Technical Note

Laboratory Investigation of Different Standards of Phase

Separation in Crumb Rubber Modified Asphalt Binders
Hakseo Kim 1 and Soon-Jae Lee 2
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Abstract: The phase separation between polymer additives and virgin asphalt binders during hot storage is an important issue in the asphalt
industry. Traditionally, it has been customary to evaluate the degree of phase separations in polymerized asphalts by laboratory testing, such
as the cigar tube test (CTB). However, the test circumstances, temperature, and storage time vary depending on different standards used in
many countries. Based on a comprehensive literature review, the range of temperatures and oven storage times were selected to be 140–180°C
and 2–7 days, respectively. The phase separation of 11 storage stability conditions selected from 12 different places using crumb rubber
modified asphalts (CRMAs) were compared and evaluated in this study. The CRMAs produced in the laboratory were made with PG 64-22
virgin binder and ambient crumb rubber with various concentrations (10, 15, and 20% by weight of virgin binder). The CTB was used as the
storage stability test method, and percent separation was obtained from the G=sin δ relationship between the top and bottom portion of
the tube. The storage stability tests indicated that the viscosity of the CRMAs had a significant influence in the phase separation of the
binders; the higher the viscosity of the binder, the less the degree of the separation. DOI: 10.1061/(ASCE)MT.1943-5533.0000751.
© 2013 American Society of Civil Engineers.
CE Database subject headings: Rubber; Asphalts; Binders (material); Laboratory tests.
Author keywords: Crumb rubber modified asphalt (CRMA); Phase separation; Cigar tube test (CTB).

Introduction
The use of asphalt modification involving polymer additives
(i.e., SBS, SBR) began in the United States, in the 1980s, with
federal regulations supporting this development resulting from in-
creasingly heavy traffic (Sun and Lu 2003; Polacco et al. 2006;
Yildirim 2007). In addition, domestic waste polymers (i.e,. crumb
rubber from scrap tires and waste plastic) have become an attractive
to virgin polymer not only because of their successful performances
but also because of their environmental and economical advantages
(Garcia-Morales et al. 2006). Ultimately, these efforts have played
a significant role in improving pavement performance such as
rutting, fatigue cracking, and thermal cracking at low temperatures
(Yu et al. 2007). Specifically, crumb rubber modified asphalts
(CRMAs) are effective in unique applications such as open-graded
friction courses (OGFC), stress absorbing membranes (SAM), and
chip seals (Cooper et al. 2007; Shen and Amirkhanian 2005).
Along with these practical uses, their effectiveness has been sup-
ported by laboratory research and field studies (Palit et al. 2004;
Bahia and Davis 1994; Way 1998). However, the field performance
of asphalt-polymer blends for extended periods at high tempera-
tures remains a concern because of the phase separation at terminal
blend products due to their poor comparability (Fu et al. 2007;
Gonzalez et al. 2004; Jin et al. 2002). For the CRMAs, it is also
1
Assistant Manager, Road Dept., Dohwa Consulting Engineers Co.,
Ltd. 942-1, Gangnam-gu, Seoul, Korea.
2
Assistant Professor, Dept. of Engineering Technology, Texas
State Univ., San Marcos, TX 78666 (corresponding author). E-mail:
soonjae93@gmail.com
Note. This manuscript was submitted on August 23, 2012; approved on
November 30, 2012; published online on December 3, 2012. Discussion
period open until May 1, 2014; separate discussions must be submitted
for individual papers. This technical note is part of the Journal of Materials
in Civil Engineering, Vol. 25, No. 12, December 1, 2013. © ASCE, ISSN
0899-1561/2013/12-1975-1978/$25.00.
common problem that the phase separation occurs when rubber
particles settle in the hot storage tank (Navarro et al. 2004; Zanzotto
and Kennepohl 1996; Bahia et al. 1998). Therefore, decreasing
the phase separation is necessary for improved quality products
and subsequently improved results in the asphalt pavement
construction.
The most common method of investigating this phenomenon
is to use the cigar tube test (CTB) and to determine the degree of
separation based on rheological properties (i.e., viscosity, softening
point, complex shear modulus, and phase angle) using samples
taken from the bottom and top of the CTB. However, the storage
conditions (i.e., storage duration and temperature in the oven) vary
widely for different countries and many states in the United States
as well. Therefore, the objective of this study was to compare dif-
ferent standards of storage circumstances from various places
(i.e., North America, South America, Africa, Europe, and Asia)
using the CRMAs.
Experimental Program
Materials
The following materials were used in the experimental program:
• Asphalt binder: One PG 64-22 asphalt binder was used in this
study. The asphalt binder was a mixture of several sources that
could not be identified by the supplier. The binder was trans-
ported to the laboratory in sealed 5 gallon containers to prevent
oxidation and premature aging and tested to collect the funda-
mental information through Superpave binder specification.
Table 1 summarizes the results through three aging phases.
• Crumb rubber: The crumb rubber produced by mechanical
shredding at ambient temperature was obtained from one
source: 40 mesh (0.425 mm). The properties of the crumb rub-
ber were analyzed in accordance with ASTM D297 (ASTM
2013) as shown in Table 2. The particle size distribution of this

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J. Mater. Civ. Eng. 2013.25:1975-1978.

 Table 1. Properties of Virgin Asphalt Binder
Aging status Properties
Unaged binder Viscosity at 135°C (kPa)
G=sin δ at 64°C (kPa)
RTFO aged residue Mass loss at 163°C (%)
G=sin δ at 64°C (kPa)
RTFO + PAV aged residue G sin δ at 25°C (kPa)
Stiffness at −12°C (MPa)
m-value at −12°C
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crumb rubber is shown in Table 3. To ensure that the consistency
PG 64-22 of the CRM was maintained throughout the study, only one
batch of crumb rubber was used in this study.
0.405
1.207
CRMA Binder Production
−0.02
2.815 The three different percentages (10, 15, and 20% by binder weight)
were decided as different agencies use different crumb rubber per-
2,970
centage. For instance, 5 and 12% CRM is used in dense and open-
183
0.311 graded hot mix asphalt (HMA) mixtures; respectively, in Florida,
10% CRM is used in HMA surface course in South Carolina,
14–23% CRM is used in California, and 20% CRM is used in

Table 2. Properties of Ambient Crumb Rubber Arizona. The mixture was reacted for 1 h at 177°C (350°F).
Properties Test values
The reaction speed was 700 rpm using a mechanical mixer based
on preliminary research indicating that this speed is effective for
Specific gravity 1.037 blending rubberized asphalt (Putman 2005).
Moisture content 0.67 The flowchart of the experimental procedures is shown in Fig. 1.
Ash content 5.36
Following the preparation of the three CRMAs, the storage stability
Carbon black content 29.75
Extract content (acetone and chloroform) 11.80 test was conducted under eleven storage conditions used in twelve
Sulfur content 1.32 different locations around the world (Table 4).

Table 3. Size Distribution of Crumb Rubber Used Storage Stability

Sieve size % Passing requirements, For the storage stability test, an aluminum cigar tube (32-mm diam-
number % Passing type Ba eter, 160-mm height) was used to estimate the phase separation of
8 — — the CRMAs as it is commonly used in approving terminal blending
10 100 100 of modified binders. The cigar tube, filled with the CRMAs, was
16 100 65–100 sealed and placed vertically in the oven at temperatures ranging
30 99 20–100 from 140–180°C from 2–7 days. The tubes were then removed
50 35 0–45 from the oven and instantaneously cooled in a freezer at −20°C.
200 2 0–5 The frozen tubes were subsequently cut into three equal sections,
a
Arizona DOT requirements. and samples obtained from the top and bottom sections were used

Fig. 1. Flowchart of experimental procedures

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J. Mater. Civ. Eng. 2013.25:1975-1978.

 Table 4. Storage Stability Conditions Used in This Study
Temperature, Duration,
°C day Country References
140 5 France DuPont (2005)
150 7 United Kingdom Morgan and Mulder (1995)
160 3 Italy Giavarini et al. (1996)
160 3 Australia Emery and O’Connell (1999)
160 3 Venezuela Becker et al. (2002)
160 3 Saudi Arabia Iqbal (2006)
160 4 Brazil
160 5 Netherlands K. Steernberg, “Preparation
process for polymer-modified
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bitumen,” International patent

WO 37,545 (1996)
160 5 Canada Ho et al. (2006)
Fig. 2. Separation of the binders containing 10% crumb rubber under
163 2 China Sun et al. (2006)
163 2 Taiwan Chen and Huang (2007) different storage conditions
163 2 S. Korea
163 5 Spain Navarro et al. (2007)
163 7 Texas K. P. Kelly and J. R. Butler,
“Method for preparation of
stable bitumen polymer
compositions,” U.S. patent
6,767,939 (2001)
165 2 United States
170 7 Japan M. Torii, H. Kato, M. Suzuki,
and T. Miyachi, “Block (co)
polymer, block copolymer
composition for asphalt
modification, process for
producing the same, and
asphalt composition,” U.S.
patent 20,060,229,391 (2006)
180 3 United Kingdom
180 3 Sweden Isacsson and Lu (1999)
180 3 Hungary Biro et al. (2001), Fig. 3. Separation of the binders containing 15% crumb rubber under
Geiger et al. (2005) different storage conditions
180 3 South Africa Hofsink et al. (2004)

to evaluate storage stability status, the rheological parameters of G

and δ based on Superpave Dynamic Shear Rheometer (DSR) Test.
A Bohlin DSR II having a 25-mm diameter plate-plate geometry
and 1-mm gap were used for this experiment at 60°C. The result of
percent separation was determined using Eq. (1):
ðG=sin δÞmax − ðG=sin δÞavg
% Separation ¼ ð1Þ
ðG=sin δÞavg

where ðG=sin δÞmax represents the higher value of either the top
or bottom section of the tube and the ðG=sin δÞavg is the average
value of both sections.

Fig. 4. Separation of the binders containing 20% crumb rubber under

Results
To determine, if the rubber concentration significantly affects the
degree of phase separation in rubberized binders, binders with
different rubber concentrations were evaluated. Figs. 2–4 show
the degree of separation for binders containing 10, 15 and 20%
rubber by weight of virgin binder, respectively. The graphs show
that as the rubber concentration increases, the degree of separation
decreases. The separation indexes were found to be 36.9, 29.4 and
23.3% for the rubber contents 5, 10 and 15%, respectively. This
may be attributable to the increase in the viscosity of the binder
as the rubber concentration increases. The results may support
the current minimum percentage of 15% specified by ASTM.
different storage conditions
With respect to the effect of storage time on the separation of
rubberized binders, the average separation values were observed
to be higher for binders stored for 7 days than those stored for
3 days. In addition, it is important to note that the storage time
appears to affect the increase in the separation of rubberized bind-
ers more than the storage temperature. This study is to compare
different standards of various storage conditions, but it is not
feasible to say that one standard is better than another due to
the limitation of test data. To generalize the findings, more

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J. Mater. Civ. Eng. 2013.25:1975-1978.

 experimental data are required using different crumb rubber types
and percentages.
Conclusions
Comparison of the phase separation of various binders with differ-
ent standards used in many countries and the rheological analyses
were carried out in this study. The following conclusions were
reached:
1. The degree of phase separation in the CRMAs decreased as the
rubber concentration increased, owing to the increase in the
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viscosity of the CRMAs.
2. The storage duration had more significant influence on
the degree of separation of the CRMAs than the storage
temperature.
3. It is recommended to conduct another study to evaluate the
chemical compatibility in asphalt binder modified with crumb
rubber. Also, more test data will be helpful to evaluate the sen-
sitivity of storage temperature and storage time.
References
ASTM. (2013). “Standard test methods for rubber products—Chemical
analysis.” D297, West Conshohocken, PA.
Bahia, H. U., and Davis, R. (1994). “Effect of crumb rubber modifiers
(CRM) on performance related properties of asphalt binders.” J. Assoc.
Asphalt Paving Technologists, 63, 414–449.
Bahia, H. U., Zhai, H., and Rangel, A. (1998). “Evaluation of stability,
nature of modifier, and short-term aging of modified binders using
new tests: LAST, PAT, and modified RTFO.” Transportation Research
Record, 1638, 64–71.
Becker, M. Y., Muller, A. J., and Rodriguez, Y. (2002). “Use of rheological
compatibility criteria to study SBS modified asphalts.” J. Appl. Polym.
Sci., 90(7), 1772–1782.
Biro, S., Bartha, L., Deak, G., and Fanto, E. (2001). “The production
and use of rubber-bitumen compositions.” Scientific Publication of
MOL PLC, 97–103.
Chen, J. S., and Huang, C. C. (2007). “Fundamental characterization
of SBS-modified asphalt mixed with sulfur.” J. Appl. Polym. Sci.,
103(5), 2817–2825.
Cooper, S. B., Jr., Mohammad, L. N., and Abadie, C. (2007). “Evaluation
of field projects using crumb rubber modified asphaltic concrete.”
FHWA, 393, 1–8.
DuPont. (2005). 〈http://www.dupont.com/asphalt/link2.html〉 (Aug. 1,
2012).
Emery, S., and O’Connell, J. (1999). “Development of a high performance
SBS modified binder for production.” 7th Conf. Asphalt Pavements
Southern Africa.
Fu, H., Xie, L., Dou, D., Li, L., Yu, M., and Yao, S. (2007). “Storage
stability and compatibility of asphalt binder modified by SBS graft
copolymer.” Constr. Build. Mater., 21(7), 1528–1533.
Garcia-Morales, M., Partal, P., Navarro, F. J., and Gallegos, C. (2006).
“Effect of waste polymer addition on the rheology of modified
bitumen.” Fuel, 85(7–8), 936–945.
Geiger, A., Biro, S., Bartha, L., Deak, G., and Miskolczi, N. (2005).
“Performance of waste polymer modified bitumens.” WasteTech-2005
Congress, Moscow.
1978 / JOURNAL OF MATERIALS IN CIVIL ENGINEERING © ASCE / DECEMBER 2013
J. Mater. Civ. Eng. 2013.25:1975-1978.
Giavarini, C., Filippis, P., Santarelli, M. L., and Scarsella, M. (1996).
“Production of stable polypropylene modified bitumens.” Fuel, 75(6),
682–683.
Gonzalez, O., Munoz, M. E., Santamaria, A., Garcia-Morales, M., Navarro,
F. J., and Partal, P. (2004). “Rheology and stability of bitumen/EVA
blends.” European Polymer J., 40(10), 2365–2372.
Ho, S., Church, R., Klassen, K., Law, B., Macleod, D., and Zanzotto, L.
(2006). “Study of recycled polyethylene materials as asphalt modifiers.”
Can. J. Civ. Eng., 33(8), 968–981.
Hofsink, W., Kong, N. Y., and Dickinson, M. N. (2004). “The performance
of seals and asphalt using SBS modified binder on the N3 toll road.”
Proc. 8th Conf. on Asphalt Pavements for Southern Africa, 12–16.
Iqbal, M. H., Hussein, I. A., Al-Abdul, H. I., and Amin, M. B.
(2006). “Rheological investigation of the influence of acrylate
polymers on the modification of asphalt.” J. Appl. Polym. Sci.,
102(4), 3446–3456.
Isacsson, U., and Lu, X. (1999). “Characterization of bitumens mod-
ified with SEBS, EVA and EBA polymers.” J. Mater. Sci., 34(15),
3737–3745.
Jin, H., Gao, G., Zhang, Y., Sun, K., and Fan, Y. (2002). “Improved proper-
ties of polystyrene-modified asphalt through dynamic vulcanization.”
Polymer Testing, 21(6), 633–640.
Morgan, P., and Mulder, A. (1995). The shell bitumen industrial handbook,
Shell Bitumen, 143–196.
Navarro, F. J., Partal, P., Garcıá-Morales, M., Martinez-Boza, F. J., and
Gallegos, C. (2007). “Bitumen modification with a low-molecular-
weight reactive isocyanate-terminated polymer.” Fuel, 86(15),
2291–2299.
Navarro, F. J., Partal, P., Martınez-Boza, F., and Gallegos, C. (2004).
“Thermo-rheological behaviour and storage stability of ground tire
rubber-modified bitumens.” Fuel, 83(14–15), 2041–2049.
Palit, S. K., Sudhakar, K., and Pandey, B. B. (2004). “Laboratory evaluation
of crumb rubber modified asphalt mixes.” J. Mater. Civ. Eng., 16(1),
45–53.
Polacco, G., Stastna, J., Biondi, D., and Zanzotto, L. (2006). “Relation
between polymer architecture and nonlinear viscoelastic behavior
of modified asphalts.” Curr. Opin. Colloid Interface Sci., 11(4),
230–245.
Putman, P. J. (2005). “Quantification of the effects of crumb rubber
in CRM binders.” Ph.D. Dissertation, Dept. of Civil Eng., Clemson
Univ, Clemson, SC.
Shen, J., and Amirkhanian, S. N. (2005). “The influence of crumb rubber
modifier (CRM) microstructures on the high temperature properties of
CRM binders.” Int. J. Pavement Eng., 6(4), 265–271.
Sun, D., and Lu, W. (2003). “Investigation and improvement of storage
stability of SBS modified asphalt.” Petrol. Sci. Tech., 21(5–6),
901–910.
Sun, D., Ye, F., Shi, F., and Lu, W. (2006). “Storage stability of SBS-
modified road asphalt.” Petrol. Sci. Tech., 24(9), 1067–1077.
Way, G. B. (1998). “OGFC meets CRM-where the rubber meets the rubber-
12 years of the durable success.” The Asphalt Conf.
Yildirim, Y. (2007). “Polymer modified asphalt binders.” Constr. Build.
Mater., 21(1), 66–72.
Yu, J., Zeng, X., Wu, S., Wang, L., and Liu, G. (2007). “Preparation
and properties of montmorillonite modified asphalts.” Mater. Sci. Eng.,
444(1–2), 233–238.
Zanzotto, L., and Kennepohl, G. J. (1996). “Development of rubber and
asphalt binders by depolymerization and devulcanization of scrap tires
in asphalt.” TRR 1530, Transportation Research Board, Washington,
DC, 51–58.