Chapter 2

Utilization of Vegetable Oil as Bio-lubricant

and Additive

Abstract  The environmental and toxicity issues of conventional lubricants as well

as their rising cost lead to renewed interest in the development of environmental
friendly oils as lubricants and industrial fluids. This chapter provides a review of
the fundamental research works carried out on tribotesters to investigate the effec-
tiveness of vegetable oil in suppressing wear and frictional force. Results obtained
in these studies are useful to explain the mechanism by which the vegetable oils
reduce friction and tool wear in machining (Chap. 3). Intensive review of the pre-
vious works shows that vegetable oils have high potential to be used as lubricant
and additive to replace conventional lubricants and additives.

Keywords Bio-additives · Bio-lubricant · Vegetable oil lubricant  · Tribotesters · 

Palm oil lubricant

2.1 Exploration for Environmental Friendly Lubricant

Additives

Additives are widely used to improve the lubricant performance of base oil.
Without additives, even the best base fluids are deficient in some features. The per-
formance of a lubricant depends collectively on the base oil, additives and formu-
lation. Phosphorus, sulphur, zinc dialkyldithiophosphates (ZDDP) are examples
of some of the widely used additives. Sulphur-containing additives are probably
the earliest known additive compounds in lubricants. In recent decades, it had
attracted a considerable amount of research efforts to further explore their poten-
tial as effective anti-wear (AW) and extreme pressure (EP) additive (Zhang et al.
1999; Bhattacharya et al. 1995).
Fatty acids, alcohols, amines and esters are some of the AW additives used to
produce a molecular film adhering to the surfaces by physical or chemical adsorp-
tion (Stachowiak and Batchelor 2005). The lubricant films are built up of orderly
and closely packed arrays of molecular layers, with the polar head of the additive

© The Author(s) 2015 7

W. Liew Yun Hsien, Towards Green Lubrication in Machining,
SpringerBriefs in Green Chemistry for Sustainability,
DOI 10.1007/978-981-287-266-1_2
8 2  Utilization of Vegetable Oil as Bio-lubricant and Additive

molecule anchored on the worn surface (Kenbeck and Bunemann 2009). There are
also strong dipole interactions between the chains. The effectiveness of the lubri-
cant depends greatly on the tenaciousness of the bond between the polar end group
of the molecular chain and the metal surface where it adheres to (Tan et al. 2002).
Sulphur-, chlorine- and phosphorus-containing compounds are commonly used
as EP additives to provide protection in EP condition (Canter 2007). These addi-
tives would form layers of iron compounds such as sulphides, chlorides and phos-
phates, respectively, through tribochemical reactions (Hsu and Gates 2005). The
mechanism of lubrication which is influenced by these additive elements involves
some chemical changes on the surface to form a surface protection film. This film
is called boundary lubricating film or a tribofilm. The tribofilm plays a major role
in determining the friction and wear of the tribological interaction. The morphol-
ogy, integrity and mechanical properties of the tribofilms may vary depending on
the properties of rubbing material as well as the type of lubricant additives used
(Biswas 2000; Kim et al. 2010).
ZDDP was initially used as an antioxidant, but their excellent AW properties
were quickly recognised and had been investigated intensively by many research-
ers. The AW function of ZDDP was attributed to its decomposed products that
led to the formation of sacrificial reaction layers on the rubbing surfaces. A vari-
ety of ZDDP decomposition mechanisms and the associated chemistry of reac-
tion film had been proposed by many researchers (Mosey et al. 2005; Fuller et al.
1997, 1998; Brancroft et al. 1997; Willermet et al. 1995; Spedding and Watkins
1982). However, the concern for the content of heavy metal zinc and phospho-
rus as environmental contaminants had resulted in efforts to find more environ-
mentally benign replacements for industrial applications (Cardis et al. 1989).
It was stated that even ashless sulphur-containing compounds do not n­ ecessarily
have good ecotoxicological profiles for environmentally friendly lubricants.
Environmentally friendly lubricants must also have high level of biodegradability
(Habereder et al. 2009).
The environmental and toxicity issues of conventional lubricants as well
as their rising cost related to a global shortage and their poor biodegradability
led to renewed interest in the development of environmental friendly lubricants.
Environmental legislation by OSHA and other international regulation authori-
ties discourage the use of mineral oil-based lubricant and environmental-harmful
additives. There has been increasing demand for green lubricants and lubricant
additives in recent years. Vegetable oils are viable and good alternative resources
because of their environmental friendly, non-toxic and readily biodegradable
nature. The majority of bio-lubricants are based on esters. There are natural esters
which are triglycerides of vegetable oils. Oleochemical esters of fatty acids such
as diesters, polyolesters and complex esters are derived from sunflower, rape-
seed, palm oil and coconut. Triglycerides of vegetable oils are more polar than
petroleum-based oils, thus they have a higher affinity to metal (Suarez et al.
2010). Owing to this character, vegetable oils and their derivatives are suitable
2.1  Exploration for Environmental Friendly Lubricant Additives 9

for lubrication applications. Conversely, their low thermo-oxidation stability,

primarily due to the presence of bis-allylic protons is the main limitation (Fox
and Stachowiak 2007; Becker and Knorr 1996). They also have poor corrosion
resistance (Ohkawa et al. 1995). Some studies have also shown that most veg-
etable oils undergo cloudiness, precipitation, poor flow, and solidification upon
long-term exposure to cold temperature (Rhee et al. 1995; Kassfeldt and Goran
1997). Erhan et al. (2006) have demonstrated that thermo-oxidative stability and
cold flow property can be improved using a combination of proper blending of
chemical additives, diluent and high-oleic vegetable oils. Another major obsta-
cle is the cost of the bio-lubricants. A bio-lubricant costs somewhere between
30–40 % more compared to a conventional lubricant. Lubricant formulations for
more environmentally benign are, therefore, being developed based on their ben-
efits and limitations.
Oils with more polar groups (like carboxylic acids and esters) possess more
sites to react and adsorb with metal surfaces to provide boundary lubrication
effects (Stachowiak and Batchelor 2005). A lubricating film with strong bonding
to the surface and adequate cohesive interaction among lubricant molecules can
effectively reduce the friction and the amount of wear. To maintain a low friction
and wear, the lubricating film has to withstand extremes of temperature variations,
shear degradation and maintain excellent boundary lubricating properties through
strong physical and chemical adsorption with the metal.
The additive molecules dissolved in the oil are attracted to the surfaces by
adsorption forces governed by their polarity (Sharma et al. 2009; Kalin et al.
2006). It was found that the friction reduction effect increased with larger amount
of adsorptive polar group of the additive in the base oil (Tohyama et al. 2009;
Kurth et al. 2007; Adhvaryu et al. 2004). In fact, the polarity of both the base
­fluids and the additives is very important because each component of the mixture
is competing for the metal surfaces reaction. A polar additive that would normally
adsorb and desorb reversibly from a metal surface in a non-polar base fluid might
have a much lower concentration on the surface than in a formulation that contains
a high concentration of polar base fluid such as ester or vegetable oil (Rudnick
2009). Works by Suarez et al. (2010) shows that the wear performance of ZDDP
additives contained in polar base fluid is better than that of ZDDP blended in a
non-polar base fluid as smaller wear track width and larger load carrying capac-
ity features were observed on the wear track produced in the former lubricant.
Hsu et al. (1988) suggested that the first and the foremost of the dynamic and
sequential competition in a solution that contains more polar groups is the pref-
erential adsorption of the most polar molecules onto the surface at a particular
temperature. However, the increase in the amount of polar compounds in the oil
could reduce the adsorption of additives on the metal surface due to competitive
adsorption, whereby the efficiency of AW additives could thus decrease (Studt
1989) and it could also provide corrosive effects (Hsu and Gates 2005; Jimenez
and Bermudez 2007).
10 2  Utilization of Vegetable Oil as Bio-lubricant and Additive

2.2 Wear and Friction Reduction by Vegetable Oil

as Bio-lubricant and Additive

Vegetable oils are viable and good alternative resources because of their environ-

mental friendly, non-toxic and readily biodegradable nature. The triacylglycerol
structure with long fatty acid chains and presence of polar groups in the vegetable
oils make them amphiphilic in character, therefore allowing them to be an excel-
lent choice as lubricants and functional fluids. These triacylglycerol molecules in
vegetable oils orient themselves with the polar end at the solid surface making a
closed packed monomolecular or multimolecular layer resulting in a surface film
that provides desirable qualities in a lubricant (Rudnick 2009). Other advantages
include very low volatility due to the high molecular weight of the triglyceride
molecule and excellent viscosity properties. Table 2.1 shows several type of vege-
table-based lubricants developed for industry applications.
Vegetable oils may not suitable to be used as lubricants in their natural form
due to their poor thermo-oxidation stability, low temperature behaviour and other
tribochemical degrading processes that occur under severe conditions of tempera-
ture, pressure shear stress and environment (Fox and Stachowiak 2007). However,
they can be used effectively as additives, in particular to improve the polarity behav-
iour of non-polar base fluid solutions, which would contribute to better tribological
performance. In the past several researchers have investigated the effectiveness of
methyl ester as additive in diesel. Sulek et al. (2010) found that the presence of fatty

Table  2.1  Several type of vegetable-based lubricants developed for industry applications

(Shashidhara and Jayaram 2010)
Type of oil Application
Canola oil Hydraulic oils, tractor transmission fluids, metalworking fluids, food grade lubes,
penetrating oils, chain bar lubes
Castor oil Gear lubricants, greases
Coconut oil Gas engine oils
Olive oil Automotive lubricants
Palm oil Rolling lubricant,-steel industry, grease
Rapeseed oil Chain saw bar lubricants, air compressor-farm equipment, Biodegradable greases
Safflower Light-coloured paints, diesel fuel, resins, enamels
oil
Linseed oil Coating, paints, lacquers, varnishes, stains
Soybean oil Lubricants, biodiesel fuel, metal casting/working, printing inks, paints, coatings,
soaps, shampoos, detergents, pesticides, disinfectants, plasticisers, hydraulic oil
Jojoba oil Grease, cosmetic industry, lubricant applications
Crambe oil Grease, intermediate chemicals, surfactants
Sunflower Grease, diesel fuel substitutes
oil
Cuphea oil Cosmetics and motor oil
Tallow oil Steam cylinder oils, soaps, cosmetics, lubricants, plastics
2.2  Wear and Friction Reduction by Vegetable Oil as Bio-Lubricant and Additive 11

acid methyl ester derived from rapeseed oil in diesel fuel resulted in 20 % decrease
in friction and twofold decrease in wear. Similarly, Sukjit and Dearn (2011) demon-
strated that adding as little as 5 % of fatty acid methyl ester derived from rapeseed
in diesel fuel could result in reduction in the wear scar diameter by 40 %.
Malaysia is often viewed as a country that evolved from dependence on tin
and rubber to export-oriented manufacturing dominated by electronics assembly,
but the commodity that made the country to the technological frontier is palm oil.
Palm oil is now a major pillar of Malaysia’s industrialization and it holds a con-
siderable lead in global markets. To ensure a sustainable growth of palm oil indus-
try in the country and remains competitive in the global market, palm oil industry
in Malaysia in recent years has been shifting to palm oil product diversification
from a conventional commercial cultivation as its main export focus until more
years to come. Research and development effort, therefore, became more critical,
in particular, to explore and develop new palm oil-based products for higher value
added in the palm oil chain. Recently, it has been promoted as a biofuel feed-
stock in compression ignition engines (diesel engines). Palm oil methyl ester has
an ester functional group which is a classic example of additive used for lubrica-
tion (Canter 2007). Characterization palm oil methyl ester can be carried out using
fourier transform infrared spectroscopy (Liew et al. 2014). Palm oil methyl ester
was produced from crude palm oil through transesterification process, whereby the
triglyceride of palm oil was reacted with an alcohol in the presence of a catalyst
as represented by general equation in Fig. 2.1. R1, R2 and R3 represent the hydro-
carbon chains of the fatty acid of the triglyceride. This reaction yielded esters and
glycerol, which are then separated, in which glycerol being removed as by-prod-
uct. The palm oil methyl ester was characterised using fourier transform infra-
red spectroscopy (FTIR). The FTIR spectra shows 1,750 and 1,150 cm−1 peaks
(Fig. 2.2) that correspond to C=O and C–O esters (Taufiq-Yap et al. 2011).
Various investigations had shown that palm oil methyl ester additives improved
the lubrication performance of the diesel base oil (Masjuki and Maleque 1996a,
1996b, 1997; Maleque et al. 2000). Masjuki and Maleque (1997) reported that
adding 5 vol% of palm oil methyl ester in the base oil lubricant resulted in low
wear rate of EN31 steel ball bearing. Palm oil methyl ester, converted from crude
palm oil through transesterification, has very low sulphur content (0.002 wt%),
and therefore is environmental friendly. Liew et al. (2014) found that in the

R1COOR
CH2 COOR1 CH2 OH
+
Catalyst
CH COOR2 + 3ROH R2COOR + CH OH
+
CH2 COOR3 CH2 OH
R3COOR

Triglyceride Alcohol Esters Glycerol

Fig. 2.1  Transesterification reaction for producing esters from oil (triglyceride)

12 2  Utilization of Vegetable Oil as Bio-lubricant and Additive

104.1

102

100

98

96
Transmittance (%)

94

92

90

88

86

84

82

80

78
4000 3600 3200 2800 2400 2000 1800 1600 1400 1200 1000 800 650
Wave numbers (cm-1)

Fig. 2.2  The IR spectrum of palm oil methyl ester (Liew et al. 2014)

Fig. 2.3  The change 0.9

in friction coefficient 0.8
0% Palm oil methyl ester
in different lubrication 5% Palm oil methyl ester
conditions at nominal load of 0.7
Coefficient of friction

1,100 N (Liew et al. 2014) 0.6

0.5

0.4
0.3

0.2

0.1

0
0 10 20 30 40 50 60 70
Sliding time (second)

presence of palm oil methyl ester in the mineral oil resulted in a shorter running-in
period and lower steady-state frictional coefficient at nominal load of between 600
and 800 N. The difference in the friction coefficient produced in mineral oil with
and without palm oil methyl ester became more apparent at loads above 800 N
(Figs.  2.3 and 2.4). The performances of lubricants in EP can also be expressed
in terms of welding load (Kabuya and Bozet 1995; Singh and Verma 1991).
Under mineral oil w ­ ithout palm oil methyl ester, complete welding of the four
2.2  Wear and Friction Reduction by Vegetable Oil as Bio-Lubricant and Additive 13

Fig. 2.4  Effect of nominal 0.7

load and lubrication condition
on the average coefficient of 0.6
0% Palm oil methyl ester

Average coefficient of friction

friction (Liew et al. 2014) 5% Palm oil methyl ester
0.5

0.4

0.3

0.2

0.1

0
0 200 400 600 800 1000 1200 1400 1600
Nominal load (N)

Table 2.2  Weld load and wear scar diameter for different lubrication condition
Lubrication condition Weld load (N) Average diameter scar
(mm) produced at the
nominal loads of
300 N 600 N 800 N
Mineral oil (without palm oil methyl ester) 1,200 0.28 1.97 2.60
Mineral oil (with 5 vol% palm oil methyl ester) 1,450 0.29 1.79 2.30

balls occurred at 1,200 N (Table 2.2). The presence of palm oil methyl ester in oil
resulted in a higher critical load of 1,450 N.
Gong et al. (2003) investigated the wear reduction bought about by two kinds
of synthetic thiophosphate (tri-n-octyl thiophosphate and tri-n-octyl tetrathi-
ophosphate) and tricresyl phosphate as additives in rapeseed oil in sliding of steel.
Synthetic thiophosphate resulted in lower wear and this could be attributed to the
tribochemical reactions between the steel and the thiophosphate, and the forma-
tion of a boundary and protective layer on the worn surfaces. A series of long-
chain dimercaptothiadiazole derivatives had been tested as AW and EP additives
in vegetable oil using a four-ball tester. The long-chain thiadiazole derivatives
were capable of improving the EP characteristic of the base colza oil. Thermal
films generated from these derivatives are composed of ferrous sulphate and a
small amount of adsorbed organic sulphide (Chen et al. 2012). Work by Gao et al.
(1999) showed that thiadiazole derivatives in paraffin oil under boundary lubrica-
tion at high loads resulted in greater friction reduction and exhibited better AW
properties than lubricant containing ZDDP. It was also found that thiadiazole
derivatives had better antioxidative and anticorrosive properties than ZPPD.
Synthesis of vegetable oil and thiols could result in the formation of hydroxyl
thioether derivatives in the vegetable oil. This process retained the vegetable oil
structure and its associated benefits such as high flash point, viscosity index,
lubricity and eco-friendly but removed poly-saturation in the fatty acid chain with
14 2  Utilization of Vegetable Oil as Bio-lubricant and Additive

addition of polar functional groups that significantly improved surface adsorp-

tion on metal leading to a reduction in wear and friction coefficient (Sharma et al.
2009). Xu et al. (2014a) demonstrated that catalytic esterification of crude bio-oil
derived from spirulina algae resulted in enhanced lubrication performance. The
coefficient of friction produced by ethanol blended with bio-oils esterified using
potassium fluoride/alumina and potassium fluoride/HZSM-5 zeolite as catalysts
was 22 and 10 % lower, respectively, than that produced by crude bio-oil blended
with ethanol. The esterified bio-oils produced lower friction coefficient because it
resulted in the formation of a better protective tribofilm on the worn surfaces.
Shi et al. (2014) studied the effect of water content in glycerol solution on the
viscosity, friction coefficient, wear loss and film thickness under elastrohydrody-
namic and boundary lubrication. Despite the viscosity and the film thickness of
the glycerol solutions decreased greatly with increasing water content, there was
an optimum amount of water in the glycerol solutions which resulted in the low-
est friction coefficient. A correlation was not found between friction coefficient
and wear volume loss. Under elastrohydrodynamic lubrication, the friction coeffi-
cient of rapeseed oil was about three times higher than that of pure glycerol. Under
boundary lubrication, the friction coefficient produced by rapeseed oil and pure
glycerol was similar. However, a more stable and lower friction coefficient was pro-
duced when the glycerol solution consisted of 5–20 wt% of water. While the water
content was beneficial for glycerol to decrease the friction coefficient, excessive
water content resulted in marked reduction in the viscosity and thus the load car-
rying capacity of the solution. These works showed that glycerol aqueous solutions
have great potential to replace rapeseed oils as environmentally friendly base oils.
Although coconut oil is more stable than many vegetable oils, it is not widely
used due to its high congelation temperature. Being a vegetable oil having typical
triacylglycerol structure, it has most of the salutary properties of other vegetable
oils as lubricants such as high viscosity index, good lubricity, high flash points and
low evaporative loss. Although it has similar disadvantages of poor properties at low
temperature, it shows much better thermal and oxidative stability owing to its pre-
dominantly saturated nature of its fatty acid constituents. Jayadas and Prabhakaran
(2006) found that adding 2 wt% of ZDDP in coconut oil resulted in significant wear
reduction in the four-ball test. The welding load of the coconut oil containing 2 wt%
of ZDDP was higher than that produced by commercial 20W50 Oil.
Quinchia et al. (2014) studied the frictional and lubricating film-forming proper-
ties of various type of improved vegetable oils based lubricants (high-oleic sunflower,
soybean and castor), using 4 wt% of ethylene–vinyl acetate copolymer and 1 wt%
of ethyl cellulose as additives. It was found that castor oil showed the best lubricant
properties, when compared to high-oleic sunflower and soybean oil, with very good
film-forming properties and excellent friction and wear behaviour. This could be
attributed to its hydroxyl functional group that increased both the viscosity and polar-
ity of this vegetable oil. Ethylene–vinyl acetate copolymer exerted a slight effect on
the lubricating film-forming properties, reducing the friction and wear mainly in the
mixed lubrication region. Ethyl cellulose, on the other hand, was much more effec-
tive mainly with castor oil, in improving both mixed and boundary lubrication.
2.2  Wear and Friction Reduction by Vegetable Oil as Bio-Lubricant and Additive 15

Alves et al. (2013) found that modified vegetable oils such as epoxidised sun-
flower and soybean oils resulted in lower friction coefficient than the mineral and
synthetic oils. However, the presence of CuO and ZnO nanoparticles in the epoxi-
dised vegetable oils resulted in higher friction coefficient and wear. It was pos-
tulated that the effect of nanoparticles on the wear and friction coefficient was
governed by the nature of the adsorption of the lubricant on the contact surfaces.
Adherence of the polar groups of the vegetable oils on the worn surface caused
the nanoparticles to roll and hence three-body abrasion to take place, resulting in
increased wear. The reduction in the wear and friction coefficient bought about
these oxides nanoparticles in mineral and synthetic oils could be attributed to adher-
ence of the nanoparticles and formation of a physical tribofilm on the worn surface.
Xu et al. (2014b) reported that emulsified bio-oil (produced form the fast pyroly-
sis of rice husk) produced the lowest coefficient of friction. This was followed by
bio-oil and diesel oil. The diesel and bio-oils produced the lowest and the highest
wear, respectively. It was concluded that the emulsified bio-oil produced the best
overall results and this was due the presence of various acidic components with
polar groups in the emulsified bio-oil. Suarez et al. (2009) demonstrated that adding
some soybean oil methyl esters and diesel-like pyrolytic fuel (produced through
­pyrolysis of soybean oil) enhanced the lubricity of diesel fuels. This result showed
the potential use of both bio-fuels as additives for improving the tribological prop-
erty of fossil fuels. Another work (Xu et al. 2010) found that the lubrication ability
of the diesel fuel blended with bio-oil (produced through fast pyrolyzing rice husk)
was better than that of the conventional diesel fuel. However, the presence of bio-oil
in the diesel fuel resulted in inferior anti-corrosion and anti-wear properties.

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