Construction and Building Materials 312 (2021) 125405

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Construction and Building Materials

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Analysis and assessment of respirable particles in asphalt pavement

recycling from perspectives of workers’ health
Shicong Mo a, Yuhong Wang a, *, Feng Xiong b, Gengren Hao a, Xingyu Chen a, Ngai Hung Tsang c
a
Dept. of Civil & Environment Engineering, Hong Kong Polytechnic University, Hong Kong, China
b
College of Architecture and Environment, Sichuan University, China
c
Occupational Safety and Health Council, Hong Kong, China

A R T I C L E I N F O A B S T R A C T

Keywords: Different groups of people are exposed to respirable particles in recycling asphalt pavement materials. In eval­
Asphalt pavement resurfacing uating the health issues of such particles posed to construction workers, existing studies mainly focus on
Respirable particles respirable crystalline silica but rarely address the organic fractions. In this study, respirable particles in reclaimed
Organic fractions
asphalt pavement (RAP) materials were collected from different sources and analyzed to determine their
Polycyclic aromatic hydrocarbons
Health assessment
morphology, elemental composition, organic content, and the content and type of polycyclic aromatic hydro­
carbons (PAHs). Focus is placed on the analysis of PAHs in the particles, for which the hazards are assessed using
benzo[a]pyrene toxic equivalent concentration. The respirable particles are found to contain much richer asphalt
content than RAP mixtures. A variety of PAHs can be found in the particles, especially those with a large number
of aromatic rings (>3). Moreover, very old RAP materials contain more PAHs, due to the oxidation reaction of
the hydrocarbons in asphalt binder. Based on the analysis data and reported exposure levels to such particles in
milling asphalt pavements, it is concluded that the health risks posed by such particles cannot be neglected.
Mitigation measures and personal protective equipment are recommended to be used in producing and handling
RAP materials.

1. Introduction hazardous substance that has received wide attention [10,24,39]. In

Highway and street pavements are the most massive civil in­
frastructures on earth. About 90% of the pavements are surfaced with
asphalt materials. As asphalt pavements deteriorate due to cumulative
traffic loading and weathering, pavement surface or the entire pavement
structure needs to be replaced. This process generates a large amount of
wastes. Nowadays, a high percentage of the asphalt pavement wastes are
recycled, creating a material known as reclaimed asphalt pavements
(RAP). Different technologies have been developed to obtain and use
RAP, including cold-in-place recycling [48,65], hot-in-place recycling
[31,68], in-plant recycling [57,58], and full depth reclamation [1].
Extensive recycling brings both environmental and economic benefits.
Asphalt binder in asphalt pavements is an organic material. As
compared with other civil infrastructure materials, a unique character­
istic of asphalt binder is that it typically needs to be heated to very high
temperatures in mixture production and construction [38,52]. The
process generates a large amount of aerosol mist called asphalt fumes—a
contrast, respirable suspended particulates (respirable particles, or
PM10) generated in recycling and using RAP materials receive little
attention, perhaps partially due to the lack of strong odor.
Different groups of people are exposed to respirable particles
generated in asphalt pavement recycling. In producing RAP, existing
pavements are milled and crushed. RAP materials are openly picked up
from the ground and transferred to collection trucks by conveyors on
milling machines. Not only workers near the machines but also pas­
sengers or residents in close proximity are exposed to considerable
amount of respirable particles. RAP materials are subsequently trans­
ported to a mixture production plant where they are stored, sorted, and
fed into new asphalt mixtures. Workers are exposed to the respirable
particles in the plants when transporting and handling the materials. In
the United States (U.S.) alone, more than 100 million tons of old asphalt
pavements need to be milled every year [18]. Approximately 351,120
and 150,860 workers are employed in highway, street, and bridge
construction and in highway maintenance, respectively [59,60]. The

* Corresponding author at: Department of Civil and Environmental Department, The Hong Kong Polytechnic University, 11 Yuk Choi Road, Hung Hom, Kowloon,
Hong Kong, China.
E-mail address: yuhong.wang@polyu.edu.hk (Y. Wang).

https://doi.org/10.1016/j.conbuildmat.2021.125405
Received 16 August 2021; Received in revised form 12 October 2021; Accepted 24 October 2021
Available online 1 November 2021
0950-0618/© 2021 Elsevier Ltd. All rights reserved.
S. Mo et al. Construction and Building Materials 312 (2021) 125405

airway disease, chronic obstructive pulmonary disease and silicosis

Sample collection
Sample preparation
Morphological and Organic fraction PAH analysis
elemental analysis analysis
Health assessment Health assessment
(Carcinogenic risk) (Non-carcinogenic risk)
Fig. 1. Diagram of the experimental and assessment procedure.
impacts of the respirable particles in RAP need to be carefully examined.
Because many types of aggregates used for asphalt mixtures contain
quartz, the airborne particles generated from producing and handling
RAP are often considered as dusts containing respirable crystalline sil­
ica. Freund et al. [13] found that workers’ exposure to respirable par­
ticles during asphalt milling could be more than four times above
background values. A study from the National Institute for Occupational
Safety and Health (NIOSH) showed that workers’ exposure to respirable
quartz could be over seven times the recommended exposure limit [29].
Studies show that exposure to this type of particles increases the risk of
[2,44,45]. Therefore, a Silica/Asphalt Milling Machine Partnership was
established by NIOSH. It advocates adding ventilation controls and a
water spray system to milling machines to prevent the excessive
dispersion of dusts and reduce workers’ exposures [40].
However, respirable particles emitted from RAP also contain organic
compounds from asphalt binder—a highly viscous fluid consisting of
complex hydrocarbons. Depending on the types of asphalt mixtures,
binder content may range from 3% to 7% by weight, with a volume
fraction often greater than 10%. The brittleness of asphalt binder in­
creases significantly with aging. As a result, RAP materials, which
typically have been aged in the field for a long period of time, may
contain significant amount of pulverized asphalt binder. If this is the
case, considering only respirable crystalline silica may seriously un­
derestimate the hazardous potentials of the fine particles in RAP.
Moreover, if aggregates are made from other types of rock such as
limestone, the primary hazard of the respirable particles in RAP may not
be from respirable quartz, but from the fine particles of asphalt binder.
As mentioned before, asphalt fumes generated from hot asphalt binder
are a hazardous substance. In particular, the benzene-soluble fraction
(BSF) and polycyclic aromatic hydrocarbons (PAHs) in asphalt fumes
have been extensively investigated. Positive associations have been
identified between fume exposure and lung function impairment and
between fume exposure and carcinogenic potentials in epidemiological
research [4,5,34,51]. Therefore, the respirable organic particles from
asphalt binder in RAP also likely pose a health risk, but this fraction has
not been well studied.

Fig. 2. Photos of sample preparation for testing: (a) Sample preparation for morphological and elemental analysis; (b) Sample preparation for PAH analysis; (c)
Sample preparation for organic fraction analysis; (d) Sample after benzene solvent evaporation.

2
S. Mo et al.
Table 1
List of RAP materials.
Sample Pavement age (years) Mixture type
SP1 12 SMA
SP2 10 SMA
SP3 – –
SP4 12 WC
SP5 4 SMA
SP6 19 WC
Note: SMA: stone-mastic asphalt; WC: wearing course
To cover the above-mentioned knowledge gap, this study aims to
characterize and assess the respirable particles (PM 10) in RAP—an
increasingly used civil infrastructure material. Focus is placed on the
organic components in the particles. The main objectives of the study
include: (1) to analyze the compositions of the organic and inorganic
fractions of the respirable particles in RAP, (2) to identify and quantify
harmful PAHs in the respirable particles, and (3) to assess the health
effects of the organic fractions of such particles. The study is anticipated
to improve the understanding of the respirable particles in RAP and
assist in the development of mitigation methods and policies.
2. Methods
Steps and methods used for the investigation are shown in Fig. 1.
Respirable particles refer to particular matters with a diameter of 10 µm
or less (PM 10) [61]. Attempts were initially made to collect respirable
particles directly from road construction sites using air pumps, cyclones,
and filter papers in accordance to NIOSH method 0600. Although the
amount of collected samples was adequate to analyze the concentration
of respirable particles in workers’ breathing zones (WBZ), the amount
was inadequate to run chemical analysis. Therefore, instead of using
WBZ samples, effort was made to separate respirable particles directly
from RAP materials. The compositions of respirable particles emitted
from RAP should be the same as the compositions of those particles in
RAP materials. Six types of RAP materials from different sites were
collected to obtain the experimental samples. After samples of respirable
particles were obtained, they were subsequently analyzed using three
approaches: (1) identification of particle morphology and elemental
compositions using scanning electron microscopy (SEM), (2) determi­
nation of benzene soluble organic matter in the particles, and (3)
identification and quantification of PAHs in the samples using gas
chromatography-mass spectrometry (GC–MS). The prepared samples for
testings are shown in Fig. 2. Based on the analysis results, the health risk
of the respirable particles in RAP was assessed from the perspectives of
both carcinogenic risk and non-carcinogenic risk.
Table 1 displays the basic information of the six types of RAP ma­
terials collected from highways in Hong Kong. The original hot-mix
asphalt mixtures from which RAP materials were obtained are
different: Three are gap-graded stone-mastic asphalt (SMA), two are
dense-graded wearing course (WC), and one is unknown. Asphalt binder
used in WC is typically neat asphalt with a penetration grade 60/70, but
either neat asphalt binder or polymer modified asphalt binder can be
used for SMA. Aggregates used in the mixtures are granite. For the five
RAP materials with known mixture types, the service period of the
original pavements varies from 4 years to 19 years.
After the RAP materials were collected, they were separated in the
lab by using standard engineering sieves. The fines (≤0.075 mm) from
RAP were further screened with an 1800-mesh sieve (less than 0.01 mm
in size, or PM10), which ensures that all the passing particles have a
diameter of 10 µm or less. The fine (respirable) particles were stored in a
dark environment at room temperature for analysis.
2.1. Reagents and instruments used for the investigation
A certified standard solution of PAH mix (CRM 47543, TraceCERT®,
3
Construction and Building Materials 312 (2021) 125405
Preparation of standard PAH
solution
Retention time correction by Sample extraction by
Scan mode of GC-MS sonication
Identification of PAHs by SIM
mode of GC-MS
Development of calibration
curves
Calculation of sample
concentration
Fig. 3. The procedure of analyzing PAHs.
lot no. XA26145V) that contains all EAP priority pollutant PAHs, and
acetone and benzene—HPLC grade, were supplied by Supelco (Sigma-
Aldrich, Bellefonte, U.S.). Hexane—HPLC grade, was supplied by Duk­
san Pure Chemicals (Ansan, South Korea). Acetone and hexane were
used as solvents for the respirable fine particles in RAP. Benzene was
used as solvent for separating benzene soluble organics from those
particles in accordance to NIOSH method 5042. The evaporation residue
of the benzene solvent is less than 5 ppm.
Disposable syringes (3 ml, NORM-JECT®, Henke Sass Wolf GMBH,
Tuttlingen, Germany), PTFE syringe filters (0.45 μm, hydrophobic,
Membrane Solutions, Dallas, U.S.), and glass Pasteur pipettes (Brand
GMBH, Wertheim/Main, Germany) were supplied by the Oriental
Chemicals & Lab. Supplies Ltd (Hong Kong, China).
The analytical balance is Sartorius TE1245 (sensitivity 0.1 mg). The
ultrasonic bath is KQ-50D (Kunshan Ultrasonic Instruments Co., Kun­
shan, China). The vacuum degassing oven is Prentex Model 9900 VDO
(Prentex Co., Ltd., America). The GC–MS is Agilent 7890B Gas Chro­
matography with 5977B Single Quadruple Mass Spectrometer (Agilent
Technologies, Palo Alto, U.S.).
2.2. Analysis of morphology and elemental composition
Images and elemental compositions (for qualitative identification) of
the respirable particle samples were obtained by using SEM TESCAN
VEGA3 equipped with energy-dispersive X-ray spectroscopy (EDX).
Samples used for analysis were transferred onto aluminum SEM sample
holders using conductive and adhesive carbon tapes. Voltage for both
image scanning and composition analysis was chosen to be 20 kV.
2.3. Analysis of organic fraction
The following steps were performed to determine benzene soluble
organic matter in the respirable particles in accordance to NIOSH
method 5042. Before use, all the weighing cups were cleaned by acetone
and hexane, respectively, as well as dried in a heating oven and cooled in
ambient temperature. The collected samples were transferred into the
weighing cups and weighed by the analytical balance. Benzene solvent
of 3 ml was added into the weighing cups, which were covered and
placed in an ultrasonic bath and agitated for 20 min. The extracts were
drawn to disposable syringes equipped with a PFTE filter and were
forced through the filters into a new pre-rinsed weighing cup. The new
cup was placed into a vacuum oven preheated to 40 ◦ C for degassing,
where negative pressure in the oven was raised to evaporate the solvent.
S. Mo et al. Construction and Building Materials 312 (2021) 125405

Table 2
PAH compounds, monitored ions by GC–MS SIM mode, and their TEF.
Compounds Abbreviations Ions (m/z) DL (ng/mL)* LOQ (ng/mL)* TEF

Naphthalene NAP 127, 128, 129 0.789 1.936 0.001

Acenaphthylene ACY 150, 151, 152 0.771 1.907 0.001

Acenaphthene ACE 152, 153, 154 0.798 1.993 0.001

Fluorene FLU 163, 165, 166 0.837 2.078 0.001

Phenanthrene PHE 176, 178, 179 0.803 1.992 0.001

Anthracene ANT 176, 178, 179 0.804 1.986 0.01

Fluoranthene FLA 200, 202, 203 0.803 1.989 0.001

Pyrene PYR 200, 202, 203 0.813 2.012 0.001

Benzo(a)anthracene BAN 226, 228, 229 0.801 1.980 0.1

Chrysene CRY 226, 228, 229 0.839 2.088 0.01

Benzo(b)fluoranthene BBF 250, 252, 253 0.802 1.979 0.1

Benzo(k)fluoranthene BKF 250, 252, 253 0.817 2.010 0.1

Benzo(a)pyrene BAP 250, 252, 253 1.959 3.915 1

Indeno(1,2,3-cd)pyrene IND 138, 276, 277 0.997 1.979 1

Dibenzo(a,h)anthracene DBA 276, 278, 279 1.019 2.030 0.1

Benzo(g,h,i)perylene BGP 138, 276, 277 1.004 2.000 0.01

*DL: detection limit; LOQ: limit of quantification

The degassed cup was weighed by the same analytical balance, and
difference between the weight of the degassed cup and the clean cup is
the weight of the benzene-soluble organic fraction.
2.4. Analysis of PAHs
The procedure of analyzing PAHs is shown in Fig. 3. PAHs in the
samples were extracted by a 5-ml mixture of solvent acetone-hexane
(1:1) in weighing cups, which were covered and placed into the bath
for 60-minute sonication treatment. The GC was equipped with an HP5
column (30 m × 0.32 mm diameter and 0.25 μm film thickness). The
injection volumes were 2 μl at splitless mode (purge flow to split vent 20
ml/min at 0.75 min). The carrier gas was helium supplied at a constant
flow of 1.5 ml/min. The details of extraction operations and GC oven
temperature are described in Mo et al. [36].
In order to trace the low concentrations of PAHs in particles, both full
scan mode and selective ion monitoring (SIM) mode in mass spectrom­
etry (MS) were used. The mass spectrum of a standard PAH solution was
recorded in full scan mode at 50–500 m/z to acquire ions for each PAH
compound. Three major ions for each analyte were acquired for further
analysis (Table 2, note that the toxic equivalency factor TEF will be
explained in the next section). The SIM mode was then used to improve
instrument sensitivity for identifying low concentration compounds in
the samples. The dwell time was 10 ms for each ion. Based on the
multiple monitored ions and relative retention time (within ± 0.1 mins)
[54], a particular PAH analyte in the samples was positively identified.

4
S. Mo et al. Construction and Building Materials 312 (2021) 125405

Table 3 where RfD is the estimated daily exposure reference of maximum

Summary of the parameters for calculating ILCR and HQ in respirable particles
permissible risk on humans.
in RAP materials.
EDI in Eq. (3) can be obtained from Eq. (5):
Symbol Indicator variable Unit Value used for Source
calculation (IR × ED × EF)
EDI = × CSBaPeq (5)
AT Average time days 365 × 45 Petit et al. AT × BW
[50]
BW Body weight kg 70 Jiang et al. where the explanations on the factors are shown in Table 3.
[20]
CSF* Inhalation cancer slope kg. 2.51 OEHHA 3. Results and discussion
factor day/ [43]
mg
ED Exposure duration year 45 Petit et al. 3.1. Morphology and elemental compositions of respirable particles
[50]
EF Exposure frequency day/ 250 Petit et al. The surface morphologies of samples obtained by SEM are shown in
year [50] Fig. 4. Fig. 4(a) shows the representative samples in a larger area, while
IR Inhalation rate m3/ 20 Petit et al.
day [50]
Fig. 4(b) and (c) show some morphological features in detail. Although
Rfc Inhalation reference µg/m3 2 × 10− 3
Rostami all the collected particle sizes are supposed to be less than 10 µm (by
concentration of BAP et al. [53] passing the 1800-mesh sieve during sample collection), SEM images
*CSF = 3.9 kg.day/mg from OEHHA [43] were adopted and multiplied by 45/70 indicate that a large number of such particles are greater than 10 µm in
to correspond with typical occupational exposure duration. size. This indicates that the fine particles tend to agglomerate when they
are scraped out of the sample container, likely due to the abundance of
asphalt particles that act as a binding agent. The morphologies of the
For quantitative analysis of each analyte, calibration curves were
particles appear to be heterogeneous: There are some coralloid objects
developed based on the integrated peak area ratio of the target ions for
with open pores (Fig. 4(b)) and some granular objects attached with fine
the diluted standard PAH solutions. The standard PAH solution was
particles. Note that coralloid objects are also reported in pure asphalt
diluted by 1 × 10^4, 2 × 10^4, 5 × 10^4, 1 × 10^5, 2 × 10^5, 5 × 10^5 and 1
binders in existing studies [12,30].
× 10^6 times. The concentrations of PAHs in the samples were calculated
EDS provides qualitative and semi-quantitative information on
based on the linear regressions of calibration curves.
typical elements (Z ≥ 5 except for nitrogen) in the sample [70]. To
ensure the completeness and reliability of the measurements, three in­
2.5. Health risk assessment
dividual areas at different locations of the sample surface were selected
to identify their compositions and average values. The most prevalent
The concept of benzo[a]pyrene toxic equivalent concentration
identifiable elements in the samples seem to be carbon and oxygen
(BaPeq) was used to assess the carcinogenic and non-carcinogenic risks
(Fig. 5). Fig. 5(a) corresponds to the particle in Fig. 4(b) while Fig. 5(b)
of the respirable particles [6,32,53]. Based on the values of BaPeq, the
corresponds to the one in Fig. 4(c). In Fig. 5(a) and (b), the ratio between
carcinogenic risk can be estimated by the incremental lifetime cancer
carbon and oxygen is 8.93 and 1.04, respectively, indicating that carbon
risk (ILCR) models, while the non-carcinogenic health risk can be
is more dominating in the particle in Fig. 4(b). For the sample shown in
calculated by the hazard quotient (HQ) index. As suggested by Nisbet
Fig. 4(c), there are more and heterogeneous types of elements including
and Lagoy [41], the PAH concentrations were converted to BaPeq con­
carbon, oxygen, calcium, silicon, aluminum, potassium, oxygen, and
centrations by multiplying the TEF shown in Table 2. It is assumed that
others.
the PAH species BAP has the effective potency of 1 since it is a proven
However, some elements in Fig. 5 are uncommon in either asphalt
human carcinogen. The toxicity of other compounds is based on their
binder or granite aggregate, including chlorine and chromium. A num­
hazardous potentials as compared to BAP. The BaPeq concentrations of
ber of researchers found that dust particles in marine atmosphere likely
all the identified PAHs are calculated by Eq. (1).
adsorb chlorine-containing particles and gases [21,69]. This may
∑
n
explain the source of chlorine in the EDX results. As for chromium (Cr),
CSBaPeq = (Ci × TEF) (1)
i=1
existing studies suggest that Cr in urban asphalt pavements is mostly
traced to vehicular traffic, including wearing of engine parts, vehicle
Where Ci is the concentration of each PAH. The risk calculation criterion body and tires. Continuous low-level exposure to hexavalent Cr is con­
suggested by [62] was followed: If the measured values are less than the cerned by researchers because of its toxicity [11,47,72].
DL and LOQ, they are replaced by DL/2 and LOQ/2, respectively. The results above suggest that the respirable particles may contain
ILCR from respirable particles due to occupational exposure can be hazardous substances from several sources—hydrocarbons in asphalt
determined by Eq (2) [9,19,56,66]. binder, respirable quartz from granite aggregate, and heavy metals from
√̅̅̅̅̅ vehicular traffic. This paper is only focused on polycyclic aromatic hy­
CSF × 3 BW × EF × ED × IR drocarbons (PAHs) in the particles, the other pollutant types may be
(2)
70
RInhalation =
BW × AT
× CSBaPeq × cf addressed in future studies.

Where cf is the conversion factor (10− 6), and other parameters used for
3.2. Organic component fractions in the respirable particles
the calculations are shown in Table 3. Note that EF, ED and IR in Table 3
are modified based on typical occupational exposures [50].
Benzene-soluble fraction (BSF) represents the total asphalt-related
The HQ was calculated based on the ratio between the concentration
organic matters in the collected samples. In asphalt fume studies and
of estimated daily intake (EDI) to the reference dose (RfD) using Eqs. (3)
monitoring, BSF is an interested indicator in assessing the hazardous
and (4) [53]:
potentials of fumes [17,37]. Similarly, in this study, it provides impor­
EDI tant information on the proportion of hazardous organic components in
HQ = (3)
RfD × 1000 the respirable particles. Fig. 2(d) shows an image of the BSF of the
collected sample after the solvent has been evaporated. The brown-
RfD =
Rfc × IR
(4) colored residual is asphalt binder from the sample. The BSFs of all the
BW samples were determined and shown in Fig. 6, which indicates that the

5
S. Mo et al.
Fig. 4. SEM images of collected respirable particles from RAP materials.
BSF ranges from 9.37% to 12.29%. Conversely, asphalt mixtures typi­
cally have an asphalt binder content of 3–7%. Therefore, asphalt binders
in the collected respirable particles are approximately two times of that
in a typical asphalt mixture.
The results imply that asphalt binder in asphalt mixtures is more
easily broken into small pieces in milling asphalt pavements. This is
likely due to two reasons. Firstly, asphalt binder is much weaker than
aggregate. Secondly, as asphalt binder ages in field pavements, it be­
comes more brittle and friable. The increased organic components in the
6
Construction and Building Materials 312 (2021) 125405
respirable particles from RAP as compared with the entire mixture
obviously pose a health concern.
3.3. Identification of the PAH compounds
The organic fractions of the respirable particles in RAP contain
various hazardous substances inherited from asphalt binder. Complete
separation of all the chemical species in the asphalt binder is impossible
[28,67]. Therefore, only PAH compounds in the organic fractions of the
S. Mo et al. Construction and Building Materials 312 (2021) 125405

shown in the figures, a variety of PAHs can be identified in the sample.

Similarly, PAHs in the other samples are identified, and all the results
are summarized in Table 4. The following observations can be made
from the table.

(1) Each sample contains at least 5 types of PAHs, with the largest
number being 11 (sample SP6). The types of PAHs detected in
these samples are also different. In fact, none of the samples
contain the same set of detected PAHs.
(2) Three PAHs—PHE, PYR and BKF—are present in all the samples,
despite differences in original mixture types and service ages.
(3) Unlike asphalt fumes, which have more types of PAHs with 2
rings [22,27], the types of PAHs in these particles consist of more
components with 3–6 rings. Note that asphalt fumes are emitted
in a hot environment, while the fine particles in this research are
generated at atmospheric temperature. Temperature difference
affects the types of PAHs detected in asphalt fumes and fine
particles. According to Table 2, increase in the number of rings
generally makes the PAHs more hazardous.
(4) BAP and IND—the most hazardous types of PAHs in Table 2 are
not detected; however, BKF is in all the samples. The hazardous
potentials of BKF are widely recognized [64].

3.4. Quantitative analysis of PAHs in the respirable particles

Figure 9 shows the total concentrations of all the detected PAHs in

the respirable particles in each sample. The figure indicates that the total
PAH concentration in sample SP6 is approximately 6 times of the con­
centration in sample SP2, which had the second highest PAH concen­
Fig. 5. EDX results corresponding to (a) Fig. 4(b) and (b) Fig. 4(c).
tration of all samples. As shown in Table 1, SP6 is obtained from a
pavement of the longest service time—19 years. Asphalt binder is sub­
ject to oxidative aging in field pavements, and PAHs have been found to
be a product of the asphalt oxidation process [49]. Similar increases in
PAHs are found in asphalt fumes collected from aged asphalt mixtures as
compared with non-aged ones [36]. Therefore, the hazardous potentials
of respirable particles in RAP likely increase with the aging severity of
RAP.
PAHs are often divided into two groups according to the number of
aromatic rings [16,25,33]. Workers exposed to asphalt fumes are more
likely exposed to PAHs with fewer rings (≤3 rings) by approximately
7–100 times [7,8,22,23,27]. In contrast, as shown in Fig. 10, the PAHs
with more rings range from 30% to almost 70% in these samples. The
results indicate that the chemical features of organic components in
RAP’s fine particles are quite different from those in asphalt fumes. This
is understandable as the organic fractions in asphalt fumes are emitted in
vapor or aerosol phases at high temperatures while those in the respi­
rable particles collected in this study are essentially solid asphalt binders
at ambiet temperatures. In addition, PAHs with fewer rings are more
easily escaped in asphalt pavements after long-term road use.
Ratios between the total amount of quantified PAHs in each sample
and the total organic matter in respirable particles are shown in Fig. 11,
which provides a general indication of the concentration of quantifiable
PAHs in the organic fractions of fine particles. In Fig. 11, the ratios range
from 0.002% to 0.087%. As a comparison, the ratio between PAHs and
total organic matter in asphalt fumes generated from hot-mix asphalt
Fig. 6. Organic and inorganic fractions in the collected samples (n = 6) and in a
paving ranges from 0.103% to 0.241% [7]. Therefore, the PAH ratios for
typical asphalt mixture (AME).
respirable particles in RAP are much lower. This is understandable as the
organic components in fine particles in this study are essentially asphalt
particles are studied in detail. For illustration purpose, the gas chro­
binder, which mainly consists of heterogeneous organic molecules of
matography (GC) chromatograms of the standard PAH solution (diluted
large molecular size. Nevertheless, a relatively high concentration of
by 1 × 104 times) and one sample (SP2) are shown in Figs. 7 and 8,
PAHs can be found in sample SP6. As discussed before, PAHs can be
respectively. Specific analytes in the extracts are positively identified
generated in asphalt binder due to the oxidative reactions of hydro­
when the retention time of the target ion of the suspected PAH com­
aromatics [49]. The longer pavement is in service, the higher concen­
pound is within ± 0.1 min of the retention time of the monitored ion
tration of PAHs will be present in asphalt binder, making the respirable
from the reference chromatograph of the corresponding PAH [54]. As
particles more hazardous.

7
S. Mo et al. Construction and Building Materials 312 (2021) 125405

Fig. 7. GC-chromatography of target ions in the standard mixture solutions of EPA 16 PAHs used as a reference: 1. NAP, 2. ACY, 3. ACE, 4. FLU, 5. PHE, 6. ANT, 7.
FLA, 8. PYR, 9. BAN, 10 CRY, 11. BBF, 12. BKF, 13. BAP, 14 IND, 15. DBA, 16. BGP.

Fig. 8. GC-chromatograph of monitored ions from particles of one sample (SP2) (the numbers correspond to the labels in Fig. 7).

3.5. Occupational exposure risk assessment

Table 4
The detected PAHs in the samples. The mean BaPeq concentrations (CSBaPeq) of all the identified PAHs
Compounds Sample from the collected samples are calculated to be 0.722 ng/mg. In this
study, the respirable particles were obtained from bulk RAP materials,
SP1 SP2 SP3 SP4 SP5 SP6
instead of workers’ or pedestrians’ breathing zones. Therefore, the in­
2-ring PAHs
cremental lifetime cancer risk (ILCR) cannot be directly calculated.
NAP ✓ ✓ ✓
ACY ✓ ✓ ✓
However, as mentioned previously, NIOSH performed extensive
FLU ✓ ✓ ✓ research on dust generated from pavement milling, including several in-
depth surveys concerning the concentrations of respirable particles to
3-ring PAHs
PHE ✓ ✓ ✓ ✓ ✓ ✓ which workers are exposed at different workplaces near a milling ma­
ANT ✓ ✓ ✓ chine [3,15]. It was found that the concentrations mostly range from
FLA ✓ ✓ ✓ ✓ ✓ approximately 1 mg/m3 to around 3 mg/m3.
≥4-ring PAHs In general, a time-weighted average (TWA) value is used to assess
PYR ✓ ✓ ✓ ✓ ✓ ✓ occupational exposure to hazardous contaminants or agents at the
BAN ✓ ✓ workplace over a specified period—usually a nominal 8-hour per day or
CRY ✓ ✓ ✓ ✓
40-hour per week. Therefore, when workers are exposed to the respi­
BBF
rable particles in RAP materials from 1 mg/m3 to 3 mg/m3 during their
✓ ✓
BKF ✓ ✓ ✓ ✓ ✓ ✓
BGP ✓ ✓ typical working periods, the corresponding ILCR values can be calcu­
Total 5 10 7 7 5 11 lated, as shown in Table 5. Note that these numbers are only applicable
to workers involved in pavement milling operations. The pedestrians’
exposures near a milling site are expected to be less, while the exposures
of those workers who handle RAP materials in a plant are unknown.
Different agencies and governments have provided thresholds for

8
S. Mo et al.
Fig. 9. Total quantified PAH concentrations (n = 3) in the respirable particles
(ng/mg).
Fig. 10. Total quantified PAH concentrations according to the number of ar­
omatic rings.
ILCR, and the one provided by [42] is widely adopted by many re­
searchers [32,50,55,71]. According to the threshold by NYS DOH, an
ILCR value less than 10-6 indicates a very low risk for cancer. An esti­
mated ILCR between 10− 6 and 10− 4 indicates potential risk. As shown in
Table 5, when the TWA exposure to respirable particles is no less than 3
mg/m3, workers will face potential carcinogenic risks. However, two
limits of this assessment need to be recognized. Firstly, the average
BaPeq concentration is used for evaluation, while the actual PAH con­
centrations may vary greatly between RAP. Secondly, respirable quartz
in dust is not considered.
Hazard quotient (HQ) values were also calculated based on the same
assumptions of average BaPeq concentration and the concentrations of
9
Construction and Building Materials 312 (2021) 125405
Fig. 11. Ratios between the total amount of quantified PAHs and the total
organic fractions.
Table 5
The ILCR and the HQ related to PAH concentrations
Assumed concentrations of respirable particles
1 mg/m3 2 mg/m3 3 mg/m3
− 7 − 7 6
ILCR 3.546 × 10 7.093 × 10 1.064 × 10−
HQ 0.865 1.731 2.596
respirable particles in the air. HQ values greater than 1 suggest that
adverse non-carcinogenic hazard is high, and values less than or equal to
1 indicate an acceptable hazard level [63]. As shown in the Table 5,
when the TWA exposure to respirable particles is more than 2 mg/m3,
the HQ will be greater than 1.73, indicating a high risk.
OSHA [46] has a permissible exposure limit (PEL) of 5 mg/m3 for
respirable particulates (8-h TWA). The ILCR and HQ results calculated
above indicate that this threshold may not be conservative in protecting
workers from the harmful effects of respirable particles generated during
asphalt pavement milling operations. The main reason is that the fine
particles in RAP contain PAHs. PAHs can not only increase DNA adducts
that lead to mutagenic activities but also induce serious non-
carcinogenic health effects, including but not limited to cardiovascular
and pulmonary disease, jaundice, kidney and liver damage, and lung
failure [14,26,35]. Therefore, more attention needs to be paid to these
unique fine particles, and it is important to develop proactive mitigation
measures and mandate the use of personal protective equipment to
reduce workplace-related exposures.
4. Summary and conclusions
RAP materials are commonly evaluated for their engineering prop­
erties. Even though the health effects of fine particles in RAP materials
received some attention, existing studies only focus on respirable silica
in the fine particles. The organic components in the respirable particles
are seldom investigated. In this research, respirable particles from six
types of RAP materials were collected and studied in detail, including
morphology and elemental compositions, content of organic fractions,
and PAH compounds in the organic fractions. Focus was placed on the
identification of the PAH compounds in the organic fractions. Based on
S. Mo et al.
the analysis results and particle concentration data reported in litera­
ture, carcinogenic and noncarcinogenic risks were assessed for workers
near pavement milling machines during construction, but risks of other
exposed groups were not evaluated due to lack of exposure data.
SEM analysis results suggest that these particles have morphological
features that are related to binder and aggregate in RAP and contain
heterogeneous elements that can be traced back to material source,
environmental exposure, and road use. The contents of the total
benzene-soluble organic matter in the particles range from slightly less
than 10% to 12%, approximately twice of the asphalt binder content in
the original asphalt mixtures. GC–MS analysis results suggest that
several types of PAH can be positively identified in the organic fraction
of the respirable particles, and the identified PAHs vary greatly in types
and concentrations among the samples. The total number of identified
PAHs ranges from 5 to 11, and the concentration ranges from approxi­
mately 2 ng/mg to less than 100 ng/mg. As compared with PAHs widely
reported in asphalt fume studies, the PAHs identified in those respirable
particles contain more aromatic rings. Moreover, RAP from very old
pavements likely contain more PAHs, especially those with more aro­
matic rings. Based on hazard assessment criteria and sampling data re­
ported in existing literature and the analysis results from this study, it is
believed that workers near milling machines and handling RAP mate­
rials face non-negligible risks if not protected. The purpose of this study
is not against the use of RAP. Instead, this study calls for attention to a
source of hazard that is often neglected in existing health assessment
studies—the organic portions of respirable particles in producing and
handling RAP. Mitigation measures and personnel protective equipment
are recommended to be used to reduce such risks.
CRediT authorship contribution statement
Shicong Mo: Data curation, Investigation, Writing – original draft.
Yuhong Wang: Conceptualization, Methodology, Writing – review &
editing, Supervision, Validation, Funding acquisition. Feng Xiong: Su­
pervision. Gengren Hao: Resources. Xingyu Chen: Resources. Ngai
Hung Tsang: Resources.
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
This paper is based on the research project (Project No. PolyU PolyU
152568/16E) funded by the Research Grant Council of Hong Kong
Special Administrative Region Government and the Occupational Safety
and Health Council of Hong Kong (Project Number: K-ZB84).
Disclaimer
The opinions expressed in this paper are those of the authors and do
not necessarily reflect the views or policies of the Government of the
Hong Kong Special Administrative Region, nor does mention of trade
names or commercial products constitute an endorsement or recom­
mendation of their use.
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