Processes: Extraction Methods of Oils and Phytochemicals From Seeds and Their Environmental and Economic Impacts

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processes

Review
Extraction Methods of Oils and Phytochemicals from Seeds and
Their Environmental and Economic Impacts
Valerie M. Lavenburg 1 , Kurt A. Rosentrater 2 and Stephanie Jung 1, *

1 Food Science and Nutrition Department, California Polytechnic State University,


San Luis Obispo, CA 93407, USA; vlavenbu@calpoly.edu
2 Department of Agricultural and Biosystems Engineering, Iowa State University, Ames, IA 50011, USA;
karosent@iastate.edu
* Correspondence: stjung@calpoly.edu

Abstract: Over recent years, the food industry has striven to reduce waste, mostly because of rising
awareness of the detrimental environmental impacts of food waste. While the edible oils market
(mostly represented by soybean oil) is forecasted to reach 632 million tons by 2022, there is increasing
interest to produce non-soybean, plant-based oils including, but not limited to, coconut, flaxseed and
hemp seed. Expeller pressing and organic solvent extractions are common methods for oil extraction
in the food industry. However, these two methods come with some concerns, such as lower yields
for expeller pressing and environmental concerns for organic solvents. Meanwhile, supercritical
CO2 and enzyme-assisted extractions are recognized as green alternatives, but their practicality

 and economic feasibility are questioned. Finding the right balance between oil extraction and
phytochemical yields and environmental and economic impacts is challenging. This review explores
Citation: Lavenburg, V.M.;
Rosentrater, K.A.; Jung, S. Extraction
the advantages and disadvantages of various extraction methods from an economic, environmental
Methods of Oils and Phytochemicals and practical standpoint. The novelty of this work is how it emphasizes the valorization of seed
from Seeds and Their Environmental by-products, as well as the discussion on life cycle, environmental and techno-economic analyses of
and Economic Impacts. Processes 2021, oil extraction methods.
9, 1839. https://doi.org/10.3390/
pr9101839 Keywords: seeds; supercritical CO2 extraction; solvent extraction; expeller pressing; enzyme-assisted
aqueous extraction; techno-economic analysis; life cycle assessment
Academic Editors: Juliana Maria Leite
Nobrega De Moura Bell,
Blanca Hernández-Ledesma and
Roberta Claro da Silva 1. Introduction
The sustainability and valorization of by-products have become an important focus
Received: 28 September 2021
Accepted: 12 October 2021
of the food industry over the past few years. According to the Food and Agriculture
Published: 16 October 2021
Organization (FAO) of the United Nations, every year, approximately 1.3 billion tons,
equivalent to 30% of total food production, is wasted globally. This volume of food waste
Publisher’s Note: MDPI stays neutral
is worth USD 750 million. Several initiatives have been implemented to combat food waste.
with regard to jurisdictional claims in
In 2013, the United States Department of Agriculture (USDA) partnered with the United
published maps and institutional affil- States Environmental Protection Agency (US EPA) to formally set a goal to reduce the
iations. country’s food waste by 50% by 2030 [1,2]. Additionally, the EPA identified a food waste
hierarchy that prioritizes feeding hungry people, feeding animals, industrial use, com-
posting, then incineration or landfilling (in order of decreasing preference) (Figure 1) [3].
The Food Recovery Act of 2017 instituted various guidelines encouraging farms, grocery
Copyright: © 2021 by the authors.
stores, restaurants and institutions to donate excess food, set up composting and anaerobic
Licensee MDPI, Basel, Switzerland.
digestion programs and reduce overall food waste [4]. In California, the legislation “Senate
This article is an open access article
Bill 1383” requires businesses to recover at least 20% of disposed edible food and divert it
distributed under the terms and for human consumption by 2025 [5].
conditions of the Creative Commons Among the various types of food waste generated, roots, tubers and fruits and veg-
Attribution (CC BY) license (https:// etables are the most notable ones, representing 45% of the total waste. In addition, a
creativecommons.org/licenses/by/ whopping 20% of oilseeds, which come from crops such as sunflowers grown specifically
4.0/). to produce edible oil, are lost during agricultural production and postharvest handling

Processes 2021, 9, 1839. https://doi.org/10.3390/pr9101839 https://www.mdpi.com/journal/processes


Processes 2021, 9, 1839 2 of 14

and storage [6,7]. This is a tremendous amount, considering that global oilseed produc-
tion was forecasted to reach 632 million tons during 2021–2022, and is expected to be
worth USD 162.5 billion by 2025 [8,9]. Furthermore, processors are aiming to reduce all
forms of seed-related waste by applying various strategies including but not limited to
valorizing by-products by extracting residual phytochemicals or oil for the food, cosmetic,
or pharmaceutical industries. For example, tomato seeds, recovered during the process-
ing of tomato-based products such as paste and ketchup, could be a source of edible oil.
Meanwhile, in recent years consumer preference has grown for foods that promote health
benefits, are environmentally friendly and offer a pleasant taste and aroma. As a result, the
market for specialty oils (which refer to non-commodity oils with functional properties that
are not further refined, bleached, or deodorized) has considerably increased [10]. Seeds in-
deed often contain desired unsaturated fatty acids and phytochemical components, which
exhibit antioxidant and anti-cancer effects [11]. Among the specialty oils, coconut and
olive oils (the latter of which is not from an oilseed) have become popular, with production
reaching 3.67 million tons and 3.1 million tons, respectively, in 2020 [12]. Other less popular
specialty oils include sesame, flaxseed and hempseed oils [13]. It should be noted that
identifying what crops are grown specifically for their oilseeds (as opposed to crops that
have seeds but are also utilized for other purposes) can sometimes be confusing. Thus, a
Processes 2021, 9, x FOR PEER REVIEW
summary of the categories of all the matrices discussed in this paper is included for 2 ofthe
15

purpose of clarity for the readers (Table 1).

Figure
Figure 1. Priorities of the 1. Priorities
food recovery of the from
hierarchy, food most
recovery hierarchy,
desirable (1) to from most desirable
least desirable (1) to least
(6). Adapted fromdesirable
[3]. (6).
Adapted from [3].
Table 1. Types of extracted seed matrices in research studies covered in this literature review.
Among the various types of food waste generated, roots, tubers and fruits and veg-
etables are the mostOilseed
notable ones, representing 45% of the totalOther SeedIn
waste. Type
addition, a whop-
Canola/Rapeseed
ping 20% of oilseeds, which come from crops such as sunflowers Almond grown specifically to
produceLinseed
edible(also known
oil, are lostas flaxseed)
during agricultural production andCoriander
postharvest handling and
Jatropha curcas Hemp
storage [6,7]. This is a tremendous amount, considering that global oilseed production
Soybean Favela
was forecasted toSunflower
reach 632 million tons during 2021–2022, and is expected to be worth
Passionfruit
USD 162.5 billion by 2025
Camelina [8,9]. Furthermore, processors are aiming
Peachto reduce all forms of
seed-related waste by applying various strategies includingElaeagnus
Castor but not limited
mollis to valorizing
Mustard Moringa
by-products by extracting residual phytochemicals or oil for the food, cosmetic, or phar-
maceutical industries. Peanut
For example, tomato seeds, recovered during Grapethe processing of to-
Forsythia suspense
mato-based products such as paste and ketchup, could be a source of edible oil. Mean-
while, in recent years consumer preference has grown for foods that promote health ben-
efits, Recently, the food industry
are environmentally has and
friendly prioritized
offer a balancing the economic
pleasant taste and aroma. andAsenvironmental
a result, the
aspects of edible oil production. This shift has been driven mainly by the consumers
market for specialty oils (which refer to non-commodity oils with functional properties who
haveare
that been
notmore conscientious
further about sustainable
refined, bleached, food has
or deodorized) production and its
considerably three pillars:
increased [10].
Seeds indeed often contain desired unsaturated fatty acids and phytochemical compo-
nents, which exhibit antioxidant and anti-cancer effects [11]. Among the specialty oils,
coconut and olive oils (the latter of which is not from an oilseed) have become popular,
with production reaching 3.67 million tons and 3.1 million tons, respectively, in 2020 [12].
Other less popular specialty oils include sesame, flaxseed and hempseed oils [13]. It
Processes 2021, 9, 1839 3 of 14

people, planet and profit. Among the oil extraction methods being considered, expeller
pressing and solvent extractions are most commonly used at an industrial scale [14]. How-
ever, both methods have some major pitfalls to overcome: a lower oil yield with expeller
pressing compared to solvent extraction can make the process economically disadvanta-
geous, and the use of organic solvents brings environmental concerns. With the increasing
focus on the environmental impact of unit operations used during processing and the
development of green chemistry, more studies have focused on improving the extrac-
tion methods so that less energy is required and less chemical pollutants are released
by these processes [15]. Supercritical CO2 (SCO2 ) and enzyme-assisted extractions are
alternatives to solvent extraction and expeller pressing, which are considered traditional
oil extraction methods.
This review includes studies on oil extractions of seeds that were published between
2010 until the present day, with the exception of a few studies that are older. The purpose
of this review is to explore the advantages and disadvantages of oil extraction methods
of seeds from the lens of sustainability and food waste reduction, as well as life cycle,
environmental impact and techno-economic analyses.

2. Mechanical Pressing
Historically, oil has been pressed out of seeds by indigenous communities for centuries,
and the mechanical pressing of soybeans dates back to the 1940s [14]. There are two broad
categories of equipment for oil extraction: expeller press and extruder (Figure 2). Expeller
pressing is often limited to small scale, on-farm seed grinding operations. For example,
Processes 2021, 9, x FOR PEER REVIEW 4 of 15
canola, sunflower, flax and safflower oils are extracted via expeller pressing in the mid-west
and northeastern United States. Due to its low cost, expeller pressing is also often used in
developing countries, such as rural India, for linseed oil extraction [14,16].

Figure 2. Major types of mechanical pressing.


Figure 2. Major types of mechanical pressing.
An expeller press has a screw that rotates in a perforated barrel. The discharge area
is partially obstructed,
An expeller exerting
press has a screwpressure ontoinseeds
that rotates to extract
a perforated oil. The
barrel. Expeller pressing
discharge areais
considered an easy method for oil extraction because it only requires mechanical
is partially obstructed, exerting pressure onto seeds to extract oil. Expeller pressing is con-power and

sidered an easy method for oil extraction because it only requires mechanical power andC
does not need organic solvents [17]. The extraction temperature can be kept under 50
to perform
does not need cold pressing,
organic which
solvents canThe
[17]. help preservetemperature
extraction nutritional compounds
can be kept of the oil
under 50 [18].
°C
However, one disadvantage of this method can be its lower oil recovery.
to perform cold pressing, which can help preserve nutritional compounds of the oil [18]. If spacing is too
small within
However, one the perforated of
disadvantage barrel, or if high
this method compaction
can be its lowerof oil
seeds resultsIffrom
recovery. pressing,
spacing is tooit
can jam the operating screw and leave 5 to 20% of the total oil in the residual cake [17,19].
small within the perforated barrel, or if high compaction of seeds results from pressing, it
Thus, there has been interest in making expeller pressing more efficient and, therefore,
can jam the operating screw and leave 5 to 20% of the total oil in the residual cake [17,19].
more economically viable.
Thus, there has been interest in making expeller pressing more efficient and, therefore,
Several parameters need to be considered to improve oil extraction yield and quality,
more economically viable.
and one such example is screw rotation. When using a pilot expeller press designed for
Several parameters need to be considered to improve oil extraction yield and quality,
cold pressing, increasing rotation from 1.2 to 18 rpm increased press capacity from 2.2 kg
and one such example is screw rotation. When using a pilot expeller press designed for
cold pressing, increasing rotation from 1.2 to 18 rpm increased press capacity from 2.2 kg
seed/h to 29.4 seed/h, while decreasing canola oil yields from 91 to 84% [20]. Additionally,
the number of presses was shown to affect the oil yield and the quality of linseed oil.
Increasing the number of presses of an expeller press from one to two increased linseed
Processes 2021, 9, 1839 4 of 14

seed/h to 29.4 seed/h, while decreasing canola oil yields from 91 to 84% [20]. Additionally,
the number of presses was shown to affect the oil yield and the quality of linseed oil.
Increasing the number of presses of an expeller press from one to two increased linseed oil
yields from 19 to 32%, while adding a third press did not significantly affect the oil yield.
Implementing a double press also led to the highest total phenol (27 mg GAE/100 g, which
was a 170% increase from a single press) and total flavonoid content (7 mg rutin eq/100 eq,
which was a 40% increase from a single press). Applying more than two presses started
to degrade these compounds due to the high pressure and temperature [16]. Another
approach to increase the oil yield was to blend oilseeds to improve the consistency of the
matrix, which enhanced the permeability and oil recovery. For example, an oil recovery of
94.7% was obtained with Jatropha seeds blended with soybean, and decreased to 88.4 and
75.4% when blended with maize and rapeseed, respectively [21].
Another way to improve oil extraction is to perform extrusion of the seeds (Figure 2).
This process, which also relies on screw configuration, is used to modify the shape and
properties in applications such as expanded snacks (such as cheerios) or obtain liquid
extracts from plant material. The end of the screw allows for seeds to be extruded through
a perforated plate and discharges oil [17,22,23]. Extrusion has been used as pretreatment
prior to expeller pressing of soybean oil, extracting over 70% of oil compared to single-step
expelling, which yielded 60% [24]. This process has also been used for simultaneous
treatment with fatty acid methyl ester as a solvent, extracting 98% of oil from sunflower
seeds [25].
Single-screw extrusion (expander) is mostly employed at a large-scale for the pressing
of oil from seeds, but twin screw systems are used in laboratory and pilot studies [18,23].
The advantage of a twin extruder is that it allows for a thermomechanical treatment of
seeds and avoids further pre-treatment steps (such as dehulling, flaking, cooking) often
necessary to obtain high oil yields from single-screw operations [17,22,23]. A twin extruder
set to 50 rpm and a flow rate of 2.27 kg/h can extract up to 50% of coriander oil without
any pretreatment [26]. Fifty percent of oil was also obtained from sunflower seeds with
parameters set to 80 ◦ C, 60 rpm and a 24 kg/h flow rate [27]. It would be worthwhile to
directly compare the oil yields obtained using single versus twin screw extrusion as a pre-
or co-treatment for expeller pressing. There is still more work to be conducted regarding
correlating research results from lab-scale expeller pressing of various seeds and scaling up
to industrial presses [17].

3. Solvent Extraction
Hexane (or n-hexane, which is its isomerized form) is the most commonly used organic
solvent in the oilseed extraction industry due to its efficiency in oil recovery, inexpensive
costs, recyclability, non-polar nature, low heat of vaporization and low boiling point
(63–67 ◦ C) [28,29]. Hexane extraction is especially utilized to produce soybean oil, which is
the most consumed vegetable oil in the U.S. [30]. However, hexane is explosive, making it
unsafe for workers in food-processing plants. In addition, it is both a neurological toxin
and a hazardous air pollutant and can cause environmental pollution [31]. Although it
is feasible to minimize these concerns with proper precautions, the production of certain
foods, such as all organic foods, is restricted from hexane use. There is indeed evidence
that hexane residue up to 21 ppm can be found in soy ingredients and in the 1 ppm range
in vegetable oils [32,33]. For soy foods, the Food and Drug Administration (FDA) has
not set maximum hexane residue limits, but the European Union (EU) prohibits hexane
residue levels greater than 10 ppm. The EU has also set other hexane residue limits that
vary depending on the food product [34].
There are many examples of the use of co-solvents during solvent extractions [35,36];
however, in this review we are only covering studies that discuss single solvent extractions.
Alternatives to hexane such as ethanol (a natural, non-toxic solvent allowed in organic
food production) have been investigated [37]. As ethanol is more polar than hexane, it has
the capability to extract more polar compounds such as polyphenols, pigments and soluble
Processes 2021, 9, 1839 5 of 14

sugars. The benefit of using ethanol vs. n-hexane was demonstrated during the extraction
of sunflower collets (ground oilcake or expanded material), with a 32% vs. 23% yield of
extracted material (oil and other compounds), respectively [38]. With sunflower collets,
ethanol extraction led to a 38% greater extractability of tocopherols and phospholipids
compared to n-hexane [38]. With castor seeds, no significant difference was found in the oil
yield between hexane and ethanol, but the extract obtained with ethanol had significantly
higher level of sterols than in the hexane extract [39].
Oil extraction yields can be improved using other organic solvents besides ethanol.
Isopropanol extracted 49 wt.% oil from favela seeds, which was significantly higher than
47% using n-hexane [40]. The extraction method itself can have an important impact on the
choice of the organic solvent leading to higher oil extraction yield. When ultrasound, shaker
and Soxhlet methods utilizing hexane, acetone, ethanol and isopropanol were compared
for the extraction of passion fruit oil, the highest oil yield (26%) was obtained using hexane
during Soxhlet extraction. Acetone was the most effective solvent for ultrasound extraction
(24% vs. 17% when using hexane) [15]. Ethyl acetate has characteristics that could be
beneficial, as it is less flammable and hazardous and 33% cheaper compared to n-hexane.
Similar oil extraction yields were obtained during the extraction of canola seeds with
hexane (21–36%) and ethyl acetate (25 to 40%), while for camelina seeds, it ranged from
9–16% for both solvents [41]. Thus, the literature provides evidence that alternative organic
solvents could replace the use of hexane for a similar oil extraction yield.

4. Supercritical CO2 Extraction


There has been a rise of SCO2 technology over the past few decades, with over 150 su-
percritical fluid extraction plants located around the world in 2014, mostly in North America
and Europe [42]. SCO2 is used to de-caffeinate coffee and tea and extract oils, antioxidants,
natural food colorings, aromas and flavors from various food matrices [43]. For oil extrac-
tion in particular, it has been applied to a wide variety of seeds such as apricot, canola,
soybean, sunflower, grape, acorn and walnut seeds [44]. During SCO2 extraction, pressur-
ized CO2 solvent is mixed with solid raw material (often ground to reduce the particle size),
which allows for the extraction of the compounds of interest. A pressurized CO2 solvent
begins to form at its critical point of 31 ◦ C and 7.38 MPa, where the gas and liquid phases
come together to form a homogeneous fluid phase beyond the supercritical fluid region.
The advantages of SCO2 extraction over conventional solvent extraction methods include
higher diffusivity, lower viscosity and surface tension and faster extraction times [43].
Additionally, using CO2 has environmental benefits such as being nonflammable and
recyclable. It allows for improved product quality by leaving no residues and maintaining
high purity of extracted materials. For these reasons, it is often considered a “greener”
extraction method compared to solvent extraction [45].
However, there are several pitfalls to using SCO2 . The non-polarity of CO2 lim-
its extraction capabilities of polar phytochemicals, such as phenols [46,47]. This extrac-
tion method is also expensive because it relies on equipment that handles high pressure,
which increases investment and maintenance costs [48]. Additionally, there is a lack and
need for continuous systems for increasing large-scale production capacity. For these
reasons, widespread adoption of this extraction method by the food industry has been
lagging [43,49]. While having benefits that other technologies do not have, the economical
competitivity of SCO2 is a major pitfall for its development [42].
The selection of the most favorable SCO2 extraction parameters for pressure, tempera-
ture, solvent flow rate, size of materials and moisture content are dependent on the type
of seed and molecules of interest. For hemp seed oil, increasing the pressure reduced the
extraction time (4.5 h at 30 MPa vs. 3.5 h at 40 MPa), while increasing the temperature from
40 to 60 ◦ C did not significantly impact the extraction yield [50]. Oil extraction of peach
seeds was improved by decreasing the particle size and increasing the temperature, flow
rate, pressure and extraction time. Applying SCO2 for 3 h at conditions of 40 ◦ C, 20 MPa
Processes 2021, 9, 1839 6 of 14

and 7 ml/min to 0.3 mm ground peach seeds led to a 35% oil yield. This was within the
range reported for peach seeds extracted using solvents [51,52].
Sometimes the benefit of SCO2 over solvents is observed in oil quality rather than
yield. When extracting samara oil from different cultivars of Elaeugnus mollis Diels seeds
using SCO2 , the oil yields ranged from 25–38%, which were significantly lower than
with hexane (47–52%). However, the use of SCO2 led to a higher quality oil due to the
greater extraction of unsaturated fatty acids, such as linoleic acid, which promotes brain
function [53]. Although the oil yield from Moringa seeds from petroleum ether extraction
surpassed that of SCO2 extractions, there was no significant difference in fatty acids,
tocopherols and sterols between the two methods [54]. The SCO2 extraction of different
grape seeds successfully led to 3.4–4.8 mg/kg extraction of lycopene, a carotenoid that
serves as an antioxidant and precursor to vitamin A. This represented an approximately
20% increase when compared to hexane [55,56].
However, the low polarity of CO2 can cause difficulty in the extraction of polar lipids,
such as phospholipids and phenols, and could be a major drawback for this technology.
This can be overcome by combining polar co-solvents with SCO2 , which improves solubility
of the solute during extraction via dipole–dipole and hydrogen bond interactions [57,58].
SCO2 extraction of camelina seeds using ethanol as a co-solvent improved the extraction
Processes 2021, 9, x FOR PEER REVIEW of phospholipids and phenols, and thus increased total lipid yields (34% vs. 23%7for of pure
15
SCO2 extraction) [59]. The highest total phenol content from grape seeds was achieved
through a sequential SCO2 extraction, in which non-polar components were removed from
grape seeds first, and then 15% mol ethanol was added to recover phenols from defatted
from defatted grape seeds. Thus ethanol-assisted SCO2 extraction may provide oils with
grape seeds. Thus ethanol-assisted SCO2 extraction may provide oils with better health
better health benefits by extracting higher yields of specific compounds [60].
benefits by extracting higher yields of specific compounds [60].
5. Aqueous Extraction
5. Aqueous Processing
Extraction Processing
TheThe
main
main benefit of of
benefit aqueous
aqueous extractions
extractions (AEP)
(AEP)forfor
seeds
seedsisisthat
thatwater
watercan
canbebeused
usedasas a
a more environmentally friendly solvent compared to organic solvents
more environmentally friendly solvent compared to organic solvents such as hexane. With such as hexane.
With solvent
solvent extractions,
extractions, thefrom
the oil oil from the substrate
the seed seed substrate is dissolved
is dissolved into the into the phase.
solvent solventThe
phase. The oil is then recovered by the evaporation of the organic solvent. With
oil is then recovered by the evaporation of the organic solvent. With AEP, oil is typically AEP, oil
is typically partitioned into the following fractions: solid residue, protein-rich
partitioned into the following fractions: solid residue, protein-rich skim, lipid-rich cream skim, lipid-
richandcream
freeand free oil 3).
oil (Figure (Figure 3). Therefore,
Therefore, additionaladditional
steps aresteps are necessary
necessary to release
to release free oil,free
such
oil,assuch as demulsification
demulsification from the from the cream.
cream. However, However, these
these steps stepsadd
could could add significant
significant costs to oil
costs to oil recovery;
recovery; therefore,therefore,
the most the most
ideal ideal extraction
extraction would be would
one that beextracts
one that
theextracts
most freetheoil.
most free oil. Hence, extraction yield is not always the best indicator
Hence, extraction yield is not always the best indicator of recovered free oil. of recovered free oil.

Figure 3. Image of partitioning in aqueous extraction slurry after centrifugation.


Figure 3. Image of partitioning in aqueous extraction slurry after centrifugation.

Regardless of the matrix, AEP usually has lower yields than the ones obtained with
organic solvents; however, some research studies have shown competitive recovery yields
up to 96% [61,62]. Pre-treatments are commonly applied prior to aqueous extractions, and
all have the same goal of breaking down/softening the seed matrix to increase oil recovery.
Processes 2021, 9, 1839 7 of 14

Regardless of the matrix, AEP usually has lower yields than the ones obtained with
organic solvents; however, some research studies have shown competitive recovery yields
up to 96% [61,62]. Pre-treatments are commonly applied prior to aqueous extractions, and
all have the same goal of breaking down/softening the seed matrix to increase oil recovery.
For example, roasting seeds can improve yields because applying heat to the substrate
can rupture cell walls and allow for better oil release [63]. Thus, using the optimized
roasting temperature and time of wild almonds led to an oil extraction yield of 35%
(w/w) [61]. Flaking and extrusion prior to aqueous extraction can also promote increased
cell disruption, allowing for better water penetration and release of entrapped compounds.
For the aqueous extraction of soybeans, oil extraction yields improved significantly when
using extruded full fat soybean flakes (68%) compared to non-treated soybean flakes
(60%) [64]. Some pretreatments were shown to specifically improve free oil recovery.
Flaxseed kernels pretreated with 0.3 M citric acid and dried at 70 ◦ C for 1 h prior to
aqueous extraction led to the development of a thinner cream layer and increased the free
oil yields from 19 to 83%. This significant increase in free oil recovery was related to the
ability of the acid treatment to affect protein properties, which led to the coalescence of
oil bodies and size reduction in protein bodies [65]. Furthermore, different instruments
can be used to perform aqueous oil extraction. The use of a twin-screw extruder for the
aqueous extraction of sunflower seeds led to 35% higher oil yield than when processed in a
blender [66].

Enzyme-assisted Aqueous Extraction (EAEP)


Enzymes are frequently used in all realms of food processing and their addition to
aqueous oil extraction offers many advantages. Oil is difficult to release from the cotyledon,
which is protected by cell wall structures made up of cellulose, hemicellulose, lignin and
pectin [28]. Thus, seeds can be treated with substrate-specific enzymes such as carbohy-
drases (i.e., cellulase, hemicellulase and pectinase) to degrade the cell wall and facilitate
oil release. Protease is utilized for hydrolyzing proteins in the cell membrane, which
increases the extraction efficiency of seeds [67,68]. Enzyme treatment is environmentally
friendly, occurs at mild temperatures and does not produce solvent residues [28,67,68].
Life cycle analyses (LCA) on enzyme usage in food, feed and pharmaceutical industries
have demonstrated that enzymatic processes lead to less impact on global warming, acidi-
fication, eutrophication, ozone formation and energy consumption [69]. Enzymes can be
expensive, but costs could be compensated by the increase in extraction yield or enzyme
recycling [67,70].
As in any process, optimizing parameters is important to obtain good extraction yields.
While the optimal pH of enzymes depends on many parameters including the type of
enzymes (for example, proteases vs. carbohydrases), it is also crucial to set the pH far
from the isoelectric pH (pI) of seed proteins. At their pI, proteins are insoluble, which can
hinder oil extractions [28,71–73]. Temperature is another important parameter to consider
when using enzymes, with the ideal range for enzymatic hydrolysis typically between
45–55 ◦ C. If temperatures are too high, enzymes can become inactive and, thus, reduce
their hydrolysis capabilities. However, temperatures that are too low can slow the reaction
rates of enzymes and the extraction rate of oils [28,71,74,75].
The benefit of EAEP has been shown in comparison to AEP of seeds. For the oil
extraction of Moringa seeds, individual addition of proteases and carbohydrases led to oil
yields ranging from 17–23% compared to 8% for the control. Protease led to highest oil
recovery due to its role in solubilizing proteins in the seed substrate [76]. Adding 0.85%
alkaline protease to an almond cake slurry extracted for 1 h at pH 9 and 50 ◦ C led to a
significantly higher oil extraction (50%) compared to the non-enzymatic control extraction
(42%) [77]. However, some studies show that enzyme addition does not improve oil
yields [78]. For example, EAEP vs. AEP of almond cake extracted using the same enzymes
and parameters mentioned above did not lead to significantly different oil extraction yields
(26 and 29%, respectively). However, the change in scale may have contributed to the
Processes 2021, 9, 1839 8 of 14

different outcomes; the first study was conducted at lab scale (50 g), while the second study
was at pilot scale (750 g) [79].
Another approach is to use a cocktail of enzymes, added simultaneously, during the
extraction. A cocktail of cellulase, pectinase and hemicellulase was used to extract oil
from yellow mustard flour through a 3-h enzyme-assisted aqueous oil extraction set to pH
4.5–5.0 and 40–42 ◦ C. Yields of 76% of oil and 75% of protein were reported, which were
significantly higher compared to aqueous extraction leading to yields of 56% of oil and 61%
of protein [73]. The oil extraction of Forsythia suspense seeds was improved using a cocktail
of cellulase, pectinase and proteinase (17 vs. 7% for AEP, respectively). This improvement
was attributed to more components within the seed cell walls being degraded [80].
Sometimes enzyme addition is more helpful during the demulsification step to release
free oil from the cream layer. Due to the composition of the cream layer, proteases and
phospholipases are often considered [81]. The mechanisms involved during enzymatic
demulsification include hydrolysis of the proteins in the emulsion, leading to larger oil
droplet coalescence and free oil recovery [71,73]. Enzymatic demulsification of cream using
0.5% alkaline protease after both AEP and EAEP of almond cake significantly improved
the free oil yield (60–63%) compared to the control (up to 39%) [78]. Cream from peanut
seed extraction was also destabilized using alkaline protease, achieving a 65% free oil yield.
This was a steep increase compared to the cream from the control, which had less than a
5% free oil yield [82]. Additionally, enzymes can be used to increase protein recovery from
the skim layer. Protease-based EAEP of almond flour set to pH 9 and then adjusted to pH
5 (the pI of almond proteins) led to the production of significantly more soluble peptides
compared to AEP (45 vs. 23%, respectively) [79]. These examples highlight the potential
for enzymes to be used on the various fractions of EAEP for multiple food applications.

6. Life Cycle and Environmental Impact Analyses


Each oil extraction method has its own advantages and disadvantages in terms of
environmental, economic and practical aspects. Therefore, the best method depends on
the matrix and specific desired outcomes. Life cycle analyses (LCA) is one way in which
environmental impacts can be assessed for the lifetime of any given food product, from
cradle-to-grave or even cradle-to-cradle. This tool has become more popular in the food
sector in the last decade, which is evident by the increasing number of publishing frequency
of LCA studies regarding food topics [83,84]. LCA, which is independent of time and
location variables, is often contrasted to Environmental Impact Analysis (EIA). The latter is
a tool that also considers the environmental impact of food products, but unlike LCA, it
also covers social impacts, such as time-related or local geographic factors [85,86].
LCA studies on edible oils frequently cover oilseed crop cultivation, oil extraction
and transportation within their system boundaries [87]. Yet, there is limited information
on the environmental impacts between extraction methods. An LCA study on mustard
seed oil demonstrated that extraction via pressing had significantly lower environmental
impacts than a combination of pressing and solvent use. The latter method showed an
8–9% increase for several impact categories, such as human toxicity and particular matter
potential. The impact based on photochemical oxidant formation potential increased by
15% due to hexane emissions [88]. When comparing the use of hexane vs. ethanol during
the soybean oil extraction process, the net present value (the economic metric representing
cash flow) was 10.2% higher for hexane extraction; however, the global warming potential
for ethanol extraction was lower by 10,600 tons of CO2eq per year [89].
Additionally, EIA has been performed to compare mass flows, energy consumption
and global warming potential between hexane, expeller and EAEP methods for soybean
oil processing (Table 2). As with mustard seeds, it was demonstrated that the use of
hexane to extract soybean oil had the highest environmental impact. Additionally, hexane
displayed a higher thermal risk and impacts on acute, chronic and eco-toxicity; however,
hexane extraction was the lowest regarding air pollutant and greenhouse gas (GHG)
emissions. The expelling process had the lowest environmental impact because it uses the
Processes 2021, 9, 1839 9 of 14

least amount of chemical additives. However, its downside was generating the highest
GHG (about 11 times more CO2 and CH4 emitted from 1 kg of soybean oil production
compared to hexane extraction) and the highest criteria pollutant emissions due to the
energy used during pressing. EAEP was concluded to be an ideal alternative candidate
because it has lower environmental impacts compared to hexane extraction, and released
less GHG and pollutants compared to expelling [90]. Although EAEP was again shown
to lower environmental impacts in another study on soybean oil extraction, it had the
highest CO2 and GHG emissions compared to pressing and hexane, which was explained
by the intensive electricity consumption used during the pretreatment (cleaning, drying,
cracking, flaking and tempering) of the soybean substrate to maximize the oil yield. As a
consequence, it was concluded that expelling, and not EAEP, was the cleanest oil extraction
method [91].

Table 2. Comparison of published techno-economic analysis and environmental impact analysis studies on soybean oil
extraction methods (adapted from [24,70,90,92,93]).

Profitable Capacity of
Extraction Method Oil Yields Revenue Sources Environmental Impact Analysis
Annual Oil Production
Similar environmental impacts
24% from oil
to expelling
EAEP 1 Over 80% >17 million kg >70% from
Lower greenhouse gas and criteria
insoluble fibers
pollutants emissions
Lowest environmental impacts
23% from oil
Extruder-expelling 72% 13 million kg Highest greenhouse gas and criteria
77% from meal
pollutants emissions
Highest environmental impact
39% from oil
Most energy efficient
Hexane Over 99% 87 million kg >60% from meal
Lowest greenhouse gas and criteria
and hulls
pollutants emissions
1 Enzyme-assisted aqueous extraction processing.

7. Techno-Economic Analysis (TEA)


Economic feasibility is the main driver in the decision process on which extraction
method to apply at an industrial scale; however, environmental impacts are increasingly
being considered. Techno-economic analysis (TEA) allows the breakdown of profits and
costs for any type of industrial process, and the analysis has been applied to oil extraction.
A wide variety of parameters need to be considered when performing TEA, including, but
not limited to, the scale of the extraction processes, type of substrate and extraction plant
location [24]. Despite some variabilities in the outcomes of studies focusing on oil extraction
methods, the valorization of co-products is of paramount importance for making profit
and offsetting the costs for advanced extraction technology in processing plants [24,70,92].
When possible and economically viable, these co-products are widely utilized as animal
feed and non-food applications instead of being discarded as food waste [24,92].
A good example illustrating this point is what occurs in the soybean oil industry
(Table 2). During expeller pressing, the solid residue made of fiber and protein often has
residual oil, which adds value to this co-product. When TEA was applied to a two-step
extruder–expelling of soybean oil extraction, it was found that soybean meal was the
driving force in profits, contributing 75% of total revenues [24]. Similarly, the importance of
soybean co-products on the techno-economic value of EAEP extraction was demonstrated.
Although EAEP led to an extraction yield that can compete with organic solvent extraction,
the enzyme and facility costs for extraction and demulsification equipment were high.
Soybean oil profits only accounted for 27% of total revenues, but co-product utilization
in soybean/corn-based ethanol production made up 74% of total revenues. Other money
saving practices may include recycling the enzymes and reusing the skim as a water
source [70].
Processes 2021, 9, 1839 10 of 14

As with soybean oil extraction, the economic feasibility of alternative green extrac-
tion methods for other seeds were demonstrated to be dependent on their co-products.
The values of the co-products (rapeseed meal and molasses) compensated for the higher
crushing costs resulting from ethanol extraction compared to the hexane extraction of
rapeseed oil [37]. The economics involved in the industrial scale of SCO2 oil extraction of
3000 ton/yr of grape marc were calculated. Selling the dried skins and exhausted seed
powder by-products for cattle feed garnered extra revenue of about 60 EUR/ton (USD
78/ton). The 2100 and 2700 tons/year of dried skins and exhausted seed powder produced,
respectively, helped meet the breakeven point of 5.9 EUR/kg (USD 8/kg) [94]. In conclu-
sion, the extraction yield and cost were not the sole indicators of the economic viability of
an oil extraction process. Co-products were an important piece of the puzzle.
TEA is a powerful tool for evaluating facility scale-up and subsequent economics
of oil extraction processes. For example, a TEA model on soybean oil hexane extraction
identified that a plant capacity of 34.6 million kg of annual soybean oil production was
needed for the process to financially breakeven [92]. For the EAEP of soybean oil to be
profitable, annual oil production could not fall below 8.5 million kg [70]. SCO2 extraction
using two extractors in series increased production efficiency of grapeseed oil from 83–86%
compared to one with only a larger single extractor. Food waste was also reduced by
utilizing grape stalks and skin by-products as thermal energy during SCO2 extraction.
The grapeseed oil market value was reported to be as high as 30 EUR/kg (USD 39/kg).
When making the assumption that SCO2 extracted oil will have similar quality and thus
comparable market value, it was demonstrated the oil has market potential [94]. Another
simulation modeled the economics of vegetable oil extraction in a SCO2 industrial plant,
investigating how adjusting the extraction time and the particle diameter of the substrate
can alter costs. Maintaining a 2.3-h SCO2 extraction time reduced the production cost to
USD 9.4/kg oil. Increasing the particle size from 0.5 to 4 mm can decrease the extraction
time from 5 to 3.6 h [42].
TEA is, therefore, an integral part of determining whether an oil extraction method is
feasible at a commercial scale. Therefore, processors must consider substrate preparation
and extraction flow processes to make large-scale, green oil extraction more economi-
cal [40]. However, it is important to note that there are limitations to studying industrial
plant economics using a simulation approach. Models typically assume laboratory scale
conditions, which set ideal parameters for substrates that are less feasible at commercial
scale. Therefore, scale-up predictions must be validated, and more research is needed to
refine the accuracy of cost estimates [42]. Further investigation and collaboration with
industrial adopters of SCO2 technology is required to better understand these large-scale
oil extraction projects.
While TEA is crucial for identifying economic feasibility, more studies are now inte-
grating an environmental component to it. A techno-economic study comparing subcritical
water, SCO2 and solvent extractions of bioactive compounds from grape marc emphasized
the energy-intensive and costly aspect of SCO2 extraction. SCO2 extractions had the high-
est cost of manufacturing (USD 88/kg product) and the lowest net present value (-USD
920,000). SCO2 extraction also had the highest environmental impact due to energy use
(11.8 kg CO2 -eq/kg product), which countered the common perception that SCO2 technol-
ogy is more environmentally friendly [47]. However, comparative studies are lacking in
the scientific literature, and future development of the edible oil industry would benefit
from more techno-economic analyses between various extraction methods.

8. Conclusions
The food industry has increasingly promoted a circular, green economy by prioritizing
sustainability and a reduction in food waste. One way to reduce waste is through the
development of functional by-products. Specialty seeds have been a target for conversion to
edible oils for human consumption. Several factors such as profitability and environmental
sustainability should be addressed when determining which of the many existing extraction
Processes 2021, 9, 1839 11 of 14

methods to implement. Ethanol and SCO2 extractions are considered viable alternatives
to using hexane. Additionally, the use of enzymes during the aqueous extraction of
seeds allows for a process with less environmental risks compared to traditional hexane
extraction. The implementation of economically feasible, greener extraction practices in an
industry setting requires the valorization of co-products and optimization of extraction
parameters. With increasing interest by consumers for sustainable food products, the
specialty oil industry would benefit from improved extraction methods supported by both
techno-economic studies and environmental impact and life cycle analyses.

Author Contributions: Conceptualization, S.J.; investigation, V.M.L. and S.J.; writing–original draft
preparation, V.M.L., K.A.R. and S.J.; supervision, S.J., project and administration, S.J., funding
acquisition, S.J. All authors have read and agreed to the published version of the manuscript.
Funding: This work was funded by the National Institute of Food and Agriculture, National Needs
Graduate Fellowship Program, United States Department of Agriculture, No. 2017-38420-26767.
Partial funding for this project has been made available by the California State University Agricultural
Research Institute (ARI) project 19-03-120.
Institutional Review Board Statement: Not applicable.
Informed Consent Statement: Not applicable.
Data Availability Statement: Not applicable.
Conflicts of Interest: The authors declare no conflict of interest.

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