Accepted Manuscript

Perspectives on Small-scale Integrated Biorefineries Using Supercritical CO2 as a

Green Solvent

Ádina L. Santana, Diego T. Santos, M.Angela A. Meireles

PII: S2452-2236(18)30120-2
DOI: https://doi.org/10.1016/j.cogsc.2018.11.007
Reference: COGSC 227

To appear in: Current Opinion in Green and Sustainable Chemistry

Received Date: 18 October 2018

Accepted Date: 20 November 2018

Please cite this article as: Á.L. Santana, D.T. Santos, M.A.A Meireles, Perspectives on Small-scale
Integrated Biorefineries Using Supercritical CO2 as a Green Solvent, Current Opinion in Green and
Sustainable Chemistry, https://doi.org/10.1016/j.cogsc.2018.11.007.

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Perspectives on Small-scale Integrated Biorefineries Using

Supercritical CO2 as a Green Solvent

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ÁDINA L. SANTANA, DIEGO T. SANTOS, M. ANGELA A. MEIRELES*

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LASEFI/DEA/FEA (School of Food Engineering)/UNICAMP (University of

Campinas) Cidade Universitária “Zeferino Vaz”, Rua Monteiro Lobato, 80,

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Campinas 13083-862, Brazil

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Author for correspondence*: maameireles@lasefi.com/LASEFI/DEA/FEA (School of

Food Engineering)/UNICAMP (University of Campinas) Cidade Universitária

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“Zeferino Vaz”, Rua Monteiro Lobato, 80, Campinas 13083-862, Brazil. Phone:
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055.19.3521.0100
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Abstract

Recent demands for the reduction and reutilization of waste have motivated scientific

research on the development of clean technologies and optimization of process

parameters to achieve sustainable production. In this context, this review aims to

provide some perspective about the applications of integrated techniques for biorefining

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of plant matrices into marketable products using supercritical carbon dioxide as a green

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solvent. Considering that Brazil has enormous potential for biorefining of renewable

raw materials, extensive scientific investigations have been performed recently to

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produce a wide variety of products from plant matrices, including high-quality extracts,

biopolymers and particle devices, with the aim of designing integrated supercritical

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fluid-based small-scale biorefineries. Thus, in this review, a compilation of the main
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recent findings in our laboratory and others are presented in detail.
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Keywords: Supercritical technology; Biorefining; Carbon dioxide; Process intensification; Particle

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formation.
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Abbreviations

COL - Cost of operational labor

COM - Cost of manufacturing
CRM - Cost of raw material
CUT - Cost of utilities

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CWT - Cost of waste treatment
FCI - Fixed capital investment

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GAE - Gallic acid equivalents

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JP - Jabuticaba peels

LPSE - Low pressure solvent extraction

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PLE - Pressurized liquid extraction
PPF - Pressed palm fiber
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RESS - Rapid expansion of supercritical solution
S/F - Solvent mass to feed mass ratio
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SAF - Supercritical antisolvent fractionation

SAS - Supercritical antisolvent
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SC-CO2 - Supercritical carbon dioxide

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SFE - Supercritical fluid extraction

SFEE - Supercritical fluid extraction from emulsions
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SWH - Subcritical water hydrolysis

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1. Introduction

An important challenge for the food industry is the reduction or elimination of wastes

through intensified use of raw materials to obtain high value-added products. The

employment of clean and economically feasible technologies contributes to the recovery of

such materials for inclusion in human diet as functional ingredients and/or for biorefinery

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purposes as cheaper resources [1-3].

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The concept of biorefinery is defined as sustainable processing of feedstocks for

bioenergy and biochemical purposes resulting in various marketable products, such as

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natural dyes, antioxidants, proteins for food and feed, lipids for biodiesel, and carbohydrates

as feedstock for bioethanol production [4-6].

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Recently, supercritical carbon dioxide (SC-CO2) has been utilized as a key green
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solvent in biorefining for the extraction and recovery of products with active properties
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inherent to various plant matrices, such as lipids from algae [7], waxes from date palm

leaves [8], polyphenols from buckwheat flowers [9] and hulls [10], volatile oils [11]**,
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pigments [12]**, starches [13]**, and particle devices from turmeric [14, 15].
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Rather than a stand-alone technology, the utilization of supercritical technology, i.e.,

processes that use supercritical fluids and pressurized liquids, as part of an integrated
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biorefinery is a recent trend for obtaining nutraceuticals [16]** and has been shown to have

a positive effect on the efficiency of processing different solid matrices [17]**.

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This review examines the current research scenario that justifies the biorefining of

crude and waste plant matrices with the use of supercritical CO2 as the first procedure for

integrated and sustainable processing of valuable constituents from these products. In

addition, this work highlights perspectives on the potential of waste matrices to produce

value-added products to replace crude ones as part of an economically feasible integrated

biorefinery. The period reviewed includes the past two years.

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2. Integrated and nonintegrated extraction methodologies applied to the recovery of

valuable products from plant matrices

Process intensification provides great opportunities to drastically improve the

performance of chemical processes [18]**. Supercritical fluid extraction (SFE)

integrated with pressurized liquid extraction (PLE) has been extensively studied as an

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efficient alternative to recover a wide variety of products, such as polyphenols from

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cocoa hulls [19] and cannabinoids from hemp wastes [20]. Comparisons have been

established between these techniques and conventional low pressure solvent extraction

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(LPSE) methods, i.e., Soxhlet and maceration, considering efficiency in obtaining

nutraceuticals. The experimental data compiled and shown in Table 1 are organized by

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the raw material common name and the product of interest. The data also include the
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experimental results obtained and the economic results calculated.
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An economic analysis of a process consists of evaluating its feasibility based on

measurements of its inputs and outcomes. This evaluation consists of determining the
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parameters that influence the cost of manufacturing (COM), i.e., fixed capital
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investment (FCI), cost of operational labor (COL), cost of raw material (CRM), cost of

waste treatment (CWT) and cost of utilities (CUT).

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The FCI involves expenses related to the implementation of the production line

(extraction units and other equipment), while the COL is related to the operators of the
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processing units and the CUT considers the energy used in the solvent cycle for steam

generation, water refrigeration and electricity requirements.

Process variables, including temperature, pressure, solvent mass to feed mass ratio

(S/F), and time of extraction highly affect the global extract and nutraceutical yields,

which consequently affect the final value of the COM.

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3. Coupled extraction and particle formation procedures to increase plant

bioactive compound yields

Table 1 also shows recently reviewed applications of coupled extraction and

particle formation from plant matrices. Particle formation is an important procedure for

the separation, stabilization and purification of active constituents of interest to the food

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and nonfood industries.

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Valorization of waste and underutilized raw materials has been proposed through

recovery of bioactive constituents for the formulation of particulate delivery systems.

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For instance, Natolino and coworkers [36] applied supercritical antisolvent fractionation

(SAF) to SFE-grape marc extracts using ethanol as the solvent and SC-CO2 as the

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antisolvent to obtain powdered extracts with enhanced polyphenol composition.
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Afterwards, Guamán-Balcázar and coworkers fractionated mango leaf extracts from
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SFE and PLE processes [33].

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4. Turmeric as a feedstock in a small-scale integrated biorefinery using

supercritical CO2 as a green solvent

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In a biorefinery, one of the most important determinants of success of a plant is a

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high-quality and consistent feedstock supply [1]. Turmeric (Curcuma longa L.) is a

widespread plant in Brazil, but its use is limited to rhizomes, while some countries such
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as Malaysia and India also use turmeric leaves as a spice [37].

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Extraction and other processes that use green solvents such as carbon dioxide,

ethanol and water are relatively new and promising techniques for obtaining valuable

biological substances from different botanical sources [38]. These procedures were

recently successfully applied for polymer modification from waste annatto seeds [39],

curcuminoid and sugar recovery from turmeric wastes [40-41], energy recovery from

paper sludge powder [42], and isolation of phenolic compounds from black carrot [43].
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Integrated processes reusing the SFE turmeric waste fraction [11] for further PLE

procedures have been successfully applied to increase the yield of curcuminoids with

the use of ethanol [12] and the yield of fermentable sugars with the use of hot

pressurized water [44]. In biorefining lignocellulosic materials, the carbohydrates in the

solid matrix are converted into sugars called cellulosic sugars or second-generation

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sugars to produce renewable chemicals and fuels [45].

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Turmeric volatile oils and curcuminoid-rich extracts are extensively used for the

formulation of medicines. Considering the poor stability and bioavailability of these

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constituents, encapsulation techniques using supercritical and compressed fluids are

promising alternatives used to improve the quality of these constituents [46].

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Considering the cited approaches, Figure 1 proposes a chart for biorefining
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turmeric based on our latest research findings [12, 13, 44, 46]. To justify the above
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process, we have previously quantified the degree of bioactive recovery in terms of the

product selling price after each unit process. Therefore, starting from crude turmeric at
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US$ 7.01/kg, we can obtain a curcuminoid-enriched fraction from the SFE-waste

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turmeric worth US$ 17.86/kg using PLE with ethanol as the solvent and subsequent

pressurized hot water extraction of curcuminoids and fermentable sugar fractions that
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retail for US$ 0.43/kg [44], thus significantly increasing the economic value of turmeric

use.
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Turmeric is already used in industry to obtain food coloring and pharmaceutical

products and may become commercially interesting as starch raw material [47]. Starch

is a cheap natural resource widely used in industry. The use of new starches, i.e.,

starches from nonconventional sources, is one of the most established alternatives to

extend the development of new products with functional properties [48].

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Alcázar-Alay and coworkers showed the potential of annatto wastes from

supercritical extraction procedures as a colorant agent, feedstock for sugar production

and complementary starch source [39, 49]**.

The chemical compounds of the volatile fraction extracted from crude turmeric

rhizomes belong to monoterpenes and sesquiterpenes, particularly zingiberene, ar-

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turmerone, α-turmerone and β-turmerone [50]. Aromatic-turmerone (ar-turmerone) is

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one of the sesquiterpenes of great interest due to its anti-inflammatory, antioxidant,

antimicrobial and anticarcinogenic properties [11].

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Curcumin and its two other important analogues, demethoxycurcumin and

bisdemethoxycurcumin, known as curcuminoids, are yellow-colored polyphenols

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responsible for the biological activity of turmeric oleoresin [51]. Experimental evidence
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has indicated beneficial health aspects of turmeric, such as antimicrobial [52], anti-
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inflammatory [53], inhibitory [54], repellent [55], and antitumor [56] activities.
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5. Pressed palm fibers and jabuticaba peels as feedstocks for small-scale integrated
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biorefineries using supercritical CO2 as a green solvent

Scientific investigations carried out by our research group in Brazil include

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obtaining extracts of bioactive constituents from plant matrices and evaluating the

process parameters using integrated or comparative SFE, PLE and LPSE processes [49,
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57-59].

In addition, the production of micro- and nanoparticles of fractionated and

encapsulated compounds has been accomplished using supercritical antisolvent (SAS),

supercritical and compressed antisolvent micronization [60], coprecipitation [46],

fractionation [61], rapid expansion of supercritical solution (RESS), and supercritical

fluid extraction from emulsions (SFEE) [62] techniques and hydrolysis of agroindustrial
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waste using sub/supercritical water + SC-CO2 to produce sugar oligomers [63]. Figure 2

reports a schematic diagram of the other two study cases performed in our research

group, and the reviewed process conditions and results are shown in Table 2.

Pressed palm fiber (PPF), waste from cold-pressing extraction applied to palm

fruits, contains a significant fraction of carotenoids. These materials have a common

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role as feedstocks for fuel production in the palm oil industry. The PPF extracts contain

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more than 5% of the residual oil and high concentrations of free fatty acids, a

characteristic that facilitates carotenoid purification when the SFE process using CO2 as

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a solvent is employed [64].

Water has been applied for the treatment of residues derived from several

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industrial plants and agriculture and municipal wastes. Yields higher than 90% of
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converted material have been obtained under mild conditions using subcritical water
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hydrolysis (SWH), i.e., temperatures up to 200°C and pressures of approximately 20

MPa [65] in the cases of ginger [66] and turmeric [67], to obtain sugars. Nevertheless,
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lower yields of converted materials with SWH have recently been obtained for the
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production of sugar oligomers from beet [68] and peptides from tuna skin collagen [69].

The use of pressurized water has been proposed as an environmentally compatible

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process to integrate the depolymerization–reaction–separation of biomass-supported

processes. Sub/supercritical water is emerging as a green solvent and reaction medium

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capable of providing selective processes while significantly reducing the reaction time,

leading to the possibility of developing compact equipment for use in decentralized

biomass production plants [70].

An effective utilization of PPF using SFE and SWH has been presented. SFE

using CO2 as a solvent of pressed palm fiber provides an oil rich in carotenoids, while

SWH produces hydrolysates with considerable amounts of fermentable sugars [71, 72].
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In addition, pressurized liquid extraction as a complementary alternative for the

recovery of carotenoid-rich extracts from these materials was performed [73] (Figure 2).

For the use of jabuticaba peel (JP) as feedstock in our proposed integrated

biorefinery concept (Figure 2), the use of supercritical CO2 as a solvent also has an

important purpose during the first step in addition to being used during the RESS

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process as a solvent. Anthocyanins are water-soluble pigments present in jabuticaba, a

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plant of the Myrciaria genus native to Brazil. The peels and waste fraction from jelly

industry production are important antioxidant sources for the human diet [76].

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Integrated and nonintegrated supercritical technologies have been applied to

obtain value-added extract products from jabuticaba peels [74, 75, 77] with further

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application in petit-suisse cheese [78] and as particles for application in food and
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nonfood industries [32]** (Table 2).
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Conclusions

The total utilization of plant matrices using multistep procedures for biorefining
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purposes is a feasible alternative for various applications in food, pharmacy, biofuel,

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and energy production.

Contemporary trends in supercritical technology have focused on the development

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of biorefinery concepts applied to waste-biomass constituents and show that this

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technology is efficient when compared to conventional ones in terms of the extraction

yield and recovery of active constituents. New perspectives on how biomasses can be

better valorized with the aid of the SFE process using CO2 as a green solvent were

shown in this article, indicating that SFE can be effectively used during the first step in

biorefinery concepts aiming for full use of biomass prior to its chemical conversion.
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Turmeric, pressed palm fibers and jabuticaba peels were considered as feedstocks in the

proposed small-scale integrated biorefineries using supercritical CO2 as a solvent.

Considering the current increase in the demand for technologies that extend the

use of raw materials, the exploitation of waste fractions using CO2 as a green solvent

may improve economic sustainability for food and nonfood crop production, in addition

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to promoting value-added products, which was demonstrated in this article and should

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be a focus in the future of scientific researchers since the use of SC-CO2 in biorefineries

should be considered key to the integral valorization of biomass.

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Acknowledgements

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Diego T. Santos would like to thank CNPq (processes 401109/2017-8; 150745/2017)
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for the postdoctoral fellowship. Ádina L. Santana would like to thank CAPES
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(1764130) for the postdoctoral fellowship. M. Angela A. Meireles would like to thank

CNPq for the productivity grant (302423/2015-0). The authors acknowledge financial
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support from CNPq (process 486780/2012-0) and FAPESP (processes 2012/10685-8;

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2015/13299-0).
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water and supercritical CO2, J Supercrit Fluid. (2016).
[40] Á.L. Santana, M.A.A. Meireles, Thin-layer chromatography profiles of non-
commercial turmeric (Curcuma longa L.) products obtained via partial hydrothermal

U
hydrolysis, Food Publ. Health. 1 6 (2016) 15-25.
[41] Á.L. Santana, G.L. Zabot, J.F. Osorio-Tobón, J.C.F. Johner, A.S. Coelho, M.
AN
Schmiele, C.J. Steel, M.A.A. Meireles, Starch recovery from turmeric wastes using
supercritical technology, Journal of Food Engineering. 214 (2017) 266-276.
[42] C. Xu, J. Lancaster, Conversion of secondary pulp/paper sludge powder to liquid
M

oil products for energy recovery by direct liquefaction in hot-compressed water, Water
Res. 6–7 42 (2008) 1571-1582.
[43] R. Aşkin Uzel, A practical method for isolation of phenolic compounds from black
carrot utilizing pressurized water extraction with in-site particle generation in hot air
D

assistance, The Journal of Supercritical Fluids. 120, Part 2 (2017) 320-327.

[44] Á.L. Santana, J.F. Osorio-Tobón, F.P. Cárdenas-Toro, C.J. Steel, M.A.A. Meireles,
TE

Partial-hydrothermal hydrolysis is an effective way to recover bioactives from turmeric

wastes, Food Sci Tech. 2 38 (2017) 280-292.
[45] A.K. Chandel, V.K. Garlapati, A.K. Singh, F.A.F. Antunes, S.S. da Silva, The path
EP

forward for lignocellulose biorefineries: Bottlenecks, solutions, and perspective on

commercialization, Bioresour Technol. (2018).
[46] Á.L. Santana, M.A.A. Meireles, Coprecipitation of turmeric extracts and
polyethylene glycol with compressed carbon dioxide, The Journal of Supercritical
C

Fluids. 125 (2017) 31-41.

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[47] M. Leonel, S.B.S. Sarmento, M.P. Cereda, New starches for the food industry:
Curcuma longa and Curcuma zedoaria, Carbohydrate Polymers. 3 54 (2003) 385-388.
[48] Á.L. Santana, M.A.A. Meireles, New Starches are the Trend for Industry
Applications: A Review, Food Publ Health. 5 4 (2014) 229-241.
**[49] S.C. Alcázar-Alay, J.F. Osorio-Tobón, T. Forster-Carneiro, M.A.A. Meireles,
Obtaining bixin from semi-defatted annatto seeds by a mechanical method and solvent
extraction: Process integration and economic evaluation, Food Res Int. 99 (2017) 393-
402.
[50] L. Zhang, Z. Yang, F. Chen, P. Su, D. Chen, W. Pan, Y. Fang, C. Dong, X. Zheng,
Z. Du, Composition and bioactivity assessment of essential oils of Curcuma longa L.
collected in China, Ind Crops Prod. 109 (2017) 60-73.
 ACCEPTED MANUSCRIPT
[51] F. Sahne, M. Mohammadi, G.D. Najafpour, A.A. Moghadamnia, Enzyme-assisted
ionic liquid extraction of bioactive compound from turmeric (Curcuma longa L.):
Isolation, purification and analysis of curcumin, Ind Crops Prod. 95 (2017) 686-694.
[52] A. Gupta, S. Mahajan, R. Sharma, Evaluation of antimicrobial activity of Curcuma
longa rhizome extract against Staphylococcus aureus, Biotech Rep. 6 (2015) 51-55.
[53] D.W. Kim, S.M. Lee, H.S. Woo, J.-Y. Park, B.S. Ko, J.D. Heo, Y.B. Ryu, W.S.
Lee, Chemical constituents and anti-inflammatory activity of the aerial parts of
Curcuma longa, Journal of Functional Foods. 26 (2016) 485-493.
[54] T.T. Dao, P.H. Nguyen, H.K. Won, E.H. Kim, J. Park, B.Y. Won, W.K. Oh,

PT
Curcuminoids from Curcuma longa and their inhibitory activities on influenza A
neuraminidases, Food Chem. 1 134 (2012) 21-28.
[55] N.G. Das, S. Dhiman, P.K. Talukdar, B. Rabha, D. Goswami, V. Veer, Synergistic

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mosquito-repellent activity of Curcuma longa, Pogostemon heyneanus and
Zanthoxylum limonella essential oils, J Infect Publ Health. 4 8 (2015) 323-328.
[56] H.S. Lee, Antiplatelet property of Curcuma longa L. rhizome-derived ar-

SC
turmerone, Bioresour Technol. 12 97 (2006) 1372-1376.
[57] P.I.N. Carvalho, J.F. Osório-Tobón, M.A. Rostagno, A.J. Petenate, M.A.A.
Meireles. Optimization of the ar-turmerone extraction from turmeric (Curcuma longa
L.) using supercritical carbon dioxide. In: 14th European Meeting on Supercritical

U
Fluids. Marseille - France: 2014.
[58] P.F. Leal, M.E.M. Braga, D.N. Sato, J.E. Carvalho, M.O.M. Marques, M.A.A.
AN
Meireles, Functional properties of spice extracts obtained via supercritical fluid
extraction, Journal of Agricultural and Food Chemistry. 51 (2003) 2520–2525.
[59] C.L.C. Albuquerque, M.A.A. Meireles. Estimate of the Cost of Manufacturing
M

(COM) of natural colorants obtained by supercritical fluid extraction. In: II

Iberoamerican Conference on Supercritical Fluids. 2010.
[60] D.T. Santos, M.A.A. Meireles, Micronization and encapsulation of functional
pigments using supercritical carbon dioxide, Journal of Food Process Engineering. 1 36
D

(2013) 36-49.
[61] R.A.C. Torres, Á.L. Santana, D.T. Santos, M.A.A. Meireles, Perspectives on the
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Application of Supercritical Antisolvent Fractionation Process for the Purification of

Plant Extracts: Effects of Operating Parameters and Patent Survey, Recent Pat Eng. 10
(2016) 121-130.
EP

[62] D.T. Santos, D.F. Barbosa, K. Broccolo, M.T.M. Gomes, R. Vardanega, M.A.A.
Meireles, Pressurized organic solvent extraction with on-line particle formation by
supercritical anti solvent processes, Food Publ Health. 6 2 (2012) 231-240.
[63] S.R.M. Moreschi, J.C. Leal, M.E.M. Braga, M.A.A. Meireles, Ginger and turmeric
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starches hydrolysis using subcritical water + CO2: the effect of the SFE pre-treatment,
AC

Brazil. J. Chem. Eng. 2 23 (2006) 235-242.

[64] L.F. França, M.A.A. Meireles, Extraction of oil from pressed palm oil (Elaes
guineensis) fibers using supercritical CO2, Food Sci Technol. 17 (1997) 384-388.
[65] Ž. Knez, M.K. Hrnčič, M. Čolnik, M. Škerget, Chemicals and value added
compounds from biomass using sub- and supercritical water, J Supercrit Fluids. 133
(2018) 591-602.
[66] S.R.M. Moreschi, A.J. Petenate, M.A.A. Meireles, Hydrolysis of Ginger Bagasse
Starch in Subcritical Water and Carbon Dioxide, J Agric Food Chem. 6 52 (2004) 1753-
1758.
[67] S.R.M. Moreschi, J.C. Leal, M.E.M. Braga, M.A.A. Meireles, Ginger and turmeric
starches hydrolysis using subcritical water + CO2: the effect of the SFE pre-treatment,
Braz J Chem Eng. 23 (2006) 235-242.
 ACCEPTED MANUSCRIPT
[68] N. Maravić, Z. Šereš, S. Vidović, A. Mišan, I. Milovanović, R. Radosavljević, B.
Pavlić, Subcritical water hydrolysis of sugar beet pulp towards production of
monosaccharide fraction, Ind Crops Prod. 115 (2018) 32-39.
[69] R. Ahmed, B.-S. Chun, Subcritical water hydrolysis for the production of bioactive
peptides from tuna skin collagen, J Supercrit Fluids. (2018).
[70] D.A. Cantero, M. Dolores Bermejo, M. José Cocero, Reaction engineering for
process intensification of supercritical water biomass refining, J Supercrit Fluids. 96
(2015) 21-35.
[71] F.P. Cardenas-Toro, T. Forster-Carneiro, M.A. Rostagno, A.J. Petenate, F. Maugeri

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Filho, M.A.A. Meireles, Integrated supercritical fluid extraction and subcritical water
hydrolysis for the recovery of bioactive compounds from pressed palm fiber, J Supercrit
Fluid. 93 (2014) 42-48.

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[72] J.M. Prado, T. Forster-Carneiro, M.A. Rostagno, L.A. Follegatti-Romero, F.
Maugeri Filho, M.A.A. Meireles, Obtaining sugars from coconut husk, defatted grape
seed, and pressed palm fiber by hydrolysis with subcritical water, J Supercrit Fluids. 89

SC
(2014) 89-98.
[73] F.P. Cardenas-Toro, S.C. Alcázar-Alay, J.P. Coutinho, H.T. Godoy, T. Forster-
Carneiro, M.A.A. Meireles, Pressurized liquid extraction and low-pressure solvent
extraction of carotenoids from pressed palm fiber: Experimental and economical

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evaluation, Food Bioprod Proc. 94 (2015) 90-100.
[74] D.T. Santos, P.C. Veggi, M.A.A. Meireles, Extraction of antioxidant compounds
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from Jabuticaba (Myrciaria cauliflora) skins: Yield, composition and economical
evaluation, J Food Eng. 1 101 (2010) 23-31.
[75] D.T. Santos, M.A.A. Meireles, Optimization of bioactive compounds extraction
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from jabuticaba (Myrciaria cauliflora) skins assisted by high pressure CO2, Innov Food
Sci Emerg. 3 12 (2011) 398-406.
[76] N.A.V. Dessimoni-Pinto, W.A. Moreira, L.d.M. Cardoso, L.A. Pantoja, Jaboticaba
peel for jelly preparation: an alternative technology, Food Science and Technology. 31
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(2011) 864-869.
[77] D.T. Santos, C.L.C. Albuquerque, M.A.A. Meireles, Antioxidant dye and pigment
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extraction using a homemade pressurized solvent extraction system, Procedia Food Sci.
1 (2011) 1581-1588.
[78] E.P.R. Pereira, J.A.F. Faria, R.N. Cavalcanti, R.K.A. Garcia, R. Silva, E.A.
EP

Esmerino, L.P. Cappato, D.B. Arellano, R.S.L. Raices, M.C. Silva, M.C. Padilha, M.A.
Meireles, H.M.A. Bolini, A.G. Cruz, Oxidative stress in probiotic Petit Suisse: Is the
jabuticaba skin extract a potential option?, Food Res Int. 81 (2016) 149-156.
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 ACCEPTED MANUSCRIPT
FIGURE CAPTIONS

Figure 1. Schematic diagram of turmeric biorefining using SC-CO2 and pressurized

liquids.

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Figure 2. Review of research applied for pressed palm fiber and jabuticaba peel

valorization.

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AN
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 ACCEPTED MANUSCRIPT

Table 1. Reviewed applications of extraction methodologies using SC-CO2 during the first step and of coupled extraction and particle formation
from plant matrices

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Raw material Product of interest Type of procedure and Results Reference
conditions
Extraction methodologies

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using SC-CO2 as first
step

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Algae Scenedesmus Carotenoids Type: Integrated Process 1: SFE [21]
obliquus Chlorophylls Process 1: SFE Extraction yield:0.41-1.15 g/100g raw
Polyphenols Temperature: 40-60 oC material

U
Pressure: 10-40 MPa Carotenoids: 2.32-48.39 mg/g extract
S/F= 75.9 Chlorophylls: 0.26-15.68 mg/g extract

AN
Polyphenols: -

Process 2: PLE Process 2: PLE

M
Temperature:50oC Extraction yield:4.83-78.04 g/100g raw
Pressure: 10 MPa material

D
S/F= 35 Carotenoids: 0.45-35.63 mg/g extract
Chlorophylls: 0.66-113.69 mg/g extract

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Polyphenols: 6.89-59.25 mg GAE/g

Annatto seeds Tocotrienols Type: Comparative [22]

EP
Bixin Process 1: SFE Process 1
Temperature: 40oC Extraction yield: 3.8-17.4 g/100g
Pressure: 20 MPa Tocotrienols: 5.7-28.9 g/100g extract
C

S/F=2
AC

Process 2: LPSE Process 2

Solvents: ethanol, water Extraction yield: -
Temperature: 60-50oC Bixin: 0.08-3.4 g/100 g raw material
S/F=8
Time of extraction: 1.58 h
 ACCEPTED MANUSCRIPT

Asparagus Polyphenols Type: Comparative [23]

Process 1: SFE Process 1: SFE

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Temperature: 50-80oC Extraction yield: 35 g/100g raw material
Pressure: 10–30 MPa Flavonolaglycone: 0.4-0.8 g/100g raw
S/F=100-500 material

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Cosolvent: ethanol and Flavonolglucosyde: 2.20-28.40
water g/100graw material

SC
Process 2: PLE Process 2: PLE:
Solvent: ethanol Extraction yield: -

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65°C Flavonolaglycone: 0.4-0.6 g/100g raw
Pressure:10 MPa material

AN
S/F=152.09 Flavonolglucosyde: 8-10 g/100g raw
material

M
Process 3: Soxhlet Process 3: Soxhlet
Solvent methanol Extraction yield: -
Temperature: 100oC

D
Flavonolaglycone: 0.6 g/100g raw
Time of extraction: 4 h material

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Flavonolglucosyde: 67 g/100g raw
material
EP
Blackcurrant pomace Polyphenols Type: Integrated [24]
Process 1: SFE Process 1: SFE
Temperature: 30-60oC Extraction yield: 12.9-14.71 g/100g raw
C

Pressure: 30-35 MPa material

S/F= 48 Yield polyphenols: 24.34 mg GAE/100g
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extract

Process 2: Soxhlet LPSE Process 2: Soxhlet

Solvent: n-hexane and Extraction yield: 17.5-18.23 g/100g raw
acetone material
 ACCEPTED MANUSCRIPT

Time of extraction: 4h Polyphenols: 27.02-119.5 mg GAE/g

extract

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Process 3: PLE Process 3: PLE
Temperature:70-130oC Extraction yield:12.3-19.05 g/100g raw
Pressure:10.3MPa material

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S/F=- Polyphenols:10.07-79.84 mg GAE/g
extract

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Process 4: EAE Process 4: EAE
Solvent: Sodium acetate Extraction yield: 16.98-39.47 g/100g

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buffer raw material
Temperature:25-55oC Polyphenols: 9.29-36.32 mgGAE/g

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Extraction time: 7h extract

Buckwheat flowers Polyphenols Type: Integrated [9]

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Process 1: SFE Process 1: SFE
Temperature: 60oC Extraction yield: 1.78-2.63 g/100g raw
Pressure: 45 MPa material

D
S/F= 32.4 Polyphenols: -

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Process 2: PLE
Temperature:70-140oC Process 2: PLE
EP
Pressure:10.3MPa Extraction yield:3.10-27.8 g/100g raw
S/F=- material
Polyphenols:11.1-75.6 g/100g raw
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material
AC

Cocoa hulls Polyphenols Type: Integrated [19]

Process 1: SFE Process 1: SFE
Temperature: 40-50 oC Extraction yield: 4.3-4.5 g/100g raw
Pressure: 20-30 MPa material
S/F=88 Polyphenols: 1.8-4.0 mgGAE/g extract
 ACCEPTED MANUSCRIPT

Process 2: PLE
Solvent: Ethanol Process 2: PLE

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Temperature: 70 oC Extraction yield: 7.2 g/100g raw
Pressure: 10 MPa material
S/F=- Polyphenols: 9.6 mgGAE/g extract

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Integrated SFE-PLE
Temperature: 40-70 oC

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Pressure: 10 MPa Integrated SFE-PLE
S/F=- Extraction yield: 35-51 g/100g
Polyphenols: 39-51 mgGAE/g

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Goldenrod Polyphenols and tocopherols Type: Integrated [25]
Process 1: SFE Process 1: SFE

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Temperature:60 oC Extraction yield:2.4-5.52 g/100g
Pressure:45 MPa Polyphenols: -
S/F= 32.4

M
Process 2: PLE Process 2: PLE
Solvent: hexane, acetone, Extraction yield: 3.86-28.9 g/100g

D
ethanol/water mixture and Polyphenols: 12.4-50.3mg GAE/g

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water
Temperature:70-140 oC Integrated SFE-PLE
Pressure: 10.3MPa Extraction yield: 15.7-24.1 g/100g
EP
S/F=- Polyphenols: 15.4-34.2 mg GAE/g

Hemp wastes Canabinoids and polyphenols Type: Integrated [20]

C

Process 1: SFE Process 1: SFE

Temperature:35-70 oC Extraction yield: 0.3-10.4 g/100g raw
AC

S/F=- material
Pressure:10-50MPa Cannabinoids: 18.3-64.2 mg/g extract

Process 2: PLE Process 2: PLE

Solvent: ethanol/water Extraction yield: 0.7-6.6g/100g raw
 ACCEPTED MANUSCRIPT

Temperature:30-130oC material
Pressure: 10.3MPa Polyphenols 0.6-10.1 mgGAE/g extract
Process 3: EAE Process 3: EAE

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Solvent: sodium acetate Extraction yield: 20.2g/100g raw
buffer material
Temperature: 40oC Polyphenols: 6.38mg GAE/gextract

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Time of extraction: 7h

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Mango leaf Polyphenols: mangiferin Type: Comparative [26]
Process 1: SFE Process 1: SFE
Temperature: 55oC Extraction yield: 5-8 g/100g raw

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Pressure: 10 MPa material
S/F=960-1,920 Yield of mangiferin: 50-700 mg/100g

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raw material

Process 2: PLE Process 2: PLE

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Solvent: ethanol Extraction yield: 15-35 g/100g raw
Temperature: 100oC material
Pressure: 20 MPa Mangiferin: 4000-6000 mg/100graw

D
S/F=360-1,200 material

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Passionfruit Tocotrienols and polyphenols Type: Integrated [27]
Process 1: SFE Process 1: SFE
Temperature: 60oC
EP
Extraction yield: 6.56 g/100g raw
Pressure: 17 MPa material
S/F=150
C

Process 2: PLE Process 2: PLE

Solvent: Ethanol Extraction yield: 33.5g/100g raw
AC

Temperature: 60oC material

Pressure:26 MPa COM: US$ 20/kg extract (500L
S/F=300 extractor volume)

Biquinho Pepper Capsaicinoids Type: Comparative [28]

 ACCEPTED MANUSCRIPT

Process 1: SFE Process 1: SFE

Temperature: 40-60°C Extraction yield:0.49-1.34g/100g g raw
Pressure: 15-25MPa material

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S/F= 420
Capsaicinoids: 0.21-0.55mg/g extract

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Process 2: Soxhlet Process 2: Soxhlet
Solvents: hexane, ethanol, Extraction yield: 2.1-38g/100g raw

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acetone, methanol material
Time of extraction: 6h Capsaicinoids: 0.02-0.0239 mg/g extract

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Pitanga Polyphenols Type: Comparative [29]
Process 1: SFE Process 1:SFE

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Temperature: 35-50oC Extraction yield:-
Pressure: 8.1-26.2 MPa Polyphenols: 18.08-73.48 µg/100g
S/F=- extract

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Process 2: PLE Process 2:PLE
Temperature: 60oC Extraction yield:-

D
Pressure: 10 MPa Polyphenols: -

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S/F=-

Turmeric Polyphenols (curcuminoids) and starch Type: Integrated [12, 13]

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Process 1: SFE Process 1: SFE
Temperature: 333 K Extraction yield: 2.4 g/100g extract
Pressure: 25 MPa
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S/F=9.5
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Process 2: PLE Process 2: PLE

Solvent: ethanol Extraction yield: 13 g/100graw material
Temperature: 60oC Curcuminoids:12.08 g/100g extract
Pressure:10MPa Starch: 36 g/100g raw material
S/F=9.5 COM: US$ 17.86/kg curcuminoids
 ACCEPTED MANUSCRIPT

extract (500 L scale)

COM: US$ 5.09/kg starch (500L scale)

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Rosemary Polyphenols: rosmarinic acid Type: Integrated [30]
Process 1: SFE Process 1: SFE
Temperature=40oC Extraction yield: 2.5g/100g raw material

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Pressure: 30MPa
S/F=2.5

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Process 2: PLE Process 2: PLE
Solvent: water Extraction yield:
Temperature: :40-172oC

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Rosmarinic acid: 0.05-0.65 mg/100g
Pressure:10MPa raw material

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S/F=0.5 COM: US$7.5/kg extract (100 L scale;
integrated SFE-PLE)
Coupled extraction and

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particle formation
Grape marc Fractionation of polyphenols Process 1: SFE Process 1: SFE [31]
(catechins) Temperature: 45oC Extraction yield: 5.03 g/100g raw

D
Pressure: 28 MPa material

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Solution flow rate: 10
kg/h
EP
Process 2: SAF Process 2: SAF
Solvent/Antisolvent: Particle size: 5-10 µm
Ethanol/ SC-CO2 Catechin: 24.23-51.73 mg/kg raw
C

Temperature: 40-45oC material

Pressure: 10-12 MPa Epicatechin: 56.93-100.29 mg/kg raw
AC

Solution flow rate: 0.12 material

L/h
SC-CO2flow rate: -
[32]
Jabuticaba Encapsulated polyphenols Process 1: PLE Process 1: PLE
 ACCEPTED MANUSCRIPT

(anthocyanins) Solvent: Ethanol Extraction yield: -

Temperature: 80oC
Pressure: 5 MPa

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Process 2: RESS Process 2: RESS
Solvent/Antisolvent: Particle size: -

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Ethanol/ SC-CO2 Encapsulation efficiency: 23.86-25.94%
Temperature: 40oC

SC
Pressure: 20 MPa
Solution flow rate: 0.030
L/h

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SC-CO2flow rate: 0.71
kg/h

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[33]
Mango leaves Fractionation of polyphenols Process 1: SFE Coupled SFE-SAF
(mangiferin) Cosolvent: ethanol Extraction yield: -

M
Temperature: 35-50oC
Pressure:10 MPa
Solvent flow rate: 5-19

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g/min

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Cosolvent flow rate: 1-15
g/min
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Process 2: PLE Coupled PLE-SAF
Solvent: ethanol and Extraction yield: -
water Coupled SAF-SFE
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Temperature: 35-50oC Particle size: 0.24-0.34 µm

Pressure: 12-20 MPa Mangiferin: 13.08-29.25 mg/g
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Solvent flow rate: 10 precipitates

g/min

Process 3: SAF Coupled: SAF-PLE

Temperature: 35oC Particle size: 0.01-0.35 µm
 ACCEPTED MANUSCRIPT

Pressure: 15 MPa Mangiferin: 56.24-94.36 mg/g

Solvent/Antisolvent: precipitates
Ethanol, water and

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mixtures / SC-CO2
Solution flow rate: 5
g/min

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SC-CO2 flow rate: 30
g/min

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[34]
Rosemary Fractionation of polyphenols (carnosic Process 1: PLE Process 1: PLE
acid and carnosol) Solvent: Ethanol Extraction yield: 39.86 g/100g
Temperature: 150-200 oC

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Carnosic acid: 109 mg/g extract
Pressure: 10 MPa Carnosol: 20.5 mg/g extract

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Process 2: SAF Process 2: SAF
Solvent/Antisolvent: Particle size: -

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Ethanol/ SC-CO2 Precipitation efficiency: 4.2-78.5%
Temperature: 40oC
Pressure: 10-30 MPa

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Solution flow rate: -

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SC-CO2flow rate: -
[15]
Turmeric Fractionation of polyphenols Process 1: PLE Process 1: PLE
EP
(curcuminoids) Solvent: Ethanol Extraction yield: 13 g/100g
Curcuminoids:12.08 g/100g precipitates
C

Process 2: SAF Process 2: SAF

Solvent/Antisolvent: Particle size: 111-829 µm
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Ethanol/ SC-CO2 Precipitation efficiency: 55-96%

Temperature: 40-60oC
Pressure: 10-20 MPa
Solution flow rate: 0.030
L/h
 ACCEPTED MANUSCRIPT

SC-CO2flow rate: 0.5-0.8

kg/h
[35]

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Onion peels Fractionation of polyphenols Process 1: PLE Coupled PLE-SAF
(quercetin) Temperature: 40-60oC Particle size: 119-234 µm
Pressure: 10-12 MPa Precipitation yield: 4.1-5.2%

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Process 2: SAF Precipitation efficiency: 12.9-26%
Solvent/Antisolvent: Quercetin: 12.9-26 g/100g precipitates

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ethanol/ SC-CO2
Solution flow rate: 0.024
kg/h

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SC-CO2flow rate: 1.020
kg/h

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PLE - Pressurized liquid extraction; SC-CO2 - Supercritical carbon dioxide; SFE - Supercritical fluid extraction; GAE - Gallic acid equivalents;
S/F - Solvent mass to feed mass ratio; EAE - Enzyme-assisted extraction; COM - Cost of manufacturing; SAF - Supercritical antisolvent
fractionation; RESS - Rapid expansion of supercritical solutions

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Table 2. Reviewed researches on the valorization of pressed palm fibers and jabuticaba

peels

Process Pressure Temperature Optimal results in Reference

(MPa) (oC) constituents obtaining

Isolated 20-30 45-55 90 mg β-carotene/g extract [64]

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SFE

Integrated

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SFE-SWH

SC
SFE 5–30 45-55 0.81mg β-carotene/g extract [71]

SWH 15 and 25 150-360 Oligosaccharides: 17.88

U
AN g/100g PPF

Total reducing sugars: 22.88

g/100g PPF
M

Isolated 20 206-256 Oligosaccharides: 2.83 g/100g [72]

SWH PPF
D

Total reducing sugars: 12

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g/100g

Isolated 0.1–8 35-45 44 mg extract/g PPF [73]

EP

PLE 305 µg α-carotene/g extract

and 713µg β-carotene/g extract

C

COM: US$13.4 and

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US$29.2/kg extract (0.5 0.5 m3

vessel capacity)

Type: Comparative SFE-

PLE

Isolated PLE 5-10 40-100 Anthocyanins: [74]

0.7-2.5 mg Cy-
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3-glycoside/g

JP

COM for

anthocyanin

fraction: 0.85-

PT
1.06 US$/g JP

(0.3 m3 vessel

RI
capacity)

SFE 10–13.5 40–80 Anthocyanins: [75]

SC
0.6-2.546 mg

Cy-3-

U glycoside/g JP
AN
PLE 11.7 80 Anthocyanins:

0.58 mg Cy-3-
M

glycoside/g JP
D

Integrated PLE-RESS
TE

PLE 5 80 [32]

RESS 10-35 40-50 Encapsulation

EP

efficiency: 50-

80%
C

PLE - Pressurized liquid extraction; SFE - Supercritical fluid extraction; COM - Cost of
manufacturing; RESS - Rapid expansion of supercritical solutions; SWH - Subcritical
AC

water hydrolysis; PPF - Pressed palm fibers; JP - Jabuticaba peels

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Highlights
- Development of novel supercritical fluid-based biorefinery concepts
- Synergy between supercritical CO2 extraction and biomass valorization
- Use of supercritical CO2 during the first-step in biorefinery concepts
- Use of multistep procedures for biorefining plant matrices into marketable products

- Using supercritical CO2 as a green solvent in small-scale integrated biorefineries

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