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A R T I C L E I N F O A B S T R A C T
Keywords: Liquid natural gas and liquid hydrogen are promising and economical clean energy sources for reducing CO2
Liquid hydrogen emissions and slowing global warming. Characterization and monitoring of the vacuum pressure inside tank
LNG containers with multilayer insulation (MLI) are essential for the safe storage and convenient transportation of
Vacuum pressure
these cryogenic fuels. Herein, a new method for characterizing the vacuum pressure of tank containers with MLI
MLI
Tank container
is proposed. A theoretical analysis revealed that the temperature of the outer surface of the MLI material (To) is a
good indicator of the vacuum pressure inside the tanks. Experimental verification was conducted using an MLI
performance-testing apparatus, To was measured under 10 different vacuum pressures. The results showed that
when the vacuum pressure was <10-1 Pa, To kept almost. However, when the vacuum pressure was >1 Pa, To
decreased sharply with the increase of vacuum pressure.
The mechanism of the proposed method was also discussed based on the thermal analysis of the experimental
system at different vacuum pressures. This study provides a simple and reliable method for vacuum pressure
monitoring of tank containers with MLI, which allows the large-scale and safe utilization of clean energy with a
low boiling temperature.
1. Introduction world (28.3%) [6]. Clean energy, including natural gas and hydrogen, is
essential for the Chinese government to achieve its goal of reducing the
Although extensive international efforts and collaborations have CO2 emissions per gross domestic product to 60%–65% of that of 2005
been made in the past decades to limit the increase in the global mean by 2030 [7]. China imports a large amount of natural gas to compensate
temperature, global warming is accelerating [1,2]. According to the for shortages and satisfy the demand [8]. Hydrogen energy—a clean
latest predictions of the World Meteorological Organization regarding form of energy—is promising for powering vehicles [9] and aircrafts
the global climate, the annual global temperature is likely to be at least 1 [10] and has the advantages of a high energy density, low costs, and low
◦
C warmer than preindustrial levels in each of the coming 5 years and is emissions [11,12].
very likely to be within the range of 0.91–1.59 ◦ C [3]. Previous studies Safe storage and convenient transportation are important aspects for
suggest that actions such as adopting clean energy [4] and replacing the the large-scale utilization of these fuels. The density of liquid hydrogen
existing energy infrastructure [5] must be taken immediately to fulfill (LH2) at 1 atm is equal to that of hydrogen gas at 193.75 MPa and 300 K,
the target of the “Paris Agreement on Climate Change.” and the density of liquid natural gas (LNG) at 1 atm is equal to that of
According to the BP statistical review of world energy, renewable natural gas at 240.18 MPa and 300 K [13]. Normally, high-pressure
energy accounted for 11.8% of the total energy consumption of China in hydrogen vessels operate at a pressure of 77 MPa; therefore, fuels
2018, which was significantly lower than the average value for the (natural gas and hydrogen) in the liquid form have the advantages of a
* Corresponding author.
E-mail address: gan_zhihua@zju.edu.cn (Z. Gan).
https://doi.org/10.1016/j.applthermaleng.2021.116569
Received 9 September 2020; Received in revised form 18 December 2020; Accepted 5 January 2021
Available online 12 January 2021
1359-4311/© 2021 Elsevier Ltd. All rights reserved.
B. Wang et al. Applied Thermal Engineering 187 (2021) 116569
low pressure and a high energy density, compared with the high-
pressure and physical or chemical adsorption in hydrides [14].
Thermal insulation is crucial for the storage of LNG or LH2 because of
the low boiling temperature and low latent heat. The boiling tempera
tures of LNG and LH2 are 111.5 and 20.2 K, respectively, at 1 atm. A
small amount of heat leaking into the low-temperature tank results in a
remarkable pressure increase and leads to the risk of cryogenic-liquid
release, combustion, and boiling liquid expanding vapor explosion
(BLEVE) [15–17]. The survey indicated that more than 1000 people died
and 10,000 people were injured because of BLEVEs from 1940 to 2005
[17].
To prevent the LNG or LH2 tanks from over pressuring and increase
the liquid storage time, multilayer insulation (MLI) with high-vacuum
conditions is widely used in the aerospace field, the gas industry, and
low-temperature physics [18–21]. The simplest MLI structure contains a
reflector layer with a low emissivity and a spacer layer with a low
thermal conductivity. The low-emissivity reflector can reduce the Fig. 1. Schematic of an LNG or LH2 tank container with MLI.
amount of thermal radiation, and the low-thermal conductivity spacer
can reduce the amount of thermal conduction. If the MLI is installed in a II). The amount of heat remains constant (Qt) in the two processes. All
high-vacuum environment, the amounts of convection and conduction three types of heat transfer occur inside the tank during process I. The
of the residential gas are reduced, benefiting from the high vacuum. heat radiates from the inside of the outer tank at a high temperature of
Many studies have been conducted on performance testing and char Ta to the MLI with a temperature of To at the outer surface. Heat is
acterization [19,22], novel structures (including layered composites) conducted through the temperature gradient of Ta and To by residential
[23], variable-density MLI [24,25], spacers [26], and MLI with a vapor- gas. Heat convection may also occur under certain conditions. The heat
cooled shield [27]. transfer during process II is similar to that during process I, but the
In addition to the material and layout of the reflector and spacer, the calculation of the three types of heat transfer is more complex and
vacuum pressure significantly affects the performance of the MLI difficult.
[19,22]. The apparent thermal conductivity of the MLI is <10-4 W/(m⋅K)
when the vacuum pressure is <10-1 Pa, and the apparent thermal con
ductivity increases significantly with the increasing vacuum pressure 2.2. Calculation of thermal resistances
when the vacuum pressure is >10-1 Pa. The vacuum pressure inside the
tanks is recommended to be <10-1 Pa for avoiding heat-load leakage. The thermal network of heat transfer inside the tank is shown in
The characterization and monitoring of the vacuum pressure of LNG Fig. 2. Thermal contact resistance between the MLI and inner tank was
or LH2 tanks (particularly tank containers) with MLI are vital for the safe neglected because the coldest layer of MLI was mounted to the wall of
and economical storage and transportation of LNG and LH2. The vacuum the inner tank directly by aluminum tape. Previous study also verified
pressure can be determined using a vacuum gauge for onsite tanks, but it the conclusion, and vacuum pressure also has a very weak influence on
is difficult for the vacuum pressures of tank containers to be monitored the temperature distribution along with the MLI [35].
over the long distance and long duration of transportation from the port The thermal resistance between Ta and To consists of the radiation
near the coast to terminal users in rural areas [28]. resistance (R1), conduction resistance (R2), and convection resistance
Few studies have been performed on the characterization and (R3), which can be calculated theoretically. The thermal resistance be
monitoring of the vacuum pressure of a tank container with MLI for LNG tween the outer surface of the MLI (To) and the liquid (Tc) is the apparent
or LH2 storage and transportation. In this paper, a new method for thermal resistance of the MLI (RMLI). RMLI is a hybrid thermal resistance
characterizing the vacuum pressure of tanks with MLI is proposed. A that includes the radiation resistance and conduction resistance of the
theoretical analysis reveals that the temperature of the outer surface of reflectors and spacers, conduction resistance, and convection resistance
the MLI material is a good indicator of the vacuum pressure inside the of the residential gas inside the MLI. It is not easy to determine RMLI
tank [29]. Experimental measurements were conducted using an MLI theoretically; therefore, empirical models such as the Lockheed–Martin
performance-testing apparatus, and the results validated the proposed model [30] and the layer-by-layer model [31] are typically used to
method. This study provides a simple and reliable method for vacuum calculate RMLI.
pressure monitoring of tank containers with MLI that allows the safe,
large-scale utilization of clean energy with a low boiling temperature 2.2.1. Radiation resistance
(LNG and LH2). In the space with a gap of δ between the outer tank and the MLI, the
radiation resistance R1 can be determined using Eq. (1):
2. Physical model and characterization method of vacuum Ta - To
R1 = (1)
pressure εσ Ao (T4a - T4o )
2
B. Wang et al. Applied Thermal Engineering 187 (2021) 116569
where Ta represents the ambient temperature, To represents the tem 2.2.3. Convection resistance
perature of the outer surface of the MLI, ε represents the mutual emis The convection resistance R3 is expressed as follows:
sivity of the outer tank and MLI system, σ represents the 1
Stefan–Boltzmann constant, and Ao represents the area of the outer R3 = (7)
Ao h
surface of the MLI.
where h represents the convective heat transfer coefficient. The heat
2.2.2. Conduction resistance convection in the finite space is dependent on the Grashof number (Gr);
The conduction resistance R2 of the gas inside the space depends on when Gr ≤ 2860, the heat convection can be neglected [34]. Gr is
the conditions within the space, and three zones are defined according to expressed as follows:
the Knudsen number, which is given as follows [32]:
gα(Ta − To )δ3
Grδ = (8)
l0 ν2
Kn = (2)
δ
where g represents the gravitational acceleration, α represents the vol
where l0 represents the mean free path of the residential gas, and δ ume expansion factor of the gas, and ν represents the kinematic vis
represents the spacing. cosity. The reference temperature for the thermal properties is the
l0 is a parameter related to the pressure and temperature of the space. average temperature of Ta and To.
The mean free path of air molecules is approximated as follows [32]:
2.3. Characterization of vacuum pressure
5T
l0 = 2.27 × 10− (3)
p
For the thermal network shown in Fig. 2, the energy-conservation
where T represents the temperature, and p represents the pressure. law requires that the heat transferred in process I (from the outer tank
When Kn > 10, the mean free path of the gas is significantly larger to the MLI) is equal to that transferred in process II (from the MLI to the
than the spacing. This is called the free molecular state. As indicated by inner tank), as the areas of the cylinder and the inner tank are almost
Eq. (3), for a certain type of molecule, the lower the pressure, and the identical. We can obtain the following:
larger the mean free path, the state is also called a high-vacuum state. In Ta − To To − Tc
the high-vacuum state, the classical Fourier conduction law is no longer 1
= (9)
1 1 1 RMLI
valid, and the conduction resistance R2f is expressed as follows [33]: R1 +R2 +R3
1 If the boundary conditions (such as Ta, Tc, R1, R3, and RMLI) are
R2f = (4) known, the relationship between the temperature of the outer surface of
Ao kap
the MLI (To) and the conduction resistance (R2) can be determined using
where a represents the thermal accommodation coefficient, which can Eq. (9). As discussed previously, in the vacuum-pressure range consid
only be determined via experimental measurement, and p represents the ered in this study, the pressure significantly affects the conduction
pressure. k is a parameter related to the properties of the gas inside the resistance R2; thus, a relationship between the temperature of the outer
space and can be determined by referencing tables, the reference tem surface of the MLI (To) and the vacuum pressure (p) can be established
perature for the thermal properties is the average temperature of Ta and using Eq. (9).
To.
The heat conduction of the gas inside the space is an intermediate 3. Experimental system and testing conditions
pressure state when 0.01 < Kn < 10. The pressure in this state is not very
high, and the scale of the mean free path of the molecule is at the same 3.1. Experimental system
level of spacing. The conduction resistance R2i in the intermediate
pressure state is expressed as follows [33]: Experiments were conducted on an MIL performance-testing plat
form to verify the characterization method proposed in Section 2. Figs. 3
R2i =
δ(1 + 2βKn)
(5) and 4 show the layout and a photograph of the experimental system,
Ao λp respectively. 50 layers of MLI materials with a thickness of 17 mm were
wrapped around the heat calorimeter, including a testing chamber in the
where δ represents the spacing, λp represents the thermal conductivity of
middle, an upper guard chamber, and a lower guard chamber. The heat
the gas at the atmospheric pressure, Kn represents the Knudsen number,
calorimeter was installed in a cylinder with vacuum pumps. A needle
and β is a parameter related to the properties of the gas inside the space.
valve connected to a compressed N2 gas source was placed between the
The reference temperature for the thermal properties is the average
cylinder and pumps to adjust the vacuum pressure inside the cylinder.
temperature of Ta and To.
The guard chamber and test chamber were filled with liquid nitrogen
The continuum state is defined at Kn < 0.01, which is the normal
during the test, several hours were taken to reach the thermal equilib
state of the atmospheric pressure, and the conduction resistance R2c in
rium after the filling, and liquid nitrogen was refilled into the chambers
this state is expressed as follows:
to carry out the actual tests. When the change of volume flow rate within
δ 1 h is less than 5%, it can be conclude that the system was in a steady
R2c = (6)
Ao λp state. Data of temperatures and volume flow rate were recorded when
the experimental system reached steady state.
As indicated by Eqs. (4)–(6), in the free molecular state and inter The vacuum inside the cylinder was controlled by the opening of the
mediate pressure state, the pressure significantly affects the conduction needle valve, and a group of 10 vacuum pressures ranges (listed in
resistance R2. Although the pressure has no impact on R2 in the con Table 1) from 1 × 10-4 to 1 × 105 Pa was chosen in this study. The
tinuum state (Eq. (6)), the pressure (atmosphere pressure) is outside of ambient temperature (Ta) was controlled by circulating water from a
the range of the vacuum pressure considered in this study; the present water reservoir connected to outer cylinder of the test apparatus, and Ta
paper focuses on a vacuum pressure between 0.01 Pa and the atmo during a single test is very stable, and the change of Ta during the whole
sphere pressure. test was about 5 K, as shown in the following section.
3
B. Wang et al. Applied Thermal Engineering 187 (2021) 116569
Fig. 4. Photograph of the MLI performance-testing platform. where Qt represents the amount of heat that leaks to the test tank, V
represents the volume flow rate of the evaporated nitrogen under
standard conditions, ρgS represents the density of nitrogen under
Table 1
Testing conditions of vacuum pressure.
Testing No. 1 2 3 4 5 Table 2
Vacuum pressure/ 5 × 10-4 4.65 × 10- 0.0425 0.0775 0.46 Uncertainties of the measured parameters.
3
Pa Parameter Instrument Producer Uncertainty
Testing No. 6 7 8 9 10
Vacuum pressure/ 3.55 13 170 1500 1.013 × Vacuum Resistance Chengdu Zhenghua ±1% of reading
Pa 105 pressure vacuum gauge
Ionization CANON ANELVA ±0.2% of reading
vacuum gauges M-341DG
3.2. Data acquisition and testing conditions Temperature Resistance TIPC, CSA ±0.1 K
thermometer
Flow rate Volume flow- MKS ±1% of reading
As shown in Fig. 3, the heat leaked to the test chamber only from the meter GE50A013203RMV020 (20%–100% full
side, as the temperatures of the upper and lower surfaces of the test scale)
chamber were kept constant by the two guard chambers. The cryogenic ±0.2% of reading
(2%–20% full
liquid in the test chamber (liquid nitrogen) adsorbed heat and
scale)
4
B. Wang et al. Applied Thermal Engineering 187 (2021) 116569
standard conditions (1250.7 g/m3), and hfg represents the latent heat of
nitrogen under the testing conditions.
The apparent thermal conductivity (Keff) of the MLI can be evaluated
using the equation of steady-state heat transfer through a cylinder of
inner diameter di, outer diameter do, and length L. The apparent thermal
conductivity (Keff) and apparent thermal resistance of the MLI (RMLI) are
expressed as follows:
Qt × ln(do /di )
Keff = (11)
2πL(To − Tc )
ln(do /di )
RMLI = (12)
2π Keff L
√̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅
⎛ ⎞2
√
√
√( )2 ( )2 ( )2 ( )
√ ∂Keff ∂Keff ∂Keff ⎜∂Keff do ⎟
σ Keff =√
√ ∂Qt σ Qt + ∂L σ L + ∂(To − Tc ) σ(To − Tc ) + ⎝∂(do ) σ di ⎠
⎜ ⎟ (14)
di
pressures. Fig. 6 shows the volume flow rate of the nitrogen gas, ambient
√̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅
( )2 ( )2 temperature (Ta), and temperature of the outer surface of the MLI (To)
∂Gr ∂Gr under a pressure of 1.0135 × 105 Pa. It can be seen from the figure, Ta
σ Gr = σδ + σ (Ta − To ) (15)
∂δ ∂(Ta − To ) remained constant and To oscillated in a limited range, but the volume
flow rate of the nitrogen gas changed significantly during the test. In this
√̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅
(
∂Kn
)2 (
∂Kn
)2 operation condition, the time from the completion of the filling to the
σ Kn = σl0 + σδ (16)
∂l0 ∂δ
According to Eqs. (13)–(16) and Table 2, the uncertainty of Qt, Keff,
Gr and Kn are 1.0%, 4.35%, 3.77% and 1.0%.
5
B. Wang et al. Applied Thermal Engineering 187 (2021) 116569
completely dry state was used to calculate the heat load. The 4.3. Discussion
“completely dry” state was defined by the volume flow rate rapidly
decreasing to a very low value. And only the average heat load could be Responding time is vital for the practical application of the proposed
determined under this condition. method. The Fig. 8 showed the change of the temperature of outer
surface of MLI (To) with the vacuum pressure. From the figure we can see
4.2. Apparent thermal conductivity and temperature of outer surface of that the temperature of outer surface of MLI changed very fast with the
MLI at different vacuum pressures change of vacuum pressure, and the result indicates that the time con
stant for the To in response to the change of the vacuum pressure is
Fig. 7 shows the apparent thermal conductivity and temperature of small, and it’s suitable for practical application in industry.
the outer surface of the MLI at 10 different vacuum pressures. The As shown in Fig. 7, in contrast to the heat flux, To initially remained
hollow circles indicate the apparent thermal conductivity, as explained steady within a wide range of low vacuum pressures and then decreased
in the Introduction. The apparent thermal conductivity remained con with an increase in the vacuum pressure. When the vacuum pressure
stant when the vacuum pressure was <10-1 Pa, and it increased when the continued to increase, the temperature of the outer surface of the MLI
vacuum pressure was >10-1 Pa. increased again. The reason for the change in To is discussed in detail in
In Fig. 7, the red triangles indicate the temperature of the outer this section.
surface of the MLI (To), the black squares represent the ambient tem As discussed in Section 2, the Knudsen number (Eq. (2)) and Grashof
perature (Ta). The change of Ta among the 10 operation conditions was number (Eq. (8)) significantly affected the heat transfer inside the space.
about 5 K. Fig. 9 shows the Knudsen and Grashof numbers at different vacuum
As shown in Fig. 7, when the vacuum pressure was <10-1 Pa, the heat pressures. The critical values for the two numbers are labeled.
load leaked to the inner tank remained almost constant, so the To also As shown in Fig. 9, Kn decreases with the increasing vacuum pres
kept almost constant as the ambient temperature did not change. sure, as the mean free path of nitrogen is inversely proportional to the
However, when the vacuum pressure was >1 Pa, the total heat load of pressure. Three zones are defined according to the critical Kn number,
liquid nitrogen increased significantly as the apparent thermal con and different equations are used to calculate the heat conduction of the
ductivity of MLI increased. A larger temperature difference was occurred residential gas. In contrast to Kn, Gr increases with the vacuum pressure,
due to the larger heat load, so To decreased sharply with the increase of and the kinematic viscosity decreases with the increasing vacuum
vacuum pressure. pressure. When Gr < 2860, the free convection inside the space can be
The trend of the heat load (flux) was identical to that of the apparent neglected. Gr reaches 2860 when the vacuum pressure is 1500, and the
thermal conductivity (Fig. 7), as the heat load was proportional to the empirical equation can be used to calculate the heat convection [34].
apparent thermal conductivity. The heat flux remained almost constant Using Eqs. (1)–(8), the heat loads at different vacuum pressures were
at low vacuum pressures and increased rapidly when the vacuum pres calculated and compared with the experimental values. As shown in
sure was >1 Pa. Fig. 10, the theoretical calculations agreed well with the experimental
As shown in Fig. 7, when the vacuum pressure inside the tank results, and heat radiation dominates the heat load leaked to the system at
container increased from a lower value (initial state, such as 10-3 Pa) to the two lowest vacuum pressures. When the Kn number falls into the in
a higher value because of outgassing or mechanical failure, the tem termediate pressure zone (as shown in Fig. 9), the heat conduction of the
perature of the outer surface of the MLI initially oscillated in a limited residential gas increases and remains almost constant at a vacuum pres
range, and when the vacuum pressure reached a certain value, the sure of >1 Pa. When the vacuum pressure is >1 Pa, the heat radiation
temperature of the outer surface of the MLI decreased significantly. increases significantly with the vacuum pressure, and the temperature
The signal for decreasing the temperature of the outer surface of the difference between Ta and To increases. As the ambient temperature is
MLI can be used to monitor the vacuum failure of the tank (the region constant, the temperature of the outer surface of the MLI (To) decreases
between the two dashed lines in Fig. 7), and overhaul must be taken to sharply with the increasing vacuum pressure in the range of 1–1500 Pa.
ensure the safe operation of the tank. The experimental results indi As indicated in Fig. 9, natural convection in a limited space occurs
cated that the vacuum pressure can be characterized by the tempera when the vacuum pressure is >1500 Pa. As the convection resistance is
ture of the outer surface of MLI, and the feasibility of the proposed much smaller than the conduction and radiation resistances, the tem
method for characterizing the vacuum pressure of tank containers is perature difference between Ta and To decreases; thus, the temperature
also verified. of the outer surface of the MLI To increases sharply when the vacuum
pressure is in the range of >1500 Pa.
6
B. Wang et al. Applied Thermal Engineering 187 (2021) 116569
vacuum pressure monitoring of tank containers with MLI and can sup
port the large-scale and safe utilization of clean energy with a low
boiling temperature (LNG and LH2).
Acknowledgements
7
B. Wang et al. Applied Thermal Engineering 187 (2021) 116569
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