buildings

Article
Research on Thermal Response Behavior of the Intumescent
Coating at High Temperature: An Experimental and
Numerical Study
Lingyun Zhang 1,2 , Yupeng Hu 2, * and Minghai Li 2, *

1 School of Aerospace Engineering, Beijing Institute of Technology, Beijing 100081, China;

[email protected]
2 Institute of Systems Engineering, China Academy of Engineering Physics, Mianyang 621999, China
* Correspondence: [email protected] (Y.H.); [email protected] (M.L.)

Abstract: Intumescent coating is able to provide effective fire protection with both practicality and
aesthetics. In this study, expansion performance and thermal physical property experiments are
firstly carried out to obtain the basic parameters at different temperatures. Then, the thermal response
model of the concrete-filled steel tubular (CFST) structure under the protection of intumescent coating
in a fire is established. Finally, based on the experimental data and thermal response model, the
effects of initial thickness, expansion rate, intra-pore emissivity and reaction heat on the structure
temperature are discussed in detail. The results of this study can provide guidance on intumescent
coating formulation design, as well as fire protection design.

Keywords: intumescent coatings; thermal insulation performance; thermal response model;

experimental study

Citation: Zhang, L.; Hu, Y.; Li, M.

Research on Thermal Response
Behavior of the Intumescent 1. Introduction
Coating at High Temperature: An Concrete-filled steel tubular (CFST) structures are widely used in modern buildings
Experimental and Numerical Study. due to their excellent mechanical and construction performance [1,2]. However, the mechan-
Buildings 2022, 12, 1014. https:// ical performance of a CFST structure degrades significantly with increasing temperatures,
doi.org/10.3390/buildings12071014 and the structure cannot maintain its strength and stiffness at high temperatures [3]. There-
Academic Editor: Karim fore, effective fire protection measures must be taken to reduce the temperature-rise rate
Ghazi Wakili of the CFST structure. Intumescent coating is able to provide efficient fire protection with
relatively less thickness, and it is a common fireproofing material for CFST structures [4].
Received: 31 May 2022
The intumescent coating will swell at high temperatures, and a porous carbon layer will
Accepted: 12 July 2022
be formed with relatively more thickness [5]. The porous carbon layer directs the path
Published: 14 July 2022
of external heat transfer into the protected structure, and the thermal conductivity of the
Publisher’s Note: MDPI stays neutral porous carbon layer is extremely low [6]. Meanwhile, the physical and chemical changes
with regard to jurisdictional claims in of intumescent coatings will absorb a large amount of heat [7]. In summary, intumescent
published maps and institutional affil- coating is able to reduce the temperature-rise rate of the protected structure with both
iations. practicality and aesthetics [8–10].
In the past decades, researchers conducted extensive studies on the thermal insulation
performance of intumescent coatings. The studies can be divided into two categories.
One type focused on the material design and formulation for intumescent coatings and
Copyright: © 2022 by the authors.
developed new components and formulations to improve the physical and chemical perfor-
Licensee MDPI, Basel, Switzerland.
mance of intumescent coatings at high temperatures. Vabdersall [11] put forward that the
This article is an open access article
distributed under the terms and
intumescent coating’s thermal performance was dependent on the quantity ratio of carbon,
conditions of the Creative Commons
nitrogen and phosphorus. Reshentnikov [12–14] found that the best thermal insulation
Attribution (CC BY) license (https://
performance was achieved when the ratio of polyphosphate to polyol was 7:3. Studies
creativecommons.org/licenses/by/ showed that expandable graphite expanded at high temperatures and formed porous car-
4.0/). bon layers with high porosity [15–18]. Researchers found that the proper addition of fillers

Buildings 2022, 12, 1014. https://doi.org/10.3390/buildings12071014 https://www.mdpi.com/journal/buildings

Buildings 2022, 12, 1014 2 of 18

improved the intumescent coating’s thermal insulation performance. For instance, the use
of magnesium hydroxide, titanium, zirconium, fire-resistant fibers and nanomaterials were
able to improve the physical and chemical performance at high temperatures [18–25].
The other type of study focused on the thermal response behavior of intumescent
coatings at high temperatures, including pyrolysis, expansion and heat-transfer mecha-
nisms. This type of study provided theoretical guidance for the design and formulation of
intumescent coatings. In the early years, semi-empirical models were developed to describe
the expansion process [26–30]. Blasi and Colomba [31,32] established a mathematical model
to characterize the pyrolysis behavior of the intumescent coating; the model described the
expansion process with some empirical parameters. Some researchers [33–35] established
comprehensive models by considering a combination of the pyrolysis, expansion and
heat-transfer process. Li et al. [36,37] adopted the constant equivalent thermal resistance to
indicate the thermal insulation performance of the intumescent coating. Cirpici et al. [38]
used the bubble growth model to describe the expansion behavior of the intumescent
coating. Zhang et al. [39] studied the couple thermal transfer mechanisms of the porous
char layer, including thermal conduction, convection and radiation.
In this paper, expansion performance and thermal physical property experiments at
high temperatures are carried out to obtain the thickness, thermal conductivity and density
of intumescent coating. Then, a numerical model is established to describe the thermal
response of CFST structures under the protection of intumescent coatings in a fire. Based
on the experimental data and numerical model, this study examines the thermal response
characteristics of the structure. The effect of initial thickness, expansion rate, intra-pore
emissivity and reaction heat are discussed in detail. This results of this study can be applied
to provide guidance on fire protection design.

2. Experiments
2.1. High-Temperature Expansion Performance Experiment
A high-temperature expansion performance experiment of a typical intumescent coat-
ing was carried out to obtain the variation in thickness with temperature. The intumescent
coating used in the experiment was produced by Wuli Coating Co. The substrate was a
surface-treated Q235 steel plate with a size of 120 mm × 120 mm × 3 mm. The initial
thickness of the intumescent coating was 3 (±0.1) mm. The specimen was placed on the
experimental table for dry maintenance. The instrument used for the experiment was the
SX2-10-13A high-temperature electric furnace produced by Chongqing Xinbang Electric
Furnace Company. The electric furnace was composed of two parts: the furnace body
and the temperature-control system, as shown in Figure 1. The maximum range of the
furnace is 1573 K, and a variety of temperature-rise rates can be set to meet the required
test conditions. The main processes were as follows.
(a) The specimen is placed on the refractory brick and surrounded by a certain amount
of sponge to prevent heat dissipation, as shown in Figure 2.
(b) The temperature of the furnace is set according to the working conditions and main-
tained for 1800 s to ensure full expansion at this temperature.
(c) After cooling, the expanded specimen is taken out and the thickness is measured by
vernier caliper.
The expansion thickness and the expansion rate, which is defined as the ratio of the
expansion thickness to the initial thickness, are shown in Table 1. In order to display the
variation trend with the change in temperature more clearly, the data in the table are plotted
as curves, as shown in Figure 3. It can be seen that in the initial stage (293 K to 573 K), the
expansion thickness and rate remained unchanged with the increase in temperature; this is
because the components of the intumescent coating have not yet decomposed. When the
temperature reached 573 K, the expansion thickness and rate increased with the increase in
temperature, which indicates that the decomposition reaction of the foaming agent and
other components started to take place. Then, the expansion thickness and rate continued
 Buildings 2022, 12, 1014 3 of 18
Buildings 2022, 12, x FOR PEER REVIEW 3 of 2

to increase and reached the maximum value at a certain temperature. Finally, the expansion
Buildings 2022, 12, x FOR PEER REVIEW 3 of 20
thickness and rate started to decrease; this is due to the intumescent coating’s oxidation at
high temperatures.

Figure1.
Figure
Figure 1.1. Electric
Electric
Electric
furnace.
furnace.
furnace.

Figure 2. Specimen in the furnace.

The expansion thickness and the expansion rate, which is defined as the ratio of the
Figure2. 2.
Figure Specimen
Specimen in the
in the furnace.
furnace.
expansion thickness to the initial thickness, are shown in Table 1. In order to display the
variation trend with the change in temperature more clearly, the data in the table are plot-
The expansion thickness and the expansion rate, which is defined as the ratio of th
ted as curves, as shown in Figure 3. It can be seen that in the initial stage (293 K to 573 K),
expansion
the expansion thickness
thicknesstoand
therate
initial thickness,
remained are shown
unchanged in Table
with the 1. in
increase In temperature;
order to display th
variation trend with the change in temperature more clearly, the data
this is because the components of the intumescent coating have not yet decomposed. in the table are plo
ted as curves, as shown in Figure 3. It can be seen that in the initial stage (293 K to 573 K
 continued to increase and reached the maximum value at a certain temperature. Finally,
the expansion thickness and rate started to decrease; this is due to the intumescent coat-
ing’s oxidation at high temperatures.

Table 1. Thickness and expansion rate (d3-373 K indicates the initial thickness is 3 mm and the
Buildings 2022, 12, 1014 experiment temperature is 373 K). 4 of 18

Specimen Initial Thickness Test Thickness Expansion Rate

1.-373
Tabled3 K
Thickness 3.13 mm
and expansion 3.13 mm
rate (d3-373 K indicates the initial thickness is 3 1mm and the
d3-473temperature
experiment K 3.06
is 373 K).mm 3.06 mm 1
-573 K
d3Specimen 3.10 mm
Initial Thickness 3.10
Test mm
Thickness 1 Rate
Expansion
d3-d3-373
673 KK 3.023.13
mmmm 9.57
3.13mm
mm 3.16
1
d3-d3-473
773 KK 3.173.06
mmmm 3.06 mm
16.95 mm 1
5.35
d3-573 K 3.10 mm 3.10 mm 1
d3-d3-673
873 KK 3.053.02
mmmm 21.60 mm
9.57 mm
7.08
3.16
d3-d3-773
973 KK 3.073.17
mmmm 21.90
16.95mm
mm 7.13
5.35
d3-873 K 3.05 mm 21.60 mm 7.08
d3-d3-973
1073 KK 3.113.07
mmmm 17.77 mm
21.90 mm
5.71
7.13
d3-1073 K 3.11 mm 17.77 mm 5.71

Figure 3. Thickness and expansion rate variation with temperature.

Figure 3. Thickness and expansion rate variation with temperature.

2.2. Thermal Conductivity Experiment

2.2. Thermal Conductivity Experiment
The instrument used for the thermal conductivity experiment was the C-Therm ther-
The instrument used for the thermal conductivity experiment was the C-Therm ther-
mal conductivity meter, as shown in Figure 4, which is based on the principle of “Modified
mal conductivity meter, as shown in Figure 4, which is based on the principle of “Modi-
Transient Plane Source”. The thermal conductivity of solids, liquids, powders and colloids
fied Transient Plane Source”. The thermal conductivity of solids, liquids, powders and
could be determined quickly and accurately. The thermal conductivity could
Buildings 2022, 12, x FOR PEER REVIEW 5 of 20 be measured
colloids could be determined quickly and accurately. The thermal conductivity could be
from 0 to 500 W/(m·K), and the temperatures were from 273 K to 423 K.
measured from 0 to 500 W/(m⋅K), and the temperatures were from 273 K to 423 K.

Figure 4.
Figure 4.C-Therm
C-Thermconductivity meter.
conductivity meter.
According to the results of the high-temperature expansion performance experiment,
the state of the intumescent coating at different temperatures varied greatly, as shown in
Figure 5. Therefore, the experiment of thermal conductivity was divided into a low-tem-
perature stage and a high-temperature stage. In the low-temperature stage (273 K-573 K),
the intumescent coating was in a dense block state, and we tested the thermal conductivity
 Buildings 2022, 12, 1014 5 of 18
Figure 4. C-Therm conductivity meter.

According
According to tothe
theresults of of
results thethe
high-temperature
high-temperature expansion performance
expansion performanceexperiment,
experi-
the state of the intumescent coating at different temperatures varied greatly,
ment, the state of the intumescent coating at different temperatures varied greatly, as shown asin
Figure
shown 5.inTherefore, the experiment
Figure 5. Therefore, of thermal of
the experiment conductivity was dividedwas
thermal conductivity intodivided
a low-tem-
into
perature stage and astage
a low-temperature high-temperature stage. In the stage.
and a high-temperature low-temperature stage (273 K-573
In the low-temperature K),
stage
the
(273intumescent
K–573 K), the coating was in a dense
intumescent coatingblock
wasstate,
in a and we block
dense testedstate,
the thermal
and we conductivity
tested the
directly. However, in the
thermal conductivity high-temperature
directly. However, instage (673 K-1073 K), thestage
the high-temperature intumescent coating
(673 K–1073 K),
reached the expansion temperature and was in a porous carbon layer
the intumescent coating reached the expansion temperature and was in a porous carbon state. We first
pressed the We
layer state. porous carbon layer
first pressed into powder,
the porous then tested
carbon layer the powder
into powder, coating’s
then tested the thermal
powder
conductivity.
coating’s thermalThe conductivity.
specimens areThe shown in Figure
specimens are6.shown in Figure 6.

FOR PEER REVIEW 6 of 20

T = 573 K T = 773 K T = 973 K
Figure
Figure 5.
5. State
State of
of the
the intumescent
intumescent coating
coating at
at different temperatures.
different temperatures.

(a) (b)
Figure 6. SpecimenFigure
for the thermal for
6. Specimen conductivity experiment.
the thermal conductivity (a) Block
experiment. (a) state; (b) powder
Block state; state.
(b) powder state.

Figure 7 displays the thermal conductivities of the intumescent coating before expan-
Figure 7 displays the thermal
sion under conductivities
different temperatures. ofbethe
It can intumescent
seen coating
that the thermal beforeincreased
conductivity expan-
sion under different
withtemperatures. It can beThe
the increasing temperature. seen that for
equation thethe
thermal conductivity
thermal conductivity and increased
the temper-
ature was obtained by linear fitting, as Equation (1). The thermal
with the increasing temperature. The equation for the thermal conductivity and the conductivity at different
tem-
temperatures (273–573 K) can be calculated by the following equation.
perature was obtained by linear fitting, as Equation (1). The thermal conductivity at dif-
ferent temperatures (273–573 K) can be calculated by the− following
λs = 0.00049T 0.0405 equation. (1)

λs = 0.00049T − 0.0405 (1)

 with the increasing temperature. The equation for the thermal conductivity and the tem-
perature was obtained by linear fitting, as Equation (1). The thermal conductivity at dif-
ferent temperatures (273–573 K) can be calculated by the following equation.

λs = 0.00049T − 0.0405 (1)

Buildings 2022, 12, 1014 6 of 18

Buildings 2022, 12, x FOR PEER REVIEW 7 of 20

Figure 7. Variations of the thermal conductivity before expansion with temperature.

Figure 7. Variations of the thermal conductivity before expansion with temperature.
Figure 8 displays the thermal conductivities of the intumescent coating after expansion
Figure
under8different the thermalλconductivities
displaystemperatures. = 0.000093
Its can of
be seen that +the0.0337
T the intumescent coating after
thermal conductivity expan-
increased with(2)
the
increasing
sion under temperature.
different By linear
temperatures. fitting,
It can multiple
be seen that equations
the thermal forconductivity
the thermal conductivity
increased with
temperature
with the increasingwere obtained,By
temperature. λslinear
as = 0.000130
Equations
fitting, T + 0.0270
(2)–(6). Theequations
multiple thermal conductivity of the
for the thermal powder
con- (3)
coating
ductivity withattemperature
different temperatures
were obtained,(673–1073 K) can be
as Equations calculated
(2)–(6). by the following
The thermal equations:
conductivity
of the powder coating at differentλstemperatures
= 0.000127(673–1073
T + 0.0324 K) can be calculated by the (4)
λs = 0.000093T + 0.0337 (2)
following equations:
λs =λ0.000127 T + 0.0362
= 0.000130T + 0.0270 (5)(3)
s

λs =λ0.000103 T ++0.0475
s = 0.000127T 0.0324 (6)(4)
λs = 0.000127T + 0.0362 (5)
λs = 0.000103T + 0.0475 (6)

Figure 8. Variations of the thermal conductivity after expansion with temperature.

Figure 8. Variations of the thermal conductivity after expansion with temperature.

2.3. Density and Porosity Experiment

The density experiment of the intumescent coating was similar to the thermal con-
 Buildings 2022, 12, 1014 7 of 18

2.3. Density and Porosity Experiment

The density experiment of the intumescent coating was similar to the thermal con-
ductivity experiment. In the low-temperature stage (273–573 K), a direct method was
adopted for testing. In the high-temperature stage (673–1073 K), there were many pores
in the carbon layer, the density was characterized into true density and apparent density
and an indirect method was adopted for testing. The specimen is shown in Figure 9. The
true density denotes the expanded carbon density without the pores, and the apparent
density means the expanded carbon density within the pores. Lastly, the porosity can
be calculated by Equation (7), which stands for the relationship of the true density to the
apparent density:
Buildings 2022, 12, x FOR PEER REVIEW φ = 1−ρ/ρ1 (7) 8 of 2

where ρ and ρ1 denote the apparent density and true density in g/cm3 , and φ is the porosity.

Figure
Figure 9. 9. Specimen
Specimen in the
in the high-temperature
high-temperature stage.stage.

The
The measured
measured density
density and and the calculated
the calculated porosity
porosity are shown
are shown in Tablein
2. Table 2. It
It can be can be see
seen
that in the low-temperature stage (373–573 K), the true density decreased from 0.791 g/cm 3
that in the low-temperature stage (373–573 K), the true density decreased from 0.791 g/cm
toto0.723 g/cm 3
0.723 g/cm. 3In this
. In stage,
this the the
stage, water and volatility
water in the in
and volatility intumescent coating escaped
the intumescent coating escape
and the mass of the coating decreased, whereas the volume remained unchanged. In the
and the mass of the coating decreased, whereas the volume remained unchanged. In th
high-temperature stage (673–1073 K), the apparent density decreased from 0.297 g/cm3
high-temperature stage (673–1073 K), the apparent density decreased from 0.297 g/cm3 t
to 0.074 g/cm3 , and the true density decreased from 0.611 g/cm3 to 0.240 g/cm3 . The
0.074 g/cm
coating
3, and the true density decreased from 0.611 g/cm3 to 0.240 g/cm3. The coatin
started to expand, the mass decreased, and the volume continued to increase.
started
The to expand,
apparent densitythe andmass decreased,
true density and
of the the volume
expanded continued
coating to increase.
both decreased with theThe appar
ent density
increasing and true density
temperature. of thethe
In addition, expanded
porosity ofcoating both decreased
the intumescent coatingwith the increasin
increased
temperature.
from 0.514 to 0.722In addition, the porosity
in the temperature rangeof(673–973
the intumescent
K), whereascoating increased
it decreased from 0.514 t
from 0.722
to0.722
0.692ininthe
the temperature
temperature range range(973–1073
(673–973K). K),The is due to
whereas the intumescent
it decreased fromcoating’s
0.722 to 0.692 i
oxidation at high temperatures.
the temperature range (973–1073 K). The is due to the intumescent coating’s oxidation at hig
temperatures.

Table 2. Measured density and calculated porosity.

T Apparent Density (g/cm3) True Density (g/cm3)

Buildings 2022, 12, 1014 8 of 18

Table 2. Measured density and calculated porosity.

T Apparent Density (g/cm3 ) True Density (g/cm3 )

Porosity
(K) 1st 2nd 3rd Avg. 1st 2nd 3rd Avg.
373 0.792 0.791 0.789 0.791
473 0.758 0.761 0.762 0.760
573 0.723 0.715 0.732 0.723
673 0.296 0.298 0.296 0.297 0.610 0.609 0.613 0.611 0.514
Buildings
7732022, 12, x 0.149
FOR PEER REVIEW
0.150 0.153 0.151 0.439 0.436 0.438 0.438 90.655
of 20
873 0.081 0.084 0.082 0.082 0.276 0.279 0.279 0.278 0.705
973 0.070 0.071 0.071 0.071 0.254 0.253 0.257 0.255 0.722
1073 0.075 0.074 0.074 0.074 0.242 0.240 0.239 0.240 0.692
3. Numerical Simulation
3.1. Physical Model
3. Numerical Simulation
3.1. A typicalModel
Physical CFST structure was selected as the research object. According to GB 50936-
2014 [40], the outer diameter of the CFST structure should not be less than 168 mm and
A typical CFST structure was selected as the research object. According to GB 50936-
the wall thickness should not be less than 3 mm. In this study, the outer diameter of the
2014 [40], the outer diameter of the CFST structure should not be less than 168 mm and the
steel pipe was taken as 180 mm and the wall thickness was 3 mm. Figure 10 shows the
wall thickness should not be less than 3 mm. In this study, the outer diameter of the steel
physical model of the CFST structure under the protection of the intumescent coating.
pipe was taken as 180 mm and the wall thickness was 3 mm. Figure 10 shows the physical
According to GB 14907-2018 [41], the thickness of the intumescent coating should not be
model of the CFST structure under the protection of the intumescent coating. According to
less than 1.5 mm.
GB 14907-2018 [41], the thickness of the intumescent coating should not be less than 1.5 mm.

Figure
Figure10.
10.Physical
Physicalmodel
modelofofthe
theCFST
CFSTstructure under
structure the
under protection
the ofof
protection intumescent coating.
intumescent coating.

3.2.
3.2.Governing
GoverningEquation
Equation
The
The thermalresponse
thermal responseofofthe
theCFST
CFSTstructure under
structure under the protection
the of of
protection thethe
intumescent
intumescent
coating in the fire is a transient heat-transfer process, and the numerical simulation fol-
coating in the fire is a transient heat-transfer process, and the numerical simulation follows
lows the three-dimensional
the three-dimensional unsteady
unsteady heatheat conduction
conduction differential
differential equation:
equation:
∂∂ ∂∂  ∂T ∂∂ 
 ∂T  ∂T
∂T ∂∂  ∂T∂T
((Tc ρ )
Tcρ) = = λ
λ +
+  λ λ +
+  λ λ  (8)(8)
∂∂t
t ∂∂xx  ∂x
∂x  ∂∂yy  ∂y
∂y  ∂∂zz  ∂z
∂z 
where
whereTTmeans
meanstemperature
temperatureininK,K,c cisisthe
thethermal
thermalcapacity
capacityininJ/(kg⋅K), ρ isρ the
J/(kg·K), true
is the density
true density
from
fromthe
thedensity
densityexperiment
experimentininkg/m
kg/m 3 , x,
3, x, y, y,
z denote thethe
z denote coordinate
coordinate system
systemin in
mm and t t
and
represents
representsthe
thetime
timeinins.s.
The temperature change along the axial direction of the CFST structure was much
smaller than that along the radial direction of the structure, so the temperature change
along the axial direction of the structure can be ignored:

∂  ∂T 
λ =0 (9)
∂z  ∂z 
 ∂ ∂ ∂T  ∂  ∂T 
(Tc ρ ) =  λ  + λ  (10)
∂t ∂x  ∂x  ∂y  ∂y 
Buildings 2022, 12, 1014 The solution to Equation (10) requires the thermal property parameters of the intu-9 of 18
mescent coating and the CFST structure. The thermal property parameters of the intumes-
cent coating in this study were obtained through the experiments, and the thermal prop-
erty parameters of the CFSTchange
The temperature were taken
alongbased on GB
the axial 50936-2014
direction [40].
of the CFST structure was much
smaller than that along the radial direction of the structure, so the temperature change
3.3. Initial
alongand
theBoundary Conditions
axial direction of the structure can be ignored:
The initial condition is as follows:  
∂ ∂T
T ( x∂z
, y ) t = 0∂z= T0= 0
λ
(11)
(9)

Substituting
where T0 denotes Equation
the ambient (9) into (8), with
temperature the governing
a value ofequation
293 K. for the thermal response of
the CFST structure under the protection of the intumescent
Solving the above heat-transfer governing equation also requires coating boundary
is obtainedcondi-
as follows:
tions. When the CFST structure is under fire, it is usually understood that external heat is
   
∂ ∂ ∂T ∂ ∂T
transferred to the structure by means ( Tcρ)of=thermal +
λ convection λand radiation, as shown in (10)
∂t ∂x ∂x ∂y ∂y
Figure 11. The boundary conditions can be expressed as:
The solution to Equation (10) requires the thermal property parameters of the intumes-
q = qconv + qrad (12)
cent coating and the CFST structure. The thermal property parameters of the intumescent
wherecoating
q, qconv in this
and qradstudy were respectively,
represent, obtained through the heat
the total experiments, and theheat
flux, convective thermal
flux property
and
parameters
radiative heat flux.of the CFST were taken based on GB 50936-2014 [40].
The convective heat flux is defined as:
3.3. Initial and Boundary Conditions
(
qconv = h f T f − Ts
The initial condition is as follows: ) (13)

T0 2⋅K), the value of hf is in the (11)

T ( x, y)|t=0in=W/(m
where hf is the convective heat-transfer coefficient
range from 10 W/(m2⋅K) to 20 W/(m2⋅K) and 15 W/(m2⋅K) is adopted in the numerical sim-
where
ulation T0 denotes
according the [42].
to Gillet ambient
Tf is temperature with a value
the gas temperature, and Tofs is
293
theK.surface temperature
Solving the
of the intumescent above heat-transfer governing equation also requires boundary conditions.
coating.
When the CFST structure is underasfire,
The radiative heat flux is defined it is usually understood that external heat is trans-
[43]:
ferred to the structure by means of thermal convection and radiation, as shown in Figure 11.
rad sys (
= ε σ Tas:4 − T 4
The boundary conditions can qbe expressed
f s ) (14)
q = qconv + qrad (12)
where εsys denotes the system emissivity with a value of 0.75, and σ is the Boltzmann
constant with 2⋅K4).
where q, qaconv
value
andofqrad
5.67 × 10−8 W/(m
represent, respectively, the total heat flux, convective heat flux and
radiative heat flux.

Figure 11. Boundary conditions of the numerical model.

The convective heat flux is defined as:

 
qconv = h f T f − Ts (13)
 Buildings 2022, 12, 1014 10 of 18

where hf is the convective heat-transfer coefficient in W/(m2 ·K), the value of hf is in the
Buildings 2022, 12, x FOR PEER REVIEW 11 of 20
range from 10 W/(m2 ·K) to 20 W/(m2 ·K) and 15 W/(m2 ·K) is adopted in the numeri-
cal simulation according to Gillet [42]. Tf is the gas temperature, and Ts is the surface
temperature of the intumescent coating.
Figure 11.TheBoundary
radiativeconditions
heat fluxofisthe numerical
defined model.
as [43]:
 
According to the boundary conditions, 4 temperature
4
qrad = ε systhe
σ Tgasf − T s Tf is the main external (14)
factor affecting the heat transfer into the structure. Therefore, it is important to describe
thewhere
temperature-rise
εsys denoteshistory of the emissivity
the system gas temperature
with aaccurately. Various
value of 0.75, andfire
σ isscenarios have
the Boltzmann
some differences
constant with a in the of
value 5.67 × 10−8 W/(m
temperature-rise 2 ·K4 ).The fire scenarios generally have two
models.
forms: (1) fire dominated
According by hydrocarbon
to the boundary substances,
conditions, the gas which is usually
temperature Tf iscaused
the mainby petro-
external
factor
leum; (2)affecting the heatby
fire dominated transfer
fibrous into the structure.
substances, which Therefore, it iscaused
is usually important to describe
by wood, paperthe
andtemperature-rise
textiles. history of the gas temperature accurately. Various fire scenarios have some
differences in the substances
For the fibrous temperature-rise
fire, themodels.
ISO 834Themodel fireisscenarios
a commonlygenerally have two
used model and forms:
can
be(1) fire dominated
expressed as: by hydrocarbon substances, which is usually caused by petroleum;
(2) fire dominated by fibrous substances, which is usually caused by wood, paper and textiles.
For the fibrous substancesTfire, the ISO 834 model t isa commonly used model and can
f = T0 + 345lg  + 1 (15)
be expressed as: 7.5 
t
Figure 12 shows the gas temperature T f = T0 +curve
345lg used + 1 (15)
7.5 in the simulations; it can be seen
from the figure that the gas temperature increased with time.
Figure 12 shows the gas temperature curve used in the simulations; it can be seen from
the figure that the gas temperature increased with time.

1400

1200
Gas temperature(K)

1000

800

600

400

200
0 2000 4000 6000 8000 10000
Time(s)

Figure 12. Gas temperature curve used in the simulations.

Figure 12. Gas temperature curve used in the simulations.
3.4. Treatments of the Nonlinear Problem in the Numerical Simulation
3.4. Treatments of the Nonlinear Problem in the Numerical Simulation
3.4.1. Heat-Absorption Effect in the Pyrolysis
3.4.1. Heat-Absorption
The intumescentEffect coatingin the Pyrolysis
pyrolysis will absorb part of the external heat and thus
The intumescent
reduces coating pyrolysis
the temperature-rise rate of the will absorb part
protected of the so
structure, external heat and thus effect
the heat-absorption re-
duces thebe
should temperature-rise
considered in therate of the protected
numerical simulation.structure, so the
The pyrolysis heat-absorption
is treated effect
as a special phase-
should
changebe process,
considered andinthe
theequivalent
numericalheat simulation.
capacity The pyrolysis
method is usedis to
treated
solve as
thea nonlinear
special
phase-change process, and
problem in the phase change. the equivalent heat capacity method is used to solve the non-
linear problem in theheat
The sensible phase change.p ,e ) is defined as:
capacity(c
The sensible heat capacity(cp,e)is defined as:
c p,s T ≤ Ts
 c p,s −ccp,lp ,s+ L

TsT<≤TTs< Tl

c p,e = (16)
 2 Tl − Ts
 c p ,s − c p ,lc p,l L T ≥ Tl

c p ,e =  + Ts < T < Tl (16)

where cp,s and cp ,l represent, respectively, 2 − Ts heat capacity before and after phase
theTlsensible
change; the value is 1000 J/(kg  ·K) andc p2000 J/(kg·K).T ≥LTis the latent heat; the value is
 ,l l
100 kJ/kg. Ts and Tl denote, respectively, the temperature before and after phase change,
withcvalues
where p,s and cof
p,l 573 K and 873
represent, K.
respectively, the sensible heat capacity before and after phase
change; the value is 1000 J/(kg⋅K) and 2000 J/(kg⋅K). L is the latent heat; the value is 100
kJ/kg. Ts and Tl denote, respectively, the temperature before and after phase change, with
values of 573 K and 873 K.
Buildings 2022, 12, 1014 11 of 18

3.4.2. Nonlinear Size Effect in the Expansion

In the high-temperature expansion performance experiment, the thickness at different
temperatures was obtained. Although the thickness of the coating changed with tem-
perature, a fixed region was still used for the numerical simulation by considering the
efficiency and feasibility. The change in the intumescent coating’s thickness is converted
into the change in the thermal conductivity equivalently, which can simplify the numeri-
cal simulation and reduce the calculation cost. The equivalent conversion processes are
as follows:
(a) Using Equation (1) to calculate the thermal conductivity before expansion and using
Equations (2)–(6) to calculate the thermal conductivity after expansion, the results are
shown in Table 3.
(b) An equivalent thermal conductivity model of the intumescent coatings is adopted to
calculate the thermal conductivity [44]:
Table 3. Thermal conductivity of the intumescent coating.

T (K) 293 373 473 573 673 773 873 973 1073
λs (W/(m·K)) 0.10 0.14 0.19 0.24 0.29 0.34 0.39 0.44 0.49
 
2 2
λ g φ 3 + 1− φ 3 λ s
λeq = λs  2   2

λ g φ 3 − φ + 1− φ 3 + φ λ s
(17)
8
λ g = 4.815 × 10−4 T 0.717 + dεσT 3
3
where λs denotes the intumescent coating’s thermal conductivity, λg denotes the air thermal
conductivity, and λeq denotes the equivalent thermal conductivity. φ indicates the porosity,
d is the average diameter of the pore with a value of 3.495 × 10−3 m, and ε is the intra-pore
emissivity with a value of 0.8. The equivalent thermal conductivity of the intumescent
coating at different temperatures is calculated by Equation (17). The results are shown
in Table 4.

Table 4. Equivalent thermal conductivity of the intumescent coating.

T (K) 293 373 473 573 673 773 873 973 1073
λs (W/(m·K)) 0.10 0.14 0.19 0.24 0.29 0.34 0.39 0.44 0.49
λg (W/(m·K)) 0.04 0.06 0.08 0.12 0.18 0.25 0.34 0.45 0.59
φ 0.514 0.655 0.705 0.722 0.692
λeq (W/(m·K)) 0.10 0.14 0.19 0.24 0.23 0.28 0.35 0.44 0.56

(c) Assuming that the thickness of the intumescent coating remains unchanged, the
thickness change is equivalently converted into the thermal conductivity change by
Equation (18). As a result, the input values in the simulation calculation are obtained,
which can be seen in Table 5:

Table 5. The input value in the numerical simulation.

T (K) 293 373 437 573 673 773 873 973 1073
n 1 1 1 1 3.16 5.35 7.08 7.13 5.71
λ0eq (W/(m·K)) 0.10 0.14 0.19 0.24 0.07 0.05 0.05 0.06 0.10

λeq
λ0eq = (18)
n
where λ0eq represents the input value in the numerical simulation, n denotes the expansion
rate from the expansion experiment, and the value is displayed in Table 1.
 Table 5. The input value in the numerical simulation.

T(K) 293 373 437 573 673 773 873 973 1073
n 1 1 1 1 3.16 5.35 7.08 7.13 5.71

Buildings 2022, 12, 1014

௘௤ (W/(m⋅K)) 0.10 0.14 0.19 0.24 0.07 0.05 0.05 0.06 0.10
12 of 18

3.5. Results and Discussion

3.5.1. Finite Element Model and Feature Point
3.5. Results and Discussion
The
3.5.1. governing
Finite Element equation
Model with initial and
and Feature boundary conditions was solved numeri-
Point
cally using the commercial software Comsol Multiphysics (Version 5.5, Comsol Inc.,
The governing
Stockholm, Sweden). The equation with initial and
quarter-symmetric boundary
model conditions
was adopted was solved
for lower cost. Thenumerically
built-
in grid module was used for grid generation, and the grid structure with a legend ofStockholm,
using the commercial software Comsol Multiphysics (Version 5.5, Comsol Inc., qual-
Sweden).
ity is shownThe quarter-symmetric
in Figure 13. The closer the model
valuewas adopted
to 1, forthe
the better lower cost.
quality Thegrid.
of the built-in
The grid
module was used for grid generation, and the grid structure
total number of grids was 20,334 and the average value was 0.95. The time step in thewith a legend of quality
is shown was
calculation in Figure
0.01 s.13. The14closer
Figure showsthe thevalue to 1,
location of the better the
the feature pointquality
1, whichof the
wasgrid.
used The
total number of grids was 20,334 and the average value was 0.95. The
for numerical analysis. In this section, numerical simulations are carried out to investigate time step in the
the temperature variation of point 1 with time. The effects of initial thickness (0, 2 mm, 3used
calculation was 0.01 s. Figure 14 shows the location of the feature point 1, which was
for numerical
mm, 4 mm, 5 mm), analysis. In thisrate
expansion section,
(0.1 n,numerical
0.2 n, n, 5 simulations are carried
n, 10 n), intra-pore out to (0,
emissivity investigate
0.2,
the temperature variation of point 1 with time. The effects of initial thickness
0.4, 0.6, 0.8, 1) and reaction heat (10 kJ/kg, 100 kJ/kg, 1000 kJ/kg, 5000 kJ/kg, 10,000 kJ/kg, (0, 2 mm,
3 mm,kJ/kg)
20,000 4 mm, are5 studied in detail. rate (0.1 n, 0.2 n, n, 5 n, 10 n), intra-pore emissivity (0, 0.2,
mm), expansion
0.4, 0.6, 0.8, 1) and reaction heat (10 kJ/kg, 100 kJ/kg, 1000 kJ/kg, 5000 kJ/kg, 10,000 kJ/kg,
20,000 kJ/kg) are studied in detail.

Buildings 2022, 12, x FOR PEER REVIEW 14 of 20

Figure 13. Grid structure of the model.

Figure 13. Grid structure of the model.

Figure 14. Location of the feature point.

Figure 14. Location of the feature point.

3.5.2. The Effect of Initial Thickness

Figure 15 shows the temperature variation of point 1 with different initial thick-
nesses. Tables 6 and 7 present, respectively, the temperature and the temperature-rise rate
 Figure 14. Location of the feature point.
Buildings 2022, 12, 1014 13 of 18
3.5.2. The Effect of Initial Thickness
Figure 15 shows the temperature variation of point 1 with different initial thick-
nesses. Tables
3.5.2. The6Effect
and 7ofpresent, respectively, the temperature and the temperature-rise rate
Initial Thickness
of point 1 with different initial thicknesses at different times. It can be seen that tempera-
Figure 15 shows the temperature variation of point 1 with different initial thicknesses.
ture of point 1 was the highest when the initial thickness was 0. This indicates that the
Tables 6 and 7 present, respectively, the temperature and the temperature-rise rate of point
intumescent coating has a thermal insulation effect on the protected structure and can
1 with different initial thicknesses at different times. It can be seen that temperature of
thus reduce the temperature and temperature-rise rate of the protected structure. In addi-
point 1 was the highest when the initial thickness was 0. This indicates that the intumescent
tion, the greater the thickness, the lower the temperature of point 1. This means that the
coating has a thermal insulation effect on the protected structure and can thus reduce the
intumescent coating’s
temperature and thermal insulationrate
temperature-rise performance increases
of the protected with theInincreasing
structure. addition, initial
the greater
thickness. Furthermore, the effect of the initial thickness on the thermal insulation
the thickness, the lower the temperature of point 1. This means that the intumescent perfor-
mance is also related
coating’s thermaltoinsulation
the time interval, and it was
performance foundwith
increases that the
the increasing
best effect occurred in
initial thickness.
the range from 2000–4000
Furthermore, s. of the initial thickness on the thermal insulation performance is also
the effect
related to the time interval, and it was found that the best effect occurred in the range from
2000–4000 s.

Figure 15. Temperature variation over time with different initial thicknesses.

Table 6. Temperature with different initial thicknesses at different times.

Temperature of Point 1 (K)

Time (s)
0 2 mm 3 mm 4 mm 5 mm
500 593.3 473.2 437.4 409.7 387.9
1000 793.1 569.1 524.3 488.7 460.3
2000 1019.0 660.5 608.3 573.5 543.9
4000 1181.7 840.9 744.0 684.8 643.7
10,000 1354.6 1173.5 1078.7 989.9 913.1

Table 7. Temperature-rise rate with different initial thicknesses at different times.

Temperature-Rise Rate of Point 1 (K/s)

Time Interval (s)
0 2 mm 3 mm 4 mm 5 mm
0–500 0.60 0.36 0.29 0.23 0.19
500–1000 0.47 0.19 0.17 0.16 0.14
1000–2000 0.23 0.09 0.08 0.08 0.08
2000–4000 0.08 0.09 0.07 0.06 0.05
4000–10,000 0.03 0.06 0.06 0.05 0.04

3.5.3. The Effect of Expansion Rate

Figure 16 shows the temperature variation of point 1 with different expansion rates.
Tables 8 and 9 present, respectively, the temperature and temperature-rise rate of point 1
 2000–4000 0.08 0.09 0.07 0.06 0.05
4000–10,000 0.03 0.06 0.06 0.05 0.04

3.5.3. The Effect of Expansion Rate

Buildings 2022, 12, 1014 Figure 16 shows the temperature variation of point 1 with different expansion rates. 14 of 18
Tables 8 and 9 present, respectively, the temperature and temperature-rise rate of point 1
with different expansion rates at different times. The expansion rate n was obtained from
the expansion performance experiment. It can be seen that the greater the expansion rate,
with different expansion rates at different times. The expansion rate n was obtained from
the lower the temperature of point 1. This indicates that the intumescent coating’s thermal
the expansion performance experiment. It can be seen that the greater the expansion rate,
insulationthe
performance increased with the increasing expansion rate. This is because the
lower the temperature of point 1. This indicates that the intumescent coating’s thermal
increasinginsulation
expansionperformance
rate led to a longer pathwith
increased for heat transfer. Inexpansion
the increasing addition, rate.
the curves
This isare
because the
very closeincreasing
to each other when the expansion rates were 5 n and 10 n. This
expansion rate led to a longer path for heat transfer. In addition,means thatthe curves
thermal insulation performance
are very close no longer
to each other when significantly
the expansionimproved
rates werewhen the10
5 n and expansion
n. This means that
rate increased to a certain level. In addition, more expansion may lead
thermal insulation performance no longer significantly improved when the to a more fragile
expansion rate
char that may get blown off the surface compared with a thinner, more
increased to a certain level. In addition, more expansion may lead to a more durable char.
fragile char
However, that
this may
paper
getfocuses
blown onoff the heat-transfer
the surface mechanism,
compared and themore
with a thinner, numerical
durablemodel
char. However,
does not include the effects
this paper focusesofon thethe
durability of the mechanism,
heat-transfer char itself. and the numerical model does not
include the effects of the durability of the char itself.

Figure 16. Temperature variation over time with different expansion rates.

Table 8. Temperature with different expansion rates at different times.

Temperature of Point 1 (K)

Time (s)
0.1 n 0.2 n n 5n 10 n
500 467.3 456.9 437.4 430.0 429.0
1000 682.0 625.3 524.3 486.7 483.6
2000 906.7 821.3 608.3 534.0 505.1
4000 1130.1 1074.4 744.0 584.5 565.7
10,000 1330.9 1304.5 1078.7 674.2 622.9

Table 9. Temperature-rise rate with different expansion rates at different times.

Temperature-Rise Rate of Point 1 (K/s)

Time Interval (s)
0.1 n 0.2 n n 5n 10 n
0–500 0.35 0.32 0.29 0.27 0.27
500–1000 0.43 0.34 0.17 0.11 0.11
1000–2000 0.22 0.20 0.08 0.05 0.02
2000–4000 0.11 0.13 0.07 0.03 0.03
4000–10,000 0.03 0.04 0.06 0.01 0.01

3.5.4. The Effect of Intra-Pore Emissivity

Figure 17 shows the temperature variation of point 1 with different intra-pore emis-
sivity. Tables 10 and 11 present, respectively, the temperature and temperature-rise rate
of point 1 with different intra-pore emissivity at different times. The intra-pore emissivity
of 0 means that radiation in the carbon layer was not considered. From the figure, the
 3.5.4. The Effect of Intra-Pore Emissivity
Figure 17 shows the temperature variation of point 1 with different intra-pore emis-
sivity. Tables 10 and 11 present, respectively, the temperature and temperature-rise rate
of point 1 with different intra-pore emissivity at different times. The intra-pore emissivity
Buildings 2022, 12, 1014 of 0 means that radiation in the carbon layer was not considered. From the figure, the15 of 18
greater the intra-pore emissivity, the higher the temperature of point 1. This indicates that
the intumescent coating’s thermal insulation performance decreased with the increasing
intra-pore
greateremissivity. The reason
the intra-pore for this
emissivity, theishigher
that the increase
the in intra-pore
temperature of point emissivity en-
1. This indicates
hances the intro-pore thermal radiation, thereby leading to an increase in equivalent
that the intumescent coating’s thermal insulation performance decreased with the increas- ther-
mal conductivity.
ing intra-poreComparing
emissivity. the
Thetemperature variation
reason for this is that at
theanincrease
intra-pore emissivityemissivity
in intra-pore of 0
and 1,enhances
the temperature difference
the intro-pore reached
thermal 326.3 Kthereby
radiation, at t = 10,000
leadings. This
to anmeans thatin
increase thermal
equivalent
radiation in the
thermal carbon layer
conductivity. formed the
Comparing by the intumescent
temperature coating
variation at intra-pore
at an high temperatures
emissivity of 0
shouldandbe1,considered.
the temperature difference reached 326.3 K at t = 10,000 s. This means that thermal
radiation in the carbon layer formed by the intumescent coating at high temperatures
should be considered.

Figure 17. Temperature variation over time with different intra-pore emissivity.

Table 10. Temperature with different intra-pore emissivity at different times.

Temperature of Point 1 (K)

Time (s)
0 0.2 0.4 0.6 0.8 1
1000 507.3 510.2 517.6 522.5 524.3 527.9
2000 571.5 578.6 592.7 602.1 608.3 610.6
4000 630.5 651.6 692.7 716.6 744.0 772.3
10,000 780.4 878.0 975.1 1020.6 1078.7 1106.7

Table 11. Temperature-rise rate with different intra-pore emissivity at different times.

Temperature-Rise Rate of Point 1 (K/s)

Time Interval (s)
0 0.2 0.4 0.6 0.8 1
0–1000 0.21 0.22 0.22 0.23 0.23 0.23
1000–2000 0.06 0.07 0.08 0.08 0.08 0.09
2000–4000 0.03 0.04 0.05 0.06 0.07 0.08
4000–10,000 0.02 0.04 0.05 0.05 0.06 0.06

3.5.5. The Effect of Reaction Heat

In the calculations, the latent heat L represents the reaction heat, but L does not appear
in the thermal governing equation (Equation (8)). Therefore, the equivalent heat capacity
method (Equation (16)) was used to transition. Figure 18 shows the temperature variation of
point 1 with different reaction heats. Tables 12 and 13 present, respectively, the temperature
and temperature-rise rate of point 1 with different reaction heats at different times. The
reaction heat represents the intumescent coating heat-absorb effect due to physical and
chemical changes. From the figure, the greater the reaction heat, the lower the temperature
of point 1. This indicates that the intumescent coating’s thermal insulation performance
increased with the increasing reaction heat. The reason for this is that the heat-absorb
 variation of point 1 with different reaction heats. Tables 12 and 13 present, respectively,
the temperature and temperature-rise rate of point 1 with different reaction heats at dif-
ferent times. The reaction heat represents the intumescent coating heat-absorb effect due
to physical and chemical changes. From the figure, the greater the reaction heat, the lower
the temperature of point 1. This indicates that the intumescent coating’s thermal insula-
Buildings 2022, 12, 1014 tion performance increased with the increasing reaction heat. The reason for this is that16 of 18
the heat-absorb effect led to a decrease in temperature rate. However, the effect of the
reaction heat on the thermal insulation’s performance is limited. Form the figure and ta-
bles, the maximum
effect temperature
led to a decrease difference rate.
in temperature is 68.9 K at t = 1151
However, s when
the effect thereaction
of the reactionheat
heaton the
thermal
increases frominsulation’s performance
10 kJ/kg to 10,000 kJ/kg. is limited. Form the figure and tables, the maximum
temperature difference is 68.9 K at t = 1151 s when the reaction heat increases from 10 kJ/kg
to 10,000 kJ/kg.

Figure 18. Temperature variation over time with different reaction heats.

Table 12. Temperature with different reaction heats at different times.

Temperature of Point 1 (K)

Time (s)
10 kJ/kg 100 kJ/kg 1000 kJ/kg 5000 kJ/kg 10,000 kJ/kg
1000 525.3 524.3 515.7 481.5 456.6
2000 610.2 608.3 603.1 577.3 546.1
10,000 1080.16 1078.7 1077.7 1074.2 1066.2

Table 13. Temperature-rise rate with different reaction heats at different times.

Temperature-Rise Rate of Point 1 (K/s)

Time Interval (s)
10 kJ/kg 100 kJ/kg 1000 kJ/kg 5000 kJ/kg 10,000 kJ/kg
0~1000 0.23 0.23 0.22 0.19 0.16
1000~2000 0.08 0.08 0.09 0.10 0.09
2000~10,000 0.06 0.06 0.06 0.06 0.07

4. Conclusions
Expansion performance and thermal physical property experiments were carried
out to obtain the basic data of intumescent coating at high temperatures. The thermal
response model of the CFST structure under the protection of intumescent coating in a fire
was established, and the effects of initial thickness, expansion rate, intra-pore emissivity
and reaction heat on the structure’s temperature were discussed based on the numerical
simulation. The following conclusions could be drawn:
(1) The thickness of the intumescent coating stayed the same at low temperatures, then
increased rapidly with the increasing temperature, finally decreasing due to oxida-
tion at high temperatures. The thermal conductivity increased with the increasing
temperature, and the calculation equations at different temperature were obtained.
(2) The initial thickness had a positive effect on the intumescent coating’s thermal insu-
lation performance. As the initial thickness increased, the thermal insulation perfor-
mance improved.
Buildings 2022, 12, 1014 17 of 18

(3) The expansion rate had a remarkable effect on the intumescent coating’s thermal insu-
lation performance, but the effect was limited when the expansion rate increased to a
certain level. In the material formulation design, appropriately increasing the quantity
of the foaming agent could effectively improve the thermal insulation performance.
(4) The intra-pore emissivity had a negative effect on the intumescent coating’s thermal
insulation performance. Thermal radiation in the porous carbon layer strength-
ened the coupled heat transfer. In the material-formulation design, specific fillers
could be used to decrease the intra-pore emissivity, thereby improving the thermal
insulation performance.
(5) The reaction heat hd a slightly positive effect on the intumescent coating’s thermal
insulation performance. In the material formulation design, modifying the com-
ponents could strengthen the heat-absorption effect, thus improving the thermal
insulation’s performance.

Author Contributions: Conceptualization, Y.H. and M.L.; methodology, L.Z.; software, L.Z.;
validation, Y.H., L.Z. and M.L.; formal analysis, L.Z.; investigation, Y.H.; resources, L.Z.; data
curation, L.Z.; writing—original draft preparation, L.Z.; writing—review and editing, L.Z.; visualiza-
tion, L.Z.; supervision, Y.H.; project administration, M.L.; funding acquisition, M.L. All authors have
read and agreed to the published version of the manuscript.
Funding: This research received no external funding.
Conflicts of Interest: The authors declare no conflict of interest.

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