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Energy
EnergyProcedia 158
Procedia 00(2019)
(2017)5329–5335
000–000
www.elsevier.com/locate/procedia
10th International Conference on Applied Energy (ICAE2018), 22-25 August 2018, Hong Kong,
10th International Conference on Applied Energy
China(ICAE2018), 22-25 August 2018, Hong Kong,
China
Dynamical mechanism of hydrate formation resulting from free gas
Dynamical The mechanism of hydrate
15th International formation
Symposium resulting
on District Heating from free gas
and Cooling
migration into seeping seafloor sediments
migration into seeping seafloor sediments
Assessing the feasibility
Bin Wanga,b,e, Jiafei Zhaoa,b,
a,b,e of using, Xin
*, Yongchen Songa,b
theLv
heat
c demand-outdoor
, Yuanping Lidd,Weixin Pangcc,
temperature
Bin Wang , Jiafei function
Zhao *,for
a,b,
a long-term
Yongchen district
Song Li, cXin
Qingping
a,b
heat demand
Lv , Yuanping
c
forecast
Li ,Weixin Pang ,
c
Qingping Li
a
Key Laboratory of Ocean Energy Utilizationa and Energy Conservation
a,b,c a of Ministry bof Education, Dalian University
c of Technology, cDalian
a I. Andrić *, A. Pina , P. Ferrão , J. Fournier ., B. Lacarrière , O. Le Corre
116024, China
Key Laboratory of Ocean Energy Utilization and Energy Conservation of Ministry of Education, Dalian University of Technology, Dalian
a
b
School of Energy and Power Engineering,116024,
Dalian University
China of Technology, Dalian 116024, China
IN+ Center for Innovation, Technology and Policy Research - Instituto Superior Técnico, Av. Rovisco Pais 1, 1049-001 Lisbon, Portugal
b c
School ofb Energy and CNOOC
Power Research Institute
Engineering, Co.University
Dalian Ltd., Beijing 100027, China
of Technology, Dalian 116024, China
Veolia Recherche & Innovation, 291 Avenue Dreyfous Daniel, 78520 Limay, France
c
dc
Shenzhen
CNOOC Branch of Institute
Research CNOOCCo. Ltd., Guangzhou
Ltd., 510240,China
Beijing 100027, China
e Département Systèmes Énergétiques et Environnement - IMT Atlantique, 4 rue Alfred Kastler, 44300 Nantes, France
Earth and Environmental Sciences
d
Area,
Shenzhen Lawrence
Branch Berkeley
of CNOOC Ltd.,National Laboratory,
Guangzhou 510240, Berkeley
China CA 94720, United Status
e
Earth and Environmental Sciences Area, Lawrence Berkeley National Laboratory, Berkeley CA 94720, United Status

Abstract
Abstract
Abstract
District heating networks are commonly addressed in the literature as one of the most effective solutions for decreasing the
Generating hydrate-bearing samples of nature-approximation in the lab is critically important for evaluating the integrated physical
greenhouse gas emissions samples
Generating from theofbuilding sector. These systems require high investments which are returned throughphysical
the heat
properties ofhydrate-bearing
hydrate-bearing sediments, nature-approximation
accurately assessing in thethe lab is critically
potential of marine important
hydrate for evaluating
resources the integrated
and establishing a safe and
sales. Due
properties to the changed sediments,
of production
hydrate-bearing climate conditions
accurately and building renovationofpolicies, heat demand in and
the establishing
future coulda safe
decrease,
efficient gas technique; however, currentassessing
databasethe onpotential marine hydrate
generating hydrate-bearing resources
samples of nature-approximation and
in
prolonging
efficient gas the investment
production return period.
technique; however, current database
the lab are still limited due to experimental challenges. Here weonreportgenerating hydrate-bearing
the dynamical formationsamples
of gas of nature-approximation
hydrate resulting from freein
The main
the scope of thisdue
paper is to assess the feasibilityHere
of usingreport
the heat demand – outdoor temperature function for heat demand
gas lab are still
migration limited
into to experimental
seeping seafloor sedimentschallenges.
through visualwe observationtheusing
dynamical formation
a magnetic of gasimaging
resonance hydrate resulting from
(MRI) device. free
The
forecast.
gas migrationTheintodistrict
seepingof Alvalade,
seafloor located in
sediments Lisbonvisual
through (Portugal), was using
observation used as a a case study.
magnetic The imaging
resonance district is consisted
(MRI) device.ofThe
665
effects of core temperature, pore pressure, gas flow rate, and solution salinity are preliminarily explored. The saturations of water,
buildings
effects thattemperature,
vary in bothpore construction period
flowand
rate,typology. Three weatherare scenarios (low, medium, high) and three water,
district
gas, andofhydrate
core are calculated based pressure,
on thegas
mean and(MI)
intensity solution salinity
of obtained MRI preliminarily
images. Theexplored. The
residual water saturations
saturation ofvariation
renovation
gas, and scenarios
hydrate were developed
are calculated based on (shallow,
the mean intermediate,
intensity deep). To estimate the error,
The obtained heat demand values were
along with gas flow direction during hydrate formation are (MI) of obtained
analyzed. Also, theMRIresidual
images. water residual
saturation water saturation
distribution in variation
the pore
compared
along are with
withvisually results
gas flow from a dynamic heat demand model, previously developed and validated by the authors.
direction during hydrate formation are analyzed. Also, the residual water saturation distribution in the pore
space presented.
The results
space showed
are visually that when only weather change is considered, the margin of error could be acceptable for some applications
presented.
(the error in annual demand was lower than 20% for all weather scenarios considered). However, after introducing renovation
Copyright © 2018 Elsevier Ltd. All rights reserved.
©scenarios,
2019 The
Copyright Authors.
©the
2018error Published
value
Elsevier by
increased
Ltd. All Elsevier Ltd. (depending on the weather and threnovation scenarios combination considered).
up toreserved.
rights 59.5%
Selection and peer-review under responsibility of the scientific committee of the 10 International Conference on Applied Energy
This
The isvalue
an open
of accesscoefficient
slope article under the CC BY-NC-ND
increased on average license (http://creativecommons.org/licenses/by-nc-nd/4.0/)
within committee
the range of 3.8%
Selection and peer-review under responsibility of
(ICAE2018). the scientific of the 10thupInternational
to 8% per Conference
decade, thaton corresponds to the
Applied Energy
Peer-review
decrease in the number of heating hours of 22-139h during the heating– season
under responsibility of the scientific committee of ICAE2018 The 10th International
(depending Conference
on the on Applied
combination Energy.
of weather and
(ICAE2018).
renovation
Keywords: scenarios
Hydrate considered).
formation; On the
gas migration, otherseafloor
seeping hand, sediments,
function intercept increasedimaging
magnetic resonance for 7.8-12.7% per decade (depending on the
coupled Hydrate
Keywords: scenarios). The values
formation; suggested
gas migration, could
seeping be used
seafloor to modify
sediments, the resonance
magnetic function imaging
parameters for the scenarios considered, and
improve the accuracy of heat demand estimations.

© 2017 The Authors. Published by Elsevier Ltd.

Peer-review under responsibility of the Scientific Committee of The 15th International Symposium on District Heating and
Cooling.
* Corresponding author. Tel.: +86-411-84706722; fax: +86-411-84706722.
* E-mail address:author.
Corresponding jfzhao@dlut.edu.cn
Tel.: +86-411-84706722; fax: +86-411-84706722.
Keywords: Heat demand;
E-mail address: Forecast; Climate change
jfzhao@dlut.edu.cn
1876-6102 Copyright © 2018 Elsevier Ltd. All rights reserved.
Selection and
1876-6102 peer-review
Copyright under
© 2018 responsibility
Elsevier Ltd. All of the scientific
rights reserved. committee of the 10th International Conference on Applied Energy (ICAE2018).
Selection and peer-review under responsibility of the scientific committee of the 10th International Conference on Applied Energy (ICAE2018).
1876-6102 © 2017 The Authors. Published by Elsevier Ltd.
Peer-review under responsibility of the Scientific Committee of The 15th International Symposium on District Heating and Cooling.
1876-6102 © 2019 The Authors. Published by Elsevier Ltd.
This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/)
Peer-review under responsibility of the scientific committee of ICAE2018 – The 10th International Conference on Applied Energy.
10.1016/j.egypro.2019.01.634
5330 Bin Wang et al. / Energy Procedia 158 (2019) 5329–5335
2 Bin Wang et al. / Energy Procedia 00 (2018) 000–000

1. Introduction

Natural gas hydrates have been recognized as a future fossil fuel, as huge amount of natural gas enclosed in hydrate
by forming hydrogen bonding water cage [1, 2]. Natural gas hydrates are ice-like inclusion compounds buried in the
permafrost regions and the deep ocean sediments where low ambient temperatures and high pore pressures naturally
coexist [3]. Extracting gas from hydrate-bearing sediments can weaken the reservoir stability due to the inevitable
phase transformation behaviour of solid hydrate dissociated into gas and liquid phases [4]. The reservoir stability,
which can cause submarine slumps or slides and further endangering seafloor infrastructure, is mostly related safety
issues during gas production [5]. Hence, investigation on the integrated physical properties of hydrate-bearing
sediments is critically essential for the safe and efficient gas extraction from hydrate reservoir [6, 7]. The physical
properties of hydrate-hosting sediments largely depend on the hydrate content, occurrence morphology, and sediment
microstructure [8-10]. Therefore, generating hydrate-bearing samples of nature-approximation in the lab is critically
important for the proper inversion of the geophysical data, stability analyses of seafloors, and evaluation of gas
production from hydrate deposits [11]. In fact, great efforts have been conducted so far, various methods to synthesize
gas hydrate-bearing sediment samples in the laboratory have been explored, including the ice-to-hydrate method, the
excess gas method, the excess water method, and the dissolved gas method [12, 13]. Among these methods, the excess
gas method, forming gas hydrates from partially water-saturated sediments, has been widely adopted as its simplicity
and the component controllability.
Given the fact that isotopic analyses results suggested that the methane within the gas hydrates is mainly from both
biogenic and thermogenic source [14, 15]. As the high temperature requirements for its production, the presence of
thermogenic gas supports that gas hydrate formed by continuous gas migration into the hydrate stability regions from
the underlying accumulations [16]. Field tests on sites including the Gulf of Mexico [17], the Cascadia margin [18],
the Caspian Sea [19], and the Blake Ridge [20, 21] have proved the occurrence of such dynamic mechanism of hydrate
formation. In addition, hydrae reformation resulting from free gas migrating into hydrate stable region when exploiting
the hydrate resource can block the gas/water flow path, therefore reducing the gas production efficiency [22, 23].
However, current database on hydrate formation characteristics as free gas upward migrating into seafloor sediments
where hydrates can stably exist are still limited.
So, the purpose of this study is to investigate the dynamics mechanism of hydrate formation resulting from free gas
migration into seeping seafloor sediments where hydrate can stably exist using a magnetic resonance imaging (MRI)
system. The effects of core temperature, pore pressure, gas flow rate, and solution salinity are preliminarily explored.
The residual water saturation, hydrate saturation, and residual water distribution were measured and analyzed. This
study can provide some basic information for the dynamical formation of gas hydrate in a seeping seafloor system as
well as the hydrate reformation behavior while exploiting hydrate resource.

2. Experimental section

2.1. Experimental apparatus and materials

(a) (b)

Fig. 1. Schematics of (a) methane hydrate formation system, and (b) pressure-temperature trajectories during hydrate formation.
 Bin Wang et al. / Energy Procedia 158 (2019) 5329–5335 5331
Bin Wang et al. / Energy Procedia 00 (2018) 000–000 3

As shown in Fig. 1(a), the experimental apparatus primarily consisted of a high-pressure vessel, an MRI system
(Varian, Inc., USA), three high-pressure pumps (260D, Teledyne ISCO Inc., USA), a thermostatic bath (FL300, Julabo
Technology, Germany), and a data acquisition system. The MRI system can detect 1H only in liquids (water in our
experiment) and produces liquid distribution images; it was operated at 400 MHz to visualize hydrate formation and
decomposition. The MRI system’s field of view (FOV) was 3030 mm; the slice thickness was 4mm, and the MRI
image matrix was 128128 pixels. Detailed descriptions of the experimental apparatus can be found in our previous
work [24, 25].
BZ-02 glass beads (As-One Co., Ltd., Japan) with a porosity of approximately 35.4% were employed to simulate
the porous media. Deionized water (prepared in lab) and methane gas (Dalian Special Gas Co., Ltd., China) with a
purity of 99.99% was used to form the methane hydrate.

2.2. Experimental Procedure

The clean glass beads were tightly packed into the vessel, and then the vessel was placed into the MRI system. The
thermostatic bath was set to maintain the vessel’s temperature at a constant value during the hydrate formation process.
Deionized water was slowly injected into the vessel until the pressure reached 6 MPa; this ensured that the porous
media was water-saturated. High-pressure nitrogen gas (approximately 5.0 MPa) was then injected from the top of the
vessel to displace the pore water, and the amount of displaced water was recorded. After the vessel was evacuated and
cooled down, the methane gas was injected into the vessel with an upstream flow direction at a constant rate controlled
by the syringe pump. The vessel pressure was maintained at a constant high pressure for hydrate formation. The
pressure-temperature trajectories during hydrate formation process was depicted in Fig. 1(b). In addition, images were
continuously obtained during hydrate formation using the MRI system. Stabilization of the mean intensity of MRI
images was taken to indicate that hydrate formation was finished. Details of the experimental parameters and initial
conditions are given in Table 1.

Table 1. The initial experimental conditions and results.a

Gas 𝑆𝑆𝑤𝑤0 T P R Salinity t 𝑆𝑆𝑤𝑤𝑤𝑤 𝑆𝑆ℎ

Exp. No.
component (%) (°C) (MPa) (mL/min) (% w/w) (min) (%) (%)
1 CH4 38.64 1 5 1 0 364.8 23.62 18.76
2 CH4 37.57 1 5 3 0 202.67 10.25 34.15
3 CH4 38.06 1 5 5 0 283.73 13.00 31.32
4 CH4 34.44 1 4 3 0 ∞ 35.27 0
5 CH4 32.86 1 6 3 0 27.73 6.78 32.60
6 CH4 35.32 0.5 5 3 0 29.87 9.12 32.75
7 CH4 31.07 1.5 5 3 0 2.13 8.42 28.31
8 CH4 36.31 1 5 3 1 198.40 8.81 34.37
9 CH4 38.59 1 5 3 3 469.33 5.32 41.58
10 CH4/C2H6 31.64 1 5 3 0 2.13 6.04 32.00
a
The symbols in this table are defined as follows: 𝑆𝑆𝑤𝑤0 is the initial water saturation (volume fraction, %); T is the core temperature (°C); P is the
pore pressure (MPa); R is the gas flow rate (mL/min); t is the hydrate formation onset time (min); 𝑆𝑆𝑤𝑤𝑤𝑤 is the residual water saturation (volume
fraction, %); and 𝑆𝑆ℎ is the formed hydrate saturation (volume fraction, %).

3. Results and Discussion

The mean intensity (MI) of MRI images, which reflecting the volume fraction of water in the whole sediment pores,
can be used to quantify hydrate saturation. Notably, 1 m3 of gas hydrate can generate 0.8 m3 of liquid water when
brought to the surface of the earth, therefore, 1 m3 of free water can form 1.25 m3 of methane hydrate at standard
temperature and pressure (STP). Thus, the hydrate saturation, 𝑆𝑆ℎ𝑖𝑖 , at time “i” (measured in minutes) can be calculated
as follows:
5332 Bin Wang et al. / Energy Procedia 158 (2019) 5329–5335
4 Bin Wang et al. / Energy Procedia 00 (2018) 000–000

I0 − Ii
Shi = 1.25   Sw0 100% (1)
I0
Ii
Swi =  Sw0 100% (2)
I0
Sgi =−
1 Shi − Swi (3)
0 I0
S=
w 100% (4)
Is
where I0 and Ii are the MI values of free water at initial time and at time “i”; 𝑆𝑆𝑤𝑤0 and 𝑆𝑆𝑤𝑤𝑖𝑖 are the water saturation at
initial time and at time “i”; 𝑆𝑆𝑔𝑔𝑖𝑖 is the gas saturation at time “i”; and Is is the MI value of the free water when the porous
medium is fully saturated.

Fig. 2. Phase saturation variation calculated based on the MI value.

The saturation variations of water, gas, and hydrate calculated based on the MI values were plotted in Fig. 2, as
well as the water phase distribution obtained from the MRI images. According to the results of Run 4 in which no
hydrate formed, the constant level of water saturation implied there was no water flowing out when gas swept through
the sediments. As observed in Fig. 2, the saturation curves were similar except Run 2. The phase saturations kept at
 Bin Wang et al. / Energy Procedia 158 (2019) 5329–5335 5333
Bin Wang et al. / Energy Procedia 00 (2018) 000–000 5

constant for a long time to induce hydrate nucleation, which was defined as the induction time for hydrate formation
in the dynamical system. Once the hydrate began to nucleate, the water saturation dropped dramatically, indicating a
rapid hydrate formation rate. But the hydrate formation gradually decreased as time went by until no hydrate
generated. However, little fluctuations in water and hydrate saturations can be observed during the rapid hydrate
formation stage, this could be the result of temperature variation due to the exothermal hydrate formation reaction. In
addition, the results in relation to induction time, residual water saturation, and formed hydrate saturation were
summarized in Table 1.

Fig. 3. Residual water saturation variation along with gas flow direction calculated based on the MI values.

Fig. 3 plotted the residual water saturation variation along with gas flow direction. The Y axis refers to the height
of FOV. As shown, the initial water saturation at top position was a higher than that at bottom position. The hydrate
can uniformly form in the sediments in an early stage, and regionally rapid hydrate formation and/or residual water
migration occurred sometimes, such as at 241 min of Run 2 and at 516 min of Run 9. In addition, Fig. 4 shown the
observed residual water distribution corresponding to Fig. 3, which indicated that water redistribution can occur during
hydrate formation because of the pore volume and capillary force change, and the migrated water can not return the
original place after hydrate formation completely.

Run 2

2.13 min 192 min 213.33 min 219.73 min 228.27 min 241.07 min 245.33 min 249.6 min 256 min 426.67 min
Run 5

4.26 min 29.87 min 38.4 min 40.53 min 42.67 min 44.8 min 49.07 min 53.33 min 68.27 min 106.67 min

Run 6

2.13 min 32 min 38.4 min 40.53 min 44.8 min 49.07 min 74.67 min 149.33 min 192 min 298.67 min
Run 9

40.53 min 469.33 min 490.67 min 501.33 min 512 min 516.27 min 533.33 min 629.33 min 650.67 min 768 min

Fig. 4. Residual water distribution during hydrate formation. Black indicates the absence of liquid water, while the colors red to blue indicate
decreasing amounts of liquid water.
5334 Bin Wang et al. / Energy Procedia 158 (2019) 5329–5335
6 Bin Wang et al. / Energy Procedia 00 (2018) 000–000

4. Conclusion

In this study, we investigated the dynamical formation of gas hydrate resulting from free gas migration into seeping
seafloor sediments through visual observation using a magnetic resonance imaging (MRI) device. The results shown
that gas hydrate always formed uniformly in the whole pore space initially, and then regional hydrate nucleation also
occurred. Due to the variation in pore volume and capillary during hydrate formation, irreversible water redistribution
was observed in our experiments. This study can provide some basic information for the dynamical formation of gas
hydrate in a seeping seafloor system as well as the hydrate reformation behavior while exploiting hydrate resource.

Acknowledgements

This study has been supported by the National Natural Science Foundation of China (Grant No. 51622603), the
Major Program of National Natural Science Foundation of China (Grant No. 51436003), and the National Key
Research and Development Program of China (Grant No. 2017YFC0307300, 2016YFC0304001).

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