Experimental analysis of the evaporation process for gasoline

Ling Zhu
a,
*
, Jiaqing Chen
a
, Yan Liu
a
, Rongmei Geng
a
, Junjie Yu
b
a
Department of Environmental Engineering, Beijing Institute of Petrochemical Technology, 19 QingYuan North Road, Beijing 102617, PR China
b
Policy Research Center for Environment and Economy, Ministry of Environmental Protection, Beijing 100029, PR China
a r t i c l e i n f o
Article history:
Received 13 January 2012
Received in revised form
5 May 2012
Accepted 5 May 2012
Keywords:
Gasoline evaporation process
Gasoline weight loss
Viscosity
RVP
NMHC
Gasoline volatility
a b s t r a c t
This paper presents the ndings from a study on the evaporation process of 93 RON (research octane
number) unleaded gasoline. The parameters measured in the experiment included the weight, the RVP
(Reid vapor pressure) and the viscosity of gasoline, the concentration of NMHC (non-methane total
hydrocarbon) in the oil vapor and the concentration of the main vapor constituent. Results showed that
the parameters changed signicantly as evaporation processed. The weight loss reached 86.36% after 300
days and presented a logarithmic curve with time. The RVP decreased from 38 kPa to 9.6 kPa. The
viscosity of gasoline increased from 8.6 10
4
Pa s to 1.51 10
3
Pa s. All the concentrations of NMHC
and the main constituent of vapor decreased in varying amounts. Most of the changes might be
attributed to the evaporation of volatile hydrocarbons.
2012 Elsevier Ltd. All rights reserved.
1. Introduction
Gasoline is a complex mixture containing hundreds of different
hydrocarbons derived fromthe distillation of petroleum. Due to the
strong volatile properties of most hydrocarbons, volatile organic
compounds (VOCs) and hazardous air pollutants (HAP) are emitted
during major gasoline transfer operations. In general, gasoline
needs to be loaded and unloaded at least 5 times from renery to
vehicle gas tanks, including production process in renery, trans-
portation to the fuel depot, loading and unloading at fuel depot and
oil station, and refueling of the vehicles. Due to its powerful vola-
tility and wide applications, gasoline vapor emissions can cause
serious gaseous pollution, especially, photochemical smog in
summer, and VOCs that serve as ozone precursors and contribute to
ground-level ozone. The primary harmful effects of gasoline vapor
emissions are the waste of energy resources and the relevant
economic losses. According to the national statistic bulletin of
China, the annual oil consumption of China in 2010 was approxi-
mately 2.46 billion tons and gasoline consumption was approxi-
mately 0.712 billion tons (NBSC, 2011). In a research report from
Beijing municipal research institute of environmental protection,
the emission factor of gasoline in an oil station could reach 2.30 kg/t
if there was no control technology. Of course, the actual loss was far
less than that because approximately 90% of gasoline evaporation
losses come from storage, loading and unloading operations of
tanks, which have been reduced by replacing xed-roof tanks with
internal oating-roof tanks since the late 1970s. Meanwhile, from
the late 1980s onwards, some oil vapor recovery systems have also
been applied in reneries, gasoline depots and service stations.
Therefore, it was estimated that the relevant annual economic loss
from gasoline evaporation in oil stations would exceed 20 billion
(RMB) in 2009 (Weiqiu, Juan, Shuhua, & Aihua, 2011).
Since the 1970s, many effective oil vapor recovery systems have
been widely used in reneries, gasoline depots and service stations
to reduce vapor emissions, such as Stage I systems, Stage II systems,
EVR systems and ORVR systems, and others. Some of these disposal
systems were certied by CARB and EVR (USA), TUV (Germany) and
others (http: //www.arb.ca.gov/homepage.htm). Many papers have
investigated the operation processes and industrial designs of these
systems (Ravanchi, Kaghazchi, & Kargari, 2009).
However, papers published on the gasoline evaporation process
are comparatively rare. Fingas M. studied the relationship between
the evaporation rate of petroleum products and related inuencing
factors, including sample weight, water concentration, held time
and wind velocity (Fingas, 2004). Fingas claried empirically that
oil products evaporated at a logarithmic rate with respect to time
and presented a simple model for predicting the weight loss frac-
tion considering different temperatures. However, oil evaporation
was not strictly regulated by boundary layer because oil evapora-
tion rates were found to be largely governed by temperature, time,
distillation data and the number of components (Fingas, 1997).
Katsuhiro O. examined changes of vapor properties for motor
gasoline during evaporation (Okamoto, Watanabe, Hagimoto,
Miwa, & Ohtani, 2009). The changes in vapor pressure and the
* Corresponding author. Tel.: 86 10 81294271; fax: 86 10 81292291.
E-mail addresses: zhuling75@bipt.edu.cn, zhuling7519@163.com (L. Zhu).
Contents lists available at SciVerse ScienceDirect
Journal of Loss Prevention in the Process Industries
j ournal homepage: www. el sevi er. com/ l ocat e/ j l p
0950-4230/$ e see front matter 2012 Elsevier Ltd. All rights reserved.
doi:10.1016/j.jlp.2012.05.002
Journal of Loss Prevention in the Process Industries 25 (2012) 916e922
evaporation rate of gasoline could be expressed as the exponential
of weight loss fraction. The prediction model for the amount of
gasoline vapor was independent of the evaporative area and the
amount of gasoline. An oil spill is another important means of oil
loss and oil evaporation. Fingas M. developed a series of models to
calculate the evaporation rate under different evaporation condi-
tions, such as the thickness of spill, the spill area, and the amount of
spill; however, this model cannot be applied to predict the amount
of gasoline vapor under different evaporation conditions because it
is an empirical model under the limited conditions (Fingas, 1998).
Shiyou Y. used the DCMC (discrete/continuous multicomponent)
model to investigate the properties and composition of realistic
multicomponent gasoline fuels, and gasoline is assumed to consist
of ve families of hydrocarbons (Shiyou, Youngchul, & Rolf, 2010).
Temerdashev Z. A. detected the trace of gasoline after evaporation
and burning, especially the composition of aromatic compounds
(Temerdashev & Kolychev, 2009). Cagliari J. monitored the
concentration of monoaromatic compounds from gasoline-
ethanol-blend fuels in laboratory sand columns during 77 days.
They found that although the content of benzene, toluene and
xylenes did not show regular change, but ethanol content had
different inuence on the concentration change of the three
compounds (Cagliari, Fedrizzi, Finotti, Teixeira, & Filho, 2010).
The above studies did not conduct a comprehensive test on the
changes in the physical properties of gasoline and vapor during the
evaporation process, which includes not only weight and pressure
of gasoline but also the NMHC value and the main vapor content
concentration of gasoline vapor. These physical properties are very
important to select a suitable purication system, to adjust the
operational parameters, and to ensure satisfactory efciencies of
recover oil vapor. Therefore, in this study, the major parameters of
liquid gasoline and gaseous vapor were measured in a continuous
evaporation process.
2. Experimental
2.1. Preparation of measured samples
Oil used in this study was 93 Research Octane Number (RON)
unleaded gasoline, purchased from China Petroleum Chemical
Corporation (CPCC) service station. Gasoline was placed in the glass
container and left open to the atmosphere under roomtemperature
to simulate the big breathing loss during the gasoline transfer
operations. The evaporation process was investigated by testing the
parameters of liquid gasoline and gaseous vapor in the container.
About 43 g liquid gasoline was transferred to a weighing bottle.
The total weight of bottle and gasoline was continually tested
during 300 days to investigate the weight change during the course
of evaporation.
Approximate 200 mL gasoline was poured into a 500 mL conical
ask. An air-tight seal syringe with a Luer lockout valve (10 mL,
Agilent) was selected as the sampler to extract oil vapor above
gasoline in the conical ask. The NMHC concentration of gasoline
vapor was measured by gas chromatogram. This test lasted 30 days.
Thirty conical asks (250 mL) with about 100 mL gasoline were
prepared in this experiment. Gasoline used to detect the Reid vapor
pressure (RVP) and the viscosity was obtained from one of the
conical asks, and this test lasted 30 days.
2.2. Gasoline weight measurement
The evaporation rate was measured by the weight loss using an
electronic balance (AL 104 Mettler) with an accuracy of 0.001 g. The
weight loss fraction a is given by Equation (1).
a
w
0
w
w
0
w
b
(1)
Here, w
0
is the initial weight of gasoline and bottle; w is the
weight of the gasoline at the time of detection, w
b
is the weight of
bottle.
2.3. Reid vapor pressure measurement
The Reid vapor pressure (RVP), as determined by the ASTM test
method D323 (Ministry of Petroleum Industry Research Institute,
1982), is widely used in petroleum industry to measure the vola-
tility of petroleum crude oil, gasoline and other petroleum prod-
ucts. It is a quick and simple method of determining the vapor
pressure at 37.8

C (100

F) for crude oil and petroleum products
which have an initial boiling point above 0

C (32

F).
The RVP of the gasoline samples was measured at 37.8

C using
an automated vapor pressure tester (ABH-1, Xufeng Scientic Ltd).
The test was performed based on China standard method GB 257-
64 (Ministry of Petroleum Industry Research Institute, 1982). A
sample cylinder bath with 30 mL of gasoline was submerged in
a water bath and was maintained at a predetermined temperature
(37.8 0.1

C). The cylinder was shaken in the water bath until the
gasoline inside the cylinder reached a constant and balanced state,
and then, the pressure in the cylinder was measured as the vapor
pressure of gasoline.
2.4. Vapor measurement of NMHC
The non-methane total hydrocarbon (NMHC) of vapor was
tested and calculated using GC 6890 (Agilent) with two FID
detectors. The test was performed based on China standard method
HJ/T38-1999 (State Environmental Protection Administration,
1999).
A stainless steel packed column (1 m 3 mm inner diameter),
lled with silylanization micro glass beads, was connected to the
front FID detector to measure the concentration of total hydro-
carbon. Another stainless steel packed column (3 m 3 mm inner
diameter), lled with GDX-104 (porous polymer beads) with
a 60e80 mesh particle size, was connected to the back FID detector
to measure the concentration of CH
4
. The concentration of NMHC
was calculated from the two different columns.
Splitless injection of a 0.1 mL sample was conducted with an
auto-sampler, and the injector temperature was 120

C. The GC
oven and detector temperature were 80

C and 300

C, respectively.
The ow rate of N
2
, the carrier gas, was 30 mL/min, and those of H
2
and air were 25 mL/min and 300 mL/min, respectively.
A standard gas containing CH
4
/N
2
(0.149% V/V) was used to
measure the concentration of NMHC. Quantization was performed
using the ve-point calibration curve for individual components.
2.5. Concentration measurements of the main vapor content
Samples were analyzed using 7890A gas chromatograph (Agi-
lent) with two FID detectors. An HP-5 silica-fused capillary column
(30 m 0.32 mm inner diameter 0.25 mm lm thickness) and an
Al
2
O
3
silica-fused capillary column (30 m 0.53 mm inner
diameter 0.25 mm lm thickness) were used to separate the
hydrocarbon components and the aromatic hydrocarbon compo-
nents, respectively.
Splitless injection of a 1 mL sample was conducted with an auto-
sampler, and nitrogen was used as the carrier gas at a constant ow
rate of 25 mL/min. The GC oven temperature was programmed at
45

C held for 2 min, followed by an increase to 160

C at a rate of
L. Zhu et al. / Journal of Loss Prevention in the Process Industries 25 (2012) 916e922 917
5

C/min and then to 250

C at 20

C/min (held for 5 min). The
injector and detector temperatures were 250

C and 230

C,
respectively. Compounds were identied by their retention times.
Quantization was performed using the ve-point calibration curve
for the individual components.
The standard gas containing 24 organic compounds was used
for quantication. Calibration curves including ve different
concentrations were constructed using the internal standard
method (Zhendi & Fingas, 1997; Zhendi, Fingas, & Page, 1999).
2.6. Gasoline viscosity measurement
Viscosity is used to indicate the friction resistance between
molecules in uid ow and also reects the uidity of the oil.
Therefore, it is a common parameter for oil quality standards.
The kinematic viscosity of gasoline was tested by a rotational
viscometer (RV1, HAAKE, Ltd.) in the range of 100 r/mine600 r/min
at 20

C.
3. Results and discussion
3.1. Gasoline weight loss
Fig. 1 shows the weight change for gasoline evaporation over
300 testing days. The weight of gasoline in the bottles gradually
decreased from 42.7155 g to 5.8265 g, and the cumulative fraction
of weight loss was 86.36%.
In this study, gasoline and the surrounding atmosphere formed
a larger space for volatile diffusion. The light hydrocarbons of
gasoline were easy to evaporate, while the heavy hydrocarbon
components, which have higher boiling points, were not as easy to
volatilize at room temperature. Therefore, the light hydrocarbons
evaporated into the air continually, while their content in gasoline
declined. As a result, the rate of weight loss became slowly, and it
can be predicted that the gasoline weight in the bottle would tend
to stabilize at the end of the process.
Fig. 2 shows photos for the initial gasoline and the sample after
300 days, and several obvious changes can be seen. First, the change
in gasoline volume was signicant. Initially, 70% of the space in the
weighing bottle was occupied in Fig. 2(a), but only the bottom of
the bottle was covered by gasoline after 300 days in Fig. 2(b). The
reduction in volume can be attributed to the volatilization of the
hydrocarbons. Second, the color of the gasoline changed fromfaint-
yellow to dark-brown, which is similar to the typical color of heavy
fuel oil (HFO), and the uidity was also modied. Furthermore,
proof of gasoline evaporation could be found at the bottleneck of
the bottle in Fig. 2(b), where the residue of the gasoline vapor
aggregated and a brown membrane was produced on the surface of
the bottleneck. The above changes all resulted from a decrease in
the concentration of the volatile hydrocarbons in the gasoline,
which is in accordance with the results of the weight experiment.
Fig. 3 shows the evaporation rate of gasoline calculated from
Fig. 1. Curve tting is also shown to describe the relationships
between a set of data in terms of the best-t equations.
In Fig. 3, a logarithmic equation t the data best for the evapo-
ration rate, with a regression coefcient R
2
of 0.9786. The result is
also in accordance with Fingas reports (Fingas, 1996). The rate of
gasoline evaporation, which consists of several volatile organic
compounds, follows in a logarithmic manner, and therefore, the
0 30 60 90 120 150 180 210 240 270 300
5
10
15
20
25
30
35
40
45
W
e
i
g
h
t

(
g
)
Time (day)

Fig. 1. Weight of gasoline vs. time.
Fig. 2. Photos for the samples: (a) origin, (b) 300 days after.
y = 16.773ln(x) - 10.436
R = 0.9786
0
20
40
60
80
100
0 50 100 150 200 250 300
E
v
a
p
o
r
a
t
e
d

F
r
a
c
t
i
o
n
(
%
)
Time (d)
Fig. 3. Logarithmic curve t to oil evaporation date.
L. Zhu et al. / Journal of Loss Prevention in the Process Industries 25 (2012) 916e922 918
loss of mass is also approximately logarithmic with time. This kind
of behavior is due to the number of components evaporating at
once, each of which has linear evaporation behavior. The envelope
of these linear rates results in a logarithmic curve, especially when
approximately 7 or more components evaporate simultaneously.
3.2. Gasoline Reid vapor pressure
The Reid vapor pressure of the gasoline sample varied with time
as shown in Fig. 4.
At any given temperature, the liquid gasoline is in equilibriumin
the fuel vapor. The pressure generated by the gasoline vapor is
called the saturated vapor pressure, which is one of the main
quality parameters and can be used to evaluate the weight loss
during the course of storage and transportation. In this study, the
PVR was adopted to characterize the saturated vapor pressure. In
Fig. 4, the values of PVR show a downward trend, decreasing from
38 kPa to 9.6 kPa over time.
Gasoline is a complex mixture of various hydrocarbons; there-
fore, the total vapor pressure cannot be calculated using the
DaltoneRaoult equation. However, according to the
ClapeyroneClausius equation, the vapor pressure can be described
as a function of temperature and composition. Normally, the
composition of gasoline changes with the penetration rates, and
the hydrocarbon components with low boiling points are easy to
volatilize and gasify, resulting in an increase in the content of heavy
hydrocarbons and a decrease in the vapor pressure.
Gasoline with a higher RVP indicates that it gasies more easily
and contains a larger amount of light hydrocarbons. As a result,
gasoline can be mixed with air more evenly, and the mixture may
achieve a more complete combustion in the cylinder. Therefore, the
higher RVP can ensure a normal combustion of gasoline, and the
combustion has the advantages of a low ignition temperature, fast
combustion speed, high combustion efciency and low fuel
consumption. But from the perspective of value, this kind of
gasoline is not suitable for storage over longer periods.
3.3. Gasoline viscosity measurement
Fig. 5 presents the change in viscosity for gasoline over 30
experimental days. Throughout the testing process, the curve did
not follow a clear trend, but it did display upward trends with the
changing slopes. The viscosity of the gasoline increased from
8.6 10
4
Pa s to 1.51 10
3
Pa s.
The main factors affecting gasoline viscosity include chemical
composition, molecular weight, temperature and pressure. More-
over, viscosity is one of the physical parameters describing the
friction between liquid molecules, and therefore, it is closely
related to the chemical composition of the gasoline. Normally,
when hydrocarbons have the same number of carbon atoms, their
viscosities are arranged in the following order:
alkanes < isoparafn < aromatic hydrocarbons < cycloalkanes. In
other words, when the molecular weights are similar, the viscosity
of hydrocarbons with ring structures is greater than that of those
with a chain structure, and a greater number of rings mean
a greater viscosity. When the hydrocarbons have the same ring
number, the longer the side-chain is, the larger is the viscosity. For
these reasons, after evaporation for a fewdays, the concentration of
heavy hydrocarbons with larger molecular weights in gasoline
increased. For the same series of hydrocarbons, with an increasing
hydrocarbon molecular weight, the attraction between molecules
strengthened; therefore, the viscosity increased approximately 1.75
times under the open evaporation test.
3.4. NMHC concentration of the gasoline vapor
Gasoline evaporation can be divided into static evaporation and
dynamic evaporation. When gasoline is in a dynamic state, it
0 5 10 15 20 25 30
8
12
16
20
24
28
32
36
40
R
e
i
d

v
a
p
o
r

p
r
e
s
s
u
r
e
(
k
P
a
)
Time (d)

Fig. 4. Reid vapor pressure (RVP) of gasoline vs. time.
0 5 10 15 20 25 30
0.0009
0.0010
0.0011
0.0012
0.0013
0.0014
0.0015
V
e
r
c
o
s
i
t
y

(
P
a
s
)
Time (d)

Fig. 5. Viscosity of gasoline vs. time.
0 5 10 15 20 25 30
0
5
10
15
20
25
30
35
C
M
N
H
C
%

(
V
/
V
)
Time (d)

Fig. 6. Concentration of non-methane total hydrocarbon (NMHC) of gasoline vapor vs.
time.
L. Zhu et al. / Journal of Loss Prevention in the Process Industries 25 (2012) 916e922 919
disperses to ne particles along the owof air and evaporates to the
surrounding atmosphere. When gasoline in the container remains
in a quiet state and the gas above the liquid surface does not ow,
the evaporation would be considered to be static evaporation.
Temperature differences between inside and outside of the
container are the main cause of evaporation, which is also dened
as small breathing losses. This kind of loss is very common during
gasoline storage.
The NMHC concentration of gasoline vapor is an important
indicator to evaluate the air pollution near oil stations and oil
depots and is also a major factor to evaluate the quality of gasoline.
An experiment was performed to test the concentration changes in
NMHC for the gasoline vapor over a month, and the result is shown
in Fig. 6. The concentration was reduced from 34.7378% (V/V) to
2.8207% (V/V) after 30 days, especially after the rst 16 days,
exceeding 83% of the nal reduction.
The process of gasoline evaporation involves many aspects, such
as thermodynamics and kinetics, and many factors may affect the
evaporability of gasoline, but it is still largely determined by the
composition. With a decrease in the weight of light hydrocarbons,
the remaining weight of the heavy hydrocarbons increases;
therefore, the concentration of gasoline vapor displays a downward
trend overall.
3.5. Concentration of the main vapor content
Gasoline is a multicomponent compound mixture, and the rate
of evaporation of each individual component will differ as a result.
Consequently, the component and the content continuously change
during the course of evaporation, especially the light hydrocarbon
components. Fig. 7 gives the gas chromatogram of gasoline vapor
when gasoline was transferred into bottle and opened in the air
only for 10 min Fig. 8 shows the concentration of C
5
, total light
hydrocarbon component and the total hydrocarbon component
during the 30 experimental days. Table 1 lists the calculated
concentration of the main vapor constituent.
In this paper, C
5
is the content of pentane in the oil vapor. The
concentration of light hydrocarbons is determined by adding
together the values of C
1
, C
2
, C
3
, C
4
and C
5
. Similarly, the concen-
tration of hydrocarbon is obtained by adding up the total constit-
uents, calculated from the GC result and compared with the
standard gas, including the 24 organic compounds. Therefore, it
must be emphasized that some trace constituents are not distin-
guished and are included in the total hydrocarbon component, and
the calculated concentration using the GC method is slightly less
than the actual value. However, if we compare the results of Figs. 8
and 6, we nd that the value of the NMHC was slightly more than
that of the total hydrocarbon component, where the original
concentrations were 34.7378% (V/V) and 33.406% (V/V), respec-
tively. Although the concentration of the NMHC was computed
with the total hydrocarbon concentration by minusing the methane
Fig. 7. The gas chromatogram of gasoline vapor.
0 3 6 9 12 15 18 21 24 27 30
0
4
8
12
16
20
24
28
32
36
C
o
n
c
e
n
t
r
a
t
i
o
n

%
(
V
/
V
)
Time (d)
C
5
light hydrocarbon
hydrocarbon

Fig. 8. Concentration of the main vapor constituents (C

5
, light hydrocarbon and total
hydrocarbon) vs. time.
L. Zhu et al. / Journal of Loss Prevention in the Process Industries 25 (2012) 916e922 920
concentration, the maximum methane concentration was only
0.0315% (V/V), which might be ignored compared to the value of
34.7378% (V/V), which was the NMHC content. This may account for
the difference in the two results.
In Fig. 8, the three proles exhibit the same downtrend. The
light hydrocarbons value decreased from 24.319% (V/V) to 4.849%
(V/V) in the rst 12 days and from 4.849% (V/V) to 0.916% (V/V) in
the last 18 days. The loss ratios were 83.19% and 16.81%, respec-
tively. That is to say, most of the volatile compounds evaporated at
the beginning of experiment, which is consistent with the weight
results and the NMHC measurements. We also found that during
the rst 12 days, the total hydrocarbon concentration decreased
from 33.406% (V/V) to 7.2886% (V/V), and 19.479% (V/V) can be
attributed to the evaporation of the light hydrocarbons. In other
words, a major portion of the reduction in total hydrocarbon
concentration resulted from the evaporation of the light
hydrocarbons.
4. Conclusion
This study examined changes in the properties of liquid gasoline
and gaseous vapor during the evaporation process. The weight
decreased from 42.7155 g to 5.8265 g, and the weight decrease can
be expressed by a logarithmic equation. The viscosity of gasoline
increased from 8.6 10
4
Pa s to 1.51 10
3
Pa s, and RVP also
decreased from38 kPa to 9.6 kPa. All the NMHC concentrations and
the main constituents of the vapor decreased with different
degrees. Most of the changes might be attributed to the evaporation
of light hydrocarbons. The concentration of light hydrocarbons
decreased from 24.319% (V/V) to 0.916% (V/V) and that of the total
hydrocarbon declined from 33.406% (V/V) to 1.559% (V/V). All of
these results indicate that the changes can be attributed to the
evaporation of volatile organic compounds, and for all the param-
eters analyzed in this study, the major changes occurred at the
beginning of the experiments.
Acknowledgment
This work was supported by grants from the Funding Project for
Academic Human Resources Development in Institutions of Higher
Learning under the Jurisdiction of Beijing Municipality (PHR
201107147, PHR 201107213, and PHR 201108365).
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