Journal of Petroleum Science and Engineering

Volume 135, November 2015, Pages 461-465

Determination of elemental sulfur deposition rates for

different natural gas compositions
J.P.L. Santos a , A.K.C. Lima Lobato b , C. Moraes c , L.C.L. Santos d

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https://doi.org/10.1016/j.petrol.2015.10.011
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Highlights
• In this study, a nucleation rate profile was determined for several gas streams.

• It was demonstrated that the amount of sulfur deposited in unrestricted

pipeline is small.
 • Serious problems of elemental sulfur deposition occur on restrictions in
pipelines.

• The composition of the gas stream influences the nucleation rate profile.

Abstract
Natural gas is increasing its share in the worldwide energy market. However, it poses several problems during
transportation. The formation and deposition of elemental sulfur (S8) in pipelines is the issue that has the greatest
impact on both operational safety and maintenance costs. The formation of S8 as a yellow powder may be influenced
by changes in operational conditions, such as pressure and temperature drops, and by the composition of the natural
gas stream. This study aims to examine the contribution of the nucleation phenomenon to the process of S8 formation
and deposition. Simulations were performed using the HYSYS® V7 process simulator, with the Peng-Robinson equation
of state, and a MATLAB routine was devised to calculate the variables affecting the nucleation rate. The influence of
natural gas composition on the nucleation rate was evaluated using thermophysical data of average gas streams from
fields of the Brazilian states of Ceará/Rio Grande do Norte (CE/RN), Espírito Santo (ES), Rio de Janeiro (RJ) and Bahia
(Fazenda Mamoeiro Field, FSP). The results show that gas composition and operational conditions may influence the
amount of sulfur deposited in the pipelines, and the nucleation rate increases by reducing the temperature.

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Keywords
Natural Gas; Simulation; Elemental sulfur; Desublimation; Nucleation
1. Introduction
Natural gas is increasing its share in the worldwide energy market because of industrial growth. Therefore, concerns
about environmental risks and safety issues during its transportation and distribution must be taken into account.
Several problems may occur during natural gas transportation, particularly the formation and deposition of elemental
sulfur (S8) in pipelines, which has high impact on both operational safety and maintenance costs.

Deposition of S8 in pipelines is an increasingly observed and studied phenomenon. Santos et al. (2013) stated that the
formation and deposition of sulfur in pipelines can cause serious consequences for the production, processing,
operation and transportation of gas. Pipe blockage caused by sulfur deposition and corrosion caused by perforated
pipes and damaged equipment failure can seriously affect the normal operation of the field, resulting in low production
or even shutdowns (Zhou et al., 2013).

Taylor and Kimtantas (2014) reported that solid elemental sulfur deposits can accumulate and cause flow constriction,
thereby reducing the separation capacity of the equipment. They can plug instrumentation connections, cause poor
process control, and require additional maintenance costs. Chesnoy and Pack (1997) have shown that elemental sulfur
deposition onto measurement instruments may cause errors of up to 2%, or even higher in some cases, on the readings
of transported gas volumes.

Pack et al. (2013) discovered that trace amounts of sulfur vapor in the gas stream could create elemental sulfur deposits
in the gas stream during local depressurization, as occurs in metering devices, through the process of desublimation,
and hence adversely impact the flow measurement accuracy.

According to Pack (2005) and Cézac et al. (2008), nucleation is the most probable mechanism to promote sulfur
deposition in natural gas pipelines. According to these authors, the process of sulfur formation and deposition basically
comprises three nucleation steps, namely particle formation, coagulation and/or condensation (particle growth), and
deposition.
Zhu et al. (2011) concluded that temperature is the dominant parameter affecting condensate formation, whereas
pressure is the dominant parameter for desublimation. In general, natural gas transportation systems operate with high
flow rates, low temperature drops (due to thermal insulation) and high pressure drops (because of turbulent flow).
Unless there is a sudden local temperature drop in the system, pressure variation seems to be an important parameter
to describe the deposition mechanism. Thus, the mechanism of elemental sulfur deposition via nucleation and
desublimation seems to be more probable.

Studies by Pack et al. (2012) validated by actual data on the deposition locations of elemental sulfur in pipelines show
that flow dynamics in pipelines with “T” junctions may be an important parameter affecting preferential deposition in
specific locations such as valves.

The problem has become more evident as natural gas consumption has increased, and has created significant operation
and maintenance problems, resulting in high costs for the industry. Thus, the understanding of the problem and the
consequent search for a solution are very important for the operation of natural gas transportation systems. Solving the
problem can help to reduce maintenance costs and lessen the need for internal equipment inspections.

Nucleation has been mentioned as one of the factors that may contribute to sulfur formation and deposition (Pack,
2005, Cézac et al., 2008). However, studies on the nucleation process are still just beginning, and more research is
needed. Therefore, investigating the mechanism of elemental sulfur formation is part of the objective of this work, and
the aim is to better understand the contribution of the nucleation phenomenon to the process of S8 formation and
deposition.

2. Methodology
The simulations in this work were performed using the HYSYS® V7 process simulator, using the Peng-Robinson
equation of state, and a MATLAB® program version R2010a was used to determine the nucleation rate. The
methodology used for the simulations in the HYSYS® was the same used by Pack (2005). Information about the
operational conditions of the Fazenda Mamoeiro Field, which belongs to the Field-School Project (FSP) of the Federal
University of Bahia, allowed the simulations to be performed using actual parameters, such as natural gas composition,
operating pressure and temperature conditions. The influence of natural gas composition on the homogenous
nucleation rate was evaluated using thermmophysical data of average gas streams produced in the fields of the
Brazilian states of Ceará/Rio Grande do Norte (CE/RN), Espírito Santo (ES), Rio de Janeiro (RJ) and Bahia (Fazenda
Mamoeiro Field, FSP), as shown in Table 1.

Table 1. Composition of natural gas samples used in the simulations

Composition (% vol) CE/RN ES RJ FSP

Methane 74.53 88.16 79.69 69.79

Ethane 10.40 4.80 9.89 14.33

Propane 5.43 2.75 5.90 6.24

i-Butane 0 0 0 1.15

Butane 2.81 1.55 2.13 1.83

Pentane 1.30 0.44 0.77 1.14

C6+ 1.40 0.44 0.44 0.49

Nitrogen 1.39 1.62 0.80 3.19

CO2 2.74 0.24 0.50 1.51

O2 0 0 0 0.33

H2S (mg/m³) 1.50 7.50 6.70 7.60

Source: Vaz et al. (2008), modified.

Nucleation in natural gas transport is the process by which small nuclei grow and disperse, until they reach a certain
size (critical nucleus) that enables the continuous growth of crystals. The nucleation process is a microscopic
phenomenon that involves from tens to thousands of molecules, so it is difficult to observe it experimentally in
pipelines.

Zhu et al. (2011) showed that the precipitation of elemental sulfur does not occur immediately at the point in the
pipeline where the gas stream flows. At this point, the initial concentration of sulfur in the vapor phase reaches the
maximum solubility in natural gas. A limit of this barrier, which is controlled by the Gibbs free energy, has to be
overcome to form a critical nucleus, based on the Classical Nucleation Theory. The nucleation rate can be obtained from
the combination of Eq. (1), (2), (3), (4), (5) according to Turk (2000):

(1)

where J is the nucleation rate (cm−3 s−1); K is the pre-exponential factor (cm−3 s−1); ∆G is Gibbs free energy (J); kB is the
Boltzmann constant (J/K); and T is the temperature (K).

The Gibbs free energy is a state function which depends only on the initial and final states. Enthalpy and entropy values
of the initial and final states can be obtained from HYSYS®, together with information on natural gas composition,
pressure and temperature. Using these values calculated for the gas streams from the desired fields, the variation of the
Gibbs energy can be obtained from Eq. (2):

(2)

where ΔG is the change in Gibbs free energy (kJ/kg); ΔH is the change in enthalpy (kJ/kg); ΔS is the change in entropy
(kJ/kg K).
The pre-exponential factor of Eq. (1) is given by:

(3)

where ϴ is the non-isothermal factor (=1 for diluted mixtures); αc is the condensation factor (m/s); vs is the solute's
molecular volume (m³); N is the number of condensable molecules (cm−3); and σ is the solute's interfacial tension
(N/m).

The solute's molecular volume can be calculated for each point as a function of temperature, according to Eq. (4):

(4)

where M is the molar volume of sulfur (mol/m³); NA is Avogadro's number (mol−1); and Tb is the bubble point
temperature (K).

The number of condensable molecules is calculated by Eq. (5):

(5)

where ρM is the density of the mixture (mol/cm³); and yE is the solute's molar fraction under the extraction conditions.

The interfacial tension of sulfur can be expressed by Eq. (6) according to Zhu et al. (2011):

(6)

where Pc is the critical pressure (MPa); Tc is the critical temperature (K); Tbr is the reduced bubble point temperature;
and Tr is the reduced temperature.
The mass of sulfur that can be deposited through the nucleation/desublimation process at a certain point, based on the
rate of nuclei formation, can be obtained using Eq. (7) according to Pack (2005):

(7)

where m is the mass of the substance (kg); n is the number of moles; and MM is the substance's molecular mass
(kg/kmol).

A MATLAB® program was developed to solve Eq. (1), (2), (3), (4), (5), (6) in each pipeline segment of the gas stream
flows. Because there is no natural gas pipeline from the Fazenda Mamoeiro field to deliver the produced gas to the
customers, the line from the wellhead to the pressure-restricting valve in the separator (points A and B of Fig. 1,
respectively) was considered as a transportation pipeline for the calculation of the nucleation rate. The steel pipeline
has an I.D. of 0.0762 meter, 35 meters length and absolute roughness of 0.000183 meter.

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Fig. 1. Fazenda Mamoeiro Field (FSP).

The field produces oil and gas at a flow rate of 7 m³/day and 7000 m³/day, respectively. Because multi-phase flow would
affect the nucleation rate calculation, only gas flows in the pipeline were considered. This consideration is not rough
and can be confirmed by determining the hold-up of liquid (λl), which is the pipe area fraction occupied by the liquid
phase. The fraction of the pipe occupied by the liquid phase can be determined by Eq. (8) according to Shoham (2006):

(8)

where qL is the liquid flow rate (m³/day); and qG is the gas flow rate (m³/day).

By inserting the oil and gas flows produced by the FSP in Eq. (8), the results show that the fraction of the area of the
pipe occupied by the liquid phase is about 0.1%. Therefore, 99.9% of the pipe area is occupied by the gas phase.

The variables were calculated by the computational routine for each pressure and temperature along the pipeline: pre-
exponential factor, density of the mixture, volume of solute, number of condensable molecules, reduced temperature,
interfacial tension and, consequently, nucleation rate for each condition. Because the pressure drop along the pipeline
causes temperature reduction, a linear relationship between pressure and temperature along the pipeline was assumed
in the calculations for simplification purposes.

3. Results and discussion

Using Eq. (1), it is possible to calculate the nucleation rate at a certain point in the pipeline. Contrary to the
methodology adopted by Pack (2005), who calculated the nucleation rate only at the point in the pipeline where the
pressure of the gas stream is reduced, a nucleation rate profile of the analyzed pipeline segment was determined in
this study, and the segment was subdivided into multiple parts. Since there is no information on the percentage of
sulfur in the gas stream of the Fazenda Mamoeiro field (FSP), fields with similar characteristics were studied to
determine this correlation. According to Alami et al. (2012), the Hasbah field in Saudi Arabia has a pressure at the choke
of 1700 psia (11617 kPa), which is the same as in the FSP.
In addition, it is noted that the choke pressure drop before the restriction is very small in the Hasbah field, which is
similar to the FSP. Given that pressure and temperature conditions from the choke onwards for the two fields are very
close and that there is no information on the sulfur concentration in the gas stream for the FSP, in this study it was
assumed that the maximum amount of sulfur in the gas at the wellhead is 0.5 ppm (equal to the Hasbah field), and it is
0.01 ppm for the conditions upstream of the separator's regulating valve. When the mixture that is leaving the choke
reaches the restriction, it becomes supersaturated with sulfur and desublimates. This implies that the amount of
desublimated sulfur is determined by the difference between the amount of sulfur in the gas stream (0.5 ppm) and the
sulfur saturation condition at the restriction (0.01 ppm). Thus, there is a desublimation of 0.49 ppm of sulfur.

A MATLAB® routine was used to calculate the variables involved in the nucleation rate. Using this routine, it was
possible to calculate the value of each variable as a function of pressure and temperature for each segment of the line
with 3 in I.D. and 35 meters length, from the wellhead to the separator. In this case, a temperature vector with 100
points was dimensioned so that the other variables were calculated from it. The input parameters used to solve Eq. (1),
(2), (3), (4), (5), (6) are shown in Table 2.

Table 2. Input parameters of the MATLAB® routine used to calculate the nucleation rate profile of the Fazenda
Mamoeiro field (FSP).

Input parameters Values

Variation of Gibbs free energy (J) −738.3×10−23

Boltzmann constant (J/K) 1.38×10−23

Pressure at the wellhead (kPa) 11617.6

Pressure upstream of the separator (kPa) 10928.2

Temperature at the wellhead (K) 350

Input parameters Values

Temperature upstream of the separator (K) 305

Sulfur molar fraction under extraction conditions (dimensionless) 4.9×10−7

Avogadro's number (mol−1) 6.023×1023

Sulfur critical temperature (K) 1314

Sulfur bubble temperature (K) 717.7

Sulfur critical pressure (MPa) 11.75

Sulfur molar volume (mol/m³) 6.45×104

Non-isothermal factor (dimensionless) 1

Condensation factor (m/s) 0.1

It was possible to obtain a nucleation rate profile along the pipeline using data from Table 2 together with the routine
developed to solve Eq. (1), (2), (3), (4), (5), (6). This nucleation profile for the set of line segments (from the wellhead to
the separator) is shown in Fig. 2.
Download : Download full-size image

Fig. 2. Nucleation rate profile as a function of temperature along the pipeline in the Fazenda Mamoeiro Field (FSP).

Fig. 2 shows the behavior of the nucleation rate along the gas flow pipeline of the Fazenda Mamoeiro field. The
solubility conditions of sulfur in the gas stream are changed as temperature falls along the line. At high temperatures
(for example, 350 K), the sulfur solubility in natural gas (0.5 ppm) is close to maximum in the gas stream. Therefore,
most sulfur remains solubilized. This means that nucleation rates are lower at high temperatures, resulting in low
amounts of deposited elemental sulfur. However, as the temperature falls because of cooling during gas flow, the
solubility of the mixture is modified, and the gas stream starts to be supersaturated in sulfur. Therefore, the amount of
sulfur that may desublimate increases, which results in an increase in the particle formation rate, as shown in Fig. 2.

It is noteworthy that the segment selected to determine the nucleation profile has no restrictions in the line that could
result in low pressure and temperatures. This explains the occurrence of a low nucleation rate along the studied line.
However, very low temperatures may occur in pressure-reduced conditions, for example in restrictions, and nucleation
rates may reach much higher values in those cases. This can be observed in the behavior of the curve in Fig. 2, which
increases exponentially to very high nucleation rates at very low temperatures, as in the case of pressure reductions.
According to Pack (2005), nucleation rates may reach values on the order of 1013 cm−3 s−1 in restrictions, which explains
why these places have larger amounts of elemental sulfur deposited downstream of valves.

The mass of sulfur deposited along the pipeline can be estimated from the nucleation rate profile. Thus, the calculated
values for the 100 points along the pipeline were used to estimate the average nucleation rate. The average nucleation
rate was 6.26×108 cm−3 s−1 for a 35-meter section of pipeline. Using the average nucleation rate, the line's operational
conditions, the gas production flow rate of the Fazenda Mamoeiro field and the gas composition given in Table 1, the
rate is 1.49×1022 nuclei/day. Using the molecular mass of sulfur (32.06 kg/kmol) in Eq. (7), the mass of sulfur deposited
in the pipeline is

The amount of sulfur deposited in the pipeline is small compared to the values that can be deposited downstream of
the restrictions. However, the small amount of deposited sulfur can be explained by two factors. First, the very short
extension of the line (35 m) resulted in a small pressure drop, which reduces the possibility of sulfur supersaturation in
the gas stream. Second, the nucleation rate was calculated for a pipe segment with no restrictions; therefore, gas was
able to flow in a wider space with less turbulent conditions. The number of molecules that collide inside the pipeline is
low under such conditions, and the particles formed are very small and can be transported together with the gas
stream for longer distances, with little deposition in the pipeline. The objective of this calculation was to demonstrate
that the amount of sulfur deposited in unrestricted pipeline sections is actually very small, and does not cause a
significant loss of flow area. However, even small amounts of sulfur deposited along the pipeline may cause corrosion
problems and affect transportation operational safety.

As previously discussed, the more serious problems of elemental sulfur deposition occur downstream of restrictions in
pipelines. In these places, the gas stream may reach very low pressures and temperatures because of the Joule-
Thompson effect. To evaluate the effect on nucleation rate at these locations, a situation was considered in which the
FSP gas was delivered to a Natural Gas Processing Unit (NGPU) with pressure and temperature similar to those of the
plant that receives the gas produced at the Hasbah field, that is, 800psia (5414.4 kPa) and 35 °F (275 K).

The nucleation rate obtained by running the MATLAB® routine for the conditions downstream of the restriction was
1.03×1013 cm−3 s−1. This value is in accordance with Pack (2005), within an order of magnitude of the 1013 cm−3 s−1 value
given by the author for restrictions. The sulfur mass that would be deposited for this nucleation rate was calculated
using the aforementioned procedure. It is noteworthy that the amount of sulfur that could desublimate at this point
was considered equal to 0.0099 ppm, as reported by Alami et al. (2012). The nucleation rate translates to 4.77×1023
nuclei per day. The sulfur mass deposited downstream of the valve, determined by Eq. (7), is as follows:

This value is on the same order of magnitude as that of Pack (2005), who estimated 1.075 kg/year of sulfur deposited
downstream of a certain point for a gas stream with 0.009 ppm of sulfur. It has to be mentioned that the author found a
lower mass for a similar sulfur concentration (0.009 ppm) because pressure and temperature conditions were different.
The author considered a temperature of 288.65 K at the reduction stage, whereas this study uses a value of 275 K.

The values obtained for the line and the restriction confirm previous results showing that a higher amount of deposited
sulfur is found downstream of the restriction points. More particle–particle collisions occur at these locations, enabling
a higher degree of agglutination and larger particle sizes. This is enhanced by the effect of a pressure and temperature
drop that makes the stream supersaturated with sulfur. Differences in nucleation at different pressure and temperature
conditions make it easier to understand why some points show visible deposition of elemental sulfur and others do
not.

The nucleation rates in the pipeline and the restrictions enable to assess the effect of pressure and temperature on the
deposition phenomenon. However, as previously discussed, the composition of the gas stream is another parameter
that may influence sulfur deposition in pipelines. Thus, the same operational conditions of pressure, temperature,
production flow rate and amount of sulfur in the FSP gas stream were used to calculate the nucleation rate profiles of
the gas streams of the CE/RN, ES and RJ fields, whose compositions are shown in Table 1. The only variable that has to
be modified in the routine for each field is the change in Gibbs free energy; the other variables are calculated as
functions of temperature. The comparative results showing the influence of natural gas composition on the nucleation
rate profile are shown in Fig. 3.

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Fig. 3. Influence of gas stream composition on the nucleation rate profile.

Fig. 3 shows that the composition of the gas stream influences the homogenous nucleation rate profile, even though
the different streams have the same operational conditions. Nucleation rates are very similar for all compositions at
high temperatures, when sulfur concentration is close to the maximum solubility in the gas stream. However, the
curves are separated when the temperature is reduced because of the cooling effect of the pipeline. Thus, the influence
of the gas composition becomes more significant at very low temperatures, as can occur in restrictions. A comparison
of the curves for gas streams from the ES and CE/RN fields, which have very different compositions, shows that, at low
temperatures, the nucleation rates of the gas from the ES field grow exponentially and reach much higher values than
those of the gas stream from the CE/RN field.

The differences between the curves can be explained by the tendency of the gas stream to form droplets at low
temperatures. When the gas stream has a higher fraction of heavy components (C3+), as in the case of the CE/RN field,
the probability of forming droplets is higher, which consequently favors heterogeneous nucleation. When the
heterogeneous nucleation is favored, homogeneous nucleation is impaired, and this results in a less homogenous
nucleation rate for the CE/RN gas stream compared to the ES field. Therefore, the comparison of nucleation rate profiles
for the four gas streams confirms that natural gas composition influences the sulfur mass that may be deposited along
a pipeline.

4. Conclusions
The following conclusions can be made based on this study:
1. Among the factors related to elemental sulfur formation, nucleation is one of the most important mechanisms
controlling sulfur deposition in natural gas pipelines. Higher homogeneous nucleation rate occurs at the point of
low pressure and temperature exactly where higher deposition rates of sulfur in gas pipelines are detected.

2. The nucleation mechanism propagates by the coagulation/agglomeration of the particles that cause nuclei
formation. As the sulfur nuclei are generated, together with other suspended particles, they agglomerate and
increase in size. When they reach a certain stage, called the critical nucleus, they may settle in the pipeline due to
gravity.

3. The flow profile of the gas stream also influences the nucleation phenomenon and consequently the sulfur mass
that is deposited in the pipeline.

4. Although the study was performed with a short-length pipe, it is important to comprehend and solve real problems
because the results showed that higher deposition rates occur at the point of low pressures and temperatures. The
 deposition along the line is very small, which shows that the deposition is more localized and concentrated at
pressure breakpoints.

Acknowledgments
The authors thank the Bahia Research Foundation (Fundação de Amparo à Pesquisa do Estado da Bahia - FAPESB) for
financing the Project, grant number APP 0008/2011, and the Graduate Studies Program in Chemical Engineering
(Programa de Pós-Graduação em Engenharia Química) of the Federal University of Bahia (Universidade Federal da
Bahia - UFBA).

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