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Article history: Inappropriate disposal of Used Cooking Oils (UCOs) can generate major problems, such as the operational
Received 20 March 2015 problems occurring in wastewater treatment plants when discharged into sewerage systems. In this
Received in revised form paper the best methods to process the UCO-to-biodiesel chain are reviewed putting emphasis on the
1 June 2015
most critical technical and practical guidelines including best practices, quality characteristics of the
Accepted 18 September 2015
collected UCO, potential implications, environmental performance and risks, and at the same time
Available online 11 November 2015
highlighting the strong and weak points of each analyzed route. The most common transesterification
Keywords: processes (homogeneous-catalyzed, heterogeneous-catalyzed, enzymatic, supercritical methanol, non-
Biodiesel catalyzed) are evaluated according to environmental, technical, health and safety, market and EU policy
Used Cooking Oil
criteria.
Transesterification
& 2015 Elsevier Ltd. All rights reserved.
Best practices
Environmental impact
Contents
1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 74
2. Existing processing technologies and practices . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 75
2.1. Biodiesel producing procedure . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 75
2.2. Common practices in transesterification . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 76
2.2.1. Homogeneous-catalyzed transesterification . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 76
2.2.2. Heterogeneous-catalyzed transesterification . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 76
2.2.3. Enzyme-catalyzed transesterification . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 77
2.2.4. Non-catalyzed transesterification . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 77
3. Crucial issues concerning the most common production practices and biodiesel distribution methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 78
4. Environmental impact analysis of UCO-to-biodiesel . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 80
5. Comparison of main biodiesel production processes using UCOs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 81
6. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 82
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 82
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 82
http://dx.doi.org/10.1016/j.rser.2015.09.039
1364-0321/& 2015 Elsevier Ltd. All rights reserved.
T.D. Tsoutsos et al. / Renewable and Sustainable Energy Reviews 54 (2016) 74–83 75
Table 1
EU Biodiesel production and capacity [5].
YEAR 2002 2003 2004 2005 2006 2007 2008 2009 2010 2011 2012 2013 2014
EU biodiesel production (kts) 1065 1034 1933.4 3183.4 4890 5713 7755 9046 9570 8607 8927 10,367 N/A
EU biodiesel production capacity (kts) N/A 2048 2246 4228 6069 10,289 16,000 20,909 21,904 22,117 23,538 24,216 23,093
16000
14000
12000
10000
8000
6000
4000
2000
0
*estimation
Table 2
Production capacity of the main EU biodiesel producers in Europe in 2013 (ts) [6].
Diester Industrie & Diester Industrie International (Sofiproteol) France France (5),Germany (1), 2,500,000
Italy (1), Belgium (1)
Neste Oil Finland Finland (2), Netherlands (1) 1,180,000
Biopetrol Industries Switzerland Germany (2), Netherlands (1) 1,000,000
ADM Biodiesel Germany Germany (3) 975,000
Infnita (Musim Mas) Spain Spain (2) 900,000
Marseglia Group (Ital Green Oil and Ital Bi Oil) Italy Italy (2) 560,000
Verbio AG Germany Germany (2) 450,000
Cargill/Agravis Germany Germany (2) 250,000
Petrotec Germany Germany (2), Spain (1) 185,000
The EU has supported the increase of biofuel consumption in oil, which is used for frying food. Inappropriate disposal of UCO
transport as means of reducing the emissions of Greenhouse Gases may generate major problems, such as operational problems
(GHGs), as well as supporting the security of energy supply, techno- occurring in wastewater treatment plants when discharged into
logical development, economic development at regional scale and job sewerage systems [14].
creation. Fig. 1 shows the biofuels consumption in transport in EU. A Strengths, Weaknesses, Opportunities and Threats (SWOT)
The major actors in the EU biodiesel market are shown in Analysis of Sustainable Management of UCOs is given below
Table 2,[7]. Since 2009, all EU Member States (MS) have been sub- (Table 3).
ject to the Renewable Energy Directive (RED) [8], which requires MS This paper displays the best methods to process the UCO-to-
to comply with a target of 10% of renewable energy in the transport biodiesel chain putting emphasis on the most critical technical and
sector by 2020, the majority deriving from biofuels, predominantly practical guidelines including best practices, quality characteristics
biodiesel. The EU is, also, committed to reduce GHG emissions to of the collected UCO, potential implications, environmental perfor-
80–95% below 1990 levels by 2050. The “Energy Roadmap 2050” mance and risks, highlighting the strong and weak points of each
adopted on 15 December 2011 [9] provides directions towards a analyzed route. Based on the field work, as well the verification of
future European sustainable energy system. Furthermore, according the existing literature done during the project period the most
to the Communication of 8 March 2011, “A Roadmap for moving to a common transesterification processes (homogeneous-catalyzed,
competitive low carbon economy in 2050" [10] the EU should heterogeneous-catalyzed, enzymatic, supercritical methanol, non-
prepare for cutbacks in its domestic GHG emissions by 40% by 2030, catalyzed) are evaluated according to environmental, technical,
and by 80% by 2050, calculated with respect to 1990 levels. Sectoral health and safety, market, EU policy criteria.
strategies should accompany this roadmap supporting technologi-
cal innovations.
The exploitation of Used Cooking Oils (UCOs) to produce bio- 2. Existing processing technologies and practices
diesel is in line with the RED, covering GHGs, biodiversity and
carbon stock. UCOs and tallow (excluding category 3 tallow) use 2.1. Biodiesel producing procedure
the EC default value for ‘waste vegetable and animal oil’. For the
use of the UCOs in the fatty acid methyl esters (FAME) production Biodiesel can be blended with petrodiesel at any percentage even
the Carbon Saving is 83% [11] to 85% [12,13]. though pure biodiesel ('B100') is equally suitable for diesel engines.
UCO is a waste produced in the domestic sector, canteens, Either primary (i.e. straight or virgin) oils or secondary (used) oils can
hotels, restaurants and food industry, existing in edible vegetable be used with no discernible difference in the product. Fig. 2 shows the
76 T.D. Tsoutsos et al. / Renewable and Sustainable Energy Reviews 54 (2016) 74–83
process of converting used cooking oils into biodiesel fuel. Technically, used as diesel fuel in compliance with the EN14214 Standard and
the methods for producing biodiesel from UCO do not differ from other national quality standards and technical norms.
conventional transesterification processes using alkaline, acid and The advantages and disadvantages of the transesterification
enzymatic catalysts. method are summarized in Table 4, as reported in relevant studies
Methanol (MeOH) is the normally used alcohol in the process and research reports.
due to its low cost, physical and chemical advantages. Homo-
2.2. Common practices in transesterification
geneous basic catalysts are the most widely used in the industry as
they accelerate the process and achieve milder reaction conditions,
Transesterification is a relatively simple process that produces
either using discontinuously (batch) or continuously systems. After
biodiesel and Fatty Acid Ethyl Esters (FAEE), according to the
the reaction, the glycerol is separated either by settling or cen- standards EN 14214 for Europe and ASTM D 6751-12 for USA.
trifuging; the organic phase (biodiesel) is then purified before being The most common processes are:
Table 5
Biodiesel production from UCO using heterogeneous catalysts.
than the novel catalytic methods, especially for the reactor and pump.
Cost of production
In order to increase the technical and economic feasibility of super-
critical transesterification, further studies are required in the direction
of optimizing the operating parameters of this process.
Moderate
Moderate
High
High
High
High
High
High
High
Low
3. Crucial issues concerning the most common production
Combined use of Lipozyme TL IM and Novozyme 435 along with tert-butanol as solvent
Stepwise addition MeOH and preincubation of enzyme in methyl oleate and soyabean practices and biodiesel distribution methods
Stepwise addition of MeOH and removal of glycerol using the solvent, iso-propanol
A novel acyl acceptor, methyl acetate which had no inhibitory effects was used
Biodiesel is highly biodegradable and has minimal toxicity; it
can replace petrodiesel often including internal combustion
engines without major modifications [29]. A slight decrease of the
engine’s performance is reported with almost zero emissions of
Stepwise addition of MeOH and removal of glycerol by dialysis
91.3
92
98
95
97
97
97
reactions that affects the components; the fatty materials are used
Ethyl acetate
MeOH
MeOH
MeOH
Novozyme 435 & Lipozyme TL IM MeOH
MeOH
BuOH
Oxidation reactions.
Hydrolysis of triglycerides.
Polymerization of triglycerides.
Novozyme 435
Novozyme 435
Novozyme 435
Novozyme 435
Novozyme 435
Novozyme 435
Novozyme 435
Novozyme 435
shown in Table 9.
Enzyme
Soyabean oil
Soyabean oil
Rapeseed oil
Jatropha oil
The transfer of water from the food to the frying oil. This is a
determinant of its degradation reactions. It is also important to
Shimada et al. (2002)
Du et al. (2004)
Xu et al. (2004)
Developer/year
Li et al. (2006)
Table 7
Reaction parameters and optimal conditions of supercritical transesterification for various oil types and alcohols.
Developer/year Oil type Alcohol temp. P (MPa) Alcohol/oil Reaction time Reactor (size/type) Extent of reaction
(mole/mole) (min)
Bunyakiat et al. Coconut and palm MeOH, 350 °C 19 42:1 7–15 251 mL 95% Methyl ester
(2006) kernel Continuous reaction in a content
tubular vesicle
Demirbas (2002) Hazelnut kernel and MeOH, 350 °C Not reported 41:1 5 100 mL 95% Methyl ester
cottonseed Batch content
Rathore and Madras Palm and groundnut MeOH, 400 °C 20 50:1 30 11 mL 95% Triglyceride
(2007) Batch conversion
Sawangkeaw et al. Palm kernel MeOH, 350 °C 20 42:1 30 250 mL 95% Methyl ester
(2007) Batch content
Saka and Kusdiana Rapeseed MeOH, 350°C 45 42:1 4 5 mL 98% Methyl ester
(2001) Batch content
Minami and Saka Rapeseed MeOH, 350 °C 20 42:1 30 200 mL Continuous reaction 87% Methyl ester
(2006) in a tubular vesicle content
Yin et al. (2008) Soybean MeOH, 350 °C 20 42:1 30 250 mL Batch 95% Methyl ester
content
Madras et al. (2004) Sunflower MeOH and 20 40:1 30 8 mL Batch 97% Triglyceride
EtOH, 400 °C conversion
Vieitez et al. (2011) Castor EtOH, 300 °C 20 40:1 Not reported 42 mL Continuous reaction 75% Ethyl esters
in a tubular vesicle content
Silva et al. (2007) Soybean EtOH, 350 °C 20 40:1 15 42 mL Continuous reaction 80% Triglyceride
in a tubular vesicle conversion
Balat (2008) Sunflower EtOH, 280 °C Not reported 40:1 5 100 mL Batch 80% Ethyl esters
content
Table 8 Table 9
Advantages and disadvantages of the transesterification processes. Results of frying.
Homogeneous-catalyzed Acceptable reac- Sensitive to FFA Oxidation reactions Fixed oxidation compounds (oxidized TG,
transesterification tion time Use of water epoxides, etc.)
Easy Glycerol quality Volatiles (hexanal, pentane, 2,4-decadienal,
Heterogeneous-catalyzed Not so sensitive to Expensive pentanol, etc.)
transesterification FFA Oxidized oligomers
Use of water Longer reaction time Sterol oxides
Glycerol quality Hydrolysis of triglycerides Free fatty acids (FFA)
Enzyme-catalyzed Not so sensitive to Very expensive Diglycerides (DG)
transesterification FFA Monoglycerides (MG)
Use of water Polymerization of triglycerides Non-polar dimers
Glycerol quality Longer reaction time Other non-polar oligomers
Supercritical MeOH Not so sensitive to Very expensive
FFA
Use of water The main harmful effects of the oil’s degradation compounds
Glycerol quality Use of energy
are presented in Table 10 below:
It is obvious that these compounds engender toxic effects, so
regarding safety of use in feeds is enormous and should be the created toxicity value is the sum of all the substances present
taken into account. in a sample. The UCOs can be toxic, so they must be handled in the
same way.
Biodiesel distribution includes activities in the storage infra-
structure, the blending, the quality assurance and the
80 T.D. Tsoutsos et al. / Renewable and Sustainable Energy Reviews 54 (2016) 74–83
Table 10
Harmful effects of the oil's degradation compounds.
Hydroperoxides Low, only at low temperatures Enzymatic dysfunction of the intestinal mucosa
Induction of colon cellular proliferation
Epoxides, TG and Oxidized FAcids Moderate (low temp.) Hepatic hypertrophy
Hepatic enzymatic dysfunction
Secondary compounds Moderate–High Hepatoxicity
Mutagenicity
Oxidized cyclic monomers Moderate–Low especially at high temperature Reduced growth and death
Non-oxidized dimers and Oligomers Moderate–High at 200 °C and low oxygen concentration Diarrhea
Oxidized dimers Predominant at high temperature with excess of oxygen Reduced growth
Oxidized oligomers Predominant at high temperature with excess of oxygen Reduced growth
Oxysterols Variable Atherogenicity
Cytotoxicity/Mutagenicity
Table 11 Table 12
Assessment of the biodiesel distribution methods. The environmental impact per 1 t biodiesel production from UCO [31,32]
FOOD
HOUSEHOLDS
INDUSTRY
Intermediate
Recycling Center
Collection of UCO
Containers
Emissions
UCO
Solid
WASTEWATER Pretreatment of UCO
Wastewater Wastes
Treatment
UCO
UCO
Reactants Glycerol
Additives Emissions
Fertilizers
biodiesel process that contributes most to human toxicity and results of the two-stage supercritical process, with reduced oper-
eutrophication is also transesterification, accounting for 66% and ating pressure, temperature and MeOH to oil ratios, will be reliably
63%, respectively. The human toxicity emanate come mostly from translated into industrial scale production [35].
the emission of volatile organic compounds during sugarcane Obviously acid, alkali, or enzymatic catalyzed and supercritical
harvesting (burning). The greatest eutrophication impact comes transesterifications are alternative approaches that have been used
from the waste produced during distillation (vinasse). for biodiesel production having both pros and cons. Amongst them
the type of feed stock is the most critical factor in the production
of biodiesel. It is essential to understand that UCO can decrease
5. Comparison of main biodiesel production processes using biodiesel production costs. On the other hand, the shortage of UCO
UCOs in EU may lead in imports, therefore the price of obtaining the raw
material may be higher in the future. However, the cooking pro-
The evaluation criteria of main biodiesel production processes cess influences negatively the oil properties and can create dif-
using UCOs (chapter 2) are: ferent types of impurities in the oil, as well as increasing the FFA
and water oil content. Hence, these obstacles increase the pur-
Environmental ification and separation costs in the downstream biodiesel
Technical production.
Health and safety The transesterification with alkali catalysts is the most common
Market Opportunities and Barriers conventional method for biodiesel production. However this
Harmonization with EU Directive and Sustainability method causes serious problems in the purification part since they
Climate/Geographical Parameters are highly sensitive to FFA and water content in the UCO. On the
contrary the acid catalyzed process is not sensitive to FFA and
The results of the above mentioned comparative analysis are water content like base catalysts, with the only drawback that the
shown at Table 13. production process is slower.
The supercritical process always generated a higher impact on The utilization of enzymatic catalysts proved very promising,
the environment, due to the requirement of large amounts of but since the catalysts are expensive, this process is not, yet, sui-
MeOH during the reaction and consequently the energy expendi- table for industrial production of biodiesel [36]. Furthermore, the
ture in MeOH recirculation. In order to make the supercritical supercritical method requires high temperature and pressure,
MeOH process feasible, from an environmental point of view, the making the process, yet, neither economical nor environmentally
distillation column in the MeOH recovery process has to be friendly.
replaced with a different less energy-intensive process technology. Therefore, scientists focus on the utilization of heterogeneous
Alternatively, it remains to be confirmed whether the promising acid and base catalysts in biodiesel production since the catalysts
82 T.D. Tsoutsos et al. / Renewable and Sustainable Energy Reviews 54 (2016) 74–83
graphical Parameters
Moderate dependent
Moderate dependent
practice. In a continuous process the reusability of the catalysts is
High dependent
High dependent
Climate/Geo-
the most important property making them economical for
industrial production. Hence, in order to reduce production costs,
reaction time, catalyst and alcohol requirements in transester-
ification reactions have demonstrated various processes such as
membrane reactor, reactive distillation, reactive absorption,
microwave, and ultrasonic. These processes increase the quality
Covering the EU Directive on
Sustainability (Medium
Sustainability (Medium
Sustainability (Medium
Sustainability (Medium
any engine modification.
Realistically, for the current time, the use of homogenous cat-
alysts is the optimum way for the UCO-to-biodiesel chain. The
following essential considerations must be taken into account:
covering)
covering)
covering)
covering)
1. KOH catalyst is less effective than the sodium based catalysts. A
catalyst concentration of 0.8 (wt%) for UCOs ensures that visc-
osity is within the limits, but then purity is lower than the
High reaction time (Med-
Increased production of
Increased production of
Increased production of
methylesters (Medium
production (Medium
purity was generally very close to the limit, better results are
Low quality (Low
methylesters.
High costs
negative)
negative)
negative)
Normal (Medium
Normal (Medium
(Low positive)
Health and
positive)
positive)
positive)
6. Conclusions
safety
(Under development
High glycerin purity
siderably reduced and the negative impact of the waste oil dis-
(Well established
(Less established
(Less established
technology)
technology)
technology)
Acknowledgments
Waste water and saponified products
The authors and all the consortium partners are grateful to the
EACI executives for their support and helpful cooperation. This
Evaluation criteria of examined biodiesel production processes.
No waste water
Environmental
transesterification.
transesterification
transesterification
Supercritical MeOH
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