Heat Transfer and Multiphase Flow with Hydrate Formation in Subsea Pipelines
A. Odukoya *, G. F. Naterer
Faculty of Engineering and Applied Science Memorial University, St. John’s, Newfoundland St. John’s, Newfoundland, Canada * Email: aodukoya@mun.ca
Abstract — This study presents a new semianalytical model to predict hydrate formation in subsea pipelines. The numerical formulation is based on a nondimensional analysis, allowing the model to be extended to various pipeline lengths and environmental conditions. The effects of change in heat transfer ratio (HTR), and pipe diameter on hydrate formation are reported in this paper. The results indicate that higher HTR between the internal and external fluids reduces the formation of hydrates which may lead to a blockage in the pipeline. The numerical results are validated against experimental results for R134a hydrates. The pipes with smaller diameters are found to reduce the possibility of hydrate formation at a constant pipeline pressure. The results show that at temperatures below 10 ^{o} C, changing thermophysical properties have limited impact on the rate of hydrate formation in the pipe.
— transfer; Phase change
Keywords
Hydrates;
Pipelines;
Multiphase
I.
INTRODUCTION
flow;
Heat
The exploration of oil and gas in deep waters and harsh environments has motivated research on multiphase flows in subsea pipelines. This requires detailed understanding of the heat and mass transfer of the oil / gas / water phases in the pipelines. One of the technical challenges remains predicting and preventing the formation of hydrates in the pipelines to ensure the flow assurance in pipelines. The environment temperature could be as low as 20 ^{o} C, which falls within hydrate forming temperatures. Hydrates are formed when the temperature falls below 303K at ambient pressure, and the specific structure formed is dependent on the type of gases flowing through the pipeline. Hydrates act like solid particles in a flow stream and if not controlled could impede the flow in the pipeline. Thermodynamic inhibitors (such as MeOH) are commonly used to prevent hydrate formation in crude oil pipelines. Other methods of reducing the hydrate formation include the use of kinetic inhibitors, low dosage hydrate inhibitors and antiagglomerates. Heated pipelines are also used to prevent hydrate formation in short pipeline networks.
The flow of hydrates in a pipeline is a multiphase flow heat transfer problem. The nucleation of the hydrate is the first step in the hydrate formation. The nucleation process has been extensively studied in past literature [14]. The hydrate starts to grow as soon as nucleation is sustained. Some of the
established models for predicting nucleation of hydrates include EnglezosKalogerakisDhalabhainBishno [5], SkovborgRasmussen [6], HerriPicGruyCournil [7], and GuanendranAmin [8] models. These studies have investigated the formation of hydrates taking into consideration the kinetics of the hydrate formation. But few studies have analyzed the combined effect of heat and mass transfer on hydrate formation. Kwon et al. [9] developed a numerical model for a fourphase fluid hydrodynamic model for oil, water, gas, and hydrates. The numerical model was solved using a fully implicit finite difference analysis. Nemeto and Balino [10] developed a numerical model for risers in oil pipelines to examine severe slugging in a mixture oil, gas, and water. The riser model considered in the latter study is a onedimensional isothermal flow and the results show nonlinearity in the fluid flow in the riser. A theoretical analysis of heat and mass transfer for interacting multiphase mixtures was outlined by Niessner and Hassanizadeh [11]. The model is well suited for nonisothermal conditions with heat transfer between phases. Shagapov et al. [12] developed a quasi –stationary model for gas hydrate dissociation in a horizontal pipe. The model shows a buildup of the hydrate toward the inlet of the pipe and indicates that the use of methanol for hydrate dissociation has limited impact on the rate of hydrate formation beyond a certain threshold during the coagulation. This paper aims at developing a new integral formulation to predict the growth of hydrates in multiphase flows.
Tolubinskiy [13] developed a general solution for transient nonlinear heat and mass transfer problems using an integral method. The solution is restricted to coupled heat and mass transfer problems, where the function of the heat source is defined as a unit pulse from experimental measurements. Mennig and Ozisik [14] developed an analytical model to account for time dependent surface conditions during heat transfer in solidification and melting. Dorstewitz and Mewes [15] reported experimental and analytical results on R134a hydrate formation in a pipe. Although heat transfer was considered in this study, the hydrate layer was modeled as a uniform layer on the ice wall. Unlike the model of Dorstewitz and Mewes [15], this paper includes the effects of the deposition of solid particles on the pipe wall, by considering both the kinetic energy of the particle and the coagulation of the hydrate layer over time. Vaze and Banerjee [16] developed experimental correlations for determining heat transfer
9781479949182/14/$31.00 ©2014 IEEE
coefficients in twophase flows. The results indicate that the heat transfer coefficient could be determined from a known Nusselt number of the flow regime.
The growth of the hydrate layer is determined by the ability of the particles to adhere to the pipe walls when formed. The particles could move along with the fluid flow or decelerate and adhere to the wall. The irregular shapes formed during solidification of particles can be defined by imposing boundary conditions and solving heat and mass balances at the defined boundaries [17]. Elperin and Fominykh [18] developed a gas – liquid slug model to predict the formation of gas hydrates, assuming perfect mixing liquid plugs. The result indicates that the heat and mass transfer of an infinite linear cluster of slugs is independent of the initial temperature. Jassim et al. [19] proposed a numerical model to determine the deposition of gas hydrate particles. A computational fluid dynamics (CFD) model taking into account the nucleation and growth of gas hydrates was used to determine the deposition mechanism of the particle. A new analytical approach is presented in this paper to determine the growth of the hydrate layer based on the deposition mechanism.
The heat transfer from the fluid in the pipe to the environment is often neglected in past models in the literature [20]. A phase change heat transfer model of Naterer [21] was incorporated into an ice growth model, to account for the heat transfer across the wall. This model is used to determine the effect of the kinetic energy of a droplet on the heat transfer across the wall. A numerical model simulating the fourphase (oil, gas, water and hydrate) flow in crude oil pipelines in the North Sea was proposed by Kwon et al. [9]. The various regions in the flow were computed using a dew point pressure line, freezing point line, and hydrate dissociation pressure line. The results were used to estimate the range of temperature and pressures that best represent the offshore pipeline temperatures.
The potential hazards of wax formation are a result of hydrate formation and mitigation techniques were reviewed by Ayejina et al.[22]. One of the current methods of preventing wax formation includes heating the pipeline beyond the hydrate formation temperature. Another established method in the oil and gas industries is the addition of kinetic inhibitors [23] to prevent the growth of hydrates. By understanding the deposition mechanism in relation to heat transfer, the kinetic inhibitors could be reduced. This paper develops a new analytical model to analyze the effects of temperature gradient and pipeline radius on the flow of the hydrate particles. This paper specifically focuses on R134a hydrates to allow for comparison with past data of Dorstewitz and Mewes [15].
II. HEAT AND MASS TRANSFER FORMULATION
A force balance on a hydrate particle is used to determine the velocity of the particle. The forces acting on the particle are highlighted in Fig. 1. Jassim et al. [19] developed a bouncing particle model to predict the forces acting on the particle. This paper extends the bouncing model to include both heat transfer and kinetic energy of the particle. When hydrate particles moving at low velocity come into contact with the pipe wall, the kinetic energy of the particle is reduced and heat is transferred across the pipe wall along with adjacent particles.
Fig. 1.
lift, gravity, and adhesive forces respectively
Schematic of problem description; FD, FL, FG, and FA are the drag,
At high velocity of the particle, it is assumed that the particle is plastically deformed. This model assumes that beyond a critical velocity, the particle will bounce and flow with the fluid. The critical velocity for the bouncing model was estimate by Friedlander et al. [24],
u
cr
⎡
= ⎢
⎣
2 σ
⎛
⎜
⎝
1 −
2
β
m
2
β
⎞⎤
⎟⎥
_{⎠}_{⎦}
0.5
(1)
where _{σ} is surface potential energy, β is the restitution coefficient, and m is the mass of the particle. The surface potential energy is defined as:
σ =
dH
12 z
o
(2)
where H is the Hamaker constant, z _{o} is the distance between the particle and the wall at steady state, and d is the diameter of the hydrate particle.
The heat transfer associated with phase change during hydrate formation is analogous to a convective heat transfer problem with initial superheat boundary conditions. The hydrates resemble freezing ice droplets in a flowing stream. Several analytical methods have been used to solve the classical phase change problem with initial boundary conditions [2529]. This paper expands on integral solutions presented by Wang and Cheng [30] by taking into account the growth of the hydrate particle using the bouncing model proposed by Jassim et al. [19]. The problem is formulated as phase change of a twophase fluid using the integral solution of a boundary layer. The temperature variation is assumed to be axisymmetric. The heat conduction equation for the hydrate layer is:
∂∂⎛
1
rr ∂∂ ⎝ ⎜
T
⎞
⎟ ⎠
1
∂
T
r
α
∂ t
r
=
(3)
where r is the internal radius of the pipe, T is the internal temperature of the fluid, and t is time. The transient term is reduced using Leibnitz’s rule and Eq. (3) is written as:
∂
r
∫
r
∂ r
f
∂
t
f
⎡
_{⎢}
⎣
α
rT
(
r t
,
)
∂
r
+
r T
r
f
∂
∂ Tr t
o
t
(
f
,) ⎤
_{⎥}
⎦
r
∂ Trt (,)
−−=
∂ r
f
∂ r
0
(4)
where r _{f} is the hydrate radius and T _{o} is the initial temperature of the fluid in the pipe. Nondimensionalizing Eq. (3) using
θ
=
T T o
− T
T f
o
− θ =
and
r
∫
r
f
rθdr
, Eq. (4) is reduced to:
d θ
dt
dr
f
⎡
⎢
⎣
∂
θ
(,)
r t
+−
α
rrr
f
dt
∂
r
−
f
∂
θ
f
r
( r
∂
,) ⎤
t
⎥
⎦
= 0
(5)
where θ is the dimensionless temperature, α is the thermal diffusivity of the fluid, and T _{f} is the final temperature of the fluid. Assuming an axisymmetric temperature distribution, the dimensionless temperature can be represented as a logarithmic function of r:
θ =
a
+
b
ln
(
r
/
r
f
)
ln
(
R
o
/
r
f
)
(6)
where a and b are proportionality constants, and R _{o} is the external radius of the pipe.
Using the following boundary conditions, Eqs. (4) and (6) can be solved as:
(
θ r
f
,)
t
=
1
(7)
∂ ∂ 
θ θ 
( , ) r t ∂ r ( r r , t ) 
) 
) 
= = ( h ) 1 r t k θ , l ρ v 
dr 
f 

h 
∂ r 2 θ 
( kT f θ − 
T o 
) 
dt l ρ 
v 

−− 

k 
( sup 
( r f , t )) 
+ 
2 
( T f 
− 
T o 
) 
u
3
p
(8)
(9)
where h _{1} and h _{2} are the external and internal convective heat transfer coefficients respectively, k is the thermal conductivity,
of
vaporization,
and u _{p} is the particle velocity. The fluid flow stream inside and outside the pipeline are defined by the following Biot numbers. The internal Biot number will vary based on the thickness of the hydrate layer, while the external Biot number is assumed to be constant in this study. This allows the model to be extended to any pipe dimension following similar boundary conditions.
ρ
is
the
density
θ
sup
of
the
fluid,
l _{v}
is
the
latent
heat
is the dimensionless superheat temperature,
Bi
f
Bi
r
=
=
h r
2
f
k
hr
1
k
(10)
(11)
Here Bi _{f} and Bi _{r} are the internal and external Biot numbers respectively.
The Biot number and dimensionless time are useful to analyze the growth of the hydrate layer for ease of comparison with experimental data and extending the model to various hydrate structures. To further simplify the solution for the non dimensional temperature, the phase change number (reciprocal
of Stefan number), heat transfer ratio (HTR) and dimensionless time are introduced in Eq. (5). These terms are given as:
P
h
θ
hr
=
=
αρ
l
v
(
kT
f
− T
a
h
2
h
1
(
θ
sup
−
)
1 )
(12)
(13)
η =
2
h
1
t
α
k
2
P
h
(14)
where P _{h} is the phase change number, the dimensionless time.
Using the nondimensional parameters (Eq. (1214)) and the boundary conditions (Eq. (79)) each term in Eq. 5 can be reduced. Integrating,
is the HTR, and η is
θ hr
θ
2
t
( ) −
2
r f
2
(15)
The first term in Eq. (5) is written as:
d
θ
dt
d
θ
dr
f
=⋅= r
dr
f
dt
f
dr
f
dt
(16)
Similarly, the third term in Eq. (5) is written as:
⎡
⎢ Bi
Bi
f
⎛
⎜
⎜
⎝
⎞
⎟
⎠ ⎟
l
ρ
v
dr
f
⎢ α ⎢
⎢
⎢
⎢
⎣
−
r
h
2
h
1
h
1
(
T
f
−
T
a
)
dt
Bit
f
sup
(
θ
−+
( )
θ
)
Bi
f
l
ρ
v
h
1
2
(
T
f
−
T
a
)
( t ) −
θ
u
3
p
⎤
⎥
⎥
⎥
⎥
⎥
⎦ ⎥
(17)
Substituting Eqs. (15) and (17) in Eq. (5) and rearranging
⎛
⎜
⎝
2
r
f
−
Bi P
fh
⎞
⎟
⎠
dr
f
h
1
dt
⎡
⎢
⎢ ⎣
αθ
Bi
r
( t )
−
Bi
f
θ
hr
+
+
Bi
f
l
ρ
v
h
1
2
(
T
f
−
T
a
)
u
3
p
⎤
⎥ =
⎥ ⎦
0
(18)
The effect of nondimensional time is introduced in Eq. (18) by using the following relationship:
dBi
dr
f
=
f
dt
d
η
d
η
⋅⋅
dt
dr
f
dBi
f
(19)
Substituting the expression for θ (Eq. (7)) in Eq. (18) the final expression for the effect of nondimensional time on Biot number can be written as:
⎛ ⎜ 
P h ⎞ ⎟ 
3 1 h 
dBi f 

− 
Bi 
α 
+ 

⎝ r f ⎡ 
f 
h 1 ⎠ 
3 kP h 
d η 

⎢ ⎢ 
Bi 
r 

α ⎢ ⎢ ⎢ ⎣ 
Bi r 
+ 
1 

ln 
( Bi 
r / Bi 
f ) 
ln 
( Bi 
r 
/ 
Bi f 
) 
2 
θ
++
f
hr
Bi
⎤
* ⎥
⎥
⎥
h 1 ⎥
⎥ ⎦
Bi U
f
(20)
= 0
where
U
*
=
l
ρ
v
2
(
T
f
−
T
a
)
u
3
p
.
The growth of the hydrate layer is dependent on kinetic energy of the particle. Using the bouncing model proposed by Jassim et al. [19], the particle size of the hydrate can be expressed as:
∂
(
nrt
f ,
)
+
∂
∂
t
∂
r
f
(
Irtnrt
f
,
f
,
(
)(
)
)
= 0
(21)
where n is the particle size distribution and I is the growth rate of a single particle which can be expressed as:
Irt
f
(
, )
=
h
1
4
π r ρ
f
2
dm
dt
(22)
The hydrate particle velocity is based on an equation of motion taking into account the free stream velocity of the fluid and can be written as:
u
pv (
∞
=−
ugτ
)(
1
−
exp
())
−
/
t τ
v
(23)
τ
v
=
2
ρ d C
hh
h
18 μ
where
bouncing model, the particle will remain on the surface if the distance of the particle from the wall is less than the boundary layer thickness determined by the critical velocity in Eq. (1). The particle velocity in Eq. (23) is used to determine the kinetic energy of the particle. The diameter of the hydrate is estimated from the previous time step by estimating the growth rate with a combination of mass transfer and kinetic reaction of the particle developed by Jassim [31],
is the residence time. In relation to the
r
p
i
−= r
p
i − 1
λ
Am
s
w
(
f
−
f
eq
)
+
⎛
⎜
⎝
n ShDm
v
w
⎞
⎟
⎠
⎛
⎜
⎜
⎝
y
−
y
eq
3000
ρ
h
ρ
2 r
lp
i − 1
⎞ ⎟ ⎟ ⎠
(24)
where f is the fugacity, λ is the kinematic constant, Sh is the Sherwood number for mass transfer, n _{v} is the vapor molar
density, m _{w} is the molar mass, y is the molar fraction, and A _{s} is the reaction surface. The first term on the right side of Eq. (24)
is the reaction kinetics component of the growth of the particle,
while the second term is associated with mass transfer.
The system of Eqs. (1), (20), (23), and (24) are solved using
a NewtonRapson algorithm to determine the growth of the
hydrate in terms of the dimensionless Biot number at each time step. The numerical model was used to investigate how key dimensionless quantities and physically measureable quantities
such as temperature (fluid, environment, and interface temperature), and pipe radius affect the hydrate growth.
III. RESULTS AND DISCUSSION
The predicted result is compared against experimental conditions reported by Dorstewitz and Mewez [15] for R134a hydrates. The assumptions for both the numerical and experimental studies are shown in Table I. The parameters which affect the hydrate formation include the temperature of the surrounding environment, fluid temperature, heat transfer characteristics of the fluids internal and external to the pipeline,
and the internal radius of the pipe. The model assumed that the thickness of the pipe has minimal effect on the heat transfer between the flowing stream and the external fluid.
TABLE I.
VARIABLES IN NUMERICAL MODEL
Volumetric density of hydrate 
302.4 
kJ/mol 
Thermal conductivity R134a 
4.35 W/mK 

Latent heat of hydrate formation 
1996 kJ/kmol 

Vapour molar density 
0.067 
mol/m ^{3} 
Reaction surface area 
0.0000375m ^{2} 

Fugacity at equilibrium temperature 
11.9 
Pa 
Kinematic constant 
3600 

Sherwood number 
2 

Molecular weight 
102.3 
mol/kg 
Molar fraction at equilibrium (y _{e}_{q} ) 
2.49x10 ^{}^{3} 
The effect of varying the HTR between the fluid in the environment and R134a/water mixture is shown in Fig. 2. The onset region in Fig. 2 is the region where hydrate nucleation takes place with no significant growth in the hydrate. An increase in the HTR reduces the thickness of the hydrate layer as a function of dimensionless time. At the highest HTR (10), the maximum thickness is approached in a short time as a result of rapid cooling of the fluid beyond the hydrate forming temperature. Increasing the HTR reduces the thickness of the hydrate layer.
The heat transfer coefficient of the fluid flowing in the pipe
can be increased to reduce the possibility of the hydrate,
leading to blockage in the pipe. Although the outer heat transfer coefficient cannot be controlled in practice, reducing the heat transfer coefficient of the surrounding fluid can achieve a similar result. The thickness of the hydrate layer is dependent on the variation of the phase change number in the transient flow regime (Fig. 3). The phase change number can be varied by either the superheat temperature or the HTR. The driving force for the hydrate formation is the temperature difference between the fluid and phase transition temperature.
Fig. 2.
Effect of HTR on hydrate growth (external temperature 3 ^{o} C)
As the superheat temperature increases, the heat transfer to the hydrate layer also increases, reducing the growth rate of the hydrate layer. The hydrate layer thickness increases by a factor of 4 when the phase change number is reduced by 25%, as the hydrate layer approaches steady state. The phase change number has minimal effect on hydrate formation when the hydrate thickness approaches steady state.
Fig. 3. Effect of phase change number on hydrate formation (pipe diameter 0.3m and external temperature 3 ^{o} C)
The effect of changing environmental conditions for specific internal flow is shown in Fig. 4. Changing the external Biot number can be accomplished by a variation in the heat flux or thermal conductivity. The peak of each curve is the instance at which the hydrate completely fills the pipeline diameter and impedes the flow of the fluid. At very low Biot numbers, it takes a longer time for the hydrate to completely impede the fluid flow. This will indicate that pipes with external surfaces with very high thermal conductivity could reduce the hydrate formation in the pipe. The regions beyond the peak in each curve in Fig. 4 are nonphysical, where the model is no longer applicable, since the hydrate cannot grow beyond the actual pipe diameter.
The numerical model was validated by comparing the results with experimental results reported by Dorstewitz and Mewez [15] for R134a hydrates (Fig. 5). The comparison shows that the predicted model in this paper is more accurate at higher dimensionless times.
Fig. 4.
inlet temperate 5 ^{o} C and pipe diameter of 0.15m)
Effect of change in external Biot number on hydrate formation (fixed
The initial discrepancy at earlier times occurs because the model does not include the initial velocity of the hydrate particle in the results of Dorstewitz and Mewez [15]. Performing a sensitivity analysis of the result, about an 8% error is observed in comparison to the experimental results at early dimensionless time. The difference between numerical and experimental results is about 1% as the dimensionless time approaches 0.5. Accounting for the hydrate particle velocity in the model is important in predicting the hydrate formation as in Fig. 5. The rate at which the hydrate blocks the flow stream is better predicted with the present model.
Fig. 5.
Comparison of predictions with experimental data for R134a hydrates
The effect of fluid flow temperature on the hydrate formation is shown in Fig. 6. In order to compare the results with experimental data in this case, similar operating conditions used by Dorstewitz and Mewez [15] were adopted in the analysis. The temperature of the internal fluid is fixed at 5 ^{o} C and the external temperature is varied between 3 and  20 ^{o} C in Fig. 6. As expected, the hydrate formation occurs faster in the colder environment. The rate of hydrate formation between temperatures of 3 and 10 ^{o} C increased by about 53%. The increase in the rate of hydrate formation between 10 and  20 ^{o} C is less significant with only a 7.3% variation. For the same internal fluid, hydrate mitigation techniques at extreme temperatures will be more expensive with limited design modifications to reduce the cost of mitigation techniques.
Fig. 6. Effect of changing external environment temperature on hydrate formation (supply temperature of 5 ^{o} C and a pipe diameter of 0.15m)
A change in the superheat temperature is a function of the interface temperature between the hydrate and fluid boundary.
The internal and external fluid temperatures are kept constant,
while the interface temperature is varied in Fig. 7. The
maximum variation in Biot number is about 0.5%, which
indicates that interface temperature has no significant effect on
the rate of hydrate formation. The dimensionless superheat
temperature
⎛
⎜
⎜
⎝
θ
sup
=
T
sup
−
a
T ⎞
⎟
⎟
T
f
−
T
a
⎠ is used to determine the superheat
temperature based on the HTR. The HTR in Eq. (13) is used to determine the dimensionless superheat temperature. The relationship between the dimensionless superheat temperature and the HTR clearly indicates that the dimensionless temperature is dependent on the ratio of the heat transfer coefficient between the internal and external fluids.
Fig. 7. Effect of superheat temperature on hydrate formation (external temperature of 3 ^{o} C and pipe diameter of 0.15m)
The effect of the pipe radius on the hydrate formation
is shown in Fig. 8. A change in pipe radius between 15 and 60
mm increased the rate of hydrate formation by about 85% for
the range of dimensionless time in this study. As the radius of the pipe increases, there is an increased flow of heat to the surrounding fluid due to the increased surface area in contact
with the environment.
Fig. 8. Effect of changing pipe diameter on hydrate formation (external temperature of 3 ^{o} C)
The effect of internal radius on the rate of hydrate formation increased at larger diameters, as a 52% increase is observed from a change of 50 and 60mm. This indicates an
optimal diameter can be determined using this model for a specific region of operation.
IV. CONCLUSIONS
A new predictive model in this paper can be used to account for hydrate formation in pipelines. The semianalytical models use reduced computational resources compared to a CFD analysis. The numerical model can be extended to handle mixtures of hydrates by taking into account mixture densities. If the temperature of the environment reduces below 10 ^{o} C, modifying any of the thermodynamic factors produces less impact on reducing the hydrate formation. Minimizing the radius of the pipe reduces the rate of hydrate formation in the pipe. The numerical model presented in this paper provides a useful predictive tool to analyze hydrate formation in real time, as this will allow for integration into existing hydrate monitoring devices.
ACKNOWLEDGEMENTS
Financial support from the Natural Sciences and Engineering Research Council of Canada (NSERC), and Research and Development Cooperation of Newfoundland and Labrador, is gratefully acknowledged.
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Carslaw,
J.C.
Jaeger,
Conduction
of heat
in
solids,
Oxford:
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