Journal of Cleaner Production 278 (2021) 123304

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Journal of Cleaner Production

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

Sustainable asphalt rejuvenation using waste cooking oil: A

comprehensive review
Muhammad Zahoor a, Sabzoi Nizamuddin a, Srinivasan Madapusi b, Filippo Giustozzi a, *
a
Civil and Infrastructure Engineering, School of Engineering, RMIT University, Melbourne, VIC, 3001, Australia
b
Chemical and Environmental Engineering, School of Engineering, RMIT University, Melbourne, VIC, 3001, Australia

a r t i c l e i n f o a b s t r a c t

Article history: Roads serve as a backbone of developing economies; thousands of kilometres of new roads are built
Received 6 February 2020 every year and old ones are continuously repaired. Due to the large areal extension, maintenance of
Received in revised form asphalt pavements generates significant economic, energy, social, and environmental impacts. ‘Rejuve-
29 June 2020
nation’ of reclaimed asphalt pavement (RAP) in roads helps minimize reliance on non-renewable re-
Accepted 11 July 2020
sources; for this purpose, various organic-based rejuvenators have been used in recent times. Waste
Handling Editor: Prof. Jiri Jaromir Kleme
s cooking oil (WCO), which contains light oil components analogous to those of the virgin bitumen, has
been proposed as a sustainable product for improving recycling of aged asphalt. The present review
Keywords: study collects state-of-the-art information on asphalt rejuvenation using WCO. It provides insights on
Waste cooking oil (WCO) the correlations between plant production methods and laboratory studies to manufacture high content
Reclaimed asphalt pavement (RAP) rejuvenated RAP mixes. In addition, WCO is comprehensively examined to provide more information
Rejuvenator about its chemical composition and the changes occurring in its chemical properties at various states of
Recycling degradation (i.e. virgin and used cooking oil). The effect of WCO on the mechanical, rheological, chemical
Bio-asphalt
and microscopic characteristics of the asphalt binder and asphalt pavements behaviour was assessed.
Organic based binder
This review highlights that the addition of WCO to the asphalt binder improves fatigue and thermal
cracking properties of the mix, but at the expense of rutting resistance unless further polymeric
modification is achieved. The increase in the acid value of the oil and its moisture content negatively
affect the asphalt binder properties. For the asphalt mixtures, an increment in WCO dosage generates an
increase in the thermal cracking resistance but reduces rutting, fatigue, and moisture resistance of the
pavement. Overall, this review article provides an overview of the positive and negative aspects of the
applications of WCO as an eco-friendly asphalt rejuvenator.
© 2020 Elsevier Ltd. All rights reserved.

Contents

1. Advantages and challenges behind bitumen rejuvenation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2

2. Methodology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
3. Correlations between plant production methods and laboratory studies to deliver high content rejuvenated RAP mixes . . . . . . . . . . . . . . . . . . . . . . . . . 3
4. WCO and its application as asphalt rejuvenator . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
5. Chemical composition of WCO . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
6. Effect of WCO on the physical properties of asphalt binders . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
7. Effect of WCO on rheological properties of asphalt binders . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
7.1. Effect of WCO on viscosity and workability . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
7.2. Effect of WCO on rutting resistance, fatigue and thermal cracking . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
8. Effect of WCO on chemical properties of rejuvenated asphalt binders . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
8.1. Effect of acid value and water content . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
8.2. Effect of WCO on molecular groups of asphalt binder (SARA) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
8.3. Effect of WCO on oxidation potential of asphalt binder . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13

* Corresponding author.
E-mail address: filippo.giustozzi@rmit.edu.au (F. Giustozzi).

https://doi.org/10.1016/j.jclepro.2020.123304
0959-6526/© 2020 Elsevier Ltd. All rights reserved.
2 M. Zahoor et al. / Journal of Cleaner Production 278 (2021) 123304

9. Effect of WCO on microscopic properties of asphalt binder . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13

10. Effect of WCO on asphalt mixture performance . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
10.1. Effect of WCO on the permanent deformation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
10.2. Effect of WCO on fatigue and thermal performance . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15
10.3. Effect of WCO on the moisture susceptibility . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15
10.4. Field performance evaluation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15
11. ‘Rejuvenators’ and ‘Softeners’: an ongoing discussion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15
12. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 16
CRediT authorship contribution statement . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 16
Declaration of competing interest . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 16
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 16
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 16

However, an increment in RAP dosage above 20% diminishes the

Abbreviations ability of the pavement to withstand intermediate (fatigue
cracking) and low-temperature cracking (thermal cracking), which
WCO Waste Cooking Oil is the primary hurdle in the utilization of RAP to its full potential
RAP Reclaimed Asphalt Pavement (He and Wong, 2008; Xinxin et al., 2018). One of the critical pa-
SLR Systematic Literature Review rameters that differentiate the recycled asphalt mixture from a new
HMA Hot Mix Asphalt one is the aging of the asphalt binder. With time, the asphalt
WMA Warm Mix Asphalt pavement ages due to its exposure to environment and traffic loads.
RA Reclaimed Asphalt As the asphalt ages, the binder loses its viscoelastic properties due
WEVO Waste Edible Vegetable Oil to loss and conversion of volatile components (i.e. maltenes) into
WEAO Waste Edible Animal Oil less volatile components (i.e. asphaltenes) making the pavement
WVO Waste Vegetable Oil material stiffer, brittle and more vulnerable to cracking (Rahmani
WFO Waste Frying Oil et al., 2017). The blending of hard and brittle asphalt binder ob-
WCVO Waste Cooking Vegetable Oils tained from RAP with the virgin bitumen results in a stiffer binder
SBS styrene-butadiene-styrene compared to the virgin binder, which affects workability and is
MSCR Multiple Stress Creep Recovery more susceptible to cracking (Ongel and Hugener, 2015).
DSR Dynamic Shear Rheometer Rejuvenation is the process of reviving the properties by restoring
BBR Bending Beam Rheometer the ratio of asphaltenes and maltenes in the aged binder with
SARA saturate, aromatic, resin and asphaltene addition of a rejuvenator. Rejuvenation tends to overcome the de-
AFM Atomic Force Microscope ficiencies associated with the incorporation of a high dosage of RAP
SEM Scanning Electron Microscope in the asphalt mixture (Shen et al., 2007b). Rejuvenators are nor-
mally petroleum-based, organic-based or engineered products and
can be of different natures, which is demonstrated by their polarity,
molecular structure, and function (Borghi et al., 2017; Taziani et al.,
1. Advantages and challenges behind bitumen rejuvenation
2017; Zaumanis et al., 2014c). In recent times, to counter the
petroleum-based binders due to their high cost and environmental
Every year, over 120 million tons of asphalt pavement is milled
effects, various other products such as engineered binders and
during the reconstruction, rehabilitation or resurfacing of the
organic-based binders are utilized to incorporate the aged binder in
existing roads (EAPA, 2018a). Recycling the aged asphalt pavement
the RAP with dual benefits of increased RAP quantity in the asphalt
has turned out to be a global practice in the last few decades to
pavement mix and excellent HMA performance (Mazzoni et al.,
enhance the energy, economic and environmental (3 E’s) efficacy
2018). It is observed that similar rheological and mechanical prop-
and resources allocation of the road systems (Dehghani et al., 2013).
erties equivalent to that of virgin binder can be obtained by the
The end-of-life material, known as reclaimed asphalt pavement
addition of rejuvenator and mixing it with aged RAP bitumen.
(RAP), possesses a great potential to be recycled as it is fully recy-
Nevertheless, rejuvenated binder’s chemical composition specifically
clable and holding useful asphalt binder and aggregate (Cong et al.,
ratio of asphaltenes to maltenes, is considerably deviating from the
2016; Mohammadafzali et al., 2017). Kandhal et al. (Kandhal and
virgin binder which affects the performance of RAP mix in the long
Mallick, 1997) mentioned 14e34% savings in terms of construc-
term (Asli et al., 2012; Ongel and Hugener, 2015; Pan et al., 2018;
tion costs by including 20e50% RAP in road pavement applications.
Shen et al., 2007b; Zargar et al., 2012). For proper utilization of re-
This not only provides economic benefits but also reduces the
juvenators in the road projects, preference should be given to the
misuse of non-renewable resources hence resulting in energy
equilibrium between rutting and cracking efficiency of the asphalt
savings and environmental benefits from reduced emissions caused
mixture. The rejuvenator should maintain its ability to resist rutting
by quarrying and transportation (Aurangzeb and Al-Qadi, 2014).
and reduce fatigue. In previous studies, it is noted that the high-
Life cycle costs analysis (LCCA) of RAP mixes has further strength-
temperature rutting resistance is reduced, however, fatigue
ened such claims (Qiao et al., 2019; Tabassum, 2016). The net pre-
cracking and thermal cracking has been improved by the utilization
sent value of the road pavement with 40% RAP costs 18.3% less due
of rejuvenators (Asli et al., 2012; Luo et al., 2017; Nur et al., 2017;
to material-saving in the production stage, 50% savings during the
Xinxin et al., 2018; Zargar et al., 2012). This study provides a review
maintenance phase and 40% savings as salvage value at the end of
of the utilization of waste cooking oil as a possible rejuvenator of
the service life; these figures provide an overall 15e25% net savings
asphalt pavements. Fig. 1 illustrates the structure of the review paper
when compared to hot mixed asphalt (HMA) (Qiao et al., 2019).
in the form of a flowchart.
 M. Zahoor et al. / Journal of Cleaner Production 278 (2021) 123304
Fig. 1. Structure of the review paper.
2. Methodology
Systematic literature review (SLR) technique (Behnood, 2019;
Tranfield et al., 2003) is adopted in this work to summarize the
impacts of asphalt binder rejuvenation utilizing the waste cooking
oil (WCO). SLR is an authentic methodology for the step by step
systematic collection of wide amounts of data (Behnood, 2019;
Esteves et al., 2019; Pacheco et al., 2017). The literature survey was
conducted using four databases, notably Google Scholar, Web of
Science, Scopus, and Transport Research International Documen-
tation (TRID), as the latter contains the largest online database for
the transport engineering field. For each of the search engines, the
following phrase strings and keywords were used: Waste Cooking
Oil; Used frying Oil; Waste Cooking Vegetable Oils; Waste Edible
Animal Oil; Waste Vegetable Oil; Waste Edible Vegetable Oil;
Rejuvenator; Asphalt; and Bitumen. The truncation “rejuv” was also
adopted to consider the numerous acceptations of “rejuvenator”,
“rejuvenation”, “rejuvenating”. Further adjustments were under-
taken within the literature search to cope with the fact that re-
juvenators are often referred by other names such as recycling
agents, softening additives and softening agents. Articles that
included the treatment of WCO (transesterification) before intro-
duction into asphalt are also included although studies conducted
on the separate components of treated WCO such as bio-oil/grease/
glycerin for asphalt rejuvenation are not as the present study fo-
cuses purely on WCO.
Particularly, this paper evaluates the following: (a) use of re-
juvenators in asphalt mixes with RAP compared to virgin bitumen;
(b) WCO rejuvenator and its chemical compositions; (c) changes in
the physical properties of the binder by addition of WCO; (d)
changes in the rheological properties of the binder by addition of
WCO; (e) changes in the chemical properties of the binder due to
WCO; and (f) difference between a rejuvenator and a softener, to
identify the advantages and shortcomings of the utilization of WCO.
3
3. Correlations between plant production methods and
laboratory studies to deliver high content rejuvenated RAP
mixes
As of today, the studies conducted at the laboratory scale have
demonstrated that using rejuvenators can significantly enhance the
aged binder’s properties and promote incorporating high RAP
content (Cooper et al., 2015; Mazzoni et al., 2018; Moghaddam and
Baaj, 2016; Tran et al., 2017b, 2017a; Xie et al., 2017; Zaumanis et al.,
2014c). Excellent field results through the management of RAP at
full-scale, production and mix-design methodologies have also
been validated (Willis and Marasteanu, 2013; Zaumanis et al.,
2014a). However, there are several drawbacks that restrict the
full-scale utilization of RAP; (i) currently available standards, (ii) the
majority of the studies being only conducted at laboratory scale,
(iii) research on production technologies at the plant level and
long-term monitoring of full-scale applications are very rare.
Similarly, the skepticism around high-content RAP mixes has
grown up due to premature failures of RAP mixtures caused by the
utilization of untreated RAP and use of HMA plants not designated
for high-content RAP mixes (Bonaquist, 2007).
The degree of blending (DOB) between the virgin binder, reju-
venator and RAP are divided into complete blending, partial
blending and no blending (black rock). Most design approaches
assume 100% degree of blending between RAP binder and re-
juvenators, although this is debatable in a plant situation where
this inaccurate assumption could cause problems in the resulting
mix design and pavement durability (Al-Qadi et al., 2007a,b;
Gottumukkala et al., 2018; Shirodkar et al., 2013; Tran et al., 2012;
Zaumanis and Mallick, 2015). Studies have revealed that there is in
fact a partial blending between RAP, rejuvenating agents and virgin
binder and this cannot be neglected (Al-Qadi et al., 2007b).
Several laboratory studies have indicated the importance of the
rejuvenator dosage as it affects the binder and mixture properties;
4 M. Zahoor et al. / Journal of Cleaner Production 278 (2021) 123304
the assumption of complete blending may lead to premature
cracking and moisture damage, or plastic deformation of the
pavement. (Shen et al., 2007a; Shen and Ohne, 2002; Silva et al.,
2012). On this note, Zaumanis et al. (2014b) developed a proced-
ure based on a laboratory study to select the optimum amount of
rejuvenator for modification of reclaimed asphalt binder as per
Superpave asphalt binder specifications. Zaumanis et al. (Zaumanis
and Mallick, 2013) correlated the laboratory studies with the plant
operation and highlighted the importance of some interaction pa-
rameters (i.e. dispersion, diffusion, and mechanical mixing) that
differentiate the high content RAP processing with rejuvenator
from conventional asphalt; furthermore, the diffusion of the reju-
venator into the aged RAP binder was simulated in a plant to
determine its softening efficiency. Based on laboratory and plant
studies, it is suggested that the diffusion rate can be enhanced
through the raise in temperature and increasing of the mixing time
(Cong et al., 2016; Zaumanis and Mallick, 2013).
Recently, to correlate the laboratory studies with plant pro-
duction methods, studies have carried out full-scale tests to eval-
uate how the pavement performance is also affected by specific
production processes (Bennert et al., 2015; Mohammad et al., 2004;
Tran et al., 2017b, 2012; Xie et al., 2017). In a detailed review
(Zaumanis et al., 2014a), insights were provided on the technolo-
gies available to produce 100% recycled hot mix asphalt, and its
performance at the laboratory and field scale. Xie et al. (2017)
studied the correlation of temperature by inspecting the labora-
tory and field performance of two different rejuvenators. They
produced the control HMA mixture as a reference and the experi-
mental warm mix asphalt (WMA) mixture at Astec Double-Barrel
Green drum plant located in Montgomery, Alabama (USA). The
results of the control HMA mixture showed better resistance to
moisture and cracking, WMA showed poor resistance to moisture
and cracking due to low WMA production temperature, low reju-
venator dosage and partial diffusion but showed high rutting
resistance. Sivilevi

cius et al. (2017) devised the principles of hot
recycling of asphalt pavement in reference to the available theo-
retical knowledge and practical experience that can act as a
guideline for developing asphalt pavement recycling methods and
technologies. Authors also specified that the asphalt plants con-
structed for RAP recycling requires special retrofitting to feed, store,
transport, drying, heating up and mixing of RAP with virgin asphalt.
However, the location for the introduction of rejuvenator in asphalt
mixing plant is not specified in the above study.
In 2018, the European Asphalt Pavement Association (EAPA)
gave its recommendations for using rejuvenators in the production
of HMA and WMA (EAPA, 2018b). In this report, the authors iden-
tified the potential dosing points for the rejuvenator depending on
the asphalt plant configuration for uniform dispersion of the reju-
venator, as each asphalt mix plant is slightly different. As per the
information contained in this report, it is suggested that the reju-
venator is to be added at the following points in the mix plant;
reclaimed asphalt (RA) crusher, RA storage, RA conveyor belt, RA
drum inlet, RA dryer and mixing unit (EAPA, 2018b). Homogeneous
distribution is needed for equal delivery of rejuvenator to RAP and
should be given enough time for the rejuvenation of the aged
binder. The report advised that to maximize the diffusion of reju-
venator into reclaimed asphalt, it would be better adding the
rejuvenator at the material discharging chute of the parallel drum;
this is expected to maximize the rejuvenator’s diffusion into the
aged binder as the material is pre-heated and about to be stored in
the silos for some time prior to mixing. This recommendation is in
agreement with results reported by Zhang et al. (Zhang and
Muhunthan, 2017) as the diffusion stage highly influences the
rheological properties. Thus, pre-heated materials needed to be
stored in the storage silos for an adequate time to enhance the
blending of RAP, rejuvenator and the virgin binder in the RAP
mixture (Zhang and Muhunthan, 2017). Adding the rejuvenating
agent during the mixing processes is also a viable option, but stage
and timing of the process needs to be considered for achieving good
results (EAPA, 2018b; Lee et al., 1983). A more practical approach
has been adopted by (Zaumanis et al., 2019); the authors discussed
five key parameters to be controlled for the use of rejuvenators and
indicated the ten potential locations (Zaumanis et al., 2019) for
rejuvenator addition into a batch asphalt plant and compared pros
and cons on the basis of environmental concerns, operability and
quality. The study narrowed down two promising locations:
namely, the RA conveyor belt and RA drier drum mixer. Similarly, in
another study they evaluated the rejuvenator addition effect on the
mechanical and chemical properties of RAP binder in the batch
plant (Zaumanis et al., 2018).
This section shows an increasing interest towards the utilization
of rejuvenators with RAP in asphalt plants, with new plant models
being developed to accommodate more RAP and existing plants
being retrofitted for the same purpose. However, further research is
needed to find robust correlations between rejuvenated asphalt
mixes produced at the plant and rejuvenated mixes produced in the
laboratory environment. At this stage plant-based research is still
considered too expensive and delayed by industrial secrets and
data sharing issues.
4. WCO and its application as asphalt rejuvenator
Rising population has increased the demand of food items that
leads to the generation of a large amount of kitchen waste, one of
the most widely used kitchen commodity is the edible cooking oil
which can be obtained from various feed sources; e.g., plant/
vegetable oils and animal fats. Both sources have two major utili-
zations: (i) food industry and (ii) industrial use. The utilization of
different resources of edible vegetable oils and animal oils gener-
ates WCO after frying and cooking (Azahar et al., 2017). As illus-
trated in Fig. 2 and Fig. 3 the global vegetable oil consumption in
2019 has reached 204.88 million metric tons, and this figure is
increasing at a pace of 2% each year (USDA-FAS, 2019).
It is evident from the above figures that there is a significant and
increasing quantity of WCO, and its end-of-life management is a
growing problem all over the world. Out of the total consumption,
only 20e30% of WCO is recycled or reused (Chen et al., 2014b). It is
suggested that WCO should be treated and managed properly as it
is considered harmful to human health and the environment when
discarded by the users into kitchen sinks, waste bins, sewerage
systems, or directly to land and water bodies (Kabir et al., 2014;
Sanli et al., 2011). Such acts chronically affect the land and water in
the form of contamination, inducing a disturbance in aquatic life by
disrupting the oxygen supply, blockage and overflow of the
sewerage system, increasing the wastewater treatment operation
and maintenance cost, hence adversely affecting the entire eco-
system. Based on a previous study in the USA (Howell et al.,
2010), approximately 40% of blockages in the sewerage system
results by pouring WCO in the kitchen sink; this increases the water
treatment cost up to 25% (Tsoutsos et al., 2019). Due to the chemical
composition of WCO, recycling will not only provide a renewable
feedstock for biofuels (i.e. biodiesel), and other bio-based products
(e.g., soap and animal feed) but also reduces environmental
pollution by mitigating the greenhouse gases (GHG) resulting from
improper handling (i.e. disposing into water and land bodies) (Tsai,
2019). Recently, Bailey et al. (Bailey and Philips, 2010) patented the
use of WCO as an asphalt rejuvenator, which powered the theory of
utilizing the WCO to rejuvenate the aged binders along with the
asphalt mixture. After this attempt, various researchers (Asli et al.,
2012; ASLI and KARIM, 2011; Wen et al., 2013; Zargar et al., 2012)
 M. Zahoor et al. / Journal of Cleaner Production 278 (2021) 123304 5

Fig. 2. Global vegetable oil consumption Worldwide by Oil Type (USDA-FAS, 2019).

Fig. 3. Global Vegetable Oil consumption Worldwide by Country (USDA-FAS, 2019).

explored the opportunity of utilizing the WCO to rejuvenate the
aged asphalt binder and improve its characteristics up to the scale
of the virgin binder. The WCO can be used directly in the asphalt
binder (virgin or aged) or after filtration of suspended impurities;
some other times, it is used after chemical treatment, which
showed enhanced results (Azahar et al., 2017). WCO is rich in un-
saturated fatty acids, which are analogous to the lower molecular
weight components (maltenes) in the asphalt binder. Throughout
the service life, the asphalt binder loses the light oil components
(maltenes) and faces the increased composition of heavy oil com-
ponents (asphaltenes); the WCO balances the lost maltenes in the
aged binder (Azahar et al., 2016a). Its abundant availability - only in
2019, 204.88 million metric tons consumption in various forms -
and possible partial similarity with bitumen components makes it a
suitable candidate for asphalt rejuvenation (USDA-FAS, 2019).
5. Chemical composition of WCO
While cooking or frying, the cooking oil is heated at 160e200
C
repeatedly and in the presence of moisture and air (Kulkarni and
Dalai, 2006). When continuously heated, the oil undergoes phys-
ical and chemical changes as - at these conditions - it suffers from
degradation reactions (i.e. oxidation, hydrolysis, and polymeriza-
tion) which leads to the increment of density, viscosity, specific
heat, total polar material (TPM), and saturated fatty acid compo-
nents (Sanli et al., 2011). These degradation reactions cause a
reduction in the number of double bonds or percentage of mono-
unsaturated and polyunsaturated components, iodine value,
peroxide value, saponification value, antioxidants (Vitamin E),
volatile components and smoke point. If this process is continued,
the oil undergoes additional degradation and becomes unfit for
cooking or frying and needs to be discarded (Choe and Min, 2007;
Das et al., 2013; Jaarin and Kamisah, 2012; Kulkarni and Dalai,
2006; Sanli et al., 2011). Researchers have utilized gas
chromatography-mass spectrometry (GC-MS) for the detection of
the chemical composition of the unknown WCO. The acidic com-
pounds of WCO are further classified into saturated, mono-
unsaturated, and polyunsaturated compounds (Azahar et al., 2017).
Saturated fatty acids include palmitic acid, stearic acid, and myristic
acid. Monounsaturated fatty acids contain oleic acid, cis-11-
6 M. Zahoor et al. / Journal of Cleaner Production 278 (2021) 123304

Table 1
Possible chemical composition of WCO (Asli et al., 2012; Azahar et al., 2017; Khalissani, 2008).

Formulation of Fatty Acids Type of Free Fatty Acid Possible % in Waste Cooking Oil (WCO) Type of Saturation

C18:1 (Cis 9) Oleic Acid 43.67 Unsaturated

C16:0 Palmitic acid 38.35 Saturated
C18:2 (Cis) Linoleic acid 11.39 Unsaturated
C18:0 Stearic acid 4.33 Saturated
C14:0 Myristic acid 1.03 Saturated
C18:3 alpha ɣ- Linolenic acid 0.37 Unsaturated
C12:0 Lauric acid 0.34 Saturated
C18:2 t Linolenic acid 0.29 Unsaturated
C20:1 Cis-11-Eicosenoic acid 0.16 Unsaturated
C21:0 Heneicosanoic acid 0.08 Saturated
TOTAL 100

Table 2
Physio-chemical properties of virgin cooking oil and WCO (Ullah et al., 2014).

Properties Values of Virgin Cooking Oil (Palm cooking oil) Values of Waste Cooking Oil (WCO)

Acid value (mg KOH/gm) 0.3 4.03

Calorific value (J/gm) ———— 39658
Saponification value (mg.KOH/gm) 194 177.97
Peroxide value (meq/kg) <10 10
Density (gm/cm3) 0.898 0.9013
Kinematic Viscosity (mm2/s) 39.994 44.956
Dynamic Viscosity (MPa.s) 35.920 40.519
Flash point (
C) 161e164 222e224
Moisture content (wt. %) 0.101 0.140

eicosenoic. Polyunsaturated fatty acids include linoleic acid, lino-
lenic acid, and ɣ- Linolenic acid (Azahar et al., 2017; Udomsap et al.,
2009). Table 1 shows the possible composition of WCO; the major
constituents are oleic acid, palmitic acid, and linoleic acid
comprising 43.67%, 38.35% and 11.39%, respectively (Asli et al.,
2012; Azahar et al., 2017; Khalissani, 2008). However, since the
fatty acid composition of various fresh and commercial oils are
different from each other (Takeoka et al., 1997), the composition of
fatty acids in WCO could not be consistent due to chemical changes
occurred during cooking and frying (Majidifard et al., 2019). As per
Ullah et al. (2014), the physio-chemical properties of WCO vary
from all types of virgin cooking oils, as shown in Table 2. The
presence of long-chain acids (e.g., saturated acid such as palmitic
acid and monounsaturated acid, such as oleic acid) increases the
probability of cracking by thermal or catalytic cracking and forming
hydrocarbon chains (Khalissani, 2008). Thus, it is concluded that
the physical and chemical composition cannot be consistent as it
depends upon the quality of cooking oil, type of cooking oil, type of
food cooked, the food composition, cooking temperature, number
of times the oil is used and duration of cooking.
The chemical properties of the cooking oil play a vital role when
it comes to blending the oil into aged asphalt. The fresh cooking oil
contains a higher amount of unsaturated compounds that, when
subjected to heating degrades and result in a high amount of
saturated compounds, increasing the acid value of the oil (Azahar
et al., 2017). The effect of acid value and water content of cooking
oil on asphalt binder rejuvenation is discussed in detail in section
8.1. When it comes to saturates, aromatics, resins, and asphaltenes
(SARA fractions), fresh cooking oil contains high saturates and ar-
omatics content but these components reduce by the degradation
of oil (Bailey and Zoorob, 2012), the effect of SARA by the addition of
cooking oil in the aged binder is provided in section 8.2. Finally,
very few studies are available on the correlation between the
chemical composition of WCO and its effectiveness as asphalt
rejuvenator. Until now, only the impact of acid value and moisture
content of the WCO on the asphalt binder performance have been
studied and more research is needed on how the usage rate,
variability and cooking-related parameters affect WCO efficacy for
rejuvenating asphalt.
6. Effect of WCO on the physical properties of asphalt binders
The physical characteristics of the binder are first evaluated by
conventional physical properties tests, including penetration test
(ASTM D5), softening point test (ASTM D36), ductility test (ASTM
D113), specific gravity test (ASTM D70), and flash & fire point test
(ASTM D92) as shown in Table 3. Penetration test identifies the
consistency and deformation resistance of the bitumen at 25
C
while softening point determines the thermal susceptibility at a
higher temperature (i.e., commonly 45e85
C). Ductility measures
the adhesion property of the asphalt binder, whereas specific
gravity helps in volume correction that fluctuates due to the change
in temperature and flash & fire point is determined for the safe
operation at the asphalt plant. As the asphalt pavement ages, it
becomes hard, brittle, and more prone to cracking, the rejuvenator
reduces the brittleness of aged asphalt at various concentrations.
Table 3 provides a summary of previous works that have analyzed
the effect of the addition of WCO on the physical properties. From
Table 3, it can be concluded that by dosing WCO, the penetration
and ductility rise though the softening point declines. The addition
of WCO also guarantees that the penetration value, ductility, and
softening point of the targeted bitumen grade are achieved. Most of
the studies experimented with the use of WCO, ranging from 1% to
20% by weight of bitumen. However, they identified to restore the
penetration value of aged bitumen groups (60/70, 50/60, 40/50, 30/
40) similar to virgin binder (80/100 penetration grade) required 1, 1,
3, 4 wt% of WCO, and to recover the softening point 4, 4, 2, 1 wt% of
WCO was required (Asli et al., 2012; ASLI and KARIM, 2011; Rasman
et al., 2018a; Zargar et al., 2012). Similarly, to improve the proper-
ties of 60/70 penetration grade and recover the properties of an
extracted RAP binder to a similar penetration grade, 1e2% WCO
dosage is suggested for recovery of penetration value and 3.5% WCO
dosage is suggested for the recovery of softening point in the
literature (Al-omari et al., 2018; Azahar et al., 2017, 2016e; 2016b;
 M. Zahoor et al. / Journal of Cleaner Production 278 (2021) 123304 7

Table 3
Summary of literature on the effect of WCO on the physical properties.

Sr Control Binder Used/Tested Rejuvenator Rej. Effect of WCO Findings Reference

No Binder Type Percentage
Penetration Softening Ductility Specific Flash
% (by mass
test Point Gravity &Fire
WCO)
Point

1 Original Virgin binder WCO 2, 3, 4, 6 e e e The study shows the effect of WCO Mahrez et al.
Bitumen artificially aged addition in the aged binders. By (2009)
with RTFO aging increasing the dosage percentage of
mode and propeller WCO, the penetration value rises,
mixer aging mode and the softening point reduces.
2 80/100 Aged 60/70, 50/60, WCO 1e5 e e e The aged bitumen groups (60/70, (Asli et al., 2012;
Penetration 40/50, 30/40 50/60, 40/50, 30/40) required 1, 1, ASLI and KARIM,
grade Penetration grade 3, 4% of WCO, respectively, to obtain 2011; Rasman
the penetration value of the target et al., 2018b;
binder (80/100 penetration grade), Zargar et al.,
while, to achieve the target binder 2012)
softening point 4, 4, 2, 1% of WCO
was required, respectively.
3 60/70 Virgin binder 60/ WCO 3, 4, 5 e e e The quality of WCO was studied by Azahar et al.
Penetration 70 PG comparing various samples of WCO (2016b)
grade sourced at three different times of
the year to prove consistency.
4 60/70 Virgin binder 60/ WCO 3, 4, 5 e e e The study showed the effect on (Azahar et al.,
Penetration 70 PG penetration and softening point of 2017, 2016e)
grade chemical treatment
(transesterification reaction via
alkali catalyst) of WCO. The treated
WCO showed better mechanical
results of its untreated version.
5 60/70 Virgin binder WVO 1, 2, 4, 6, 8 The authors studied the effect of Al-omari et al.
Penetration 60/70 PG WVO addition in virgin pen 60/70 (2018)
grade binder.
6 60/70 Extracted RAP WCO 2, 3, 3.5, 4 e e e The effect of WCO on RAP was El-Shorbagy
Penetration binder analyzed. The extracted RAP binder et al. (2019)
grade required 2% of WCO to achieve the
penetration value of target binder
grade, while, 3.5% of WCO was
required to achieve softening point.
7 PEN 70 Virgin binder WVO 5, 10, 15, 20 e The study identified 13.4% WVO as Xinxin et al.
artificially aged in the optimal amount to reinstate the (2018)
RTFO and PAV physical properties of aged asphalt
and make it equivalent to the virgin
asphalt.
8 PEN 70 Virgin binder WCO 1e5 e e The study showed that a higher Li et al. (2019a)
artificially aged in dose of WCO is required to achieve
RTFO at different the penetration value and ductility
aging times (5 h, of virgin binder as the aging time
7 h, 9, 11 h, 13 h increases. The softening point
and 15 h) requirements could be satisfied
with smaller dosages at more than
10 h aging.
9 70# asphalt Virgin binder WEAO 3-7 by e e It was observed that 6% WEAO Sang et al.
SBS artificially aged in mass content makes the PAV aged binder (2014b)
modified RTFO and PAV 70# asphalt to resemble the
asphalt physical properties of virgin one.
However, for SBS-modified asphalt
the optimal dosage was 4%.
10 60-80 Virgin binder WEVO 3-7 by e e e Results showed that WEVO can Chen et al.
Penetration artificially aged in mass effectively rejuvenate the aged (2014a)
Grade RTFO and PAV binders and the optimum dosage to
40-60 resemble basic properties of virgin
Penetration binders found to be 6.6, 5.2, 4.8% of
Grade WEVO, respectively.
40-60
Penetration
Grade þ SBS
11 70/100 Virgin binder WVCO 2, 4, 6, 8, 10 e e e The study analyzed the potential of Go€kalp and Uz
Penetration artificially aged by WVCO as an anti-aging agent in (2019)
grade RTFO, PAV and oxi- both short and long-term aging. The
aging method (SHT high dose was required for long
& LHT) term aged binder, but a small dose
was required for short term aged
binder.
12 PG 64-22 Binder recovered WCVO 2, 4, 6, 8, 10 e e The physical properties showed Ji et al. (2017)
from RAP that the WCVO can successfully
(continued on next page)
8 M. Zahoor et al. / Journal of Cleaner Production 278 (2021) 123304

Table 3 (continued )

Sr Control Binder Used/Tested Rejuvenator Rej. Effect of WCO Findings Reference

No Binder Type Percentage
Penetration Softening Ductility Specific Flash
% (by mass
test Point Gravity &Fire
WCO)
Point

recover the aged asphalt binder

with a 6e8% dose.
13 50/70 Binder was WVO 2, 3, 4, 5, 6 e e e The results confirmed that a 5.1% Aghazadeh
Penetration extracted from 12 dosage of WVO can revive physical Dokandari et al.
grade years old RAP. properties in aged RAP binder like (2017)
Virgin 50/70 pen grade.
14 50/70 Virgin binder was WFO 1, 3, 5 e e e WFO utilization in HMA was Eriskin et al.
Penetration used studied as a binder modifier to (2017)
grade reduce the amount of bitumen.
15 AH-90 Virgin binder WCO 6 e e In this work, higher quality (D. Zhang et al.,
Asphalt artificially aged in (reduced number of heating cycles) 2017b)
Binder RTFO and PAV WCO proved superior results in
terms of physical properties, while
continuously used or repeatedly
heated WCO showed poor results
for the rejuvenation of aged asphalt
binder.
16 40/50 Binder (20/30) WVO 1e3 The optimum percentage of WVO Joni et al. (2019)
Penetration penetration grade) was 1% that returned aged asphalt
grade was extracted from binder to its virgin properties.
6 years old RAP.
17 Natural Natural asphalt is WVO 17.90 e e e The produced new binder Some et al.
Bitumen used with hard resembled Pen 35/50. (2016)
bitumen Pen 15/25

El-Shorbagy et al., 2019). 5.1 wt% dosage is suggested to revive the
basic properties in aged RAP binder similar to 50/70 and 40/60
penetration grade and the utilization of RAP binder is definitely
beneficial due to the reduction of the amount of fresh bitumen
required (Aghazadeh Dokandari et al., 2017; Chen et al., 2014a;
Eriskin et al., 2017). In other studies, 13.4 wt% dosage has been
identified to rejuvenate the physical properties of aged asphalt (up
to 15 h. RTFO aged) and make it equivalent to the virgin asphalt
(Pen 70) (Li et al., 2019a; Xinxin et al., 2018). For the modified
asphalt with styrene-butadiene-styrene (SBS), approximately 4.8%
dosage of WEVO or WEAO has been suggested to reinstate the basic
properties of an aged binder (Chen et al., 2014a; Sang et al., 2014a).
Dong et al. (Dong Zhang et al., 2017a) found that increasing the
number of times cooking oil is used (heated), actually drops its
quality due to deterioration reactions which decrease its ability to
rejuvenate the aged asphalt binder. The fresh cooking oil showed
better results for asphalt binder rejuvenation than the one which
was heated for 16 h. From the above studies, it can be concluded
that the more aged is the bituminous binder, the higher dosage of
rejuvenator is required to recover the penetration value and soft-
ening point. The ductility has been determined in a few studies (Al-
omari et al., 2018; Ji et al., 2017; Joni et al., 2019; Li et al., 2019a;
Sang et al., 2014a; Xinxin et al., 2018) which showed how as the
WCO dosage increases in the aged binder, so does the ductility. The
effect of WCO dosage on the specific gravity was found in two
studies (Al-omari et al., 2018; Joni et al., 2019); both studies
revealed that the dosing of WCO in the binder results in the
reduction of the overall specific gravity. Dosage of WCO can vary
the flashpoint of the asphalt binder; this information is significant
for the plant during production. Although only three studies
considered the flash and fire point variation, results were con-
trasting in saying the effective change in flashpoint by using WCO
as two of them highlighted an increase of flash point temperature
of rejuvenated binder (Al-omari et al., 2018; Joni et al., 2019) while
the other one claimed a possible reduction in the flash and fire
point of the rejuvenated binder (Xinxin et al., 2018).
7. Effect of WCO on rheological properties of asphalt binders
7.1. Effect of WCO on viscosity and workability
If the binder is too viscous it is more prone to thermal cracking
while a too low viscosity will make it more vulnerable to rutting
and fatigue (Zaumanis et al., 2014a). Normally, Brookfield rotational
viscometer (ASTM D4402) is utilized to quantify the asphalt
binder’s viscosity. Mahrez et al. (2009) demonstrated the effect of
WCO addition on the viscosity at various temperatures for the first
time. The results confirmed that with the surge in temperature and
concentration of WCO the rotational viscosity of the binder reduces
gradually. At 6% WCO the viscosity of RTFO aged binder has reduced
by half. In previous studies (Asli et al., 2012; ASLI and KARIM, 2011;
Rasman et al., 2018b; Zargar et al., 2012), used WCO (1e5%) in the
aged bitumen (penetration grade 50/60, 40/50, 30/40) and
compared its viscosity at different temperatures (from 90
C to
180
C) to the viscosity of the control binder (penetration grade 80/
100). It was observed that at 110
C, 2, 4, and 5% WCO is needed in
aged bitumen groups to resemble the viscosity of the control
binder. However, rise in the temperature (e.g. 135
C and 150
C)
makes the WCO dosage requirement to increases as to reach the
viscosity of the control binder. Similarly, in studies by (Al-omari
et al. (2018); Azahar et al., 2017, 2016e, 2016b; El-Shorbagy et al.,
2019) the control binder (penetration grade 60/70) was artificially
aged and RAP binder was used and rejuvenated using WCO at
1e8 wt%, the viscosity of the rejuvenated binder was determined at
various temperatures (135e165
C) to compare with the control
binder. At 165
C, the WCO concentration between 1 and 4%
showed equivalent to control binder. The treated WCO (pre-treated
with transesterification reaction via alkali catalyst) (Azahar et al.,
2016e) showed better internal resistance as well as higher viscos-
ity than the untreated one due to its high adhesion properties after
chemical treatment.
Several other studies (Aghazadeh Dokandari et al., 2017; Chen
et al., 2014a, 2014b; Eriskin et al., 2017; Go € kalp and Uz, 2019; Ji
et al., 2017; Joni et al., 2019; Li et al., 2019a; Sang et al., 2014b;
Some  et al., 2016; Xinxin et al., 2018; Dong Zhang et al., 2017a), used
 M. Zahoor et al. / Journal of Cleaner Production 278 (2021) 123304
multiple control binders and found that at different temperatures
and WCO concentrations, the addition of WCO decreases the vis-
cosity. Although this was widely expected, the numerous studies
confirmed that WCO, variable in nature, can provide consistent
outcomes in terms of viscosity reduction. Looking at the energy,
environmental and economic approach, low viscosity binder is
beneficial as it eases the workability (mixing and compaction
temperatures), requires less energy, consumes less fuel favoring the
environment and increasing savings.
7.2. Effect of WCO on rutting resistance, fatigue and thermal
cracking
Rutting, fatigue and thermal cracking resistance can also be
ascertained by looking at the rheological properties of a binder.
Rutting and fatigue characteristics of unaged, RTFO and PAV-aged
asphalt binders at different temperatures, frequencies and loads
are commonly determined by dynamic shear rheometer (DSR)
(ASTM D7175) to confirm the performance of the binder or changes
in the shear resistance by the addition of WCO (Hidayah et al.,
2013). The behavior of the binders in the high and medium tem-
perature range is partially elastic and partially viscous; rutting
behavior is studied at elevated temperature, while fatigue is stud-
ied at intermediate temperature. The DSR test measures funda-
mental rheological characteristics such as the complex shear
modulus (G*) and phase angle (d). The complex shear modulus (G*)
is the total resistance of the binder to deformation resulting from
shear loading, and the phase angle (d) is the delay in time between
shear strain and shear stress (Azahar et al., 2016b). Commonly, G*/
sind is used to show rutting resistance at high temperature, while
G*sind evaluates fatigue resistance at an intermediate temperature
according to the Superpave program (Speight, 2016). Table 4 shows
the list of references in which WCO is utilized as rejuvenator and its
effect on G*, d, G*/sind and G*sind are studied at varying WCO
dosages, temperature-dependency (isochronal) and frequency-
dependency (isothermal) in different control, aged and extracted
binders. It can be noted that WCO dosage 1%, 1%, 3% and 3% is
required to revive the G* of the aged binders (pen 60/70, 50/60, 40/
50 and 30/40) while for the d, WCO dosage requirement is 1%, 3%,
4% and 5% to resemble the phase angle of virgin binder (penetration
grade 80/100) (ASLI and KARIM, 2011; El-Shorbagy et al., 2019;
Nordiana et al., 2019; Rasman et al., 2018a; Zargar et al., 2012). Chen
et al. (Chen et al., 2014b, 2014a) in their studies, mentioned 5% WCO
is needed to restore the rutting resistance of artificially aged and
RAP-extracted binder similar to the pen grade 40e60 and PG 64-22
binders. Similar results have been found by Ji et al. (2017) for aged
RAP binder by addition of 6% WCO; it was demonstrated that
rutting and fatigue properties were similar to the virgin PG 64-22
bitumen. Azahar et al. (2016b) showed that WCO with higher acid
value and water content reduces G* and increases d, thus reducing
the overall resistance to rutting while increasing fatigue resistance
of WCO-rejuvenated binder. Zhang et al. (Dong Zhang et al., 2017a)
studied the effect of acid value on the rheology of the rejuvenated
binder, it is reported that the value of G*/sind is influenced by the
quality of WCO (acid value). The acid value changes by heating the
oil for a known amount of time. The rejuvenated binder blended
with a low acid value WCO brings the rutting factor of the aged
binder to the level of a virgin binder. The recommended range of
acid value to restore the value of G*/sind is between the range of
0.4e3.2 mg KOH/gm. Azahar et al. (2017) studied the addition of
unmodified and chemically-modified WCO in aged asphalt binder;
the findings demonstrated that the chemically treated WCO-
rejuvenated binder has better rutting and fatigue resistance when
compared with the untreated WCO-rejuvenated binder (Azahar
et al., 2017, 2016e). Thus, from the above studies, it is found that
9
increasing the WCO concentration in the aged asphalt binder re-
duces the resistance to deformation and recovery efficiency of the
control and aged binders due to decreased complex shear modulus
and increased phase angle. As a result, the value of G*/sind is
reduced, which leads to a reduction of the rutting failure temper-
ature while G*sind value reduces, hence increasing the overall fa-
tigue resistance of the binder (ASLI and KARIM, 2011; Azahar et al.,
2016e; Chen et al., 2014b; Go €kalp and Uz, 2019; Leng et al., 2014;
Maharaj et al., 2015; Mahrez et al., 2009; Singh-ackbarali et al.,
2017; Zargar et al., 2012; Zaumanis et al., 2014d).
However, newer tests such a Multiple Stress Creep Recovery
(MSCR) and Linear Amplitude Sweep (LAS) are now being utilized
to test rutting potential and fatigue behavior of the binder (Cao
et al., 2018; Wen et al., 2013; Xinxin et al., 2018; Zaumanis et al.,
2015). MSCR test is used to determine the permanent deforma-
tion potential of the binder at elevated temperature. MSCR offers
the response of modified asphalt binder under stress by providing
two important parameters: the non-recoverable creep compliance
(Jnr) and percentage recovery (%). The non-recoverable creep
compliance (Jnr) has been shown to provide good correlation with
rutting resistance; an increased value of Jnr means reduced rutting
resistance and increased thermal resistance of the binder (Cao et al.,
2018). The increment of WCO dosage into the binder commonly
results in raising the Jnr value thus showing a reduction in rutting
resistance and improved thermal resistance (Wen et al., 2013). The
cumulative strain curve of time-strain responses at different
stresses (0.1 kPa and 3.2 kPa) during the MSCR test showed that the
virgin binder has greater cumulative deformation than the aged
binder but the addition of WCO increases the cumulative defor-
mation of the aged asphalt binder. The higher the dosage of WCO,
the greater will be the cumulative deformation (Xinxin et al., 2018).
Similarly, Wang et al. (2018) reported the Jnr value of the binders
under two creep stress levels, these results show that addition of
5 wt% WCO increases the Jnr value by two-folds. Also, time-strain
curves show the adverse effects of bio-oil addition on the perma-
nent deformation resistance (Wang et al., 2018).
In summary, WCO addition to the binder increases the softness
of the binder and leads to increment in the non-recoverable creep
compliance and reduction in the permanent deformation resis-
tance. Therefore, rutting resistance should be taken into account
before adding WCO into the binder with cautions depending on the
climatic conditions of the site.
The linear amplitude sweep (LAS) test is conducted at inter-
mediate temperature to assess the binder resistance to the damage
occurring due to the cyclic load with a linear amplification of strain
at a constant frequency (AASTHO TP 101-14, 2014). The test is
divided into two stages, namely; (1) frequency sweep test to
measure the alpha “a” parameter for damage analysis and (2)
amplitude sweep test to determine the damage accumulation in
the samples against the loading cycles. Limited studies are available
for what concerns LAS tests on the binder containing WCO. For
instance, Zaumanis et al. (2015) demonstrated the results of fatigue
life prediction as logarithmic LAS cycles to failure vs. strain (%).
According to the results, at 2.5% strain, the virgin binder performs
poorly and has low fatigue life but shows better performance at 10%
strain and has greater fatigue life than RAP and rejuvenated
binders. While RAP binder has high fatigue life at very low strain %,
fatigue life reduces to a minimum for 10% strain level. The waste
vegetable oil-rejuvenated binder, on the other hand, has a great
fatigue life both at lower and at high strain %, and performs almost
similarly to the virgin binder. Wang et al. (2018) have also pre-
sented the effect of WCO addition on the fatigue life and reported
that the WCO dosage to the binder improves its resistance to fa-
tigue against the loading cycles.
Therefore, it can be concluded that the WCO addition to the
10 M. Zahoor et al. / Journal of Cleaner Production 278 (2021) 123304

Table 4
Literature study of complex shear modulus, phase angle, rutting and fatigue resistance.

Sr No Control Binder Binder Tested Rej. Type Rej. Effect of increase Isochronal behavior Isothermal Mainfindings/ Reference
content in WCO % (constant frequency) behavior Optimumdosage to
(%) (constant resemble control
temperature) binder

G* d G*/sin d G*sin d G* d G*/sin d G*sin d G* d

1. Original Virgin binder WCO 2, 3, 4, 6 ✓ ✓ To restore G* Mahrez et al.
Bitumen artificially aged in After RTFO: 4.6% (2009)
RTFO aging mode After Mixer: 6%
and Mixer aging To restore d
mode After RTFO: 6%
After Mixer: >6%
2. 80/100 Aged 60/70, 50/60, WCO 1e5 ✓ ✓ To restore G* ASLI and
penetration 40/50, 30/40 60/70: 1% KARIM (2011)
grade Penetration grade 50/60: 1%
40/50: 3%
30/40: 3%
To restore d
60/70: 1%
50/60: 3%
40/50: 4%
30/40: 5%
3. 70/100 40/60 Penetration UVO 4e8 ✓ ✓ Not Given Bailey and
penetration grade þ 6% oil Zoorob (2012)
grade (Vegetex 50)
4. 80/100 Aged binder 40/50 WCO 1e4 ✓ ✓ 3% to restore G* Zargar et al.
penetration penetration grade 4% to restore d (2012)
grade
5. 60-80 Virgin binder WEVO 3e7 ✓ ✓ ✓ Pen 60e80: Chen et al.
Penetration artificially aged in 6% (2014a)
Grade RTFO and PAV Pen 40e60:
40-60 5%
Penetration Pen 40e60 þ 4%
Grade SBS
40-60
Penetration
grade þ SBS
6. PG 64-22 Binder extracted WCO 0, 5, 10 ✓ ✓ ✓ 5% Chen et al.
from RAP (2014b)
Mass ratio
recovered aged
binder: Virgin 1:3
7. PG 58-28 Virgin binder WVO 12 ✓ ✓ WVO reduced G* Yu et al. (2014)
PG 58-10 artificially aged in below virgin level,
RTFO and PAV while, increased
the d above virgin
level
8. PG 64-22 Extracted RAP WVO 12 ✓ WVO reduced the Zaumanis et al.
binder (PG 94e12) G*sind below the (2014d)
limit of virgin
binder <2000 kPa
9. TLA Virgin binder WCO 2e10 ✓ ✓ ✓ ✓ ✓ ✓ ✓ ✓ ✓ ✓ TPB has minimum Maharaj et al.
TPB G*sind value (2015)
50: 50 TLA: TPB meaning highest
fatigue resistance
TLA has the highest
G*/sind showing
the highest rutting
resistance.
10. 60/70 Virgin binder WCO 3e5 ✓ ✓ Binder with high (Azahar et al.,
Penetration 60/70 PG quality (low acid 2016b, 2016c)
grade value) showed
rutting resistance.
However, non-
reached equivalent
to original bitumen.
11. 60/70 Virgin binder WCO 3e5 ✓ The treated WCO Azahar et al.
Penetration 60/70 PG binder showed (2016e)
grade better rutting
resistance than the
untreated one.
12. PG 64-22 Binder recovered WCVO 2e10 ✓ ✓ G*/sind: 6% Ji et al. (2017)
from RAP G*sind: 6%
13. Natural Natural asphalt is WVO 17.9 ✓ ✓ G*and d showed Some et al.
Bitumen used with hard that the produced (2016)
bitumen P15/25 binders are softer
 M. Zahoor et al. / Journal of Cleaner Production 278 (2021) 123304 11

Table 4 (continued )

Sr No Control Binder Binder Tested Rej. Type Rej. Effect of increase Isochronal behavior Isothermal Mainfindings/ Reference
content in WCO % (constant frequency) behavior Optimumdosage to
(%) (constant resemble control
temperature) binder

G* d G*/sin d G*sin d G* d G*/sin d G*sin d G* d

than the original
one.
14. 60/70 Virgin binder (WVO) 1, 2, 4, 6, 8 ✓ ✓ ✓ ✓ G*/sind: Failed to Al-omari et al.
Penetration 60/70 PG satisfy Superpave (2018)
grade criteria at all
temperatures and
WVO%
G*sind: Satisfied
Superpave criteria
on all temperatures
and WVO%
15. TLA Virgin binder UFO 2e10 ✓ ✓ ✓ ✓ Value of G* reduced Singh-ackbarali
TPB while d is increased. et al. (2017)
G*/sind rutting
resistance is
reduced while
G*sind fatigue
resistance
increased.
16. 80/100 Virgin binder WCO 6 ✓ ✓ ✓ High-quality WCO (Dong Zhang
Penetration artificially aged showed better G*/ et al., 2017a)
grade sind, as the quality
deteriorates the
rutting resistance
went down also.
17. 80/100 Virgin binder WCO 1e3 ✓ The addition of 2% Rasman et al.
Penetration WCO made the (2018b)
grade rutting resistance
comparable to the
unmodified binder
18. 60/70 Extracted RAP WCO 2, 3, 3.5, 4 ✓ ✓ 3.5% WCO in El-Shorbagy
Penetration binder extracted RAP et al. (2019)
grade binder made G*/
sind identical to the
control binder and
reduced the G*sind
19. 70/100 Virgin binder WVCO 2e10 ✓ ✓ ✓ The study analyzed Go€ kalp and Uz
Penetration artificially aged by that 7% WVCO dose (2019)
grade RTFO, PAV and oxi- makes the rutting
aging method (SHT factor and fatigue
& LHT) factor of aged
bitumen to
resemble the virgin
binder.
20. PEN 70 Virgin binder WCO 1e5 ✓ ✓ ✓ G* and G*sind with Li et al. (2019a)
artificially aged in aging and an
TFOT at different increase in WCO
aging times (5 h, dosage decreases
7 h, 9, 11 h, 13 h, and d increase. 1
and 15 h) e3% WCO proved
to be the optimum
dosage for high-
temperature
performance.
21. 60/70 Virgin binder WCO 3e5 ✓ The outcomes Nordiana et al.
Penetration exhibited that G*/ (2019)
grade sind and failure
temperature of
treated WCO
dosage 5% showed
identical results as
of the virgin binder
22. VG 30 Artificially aged and WCO 2e6 ✓ ✓ Rutting resistance Durga
extracted RAP reduces while the Prashanth et al.
binder fatigue resistance (2019)
rises with the
addition of WCO.
6% WCO is the
optimum dosage.
12 M. Zahoor et al. / Journal of Cleaner Production 278 (2021) 123304
binder offers fatigue enhancements on the basis of rheological test
outcomes.
The binder’s performance at low temperature is characterized
by creep stiffness and m-value, these parameters associated to the
cracking resistance of the asphalt pavement; they are commonly
evaluated by a bending beam rheometer (BBR) (ASTM D6648). The
test is conducted on a PAV-aged binder. Creep stiffness is the esti-
mate of stresses resulting from thermal contraction, and the m-
value is the creep rate or ability to relax stresses. As per the virgin
binders, the creep stiffness increases at low temperature while m-
value decreases; the latter increases the risk of thermal cracking
(Cambridge Systematics et al., 2006). Yu et al. (2014) presented the
results of the BBR of the virgin, aged, and rejuvenated binder
at 18
C. The results of rejuvenated asphalt with waste vegetable
oil (WVO) showed a tenfold decline in the creep stiffness and more
than twice the increment in the m-value as compared to the virgin
one. Ji et al. (2017) determined the effect on creep stiffness due to
the dosage of WCVO rejuvenator in the asphalt binder. The results
demonstrated that the stiffness of the rejuvenated binder at low-
temperature gradually reduces with the rise in concentration of
WCVO, advising that the thermal cracking resistance has been
increased and chances of thermal cracking are greatly reduced.
Similarly, Al-omari et al., 2018 determined the effect of temperature
(12
C, 6
C and 0
C) and WVO concentration on the creep
stiffness and m-value. The creep stiffness and m-value satisfy the
Superpave criteria at 4% WVO at all temperatures, however, as the
concentration of WVO increases the value of creep stiffness further
reduces beyond 300 MPa. Zhang et al. (Dong Zhang et al., 2017a)
determined the effect of quality of the WCO on the thermal
cracking. The value of stiffness rises whereas, the m-value reduces
with the higher number of times the WCO was cyclically re-heated.
Similarly, other studies (El-Shorbagy et al., 2019; Go € kalp and Uz,
2019; Xinxin et al., 2018) demonstrated that the addition of WCO
is beneficial in terms of low-temperature properties. Thus, it can be
inferred that the dosing of WCO improves the thermal cracking
resistance of the asphalt binder although both creep stiffness and
m-value are affected by the type and quality of WCO used as asphalt
rejuvenator.
8. Effect of WCO on chemical properties of rejuvenated
asphalt binders
8.1. Effect of acid value and water content
During the preparation of food, the oil is continuously or
repeatedly heated between 160 and 200
C for an extended period
in the presence of air, moisture, and light. Based on frying time,
frying temperature, and concentration of cooking oil (varies from
source to source), the oil undergoes deterioration that causes sig-
nificant changes in the chemical and physical properties of the oil
(Kulkarni and Dalai, 2006; Sanli et al., 2011). The major degradation
reactions that occur under the standard operating conditions are (i)
hydrolysis, (ii) oxidation, and (iii) polymerization. In the hydrolysis
reaction, the moisture content of the food causes the oil’s double
bond to rupture and increases the free fatty acids (FFA) composition
and saturation degree (Kulkarni and Dalai, 2006). The quality of
WCO is usually determined by the acid value, which determines the
concentration of free acids and water content value identifying the
amount of water present in WCO. (Azahar et al., 2016b). Azahar
et al. (2016b) studied the effect of acid value and water content
on asphalt rejuvenation, and the results showed that the WCO
rejuvenated binder with higher acid value and water content pre-
sented poor properties while, the WCO rejuvenated binder with
lower acid value and water content displayed better results in
terms of physical, rheological and chemical properties. In another
study by Azahar et al. (2017), untreated and chemically treated
WCO addition in the aged binder is compared. The untreated WCO
with higher acid value and water content showed poor results
concerning physical, rheological, and chemical properties. In
contrast, the treated WCO with lower higher acid value and water
content showed better results in the respective properties. Zhang
et al. (Dong Zhang et al., 2017a) studied the effect of WCO quality -
denoted by its acid value - on the physical, rheological, and
chemical properties of the rejuvenated binder. It is reported that
the acid value has a significant influence on the properties of the
asphalt binder. The rejuvenated binder with fresh cooking oil - or
WCO of lower acid value - effectively restores the aged binder to the
level of a virgin binder. The recommended range of acid value to
restore the performance of the aged binder was in the range of
0.4e7 mg KOH/gm.
The high acid value increases the softening point, viscosity, and
colloidal instability index of the binder that results in the reduction
of penetration value, ductility, and rutting resistance. The low acid
value and water content of WCO contribute towards maintaining
the properties of the rejuvenated binder close to the level of virgin
asphalt binder. Thus, it makes the acid value an excellent indicator
of the rejuvenation efficiency of WCO; to achieve a greater reju-
venation effectiveness, it is recommended to perform preliminary
chemical treatments to reduce the free fatty acid and water content.
8.2. Effect of WCO on molecular groups of asphalt binder (SARA)
Since the asphalt binder is a fraction of the crude oil, it is evident
that its composition is a combination of complex organic com-
pounds with various molecular groups. These groups are based on
size, molecular weight, and polarity, and are commonly charac-
terized as Maltenes and Asphaltenes. The maltenes are subdivided
into saturates, aromatics and resins. Maltenes are the low molec-
ular weight oily medium, while, asphaltenes are high molecular
weight micelles. The combination of all these molecules is referred
to as the four components of asphalt; specifically, saturate, aro-
matic, resin, and asphaltene (SARA). SARA fractions have proved to
the influence on the physical, chemical, and rheological properties
of the asphalt binder. SARA fractions are separated by utilizing thin-
layer chromatography with flame ionization detection (TLC-FID)
(Chen et al., 2014a; Yu et al., 2014). As the bitumen ages, the con-
centration of maltenes decreases due to the oxidation and volatil-
ization, causing an increase in the composition of asphaltenes,
making the asphalt pavement stiffer due to the imbalance of
asphaltenes and maltenes. The variation of SARA is responsible for
the performance enhancement or degradation of the physical,
rheological, and chemical properties of asphalt during rejuvenation
and aging (Behnood, 2019).
Bailey et al. (Bailey and Zoorob, 2012) summarized the SARA
analysis of various virgin, aged, and rejuvenated binders. The re-
sults showed saturates, resins, and asphaltenes values are higher in
the aged binder and rejuvenated binder than the virgin binder,
while aromatics are decreased in aged and rejuvenated binder.
However, the results showed that rejuvenation does not follow any
logical mechanism as virgin and WCO (both rich in resins) changed
the SARA fractions differently when added to the aged binder;
specifically, 0.54 CI for asphalt binder rejuvenated with virgin
cooking oil and 1.13 CI for the binder rejuvenated with WCO (Bailey
and Zoorob, 2012). Zargar et al. (2012) compared the asphaltenes to
the maltenes ratio of the virgin, aged, and rejuvenated binder, and
the results demonstrated that the binder rejuvenated with WCO
nearly equals the value of asphaltenes to maltenes ratio. In a study
by Zhang et al. (Dong Zhang et al., 2017a), the authors presented the
influence of WCO quality on the SARA fraction of virgin, aged, and
rejuvenated asphalt. The good quality or less used WCO shows a
 M. Zahoor et al. / Journal of Cleaner Production 278 (2021) 123304 13

Table 5
Observation of FTIR analysis of various virgin, aged and WCO rejuvenated asphalt binders.

Sr No Material Observation of peaks (Yes ¼ O and No ¼ X) Reference

600-1400 cm1 1600-1800 cm1 2700-3500 cm1

CeC CeO C¼C C¼O CeH bond Alcohol

Alkane group bending Alkyl group Stretch aromatics Stretch OeH stretch

1. Virgin binder (pen 80/100) O X O X X X Zargar et al. (2012)

Aged binder (pen 40/50)
WCO
WCO-rejuvenated binder
2. Virgin binder (pen 60/70)
WCO
WCO-rejuvenated binder
3. Untreated WCO based binders
Treated WCO based binders
4. WCO-rejuvenated asphalt binder
5. Virgin asphalt binder (pen 50)
WVO
WVO-Rejuvenated binder
6. Virgin asphalt binder (pen 60/70)
Aged binder
Aged binder þ 3.5% WCO
7. Virgin asphalt binder (pen 70)
Aged binder
WCO-rejuvenated binder
O X
O O
O O
O X
O O
O O
O O
O O
O O
O X
O O
O O
O X
O X
O O
O X
O X
O O
O O X X
X O X X
O X* X X
O X O X Azahar et al. (2016d)
X O O X
O X* O X
O O O X Azahar et al. (2016e)
O X* O X
O X** O X (Dong Zhang et al., 2017a)
O X O O Cao et al. (2018)
O O O O
O X* O O
O O O O El-Shorbagy et al. (2019)
O O O O
O X* O O
O O O X Li et al. (2019a)
O O O X
O X* O X

X* means reduced or negligible amount of C¼O peak.

X** means reduced value C¼O for high-quality WCO in bitumen. High-quality WCO corresponds to a product that has been subject to less heating cycles compared to a
standard WCO.

high content of saturates and aromatics, a reduced amount of
resins, and nearly half of the content of asphaltenes compared to
aged asphalt. The results demonstrated that as the quality of WCO
reduces so the colloidal instability index (IC), expressed as the ratio
of the sum of asphaltenes and saturates to the sum of resins and
aromatics (Bailey and Zoorob, 2012). The colloidal instability index
(IC) of the virgin asphalt determined by Zhang et al. (Dong Zhang
et al., 2017a) is 0.30 which is almost identical to the high-quality
WCO-rejuvenated asphalt binder, however, as the heating time
elevates, the WCO quality deteriorates, and the colloidal instability
index (IC) increases which is still tolerable as the IC of the aged
binder is much higher (i.e., 0.41) (Dong Zhang et al., 2017a). Chen
et al. (2014a) reported that WCO addition slightly alters the
composition of the four SARA fractions by reducing the overall
asphaltenes content and adding up more resins compared to the
aged asphalt. Similarly, in other studies (Gong et al., 2016; Li et al.,
2019b, 2019a; Osmari et al., 2017; Yu et al., 2014) the effect of WCO
dosage on SARA fractions of various asphalt binders was studied; it
was concluded that WCO, by reducing the asphaltenes and raising
the maltenes in the aged asphalt, can rejuvenate the aged asphalt
by significantly affecting the macro scale properties. It increases the
penetration value, ductility, and phase angle of the aged binder and
reduces the softening point, viscosity, and complex shear modulus.
However, predicting the molecular interactions among the chem-
ical components of the binder and rejuvenator remains very com-
plex; in fact, only a general rearrangement of different fractions is
predicted by the colloidal index.
8.3. Effect of WCO on oxidation potential of asphalt binder
The characterization and identification of functional groups in
the different samples are determined by using Fourier Transform
Infrared Spectroscopy (FTIR). FTIR spectroscopy measures the
coherence of the radiating source at ambient temperature utilizing
space or time domain determination of electromagnetic radiations
(Chen et al., 2014a). Table 5 summarizes the studies that looked into
the FTIR spectroscopy of various virgin, aged, and WCO-
rejuvenated asphalt binders. It is clear from Table 5 that all
binders along WCO have similarities in the CeC and CeH bonds
based on their similar elements, e.g., hydrogen, carbon, nitrogen,
and sulfur that are also building blocks of asphalt (Gong et al.,
2016).
The degree of aging and rejuvenation is determined by
analyzing the intensities of the carbonyl (C]O) and sulfoxide (S]
O) peaks; when the asphalt ages, it loses its lighter oily components
and oxidation reactions modify the carbonyl (C]O) and sulfoxide
(S]O) groups, which correlate to the rise in the polar components
(asphaltenes). Asphaltenes are high molecular weight micelles.
When the asphalt is rejuvenated with WCO, new absorption peaks
can be observed at 1160 cm1 and 1744 cm1 that belong to the
alkyl group (CeO) and the ester carbonyl group, respectively.
It is noticed that the carbonyl (C]O) peak is reduced drastically
by the rejuvenation of WCO when compared with the aged binder
resulting in the enhancement of physical and rheological properties
of the rejuvenated binder (Azahar et al., 2017; Li et al., 2019a; Zargar
et al., 2012). It is also reported that as the quality of WCO improves
(i.e. lower usage rate), the carbonyl (C]O) peak and the sulfoxide
(S]O) peak reduce gradually (Dong Zhang et al., 2017a). Similarly,
Azahar et al. (2016e) demonstrated that the carbonyl (C]O) peaks
are significantly reduced in the treated WCO based binder. Thus,
from the analysis of the above studies, it can be observed that as the
polar compounds (high molecular weight molecules) rise with the
aging of the asphalt binder, so does the carbonyl (C]O) peak. The
addition of WCO-based alkyl groups and ester functional groups
helps reduce the asphaltenes content, which leads to the reduction
in the carbonyl (C]O) peak hence reducing the effect of aging
without fully recovering the carbonyl (C]O) peak to the virgin
asphalt binder level.
9. Effect of WCO on microscopic properties of asphalt binder
Asphalt binder is a mixture of complex organic compounds of
various sizes and polarities obtained from the processing of crude
oil. There is widespread acceptance that asphalt binder is a
14 M. Zahoor et al. / Journal of Cleaner Production 278 (2021) 123304
heterogeneous and multiphase system; however, it comprises mi-
crostructures formed by the high chemical contents variability with
diverse micro-mechanical properties which influences the physical
properties of asphalt binder including stiffness, plasticity, hardness,
adhesion, healing and quantitative sample deformation (Das et al.,
2016). Technologies commonly available to study microstructure
and morphology are atomic force microscope (AFM), transmission
electron microscope (TEM), scanning electron microscope (SEM),
fluorescence microscope, and environmental scanning electron
microscope (ESEM) (Hossain and Hossain, 2019). Atomic force mi-
croscope (AFM) is the most widely utilized tool to examine the
three-dimensional micro-structure and morphological behavior of
asphalt binder. Two types of information can be taken from the
microstructure image formed by AFM, namely (i) surface topog-
raphy (roughness) and (ii) surface force (adhesion). Additionally,
three phases are distinguished from the microstructure image of
the AFM: (i) catana phase, (ii) peri-phase, and (iii) para phase
(Hossain and Hossain, 2019; Osmari et al., 2017). The catana phase
forms a bee-like structure due to ridges and valleys within the
phase (Loeber et al., 1996). It was noted that the bee structure is
linked to the rheological performance of asphalt, as the binder ages
the number of bee structures increases, although the process is
reversed after the rejuvenation occurs (Osmari et al., 2017; Soenen
et al., 2008). It was also shown that the rejuvenator does not always
change the microstructure development of virgin or aged binder,
which led to the point where the performance of rejuvenated
binder cannot be simply evaluated based on the microstructure
(Chen et al., 2018; Yu et al., 2014). In spite of this, few researchers
have conducted studies on the micro-mechanical behavior of WCO-
based rejuvenated asphalt binder (Azahar et al., 2017; Osmari et al.,
2017; Yu et al., 2014). Yu et al. (2014) studied the effect of WCO on
microscopic properties for the first time. This study shed some light
on the WCO-rejuvenation mechanism at a microscopic scale by
demonstrating the difference between virgin, aged, and rejuve-
nated bitumen AAD (PG 58e28) and ABD (PG 58e10). The virgin
ABD binder shows a flake-like structure, while the AAD binder
shows elliptical domains with bee-structures. Upon aging, the size
of flake-like structures reduces, and the quantity increases in the
ABD binder; however, the bee-structures resulting in less pro-
nounced changes between the virgin and aged binder. The addition
of WCO shows darker flake-like structures like the aged binder but
with a smooth surface. On the other hand, the bee-structure re-
mains the same, but the density increases when compared to the
aged binder. Thus, it can be observed that some enhancement in the
morphological characteristics was provided by WCO compared to
the aged binder; however, WCO rejuvenation did not reproduce the
surface structure of the original virgin binder. Azahar et al. (2017)
studied the surface characteristics of a control binder (60/70
penetration grade) and modified binder based on untreated and
treated 5% WCO (Azahar et al., 2017). The 3D topographical obser-
vations showed the rise and fall of the peaks in all the samples. The
control sample had high surface roughness due to the greater cat-
ana phase than the other samples. The modified binder with
chemically-treated WCO showed minimum surface roughness
1.791 nm when compared to the virgin binder, which had a surface
roughness of 2.705 nm; this demonstrated enhanced adhesion and
coating possibility with the aggregate to produce high-
performance asphalt (Azahar et al., 2017). Therefore, it can be
inferred that the chemically modified WCO minimizes the surface
roughness caused by the loss of low molecular weight compounds
as the bitumen ages. Osmari et al. (2017) analyzed two control
binders (PG 64-22 S and PG70-22 S) in virgin, aged, and rejuve-
nated condition. The aged binders showed a high density of bees
than the virgin binder, and the WCO reduced the catana phase and
peri phase by 47% and 48%, respectively. It also increased the para
phase by 147% in PG 64-22 S, and similar trends were noticed in PG
70-22 S. Outcomes of this study show that the addition of re-
juvenators provides help in recovery the characteristics of the vir-
gin binder. In 2019, El-Shorbaghy et al. (El-Shorbagy et al., 2019)
utilized the SEM and energy dispersion x-ray (EDX) and compared
the composition of aged and rejuvenated binder; the results
showed that WCO had enhanced the CaCO3 from 89.31% in the aged
binder to 93.94% in the rejuvenated binder. The WCO rejuvenated
binder’s SEM image showed that the smooth surface as SiO2 was
completely dissolved, which caused spread bores of different sizes.
From the above studies, it can be concluded that the WCO-
rejuvenation has the potential to recover the microscopic charac-
teristics of a virgin binder. Bitumen rejuvenation with WCO causes
a reduction in the catana and peri phase and increases the para
phase in the aged binder, which retrieves the characteristics of the
virgin binder. However, one study reported no significant change in
the microscopic properties of the aged binder by the addition of a
WCO-rejuvenator. Due to very limited studies in this area and some
conflicting outcomes, there is a need for further exploration in this
area.
10. Effect of WCO on asphalt mixture performance
10.1. Effect of WCO on the permanent deformation
The low viscosity of WCO contributes towards the formation of a
softer binder. The softer binder has more susceptibility towards
rutting, which leads to permanent deformations of the asphalt
pavement (Hidayah et al., 2013). The incremental dosage of WCO
plays a role in the constant reduction of rutting resistance and
stiffness of the asphalt. A few studies are available in which ex-
periments are conducted for predicting the effect of WCO on the
rutting performance of the asphalt mixture, especially including
RAP/RAS (Aghazadeh Dokandari et al., 2017; Taherkhani and
Noorian, 2018; Wen et al., 2013; Zaumanis et al., 2014d). Wen
et al. (2013), evaluated the effect of WCO on HMA. The dynamic
repeated creep load test conducted to analyze the rutting potential
showed that the asphalt mixtures with a high dosage of WCO
exhibit a reduction in rutting resistance (i.e. reduction of the flow
number). These results correlate to what was already discussed for
the binder rutting tests based on complex shear modulus, phase
angle, and Jnr. Taherkhani et al. (Taherkhani and Noorian, 2018)
conducted IDT strength tests on asphalt mixtures including WCO. It
was reported that 3%, 6%, and 10% dosage of WCO for asphalt
mixtures with 25%, 50%, and 75% RAP, respectively, provide an
equivalent (or slightly inferior) IDT strength to the control mixture.
Similar results are reported by Zaumanis et al. (2014d) where 12%
dosage of rejuvenator in 100% RAP mixture resulted in an overall
reduction of IDT strength. It is concluded that the addition of RAP
increases the IDT strength of the mixture, although - when the
WCO is added - due to its softening effect, the IDT strength reduces
with the increment in the dosage of WCO. For the dynamic
repeated creep load test, it is reported that mixtures with 75% RAP
offers better resistance to permanent deformation although the
optimal dosage of WCO should be carefully selected; in this study,
10% WCO provided the best resistance to permanent deformation
and similar to the initial control mixture, while 5% and 15% WCO
dosage showed poorer rutting performance (Taherkhani and
Noorian, 2018). The high RAP content mixes have substantial
aged binder with high molecular weight components favoring a
greater resistance to permanent deformation; 10% WCO re-
juvenates more aged binder than its 5% WCO counterpart while 15%
WCO provides excessive quantity of rejuvenator in the mix hence
softening it.
 M. Zahoor et al. / Journal of Cleaner Production 278 (2021) 123304
10.2. Effect of WCO on fatigue and thermal performance
Wen et al. (2013) reported fatigue test results and showed that
as the dosage of WCO increases in the mixture, a correspondent
reduction in asphalt fatigue can be observed. Similar results are
reported in other studies where excessive WCO dosage causes a
reduction in the fatigue resistance of the asphalt mixes containing
RAP (Taherkhani and Noorian, 2018; Zaumanis et al., 2014d).
Strength tests at low temperature indicate that incremental dos-
ages of WCO increase the critical strain energy density (CSED)
hence indicating an enhanced resistance to thermal cracking (Wen
et al., 2013). Similarly, it is reported that low temperature bending
test showed high flexural failure strain (2900 mε) for the WCO-
based asphalt mixes compared to conventional asphalt mixture
(2000 mε) and polymer modified asphalt mixture (2500 mε) (Sun
et al., 2017). This shows that WCO-based asphalt mixture pro-
vides good low-temperature cracking resistance (Sun et al., 2017). It
is concluded that the excessive concentration of WCO causes the
specimens to fail at lower deformation, which consequently results
from the reduction of cohesiveness of the binder leading to reduced
fatigue resistance. At the same time, it enhances the thermal
cracking resistance of the asphalt mixture. However, although
several studies are available on fatigue and thermal cracking
properties of asphalt mixes with various rejuvenators, limited
study is available on the specific effect of WCO.
10.3. Effect of WCO on the moisture susceptibility
The presence of water inside the pavement can make the HMA
prone to moisture damage. This can affect the pavement by causing
stripping between the binder and the aggregate, hence leading to
potholes on the road, which ultimately affect the traffic flow and
safety (Ahmed and Hossain, 2020). Moisture susceptibility of
asphalt pavement is often denoted by the tensile strength ratio
(TSR). Wen et al. (2013) have studied the effect of WCO addition on
moisture susceptibility of asphalt mixes; the results show that all
the samples containing WCO satisfied the minimum criteria as set
by AASTHO for TSR (i.e. > 80%). However, Majidifard et al. (2019)
reported that asphalt mixture with virgin bitumen had the great-
est moisture susceptibility, but 60% RAP þ WCO reduced the
moisture susceptibility. Similar results are reported by Zaumanis
et al. (2014d) where 100% RAP rejuvenated asphalt containing
12% WCO increased the susceptibility to moisture damage and
failed the minimum TSR requirement. From the above studies, it
can be inferred that an excessive dosage of WCO can result in loss of
adhesion and cohesion, which facilitates moisture damage.
10.4. Field performance evaluation
Field studies are available on the effectiveness of rejuvenators
with high RAP content mixes (Giustozzi et al., 2015). However, only
a very limited number of studies presents on the field experiences
using WCO-rejuvenated asphalt. Hugener et al. (2014) reported
cold asphalt recycling with 100% RAP and cooking oil-based re-
juvenators. The study utilized a commercial rejuvenator, virgin
cooking oils (rapeseed oil and linseed oil), and Waste oil (frying oil)
as possible rejuvenators for reclaimed asphalt. Cold mixture field
trial samples when compared against the laboratory mixtures
illustrated greater uniaxial compression test (UCT) resistance. The
results confirmed the laboratory tests where all the rejuvenators
demonstrated similar UCT resistance but waste oil based mixture
showed slightly lower UCT-resistance than the virgin oil (Hugener
et al., 2014). However, WCO þ fresh bitumen showed poorer per-
formance than WCO alone. The laboratory and field tests were also
enhanced by using the wheel tracking test; the virgin cooking oils
15
and WCO showed similar rutting depth and agreed with the out-
comes from UCT tests. Xie et al. (2017) studied the effect of re-
juvenators on high recycled content asphalt mixes by conducting
laboratory and field performance examinations. Different experi-
mental mixes prepared in this work, out of these mixes, one reju-
venated mix is based of fatty acids of cooking oil (rejuvenator), 25%
RAP, and 5% RAS as a warm mix asphalt (experimental mix 1). The
laboratory and early field performance (after two years of service)
showed that the control mix possesses similar rutting resistance to
the experimental mix, but the rejuvenated mix (experimental-1)
offers lower resistance to cracking and reduced moisture suscep-
tibility. Notably, the field cracking was in agreement with the
overlay test (OT) and I-FIT test results conducted in the laboratory
(Xie et al., 2017).
It can be concluded that the effect of WCO on pavement per-
formance correlates well with the outcomes from laboratory
studies. However, due to the limited long-term monitoring studies,
additional research is needed to assess the performance of WCO-
rejuvenated high RAP/RAS content pavements.
11. ‘Rejuvenators’ and ‘Softeners’: an ongoing discussion
In recent times, a debate has been started between researchers
on a distinction between two recycling agents: rejuvenators and
softeners. In 2007, Chen et al. (2007) and Shen et al. (2007a)
mentioned in their work that the softening agents are added in
the aged binder to improve their viscosity, while, the effect of the
rejuvenators is to restore the mechanical, chemical and rheological
properties of an aged binder giving it a new service life that is
equivalent to the service life of virgin asphalt binder. Similar
statements have also been reiterated by Grilli et al. (2017) and
Tabakovi c et al. (2017) who mentioned that softening agents are
more concerned with the viscosity behavior only, while re-
juvenators attempt to recuperate the basic, rheological and chem-
ical properties of an aged binder, thus ensuring a new life to HMA.
However, Tabatabaee et al. (Tabatabaee and Kurth, 2016) provided a
more clear picture of the difference between rejuvenators and
softeners. The recycling agents are further classified into the
following: (i) soluble softener, (ii) compatabilizer, and (iii) incom-
patible softener (Tabatabaee and Kurth, 2017). Soluble softeners
supplement the solvent phase and mostly consist of low polarity
naphthenic aromatic fractions of the bitumen colloidal structure.
This type of additives reduces the modulus and viscosity of the
bitumen, however, self-assembly of polar micelles and intermo-
lecular agglomeration might be affected. Meanwhile, the incom-
patible softeners are less compatible with low polarity napthenic
aromatics and polar fractions due to the involvement of saturated
and paraffinic materials. They reduce the viscosity and stiffness
modulus of bitumen, although increasing the dosage of insoluble
softeners results in increased colloidal instability and affects the
bitumen in the long run (Johnson and Hesp, 2014). The compati-
bilizers are engineered products that have an affinity for multiple
fractions. They reduce the binder viscosity and decrease the con-
tent of higher molecular weight components. The rejuvenators
cannot undo the oxidative aging occurred to the binder, however, it
can only reverse the impact of aging on the asphalt performance,
properties, damage resistance, and durability by restoring the bal-
ance of maltenes and asphaltenes fractions, phase stability, healing
ability, reducing the low temperature and cracking resistance and
giving equal or better aging behavior than the virgin binder.
Therefore, rejuvenator is a recycling agent that demonstrates the
properties of both “softner” and “compatibiliser” while reversing
the impact of aging on asphalt (Tabatabaee and Kurth, 2017, 2016).
16 M. Zahoor et al. / Journal of Cleaner Production 278 (2021) 123304
12. Conclusions
This study reviews various aspects of restoring the initial
properties of aged asphalt with WCO. In recent years, many studies
have been conducted to evaluate the possibility of using WCO as an
asphalt rejuvenator. Based on the present review of the literature,
the following conclusions can be drawn:
 The properties of WCO-rejuvenated bitumen are significantly
affected by the concentration of the oil. The physical properties
are highly influenced as more lighter oil components are
introduced by the incremental dosage of WCO, which reduce the
overall viscosity of the bitumen and result in greater penetration
value, ductility and reduced softening point and specific gravity.
WCO addition into the binder also enhances its flexibility at
lower temperature leading to high thermal resistance; however,
this makes the binder more prone to permanent deformation
unless further polymer modification is provided.
 Rheological evaluation of WCO-based rejuvenated bitumen
shows an overall reduction of stiffness. As the dosage of WCO is
increased, the less viscous oil contributes by reducing the
complex shear modulus G* and creep stiffness of the binder,
while phase angle (d) and m-value showed improvements. Thus,
WCO addition in the binder is commonly acknowledged to
reduce rutting resistance while improving bitumen fatigue and
resistance to thermal cracking.
 The efficiency of the rejuvenation process is significantly
affected by the acid value, water content and overall quality of
WCO. As the quality of WCO deteriorates, the acid value and
water content rise gradually and cause a reduction of the reju-
venation potential. Some studies showed how preliminary
treatments of WCO could reduce the acid value and water
content, hence enhancing its rheological and chemical
performance.
 The results of the oxidative analysis using FTIR showed that the
untreated WCO accommodates undesirable components - e.g.
C]O stretch - which are accountable for deprived rutting per-
formance of the WCO-rejuvenated binder. The treated WCO-
based binder has a nearly negligible number of undesirable
compounds; e.g. C]O stretch.
 It is found that WCO rejuvenation does not reproduce the sur-
face structure of the original virgin binder but retrieves some
characteristics of standard bitumen. WCO reduces the catana
phase and peri phase up to 50% of the aged asphalt binder,
reducing the overall surface roughness caused by the loss of low
molecular weight compounds. However, limited studies are
available on this domain.
 For the asphalt mixtures, high RAP content mixes with WCO-
rejuvenator favours improved resistance to permanent defor-
mation. Also, an increase of WCO dosage causes a general
reduction in fatigue resistance of asphalt mixes with RAP while
enhancing the thermal cracking resistance at low temperature.
However, available studies on this domain are limited for WCO.
 A rejuvenator is a recycling agent that demonstrates the prop-
erties of both a “softner” and a “compatibiliser” while reversing
the impact of aging on asphalt. Rejuvenators cannot undo the
oxidative ageing but can reverse their impact by improving the
physical, rheological and chemical properties of bitumen by
providing equal or better ageing behavior than the virgin binder.
This review paper emphasizes the efficiency enhancement of
asphalt binder using WCO as a rejuvenator, also exploring the
possibility of utilizing it with RAP. Many studies have shown
promising results with improvement in physical, rheological,
chemical, and micro properties of the asphalt binder. However,
there are several shortcomings related to the usage of WCO in the
asphalt pavements. The overview of the shortcomings is given
below:
 The optimal dosage of WCO rejuvenator for RAP in full-scale
applications is still highly debated, mainly due to the lack of
long-term performance data.
 Inadequate data is available on the effect of WCO chemical
components on the properties of WCO-rejuvenated binders.
 There is a general lack of field performance studies of WCO-
rejuvenated asphalt pavements; e.g. high-RAP content HMA or
WMA rejuvenated with WCO.
 There is room for combining the rejuvenation effect of WCO
along with other modifiers e such as plastomeric polymers
(Bonicelli et al., 2017) - to enhance the performance of asphalt in
specific climatic conditions (i.e. warm climates).
CRediT authorship contribution statement
Muhammad Zahoor: Conceptualization, Data analysis, Meth-
odology, Writing - original draft, Writing - review & editing. Sabzoi
Nizamuddin: Conceptualization, Data analysis, Methodology,
Writing - original draft, Writing - review & editing. Srinivasan
Madapusi: Conceptualization, Methodology, Writing - review &
editing, Supervision. Filippo Giustozzi: Conceptualization, Meth-
odology, Writing - review & editing, Supervision, Project adminis-
tration, Funding acquisition.
Declaration of competing interest
The authors declare that they have no known competing
financial interests or personal relationships that could have
appeared to influence the work reported in this paper.
Acknowledgments
The Authors would like to acknowledge Cookers Oil Pty. Ltd. for
sponsoring the doctoral scholarship “Exploring the possibility to
reuse Waste Cooking Oil in asphalt pavements as rejuvenator” to
Muhammad Zahoor.
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