation Hydrotreating

Anaerobic Digestion/Hydrothermal gasification

Aqueous Phase

Aqueous Fertilizer Process Heat andPower Integration

H2

WaterRecirculation

Biochar/fertilizer

Hydrocarbon Fuels

Fig. 2. Process flow diagram of HTL process of lignocellulose biomass adopted from Biller and Ross [148].

Water &NutrientsWater &Nutrients

AlgaeCultivation Water Removal Hydrothermal

Liquefaction Hydrotreating

Catalytic HydrothermalGasification

Hydrocarbon Fuels

H2

Process Heatand PowerIntegration

Aqueous Phase

Solids, P recycle

Nutrients & CO2

CO2

Fig. 3. Process flow diagram of HTL process of algal biomass/wet biomass adopted from Biller and Ross [148].

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and a pressure of 150 bar for 15 min approximately. Phase separationoccurs spontaneously at these operating conditions resulting thegaseous stream of CO2, solid residue, bio-crude and small traces ofaqueous phase [149]. The aqueous phase/water can be recirculated toHTL unit which reduces the water requirement and enhance the bio oilyield. The other stream of the water that is generated through HTLprocess can be treated anaerobically or via catalytic hydrothermalgasification technique to produce methane rich or hydrogen richsyngas. Anaerobic digestion of the water from the HTL process can’tbe treated to full extent due to the presence of phenols and furfuralsthat delimits the anaerobic digestion process.

During the phase separation process the obtained solid phasematerial can be directly used as a bio char/fertilizer. The producedbio-crude may not be directly used as an alternate which requiresfurther hydrotreatment for commercial utilization. However, compli-cated reaction mechanism is not required for the upgrading procedureas the bio-crude obtained through HTL is less in moisture, oxygencontent and hence the fine hydrotreatment will enhance the quality ofbio-crude. Finally, the amount of the heat generated through the entireprocess can be efficiently utilized to operate the hydrothermal gasifierthat refines the process economy.

3.4.2. HTL of wet/algal biomassThe major benefit of processing algae/wet biomass is the potential

for recycling of nutrients back to cultivation. The procedure of treatingwet biomass is similar to that of treating lignocellulose with a fewmodifications. The schematic of the procedure treating the wet/algalfeedstock is presented in Fig. 3 adopted from Biller and Ross [148].

The major difference lies in treating the wet feedstock compared to dryfeedstock is ignoring the pre-treatment step.

Generally, pre-treatment is essential as the particle size of the microalgae is quite small compared to lignocellulose that eliminates thecomplexities of pumping slurries to the reactor. Further, dewateringprocedure at harvesting step tends to produce the feedstock slurry with20% solids. Then the slurry is passed through the HTL reactor yieldsbio crude that has to be hydro-treated further to produce hydrocarbonfuels. During the HTL process the aqueous phase generated isrecirculated back to the algae cultivation procedure, CO2 that isreleased can be utilized in the process of photosynthesis in the growthof algae for next batch. During hydrotreatment the nutrients areseparated that are sent back to the algae cultivation procedure. Thisovercomes the shortfalls of the HTL process economy.

4. Energy efficiency of HTL process

The ultimate target of the hydrothermal liquefaction procedure is toconvert the biomass to bio crude that can be utilized as an alternate tothe commercial fossil fuels. However, the economy of the process ishighly questionable due to the utilization of higher pressure conditions.Fig. 4 describes the utilization of various product streams that canaffect the energy efficiency in terms of materials and feedstock. HTL ofwet biomass i.e., algal feedstock is a multifaceted processing techniquethat can generate the nutrients which can be recycled for the growth ofalgae, waste water can be used for the water requirements and CO2 forthe photosynthesis reaction.

It has the potential to bottleneck the current algal refiningprocedure including consumption of water, fertilizer and energy input.One of the cutting edge benefits of this HTL process is it consumes 10–15% of the energy in the feedstock biomass yielding energy efficiency of85–90%. HTL can recover more than 70% of the feedstock carboncontent that can be utilized for the carbon capture procedures. Theother technical edge of this process is the bio-crude that is obtainedfrom this process doesn’t require much treatment/upgrading proce-dures for the commercial utilization. From Fig. 4, it is seen that severalby-products are obtained through this HTL process like fertilizer in theform of a solid content, bio crude alternate to fossil fuels, the processedwater can be treated for the utilization and the nutrient cycle for the

Fig. 4. Schematic of Energy efficient usage HTL process using algal biomass. This figure was drawn from Refs. [150–156].

Table 3Comparison of bio-crude by HTL and pyrolysis adopted from Elliot et al. [157].

Elemental composition Hydrothermal liquefaction Pyrolysis

C (wt%) 73 58H (wt%) 8 6O (wt%) 16 36S (ppm) < 45 29Moisture 5.1 24.8HHV (MJ/kg) 35.7 22.6Viscosity (cPs) 15,000 59

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regeneration of the algal growth. A comparison on the bio-crudesobtained via pyrolysis and hydrothermal liquefaction procedures areshown in Table 3 whereas, the major product compounds obtained byHTL are presented in Table 4. From Table 3 it can be observed thatexcept the sulphur contents and viscosity, the performance of HTL issuperior to pyrolysis.

5. Conclusion

Because of the ordinant dictations for the fuels, the alarming levelsof CO2 emissions into atmosphere, and depletion of conventional fossilfuels the desideratum for the renewable fuels is evident. In this context,biomass derived fuels seems to be the promising path which isrenewable and redundant. Various techniques are available for thebiomass processing such as pyrolysis, transesterification, hydrothermalliquefaction, steam reforming, etc. However, bio-oil (or bio-crude)obtained from various process suffers from several demerits such ashigh oxygen content, rendering its acidic value, instability, miscibility,low heating values, etc. Hence utilization of bio-crude requires theoptimal processing technique to efficiently convert the biomass to bio-crude i.e., an alternate for future use. Amongst the aforementionedtechniques hydrothermal liquefaction of biomass seems to be thepromising route for the engenderment of bio-oil equipollent to

conventional crude oil. Briefly, this article enlightened the elementalcomposition of bio-crude obtained by HTL, different types of feedstockadopted for HTL, mechanism of HTL processes, possible process flowdiagrams for HTL of both wet and dry biomass; advantages/disadvan-tages and energy efficiency of the process. Finally, challenges stillsubsist with this field which could serve as future scope for concernedresearchers. A very few of these challenges are listed below:

1. Set up an HTL pilot plant by analyzing the effects of feedstock (wetbiomass) conversion efficiency.

2. Analyze the complexities of the critical parameters like temperature,pressure and the residence time for HTL of a given feedstock.

3. Examine possible pathways for optimized conversion via HTL (ofboth wet and dry biomass feedstock and their mixtures).

4. Explore the relationships between bio-crude oil yield and valueadded chemical species and study the effects of catalyst on produc-tion of individual specific chemical compounds.

5. Investigate the reaction pathways of HTL process of model com-pounds as well real biomass.

6. Develop theoretical, especially computational fluid dynamics based,models to analyze the complex inherent properties like thermody-namic properties of the bio-crude, viscosity effects etc. so that tooptimize the processing parameters.

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Table 4Major product compounds of bio-oil obtained by HTL process.

Product compounds Reference

MonoaromaticsPhenol Duan and Savage [158]Benzene/Toluene/Styrene Ross et al. [75]Cholesterol and Cholestene Jena and Das [77]Vitamin E Zou et al. [76]Fatty AcidsMyristic acid Brown et al. [159]Palmitic acid Shuping et al. [160]Steric acid/oleic acid Valdez et al. [161]Tetradecanoic and Octanoic acid Biller and Ross [40]Hexadecanoic acid Jena et al. [162]Arachidic acid Duan and Savage [158]Eicosapentaenoic acid Brown et al. [159]Alkane/AlkeneHexadecane/hexadecane Yang et al. [163]Heptadecane/Heptadecene Biller and Ross [40]Pentadecane/Pentadecene Zou et al. [76]Phytane/Phytene Shuping et al. [160]Docosane and Cholestane Valdez et al. [161]Cycloalkane Anastasakis and Ross [24]Eicosane, Coprostane, Triconate, Hentriaconate,

DotriaconateDuan and Savage [158]

Polyaromatic compoundsNaphthalene Yang et al. [163]Quinoline Jena et al. [162]Indene Brown et al. [159]Anthracene and Phenanthrene Yang et al. [163]Pyrene and carbozole Zhou et al. [164]Fluorene Duan and Savage [158]Nitrogen compoundsPiperidines Jena and Das [77]Pyrrols/Pyrrolidines Biller and Ross [40]Indoles Yuan et al. [100]Pyridines Valdez et al. [161]Pyrazines Zhou et al. [164]Pyrrolidinones Shuping et al. [160]Amides Valdez et al. [161]Amines and nitriles Zou et al. [76]Other Oxygenated compoundsEsters Jena et al. [151]Aldehydes Anastasakis and Ross [24]Ketones Ross et al. [75]Alcohols Yang et al. [165]Acetic acid Jena and Das [77]Furans Jena et al. [162]

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