Accepted Manuscript The mechanism and verification analysis of permafrost-associated gas hydrate formation in the Qilian Mountain, Northwest China Bing Li, Youhong Sun, Wei Guo, Xuanlong Shan, Pingkang Wang, Shouji Pang, Rui Jia, Guobiao Zhang PII:
S0264-8172(17)30202-7
DOI:
10.1016/j.marpetgeo.2017.05.036
Reference:
JMPG 2929
To appear in:
Marine and Petroleum Geology
Received Date: 11 March 2017 Revised Date:
21 May 2017
Accepted Date: 25 May 2017
Please cite this article as: Li, B., Sun, Y., Guo, W., Shan, X., Wang, P., Pang, S., Jia, R., Zhang, G., The mechanism and verification analysis of permafrost-associated gas hydrate formation in the Qilian Mountain, Northwest China, Marine and Petroleum Geology (2017), doi: 10.1016/ j.marpetgeo.2017.05.036. This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain.
ACCEPTED MANUSCRIPT
The mechanism mechanism and verification analysis of permafrostpermafrost-associated gas
2
hydrate formation in the Qilian Mountain, Mountain, Northwest China
3
Bing Li a,b, Youhong Sun a,b,*,Wei Guo a,b,*,Xuanlong Shan c, Pingkang Wang d,Shouji Pangd, Rui Jia a,b,Guobiao
4
Zhang a,b
5
a
6
b
7
University, Changchun 130026, PR China
8
c
9
d
College of Construction Engineering, Jilin University, Changchun 130026, PR China
RI PT
1
College of Earth Sciences, Jilin University, Changchun 130061, PR China Oil and Gas Survey, China Geological Survey, Beijing 100029, PR China
SC
Key Laboratory of Drilling and Exploitation Technology in Complex Condition, Ministry of Land and Resources, Jilin
* Corresponding author (Youhong Sun, E-mail address:
[email protected], Tel. and Fax: +86 431
11
88502678; Wei Guo, E-mail address:
[email protected] )
12
Present address: No. 6 Ximinzhu Street, Changchun City, Jilin Province, PR China, 130026
13
Abstract
TE D
M AN U
10
Muri Basin in the Qilian Mountain is the only permafrost area in China where gas
15
hydrate samples have been obtained through scientific drilling. Fracture-filling hydrate is the
16
main type of gas hydrate found in the Qilian Mountain permafrost. Most of gas hydrate
17
samples had been found in a thin-layer-like, flake and block group in a fracture of Jurassic
18
mudstone and oil shale, although some pore-filling hydrate was found in porous sandstone.
19
The mechanism for gas hydrate formation in the Qilian Mountain permafrost is as follows:
20
gas generation from source rock was controlled by tectonic subsidence and uplift--gas
21
migration and accumulation was controlled by fault and tight formation--gas hydrate
22
formation and accumulation was controlled by permafrost. Some control factors for gas
23
hydrate formation in the Qilian Mountain permafrost were analyzed and validated through
24
numerical analysis and laboratory experiments. CSMGem was used to estimate the gas
25
hydrate stability zone in the Qilian permafrost at a depth of 100-400 m. This method was used
AC C
EP
14
1
ACCEPTED MANUSCRIPT to analyze the gas composition of gas hydrate to determine the gas composition before gas
27
hydrate formation. When the overlying formation of gas accumulation zone had a
28
permeability of 0.05 × 10-15 m2 and water saturation of more than 0.8, gas from deep source
29
rocks was sealed up to form the gas accumulation zone. Fracture-filling hydrate was formed
30
in the overlap area of gas hydrate stability zone and gas accumulation zone. The experimental
31
results showed that the lithology of reservoir played a key role in controlling the occurrence
32
and distribution of gas hydrate in the Qilian Mountain permafrost.
33
Keywords
34
Qilian Mountain permafrost; Mechanism of gas hydrate formation; Gas hydrate stability zone;
35
Gas migration and accumulation; Verification analysis
36
0 Introduction
M AN U
SC
RI PT
26
Gas hydrate is one kind of cage compound formed by natural gas and water that exists in
38
enormous quantities in the permafrost and offshore environments (Collett, 2002). Recently,
39
gas hydrate samples were obtained in the Sanlutian region of Muri Basin, Qilian permafrost
40
(Zhu et al., 2010a; Wen et al., 2015). As a result, China became the fourth country to discover
41
the permafrost-associated gas hydrate and the first country to discover permafrost-associated
42
gas hydrate in the low-middle latitude permafrost of the world (Bily and Dick, 1974; Collett,
43
1993; Yakushev and Chuvilin, 2000).
AC C
EP
TE D
37
44
Based on guiding concepts for conventional oil and gas exploration, Collett et al. (2011,
45
2009) proposed the concept of a gas hydrate petroleum system, which was used to identify
46
and assess the mechanism of gas hydrate formation in the Alaska North Slope. They proposed
47
that the factors that contribute to formation of gas hydrate mainly included gas hydrate
48
pressure-temperature stability conditions, gas source, gas migration, and suitable host
49
sediment or “reservoir”. The mechanism of gas hydrate formation in the Alaska North Slope 2
ACCEPTED MANUSCRIPT can be summarized as follows: the thermo-genic gases from deep source rocks migrated to the
51
shallow formation along permeable pathways such as Mount Elbert fault systems; the gases
52
migrated into porous-permeable sediment layers and accumulated in the permeable sand layer
53
that was controlled by a tight sand layer over a permeable sand layer; with the arrival of the
54
Quaternary glaciation, the hydrate stability condition was reached, and the gas hydrate
55
reservoir formed in the Alaska North Slope. The sedimentary environment of gas hydrate,
56
which mainly occurred in porous-permeable sedimentary sand in Mackenzie Delta in Canada
57
and Messoyakha Gas Field in Russia were similar to that of the Alaska North Slope, and the
58
main mechanism for gas hydrate formation was similar as well (Yakushev and Chuvilin, 2000;
59
Majorowicz and Osadetz, 2001). However, gas hydrate in the Qilian Mountain permafrost
60
mainly occurred in the fracture of Jurassic mudstone and oil shale, while a small amount of
61
gas hydrate was distributed in the fissures and pores of sandstones (Zhu et al., 2010a; Wang et
62
al., 2011; Wang et al., 2015; Pang et al., 2013).
M AN U
SC
RI PT
50
Zhang et al. (2013) analyzed the gas hydrate accumulation pattern in the Qilian
64
Mountain permafrost. They proposed that gas hydrate formed from deep pyrolysis gas and
65
shallow coalbed methane under the tectonic uplift. However, they did not consider in detail
66
the gas hydrate stability zone, gas hydrate formation time and the role of tectonic movement
67
to control gas migration. Li et al. (2014, 2012) discussed the gas hydrate formation condition
68
in the Qilian Mountain permafrost from four aspects: the material source, reservoir, cap rock
69
and gas migration conditions. They postulated that coalbed methane was the main gas source
70
for gas hydrate. With the Qinghai-Tibet Plateau uplifting, the formation temperature was
71
reduced and the gas hydrate stability zone formed gradually. They proposed that the
72
accumulation mode at Muri area was a self-born self-storage and short-range migration
73
reservoir. Zhai et al. (2014) and Lu et al. (2013a) hypothesized that the gas source for gas
74
hydrate in the Qilian Mountain permafrost was mainly composed of oil-typed thermo-genic
AC C
EP
TE D
63
3
ACCEPTED MANUSCRIPT 75
gases that were mainly derived from lower or deeper Upper Triassic or Permian. Gas hydrate
76
occurrence and gas migration in gas hydrate scientific wells DK-1, DK-2, DK-3, DK-7, DK-8,
77
DK-9, and DK-12 were controlled by F1 and F2 faults. They described the gas hydrate
78
geological
79
hydrocarbon-generation, fluid-migration, and gas hydrate accumulation subsystems and the
80
coupling relationship of these subsystems as determined by gas hydrate distribution. In
81
addition, Lu et al. (2015a) also analyzed the control effect of F1, F2 and F30 faults on gas
82
hydrate formation and distribution by testing drilling samples provided by Shenhua Qinghai
83
Energy Co., Ltd. Li et al. (2013) noted that the well permeable sand formations and
84
unconformity contact planes can also act as a gas migration system in gas hydrate
85
accumulation pattern in the Qilian Mountain permafrost apart from faults.
in
the
Qilian
Mountain
permafrost
as
mainly
including
M AN U
SC
RI PT
system
Based on the literatures, we can only roughly infer the mechanism of gas hydrate
87
formation in the Qilian Mountain permafrost. A more detailed and systematic mechanism,
88
however, is needed. Discussion of the mechanism in the literature did not include information
89
of all the gas hydrate scientific drilling data in the study area. These previous studies only
90
combined geological data and theoretical analysis, while related laboratory experiment and
91
numerical simulation were not conducted. To fill these gaps, our study systematically
92
summarizes all of the existing gas hydrate scientific drilling data and discusses the
93
mechanism of gas hydrate formation in detail. Then, some parts of factors for the mechanism
94
of gas hydrate formation are verified through numerical analysis and laboratory tests.
95
1 Gas hydrate in the Qilian Mountain permafrost
AC C
EP
TE D
86
96
As of October 2015, permafrost-associated gas hydrate in China had been found only in
97
the Qilian Mountain permafrost. Twenty-nine wells were implemented by China Geological
98
Survey and Shenhua Qinghai Energy Co., Ltd, as shown in Fig. 1 and Table 1 (Wang et al.,
99
2011; Wang et al., 2015; Zhai et al., 2014; Lu et al., 2015a). 4
M AN U
SC
RI PT
ACCEPTED MANUSCRIPT
100
Fig.1. The simplified tectonic map of Sanlutian of Muri Basin, Qilian permafrost and wells location (modified from
102
Wang et al., 2015). 1-Upper Jiangcang; 2-Lower Jiangcang; 3-Upper Muli; 4-Lower Muli; 5-Lower Jurassic; 6-Upper
103
Triassic; 7-Concordant stratigraphic boundary; 8-Discordant stratigraphic boundary; 9-Normal fault; 10- Supposed
104
fault; 11- Reverse fault; 12-No hydrate hole; 13-Exploration line; 14-Research boundary; 15- Hydrate hole.
105
Table 1 Gas hydrate scientific wells in the Qilian Mountain permafrost
TE D
101
Agency
Well category
China Geological
Exploration wells
Gas hydrate sample
Gas hydrate abnormal*
Survey
EP
DK-1、DK-2、DK-3、
AC C
Production wells
Shenhua Qinghai
DK-8、SK-0、SK-2
SK-1 DK2-25、DK2-26、DK4-23、DK4-24、
DK8-19、DK11-14、 DK5-22、DK6-21、DK7-20、DK10-16、
Exploration wells
Energy Co., Ltd
DK-4、DK-5、DK-6、DK-10、DK-11
DK-7、DK-9、DK-12
DK12-13、DK13-11 DK10-17、DK10-18
106
* A series of hydrate-related anomalies were found, which mainly included unusual high pressure gas in the drilling
107
process, gas blowouts near wellhead, incessant water seepage from rock fracture and pore, and abnormal low
108
temperature of infrared imaging in the rock fracture surface.
5
ACCEPTED MANUSCRIPT 109
1.1 Geological setting Sanlutian area is located in the Juhugeng mine area, Muri Coalfield, Qilian Mountain.
111
The basic structural pattern in Muri coalfield is a thrusting-folding type. Under the influence
112
of regional fault zones and coal-bearing basement structures, fault structure is a complete
113
evolution and thrust fault is dominant (Lu et al., 2015b). The Juhugeng mine area is located in
114
the west Muri coalfield, and the overall tectonic morphology is shown as NW multiple
115
syncline (Lu et al., 2015a). Juhugeng mine area is separated into three open pits and four mine
116
fields. Sanlutian area is one pit and located in the south syncline tectonic unit of Juhugeng
117
mine area multiple syncline. The exposure strata in Sanlutian area are mainly the Quaternary,
118
Middle Jurassic and Upper Triassic. The upper Triassic is dominated by black mudstone,
119
siltstone and thin coal seams (Wang et al., 2011; Wang et al., 2015). The Middle Jurassic
120
includes Muri and Jiangcang formations. The Muri formation is dominated by white
121
medium-coarse-grained sandstone, gray fine-grained sandstone and siltstone. The Jiangcang
122
formation is mainly composed of dark gray mudstone and siltstone, dark mudstone, black oil
123
shale and multiple thin coal seams. The elevation of Muri coalfield is 4000-4300m, where the
124
annual average temperature is -5.1 ℃, and the depth of permafrost is generally 60-95m
125
(Wang et al., 2011).
126
1.2 The characteristic of gas hydrate in the Qilian Mountain permafrost
AC C
EP
TE D
M AN U
SC
RI PT
110
127
The gas hydrate samples from thirteen wells were obtained below permafrost in the
128
range of 124.1m~396.0m. The distribution and characteristic of gas hydrate in the Qilian
129
Mountain permafrost are shown in Table 2 (except DK-12) (Wang et al., 2011; Wang et al.,
130
2014; Wang et al., 2015; Pang et al., 2013; Zhu et al. 2010b; Huang et al. 2011; Lu et al.
131
2010a; Pang, 2012; Hou et al. 2015; Chen et al. 2015a; Lu et al. 2010b; Yang et al. 2015; Li
132
et al. 2015; Meng et al. 2015; Tang et al. 2015a; He et al. 2015; Xu et al. 2015; Tang et al. 6
ACCEPTED MANUSCRIPT 133
2015b; Jiang et al. 2015; Lu et al. 2013b; Chen et al. 2015b; Lu et al. 2015b). Compared with
134
gas hydrate in polar permafrost, gas hydrate in the Qilian Mountain permafrost has the
135
characteristics of thin layer, shallow burial, fractured-filling type, complex spatial distribution,
136
gas composition and gas source. Fracture-filling as the main occurrence type of gas hydrate, which is white or pale yellow
138
white ice or jelly in the Qilian Mountain permafrost, occurs as the thin-layer-like, flake, block
139
group in the fracture of low porosity and low permeability rocks such as mudstone, oil shale
140
and siltstone. Pore-filling hydrate disseminated occurs in the porous of sandstone and is
141
difficult to observe by the naked eye, but can be indirectly speculated by continuously
142
emerged bubbles and the water drops, and dispersion-like abnormal low temperature of
143
infrared imaging from the core. As shown in Table 2, the fracture-filling gas hydrate reservoir
144
and fracture-filling + pore-filling gas hydrate reservoir account for about 80% of the hydrate
145
reservoir, and the pore-filling gas hydrate reservoir and the pore-filling + fracture-filling gas
146
hydrate reservoir account for about 20% of the hydrate reservoir (Fig. 2). The statistical
147
results of cores indicate that the gas hydrate reservoirs are in good agreement with the
148
reservoir fracture zone (Wang et al. 2011). From Table 2, we can know that gas hydrate in the
149
Qilian Mountain permafrost has the characteristics of shallow burial, thin layer, large span in
150
vertical distribution and significant difference in horizontal distribution.
EP
TE D
M AN U
SC
RI PT
137
The gas composition of gas hydrate in the Qilian Mountain permafrost is relatively
152
complex and varies in different proportions. However, the overall trend is basically identical,
153
C1 61.3%~71.58%,C2 6.8%~10.9%,C3 9.8%~25.2%,i-C4 1.1%~3.3%,n-C4 0.8%~5.88%,
154
C5 0.5%~2.04%,C6+ 0.1%~4.09%,CO2 0.28%~1.56%,individual samples can be as high as
155
45.1%. The average δ13C values of C1, C2 and C3 of adsorbed gas from hydrate-bearing core
156
are -50.07 ‰, -35.90 ‰ and -32.25 ‰, and the average δD values are -251 ‰, -267 ‰ and
157
-233 ‰, all of which were δ13CC1 <δ13CC2 <δ13CC3, so hydrocarbon gas is typical organic
AC C
151
7
ACCEPTED MANUSCRIPT origin (Cheng et al. 2017). It is shown that gas source in the study area is of mixed geneses,
159
which are dominated by thermo-genic gases, and some biogenic gas may be mixed in some
160
drilling holes (He et al. 2015).
SC
RI PT
158
EP
TE D
Fig.2. Proportion distribution of gas hydrate occurrence in the Qilian Mountain permafrost.
AC C
162
M AN U
161
8
ACCEPTED MANUSCRIPT
Table 2 Distributions and characteristics of gas hydrate in the Qilian Mountain permafrost
Gas hydrate Well
Formation
layer
Depth/m
Lithology and characteristics of reservoir
Characteristics of cores
Average gas composition
RI PT
occurrence Middle Ⅰ
133.5~135.5
Gray fine grained sandstone
Jurassic Middle
Fracture 142.9~147.7
Gray-dark grey silty mudstone
Jurassic
F-F C3 9.10%、i–C4 1.12%
Local fracture development. core
Ⅲ
165.3~165.5
Dark gray - gray mud-siltstone
Jurassic
M AN U
Middle
n–C4 5.58%、C5 0.84% F-F, P- F
crushing
Middle
Fracture
Ⅳ
169.0~170.5
Gray siltstone
Jurassic
C6 4.06%、CO2 0.98% development,
core P- F, F- F
crushing
Ⅰ
Light gray-dust color medium- fine grained
Fracture development, local core
sandstone
crushing
144.4~152.0
Jurassic Middle 156.3~156.6
Jurassic DK-2 Middle Ⅲ
235.0~291.3
Jurassic Middle Ⅳ
377.3~387.5
Dark brown oil shale
EP
Ⅱ
TE D
Middle
F- F, P- F
More fracture development
F- F
C1 71.584 %、C2 10.92% C3 13.07%、i–C4 1.20%
Local
fracture
development,
Brown-gray black oil shale, mudstone
F- F calcite filling
n–C4 2.58%、C5 0.84%
Local fracture development, core
Dark-medium grained sandstone
P- F
Jurassic Middle
C1 68.75 %、C2 8.65%
core
crushing
DK-1
DK-3
development,
SC
Ⅱ
F-F1, P-F2
Local core crushing
AC C
163
crushing Ⅰ
133.0~156.0
Dust color- dark brown oil shale, mudstone 9
More fracture development, local
F-F
NA
ACCEPTED MANUSCRIPT
Jurassic
core crushing
Middle
Fracture development, local core Ⅱ
225.1~240.0
Gray-dark gray oil shale, mudstone
F-F crushing
Middle Ⅲ
Gray- brown grey fine grained sandstone,
Local
siltstone
more core crushing
367.7~396.0
Jurassic
RI PT
Jurassic
Middle
fracture
development, P- F, F-F
High angle fracture development, 136.6~138.0
Gray-dark gray siltstone
P- F, F-F
SC
Ⅰ Jurassic
core integrity well
Middle
Fracture development, local core
Ⅱ
143.4~146.7
NA
Dark gray mudstone, dust color- oil shale
Jurassic
F-F
crushing
Fracture
Middle Ⅰ
147.8~155.9
Dark gray fine grained sandstone
Jurassic
development , core P- F, F-F
integrity well
Middle Ⅱ
171.6~175.0
Jurassic Middle
TE D
DK-8
Gray-black mudstone, dust color- oil shale
Ⅳ
265.9~291.2
Dark brown oil shale, gray-black mudstone
Middle Ⅴ
301.8~304.2
Little fracture development, local F-F core crushing
Calcite filling、, core crushing
Fracture
AC C
Jurassic
EP
226.3~236.5
Middle
NA
Gray-black mudstone, dust color- oil shale
Ⅲ Jurassic
DK-8
M AN U
DK-7
development,
F-F
core F-F, P- F
crushing Fracture
development , core
Gray-black muddy siltstone
P- F, F-F
Jurassic
integrity well
10
NA
ACCEPTED MANUSCRIPT
Middle
Fracture development, local core Ⅰ
188.2~202.4
Gray mudstone, fine grained sandstone
F-F, P- F
Jurassic
crushing
Middle
Fracture development, local core 259.8~271.9
mudstone, siltstone
RI PT
Ⅱ Jurassic
crushing
Middle
Fracture
DK-9 Ⅲ
300.1~302.2
Gray mudstone
F-F
crushing
Middle
Fracture development, local core Ⅳ
357.5~367.6
mudstone, fine grained sandstone
F-F, P- F
crushing
M AN U
Jurassic
Fracture
NA
NA core
SC
Jurassic
development,
F-F, P- F
Ⅰ
184.5~185.5
Gray-brown oil shale
development,
core F-F
crushing
SK-0
Fracture
SK-2
NA
NA
DK
Ⅱ
Ⅲ
250.0~262.0
350.5~354.7
Gray mudstone
F-F
crushing Fracture development, local core F-F crushing Fracture development, local core F-F
NA
crushing Fracture development, local core
Fine grained sandstone
P- F, F-F crushing Fracture
124.1~129.7
core
Mudstone, silty mudstone
Middle Ⅰ
8-19
178.0~199.0
Gray-brown oil shale
TE D
Ⅰ
195.5~196.5
EP
NA
Ⅱ
AC C
NA
NA development,
Gray brown-dark gray mudstone, oil shale
Jurassic
core F-F, P- F
crushing 11
development,
C1 69.04 %、C2 8.83%
ACCEPTED MANUSCRIPT
Middle
Fracture development, local core Ⅱ
133.4~136.1
Silty mudstone
C3 17.11%、i–C4 1.83% F-F
crushing
Jurassic
n–C41.03%、C5 0.5%
Middle 141.5~144.2
Gray muddy siltstone
Local fracture development,
F-F
Ⅰ
293.2~295.5
Dark gray mudstone
Fracture development, soft
F-F
RI PT
Ⅲ Jurassic Middle
Middle 320.6~322.4
Dark gray mudstone, gray-black oil shale
Jurassic
Fracture
Ⅰ
202.8~205.3
Light gray siltstone
Jurassic Middle
Fracture
Jurassic
Ⅲ
311.6~313.4
core P- F, F-F
Ⅰ
267.5~269.4
C1 65.65 %、C2 7.89% C3 19.96%、i–C4 2.96%
core F-F
crushing Fracture
n–C4 1.19%、C5 1.37% development,
core F-F
C6 0.65%、CO2 0.33%
crushing C1 66.43 %、C2 6.53%
AC C
Middle
development,
Gray - dark gray mudstone, oil shale
EP
Jurassic
Jurassic
development,
Brown black - gray black mudstone, oil shale
TE D
262.8~263.7
Middle
13-11
C6 0.28%、CO2 0.38%
crushing, scratches visible
Ⅱ
DK
n–C4 0.87%、C5 2.04% P- F, F-F
leafy
Middle
12-13
C3 25.2%、i–C4 3.2%
Fracture development, massive – Ⅱ
DK
C1 61.3 %、C2 6.8%
SC
11-14
Jurassic
M AN U
DK
C6 0.1%、CO2 1.56%
Fracture
development
well, C3 21.33%、i–C42.49%
Light gray - dark gray silty mudstone
calcite filling, scratches and fault
F-F n–C4 0.89%、C5 1.43%
breccia visible C6 0.16%、CO2 0.74%
164
1. Fracture-Filling gas hydrate reservoir; 2. Pore-Filling gas hydrate reservoir; 12
ACCEPTED MANUSCRIPT 165
2 Mechanism of gas hydrate formation in the Qilian Mountain permafrost Gas hydrate in the Qilian Mountain permafrost was formed under a series of complicated
167
processes, including sedimentation and tectonic movement. As shown in Fig. 3, mechanism of gas
168
hydrate formation in the Qilian Mountain permafrost was related to source rock, hydrocarbon gas,
169
migration pathway, cap rock, reservoir, permafrost, gas hydrate stability zone and others. It mainly
170
included three processes: gas generation, gas migration and accumulation and gas hydrate formation.
171
Source rocks associated with gas hydrate formation in Sanlutian area in the Qilian Mountain
172
permafrost are mudstone from Upper Triassic Galedesi formation and coal-bearing mudstone from
173
Middle Jurassic Yaojie Formation (Xu et al. 2015; Tang et al. 2015b). During the Early Jurassic to
174
Late Cretaceous periods, Sanlutian area was in the subsidence stage. At the end of the Early
175
Cretaceous, the burial depth of Upper Triassic mudstone and Middle Jurassic coal-bearing mudstone
176
was approximately 3000 m, where the formation temperature was up to 120 ℃ and source rock was
177
in the mature-high mature stage. Such conditions were beneficial for generating gas (Jiang et al.
178
2015). Gas is mainly composed of crude oil-associated gas and crude oil cracking gas, and includes a
179
small amount of condensate-associated gas, kerogen cracking gas, coalbed gas, and others. In
180
addition to methane, hydrocarbon gases were also mixed with ethane, propane and butane, as well as
181
a small amounts of C5 + and CO2 (Lu et al. 2010a; Lu et al. 2013b). Since the Late Cretaceous, the
182
regional began to uplift, and the formation was eroded. The maximum temperature of coal-bearing
183
mudstone dropped, which led to sharply declining hydrocarbon generation until no more was
184
generated (Jiang et al. 2015).
AC C
EP
TE D
M AN U
SC
RI PT
166
13
185 186
AC C
EP
TE D
M AN U
SC
RI PT
ACCEPTED MANUSCRIPT
Fig.3. Mechanism of gas hydrate formation in the Qilian Mountain permafrost.
187
During the Yanshan movement in the Late Middle Jurassic to the Early Cretaceous, NW-SE
188
thrust faults were formed in this area (Fig. 1). In the middle and western Sanlutian region, the deep
189
hydrocarbon source rock and shallow formation were connected with F25 and F27 faults, and the deep
190
thermo-genic gases migrated from deep to shallow depths. The thrust faults of F1, F2 and F30 that
191
formed at a relatively late stage of this period were characterized by continuous compression and 14
ACCEPTED MANUSCRIPT effective sealing properties for gas migration (Lu et al. 2013b; Chen et al. 2015a). The Xishan
193
movement in this area had an inheritance effect on F1 and F2 faults, especially in the middle and
194
western regions, which is favorable for gas migration and accumulation. The faults, including F25,
195
F27, F1, F2 and F30, played a role in the migration pathway and effective plugging for gas in the
196
process of gas hydrate formation in Sanlutian area. The gas entered into the broken zone or rock
197
fracture at different depths in the process of gas migration along the main faults. The tight and
198
complete mudstone and oil shale above the fracture zone acted as cap rocks. Under its effective
199
plugging, the gas accumulation zone was formed in fractured reservoirs, such as mudstone, oil shale
200
and siltstone, in the upper part of the Middle Jurassic Jiangcang Formation. A small amount of
201
microbial biogenic gas or coalbed gas may be added locally to the shallow gas accumulation (He et
202
al. 2015; Lu et al. 2015b).
M AN U
SC
RI PT
192
The Qinghai-Tibet Plateau reached its present altitude after the Kunhuang movement and
204
Gonghe movement. With the interaction of Quaternary glacial, the permafrost in the Qilian
205
Mountains has extensively and steadily developed since the Early Middle Pleistocene (Jiang et al.
206
2015; Wang et al. 1989). The inclusion of ethane, propane and CO2 reduced the temperature and
207
pressure condition for gas hydrate formation. Therefore, although the permafrost in the Qilian
208
Mountains was thinner than it in Arctic, there was a gas hydrate stability zone. Gas hydrate samples
209
were found at the depth range of 124.4 to 396 m, which indicated that the temperature and pressure
210
conditions of this range met the need for gas hydrate formation. According to the current drilling
211
data, we consider the depth range of 124.4 to 396 m as a gas hydrate stability zone. Under joint
212
control of the fractured system and lithology, gas hydrate reservoirs formed in the overlap of the gas
213
hydrate stability zone and gas accumulation zone in Sanlutian area, with the fracture-filling type
214
being the main gas hydrate reservoir.
AC C
EP
TE D
203
215
Gas hydrate in Sanlutian area formed under joint control of sedimentation, paleoclimate, and, in
216
particular, tectonic movement. According to the previous description, the mechanism of gas hydrate 15
ACCEPTED MANUSCRIPT formation in this area can be summarized as follows: gas generation from source rock was controlled
218
by tectonic subsidence and uplift--gas migration, accumulation was controlled by fault and tight
219
formation--gas hydrate formation, and accumulation was controlled by permafrost. Due to different
220
gas sources, gas accumulation zone, permafrost thickness and their matching relationships, the
221
distribution of gas hydrate in the vertical section and horizontal plane were heterogeneous in the
222
Sanlutian area.
223
3 Verification analysis on mechanism of gas hydrate formation
224
3.1 Analysis of the gas hydrate stability zone
SC
RI PT
217
The gas hydrate stability zone was mainly determined by the annual mean surface temperature,
226
geothermal gradient, water salinity and gas composition. The annual mean surface temperature and
227
geothermal gradient in permafrost determine the depth of permafrost, as well as control the
228
temperature and pressure conditions for formation. Since the salinity value of groundwater in this
229
area is relatively small, it has little influence on the gas hydrate phase equilibrium condition and
230
liquidus temperature of water. So we can assume that the salinity was 0 in our study (Collett and
231
Dallimore, 2000). As shown in Table 2, the gas components of gas hydrate samples in different wells
232
are not the same, but the proportions of each component are roughly the same. For this reason, gas in
233
DK 12-13 was taken as an example to analyze the gas hydrate stability zone in the Qilian Mountain
234
permafrost.
AC C
EP
TE D
M AN U
225
235
The gas composition in mixed gas hydrate was not exactly the same as the original gas
236
composition (Herri et al., 2011). Therefore, we first needed to infer the original gas composition
237
according to the gas composition in gas hydrate obtained in DK12-13. Then, the equilibrium
238
condition for gas hydrate in Muri basin was predicted. At last, the gas hydrate stability zone was
239
inferred according to the gas hydrate equilibrium condition, and temperature and pressure conditions
240
of formation. 16
ACCEPTED MANUSCRIPT
242
3.1.1 Temperature and pressure distribution of formation
We obtained the temperature distribution for formation by using the equation:
243
=
+
244
=
+
245
where
≤ −
(1)
>
is formation temperature,
(2)
RI PT
241
is annual average surface temperature,
246
temperature of the bottom of permafrost,
247
geothermal gradient below permafrost,
248
bottom of permafrost.
is geothermal gradient of permafrost,
is
is the depth of the
M AN U
SC
is the depth of formation, and
is the
249
The annual average surface temperature in the Muri area is approximately -2.0 ℃ (Li et al.,
250
2014; Zhu et al., 2006). Based on analysis of logging temperature data of DK-1, DK-2 and DK-3, the
251
depth of the bottom of permafrost in the middle and western of Sanlutian area is approximately 95 m
252
(Zhu et al., 2010b). We assumed that
253
Therefore,
254
the Muri basin, the average geothermal gradient of permafrost in the region was 0.026 ℃/m (Cao et
255
al., 2013). According to the temperature logging data of gas hydrate scientific wells DK-1 and DK-8
256
in the middle and western Sanlutian region, the geothermal gradient below permafrost in this area
257
was about 0.286 ~ 0.0404℃/m (Jin et al., 2011). Therefore, in our study, the geothermal gradient of
258
DK 12-13 was assumed to be 0.026℃/m, 0.028℃/m, 0.032℃/m, 0.036℃/m and 0.040℃/m
259
respectively. This temperature profile was shown in Fig. 4.
TE D
is 0 ℃, which was independent of the formation pressure.
AC C
EP
was 0.02105 ℃/m. According to the simple temperature logging data of coal holes in
260
The local gas pressure anomaly was not considered during the formation pressure analysis; only
261
the confining pressure of formation was considered. The relationship between formation pressure
262
and depth was dependent on hydrostatic pore pressure (Sloan and Koh, 2007); therefore, we can
263
obtain the formation pressure-depth relationship. 17
ACCEPTED MANUSCRIPT 264
265
3.1.2 The original gas composition of gas hydrate in DK 12-13
The average gas composition from gas hydrate samples in DK 12-13 is C1 65.65%, C2 7.89%,
266
C3 19.96%, i-C4 2.96%, n-C4 1.19%, C5 1.37%, C6
267
composition was predicted to be C1 94.091%, C2 4.13%, C3 0.845%, i-C4 0.0535%, n-C4 0.275%,
268
C5+ 0.0655% and CO2 0.54% according to an analysis using CSMGem software developed by Center
269
for Hydrate Research, Colorado School of Mines. The average gas composition of headspace gas of
270
DK 12-13 was C1 95.32%, C2 3.41%, C3 1.00%, i-C4 0.07%, n-C4 0.15% and C5 + 0.05% (Tang et al.,
271
2015c), was consistent with the prediction. Therefore, the reliability of the prediction was verified.
272
The minor differences in gas compositions may be associated with later gas migration or new
273
biogenic gas incorporation.
274
3.1.3 Gas hydrate equilibrium condition and gas hydrate stability zone
0.65% and CO2 0.33%. The original gas
M AN U
SC
RI PT
+
The equilibrium temperature of mixed gas hydrate in the formation was predicted by CSMGem
276
software based on the formation pressure, and the mixed gas hydrate equilibrium curve in the
277
formation was obtained, as shown in Fig. 4. The range between two intersection points for the
278
temperature profile and the mixed gas hydrate phase equilibrium curve was called the gas hydrate
279
stability zone.
EP
As shown in Fig. 4, the gas hydrate stability zones of the two gas components had a large
AC C
280
TE D
275
281
difference. For example, the range of gas hydrate stability zone for
282
m for gas component 1 and 25 - 785 m for gas component 2. However, the gas hydrate samples in
283
this area were only found in the range of 124.4 - 396 m, and there was no gas hydrate in permafrost,
284
which was close to the predicted value for gas component 1. The correctness of selecting the original
285
gas components for gas hydrate stability zone analysis was verified.
18
0.032 ℃/m was 108 - 485
M AN U
SC
RI PT
ACCEPTED MANUSCRIPT
286 287
Fig. 4. Gas hydrate stability zone in the Qilian Mountain permafrost. Gas component 1: the original gas component before gas
288
hydrate formation; Gas component 2: the gas component from gas hydrate sample.
Fig. 4 showed that
had little effect on the top boundary of the gas hydrate stability zone,
TE D
289 290
whereas gas component 1 was within 100 - 120 m. However, the bottom boundary of gas hydrate
291
stability zone had a large difference. When
292
/m and 0.026 ℃/m, the corresponding bottom boundary of gas hydrate stability zone was 332 m,
293
398 m, 485 m, 598 m and 667 m, respectively. In comparison with the distribution interval of gas
294
hydrate samples from DK 12-13, which were 202.8 - 313.4 m, and the actual distribution interval of
295
gas hydrate in Sanlutian,which was 124.4 - 396 m, it can be deduced that the
296
0.036℃/m. This value coincides with the
297
method for analyzing the gas hydrate stability zone.
298 299
AC C
EP
was 0.040 ℃/m, 0.036 ℃/m, 0.032 ℃/m, 0.028 ℃
was 0.040℃/m -
of DK 8, which was used to verify the validity of the
Based on the described analysis, it can be inferred that the gas hydrate stability zone in the Qilian Mountain permafrost was 100 m - 400 m depth.
19
ACCEPTED MANUSCRIPT 300
3.2 Numerical simulation of gas accumulation The gas from deep formation entered into the broken zone or rock fracture in the process of gas
302
migration along the main fault. Under effective plugging of the tight formation above the broken
303
zone, the gas accumulation zone was formed in the fractured reservoirs. Based on the analysis of the
304
hydrocarbon gas content in headspace gas, the content of hydrocarbon gases in the fracture zone was
305
high, and they in the formation above the fracture zone decreased as the distance from the fracture
306
zone increased. This showed the property of gas accumulation in the fracture zone and gas migration
307
along the fracture zone or fault, and also indicated that low porosity and low permeability formation
308
effectively seals against gas migration.
M AN U
SC
RI PT
301
To verify the process of gas migration and accumulation, and analyze the influencing factors,
310
the numerical simulation was conducted using TOUGH+HYDRATE software. The interval between
311
125.0 m and 138.5 m in DK 8-19 was chosen as the target layer. The depth of 135.50 - 138.28 m was
312
the fracture zone and the content of hydrocarbon gas was very high. In addition, gas hydrate was
313
found at 135.87 m. From the fracture zone to 128.70 m, the content of hydrocarbon gas gradually
314
decreased.
315
3.2.1 Numerical model and parameters
317 318 319 320 321 322
EP
To conduct this numerical simulation, we must make some simplifications and assumptions,
AC C
316
TE D
309
which were as follows:
(1) The formation was simplified to two types of formation: the fracture zone (135.5-138.5 m) and its overburden(125-135.5 m), as shown in Fig. 5; (2) Each formation was homogenized, and the fracture zone was described by increasing the porosity and permeability; (3) Methane is the only gas.
20
ACCEPTED MANUSCRIPT The basic physical parameters of the interval were obtained from literature, as shown in Table 3
324
(Li et al., 2012; Li et al., 2015; Lu et al., 2010c). In our study, the porosity of overburden was set at
325
0.04 and the fracture zone was set at 0.08.
SC
RI PT
323
327 328
M AN U
326
Fig.5. A simplified diagram of the fracture zone and its overburden. Table 3 The physical properties of the fracture zone and its overburden
Formation
Porosity (including fracture)
Permeability /10-15 m2
Overburden
0.03-0.05
0.01-1
0.07-0.09
1-20
329
TE D
Fracture zone
3.2.2 The setup of numerical simulation
At present, there are few reports on the water saturation of the fracture zone and its overburden
331
in the Qilian Mountain permafrost. To explore the effect of initial water saturation of overburden on
332
the sealing performance of gas, six different initial water saturations (0.95, 0.9, 0.8, 0.7, 0.5 and 0.2)
333
were selected for numerical simulation. Similarly, four different permeability (0.01×10-15 m2、
334
0.05×10-15 m2、0.1×10-15 m2 and 1×10-15 m2) were used.
335
3.2.3 Results and Analysis
AC C
EP
330
336
Fig. 6 shows the final distribution of gas saturation at different initial water saturation. When
337
the initial water saturation was high, gas saturation in the fracture zone was approximately 0.7, which 21
ACCEPTED MANUSCRIPT exceeded the initial gas saturation and indicated that the entry of deep high-pressure gas caused the
339
movement of water in the fracture zone and its adjacent overburden. When the initial water
340
saturation was low (as in the case of 0.2), gas from deep reservoirs had enough space and relatively
341
large permeability in the fracture zone; therefore, there was almost no water migration. When the
342
initial water saturation was 0.9 and 0.95, the gas saturation decreased sharply from 128.5 to 129 m
343
and from 126.5 to 127 m, respectively, and there was no change between the final gas saturation
344
above this interval and the initial gas saturation. This indicated that the overburden played a role in
345
gas sealing, when the initial water saturation was higher than 0.8. When the initial water saturation
346
was less than 0.8, the gas saturation in the formation is gradually reduced, and there is no sharp
347
decrease, which indicates that the overburden had no role in gas sealing.
348 349
AC C
EP
TE D
M AN U
SC
RI PT
338
Fig.6. The distribution of gas saturation at different initial water saturations.
350
Fig. 7 shows the final distribution of gas saturation at different permeability of overburden.
351
When the permeability of overburden was 0.01 × 10-15 m2 and 0.05 × 10-15 m2, the gas saturation
352
decreased sharply at depths of 132 m and 128.7 m, respectively. This indicated that the overburden 22
ACCEPTED MANUSCRIPT played a role in gas sealing. However, when permeability was more than 0.1 ×10-15 m2, there was no
354
sharp decrease, which indicated that the sealing property of the overburden was poor.
M AN U
SC
RI PT
353
355
Fig.7. The distribution of gas saturation at the different permeability of overburden.
TE D
356
In summary, in addition to the effect of porosity, the sealing property of the overburden was
358
mainly controlled by rock permeability and the initial water saturation. When the initial water
359
saturation was 0.9 and the permeability was 0.05 ×10-15 m2, gas saturation rapidly decreased from
360
128.5 to 129 m, which was close to the depth of 128.7 m observed in drilling. This indicated that the
361
overburden was an effective sealant, which could achieve gas accumulation in the fracture zone, and
362
provided adequate gas for gas hydrate formation. The values of the permeability obtained by
363
numerical simulation were close to those measured in the laboratory, which proved that the
364
numerical simulation was valid. For the mudstone, which had less porosity and permeability, an
365
effective sealing effect for gas accumulation can be achieved.
AC C
EP
357
366
Numerical simulation was used to further verify that the low-porosity and low-permeability
367
formation with high water saturation can effectively seal gas and form gas accumulation zone. This
23
ACCEPTED MANUSCRIPT 368
supported the hypothesis that gas hydrate formation occurred after the formation of gas accumulation
369
zone.
370
3.3 Experimental Study on Synthesis of Gas Hydrate in Different Lithology Gas hydrates in the Qilian Mountain permafrost mainly occurred in the fracture of mudstone, oil
372
shale, siltstone and fine sandstone and in the pores of siltstone and fine sandstone. To investigate the
373
effect of lithology on synthesis of gas hydrate, three different lithologies were used.
374
3.3.1 Experimental preparation
SC
RI PT
371
Mudstone, sandstone and granite core with fractures were selected as the experimental medium
376
in this paper. Mudstone is one of the main lithology containing gas hydrate in the Qilian Mountain
377
permafrost. It is a type of clay rock with low permeability and porosity, and has good water
378
absorption and water retention. Sandstone is the main lithology for pore gas hydrate. Granite is also a
379
type of rock with the low permeability and porosity, but its water absorption and water retention is
380
very poor.
TE D
M AN U
375
The experimental apparatus for synthesis of gas hydrate mainly includes the reactor system, the
382
control system for temperature and pressure, and a detection and recording system, as shown in Fig.
383
8.
AC C
EP
381
384 385
Fig.8. The schematic diagram of experimental apparatus for synthesis of gas hydrate. 1 Methane cylinder; 2 Gas pressure
386
reducing valve; 3 Shut-off valve; 4 Reactor; 5 Temperature sensor; 6 Constant temperature water bath; 7 Pressure sensor; 8
387
Pressure gauge; 9 Vent valve; 10 Paperless recorder. 24
ACCEPTED MANUSCRIPT 388
3.3.2 Experimental result
Methane hydrate was formed in all three fissures, most of which occurred in mudstone fissures;
390
there were few methane hydrates in sandstone fissures and granite fissures. The pore-filling hydrates
391
were present only in the pore of sandstone cores. The experimental results are as follows:
RI PT
389
(1) Methane hydrate distribution in mudstone fracture
393
Most methane hydrates were found in mudstone fractures, and they were milky white and
394
occurred as layers or nodules. Both the horizontal and oblique fractures had large amounts of gas
395
hydrate. The hydrate layer in the horizontal fracture was thicker than the hydrate layer in the oblique
396
or vertical fracture. Methane hydrate in the vertical fracture or high-angle oblique fracture occurred
397
as nodular or wavy, as shown in Fig. 9-a. Methane hydrates in the mudstone fracture were flammable
398
and boiling during combustion, as shown in Fig. 9-b.
400
AC C
399
EP
TE D
M AN U
SC
392
Fig.9. Methane hydrate in mudstone fracture and ignition.
401
(2) Gas hydrate distribution in sandstone
402
Only a small amount of methane hydrates were formed in the sandstone fracture, and it
403
decomposed during the reactor disassembly. Because sandstone pore is small, pore-filling gas
404
hydrates could not be visually observed by the naked eye. The presence of gas hydrates in the pore
405
were determined by the strong bubbling in water, as shown in Fig. 10.
406
(3) Gas hydrate distribution on granite fracture 25
ACCEPTED MANUSCRIPT There was a very small amount of methane hydrate on the horizontal surface of the granite and
408
it appeared only in low-lying areas of horizontal surface or at the core edge. No methane hydrate was
409
formed in vertical fractures or high-angle fractures, as shown in Fig. 11.
410 Fig.10. Strong bubbling caused by hydrate dissolution in sandstone.
412
3.3.3 Analysis and discussion
Fig. 11. Little methane hydrate on the granite fracture.
M AN U
411
SC
RI PT
407
Granite and mudstone cores were low-porosity and low-permeability rock, there was only a
414
very small amount of methane hydrate on the granite fracture. However, a large amount of methane
415
hydrate formed in the mudstone fracture, which was mainly controlled by effective water absorption
416
and water retention in the mudstone and water migration during hydrate formation. There was a
417
thickness of free water film in the mudstone fracture, which could provide full contact with gas and
418
transformed into methane hydrate under appropriate condition. When methane hydrate formed in the
419
mudstone fracture, a suction effect on the water in the micro-pore or micro-fissure and in the
420
metastable state and unstable state in clay minerals was induced. This resulted in a migration of
421
water to fracture surface that continued to form hydrate. According to the experimental results,
422
methane hydrate was mainly distributed in the fracture for low-porosity and low-permeability rock,
423
and its occurrence was mainly controlled by water distribution and migration.
AC C
EP
TE D
413
424
Since the mudstone pores were mainly microporous and mesoporous, the formation of methane
425
hydrate was difficult. Therefore, the pore-filling methane hydrate was not observed in mudstone in 26
ACCEPTED MANUSCRIPT the experiment. The pore of the sandstone was relatively large, and most pores had no effect on the
427
methane hydrate phase equilibrium condition. In addition, the free water saturation in the sandstone
428
pore was low relative to the mudstone; therefore, the gas can diffuse and migrate in the sandstone
429
pore and form methane hydrate with water. The water film on the sandstone fracture was relatively
430
thin; therefore, the amount of gas hydrate in the fracture was less. As porosity of sandstone increased,
431
the thickness of the water film decreased (Wang et al., 2012), and the gas relative permeability
432
increased. Therefore, the amount of gas hydrate in the fine or medium grained sandstone fracture
433
was little or zero, while the amount of gas hydrate in the pores increased. The formation of gas
434
hydrate in the sandstone was mainly controlled by pore size and clay content, which further
435
controlled water distribution and gas permeability.
M AN U
SC
RI PT
426
The occurrence of methane hydrate in the lab experiment was consistent with observations in
437
the field, which verified the hypothesis that the occurrence of gas hydrate was controlled by lithology
438
and the fracture system.
439
4 Conclusions
TE D
436
1. Gas hydrate in the Sanlutian region formed under the joint control of tectonic movement,
441
sedimentation and paleoclimate. The mechanism of gas hydrate formation in this area can be
442
summarized as follows: gas generation from source rock was controlled by tectonic subsidence and
443
uplift--gas migration and accumulation was controlled by fault and tight formation--gas hydrate
444
formation and accumulation was controlled by permafrost. At the end of the Early Cretaceous, the
445
Upper Triassic mudstone and Middle Jurassic coal-bearing mudstone began to generate gas. Gas
446
entered into the broken zone at different depths during the process of gas migration along the main
447
fault, such as F25, F27, F1, F2 and F30, which was formed in the Yanshan movement and the Xishan
448
movement. Under effective plugging of the tight and complete mudstone and oil shale formation
449
above the fracture zone and fault F1 and F2 with continuous compression, the gas accumulation zone
450
was formed in the fractured reservoirs. Under joint control of the Qinghai-Tibet Plateau uplift and
AC C
EP
440
27
ACCEPTED MANUSCRIPT 451
the Quaternary glacial, the depth of permafrost in this area reached approximately 90 m, which
452
provided the temperature and pressure condition for gas hydrate formation. Finally, gas hydrate
453
reservoirs formed in the overlap of the gas hydrate stability and gas accumulation zones in the
454
Sanlutian area. 2. The permafrost-associated gas hydrate samples in China were only obtained beneath
456
permafrost in the range of 124.4-396.0 m in the Sanlutian region, and the gas composition was
457
complex. The original gas composition before gas hydrate formation in DK 12-13 was predicted to
458
be C1 94.091%, C2 4.13%, C3 0.845%, i-C4 0.0535%, n-C4 0.275%, C5+ 0.0655% and CO2 0.54% by
459
using CSMGem software, which was used to analyze the range of gas hydrate stability zone in
460
DK12-13 at 108-485 m. Combined with the range of gas hydrate samples, it can be inferred that the
461
gas hydrate stability zone in the Qilian Mountain permafrost was 100-400 m depth.
M AN U
SC
RI PT
455
3. The results of numerical simulation of gas distribution in the interval of 128.70-138.28 m
463
indicated that the sealing property of the overburden was mainly controlled by porosity, rock
464
permeability and initial water saturation. When initial water saturation was 0.9 and permeability was
465
0.05 × 10-15 m2, gas saturation rapidly decreases from 128.5 to 129 m, which was close to the depth
466
of 128.7 m that was observed in drilling. This indicated that the overburden was an effective sealant,
467
which could achieve gas accumulation in the fracture zone, and provided adequate gas for gas
468
hydrate formation. This supported the hypothesis that gas hydrate formation occurred after the
469
formation of gas accumulation zone.
AC C
EP
TE D
462
470
4. Gas hydrate mainly occurred in the fracture of low-porosity and low-permeability rocks such
471
as Jurassic mudstone and oil shale. Through laboratory experiments and numerical simulations, it
472
was found that methane hydrate was more likely to form in mudstone fractures. This was mainly
473
controlled by effective water absorption and retention of the mudstone and water migration during
474
hydrate formation. The water film on the sandstone fracture was relatively thin; therefore, there was
475
little methane hydrate in the fracture. The formation of methane hydrate in the sandstone was mainly 28
ACCEPTED MANUSCRIPT controlled by the pore size and clay content, which further controlled the water distribution and gas
477
permeability. The occurrence of methane hydrate in the lab experiment was consistent with field
478
observations, which verified the hypothesis that the occurrence of gas hydrate was controlled by
479
lithology and the fractured system.
480
Acknowledgments
RI PT
476
This study has been supported by National Natural Science Foundation of China (Grant
482
No.51474112, Grant No.51304079), and China Geological Survey Project (GZHL201400307,
483
GZHL20110326).
484
Nomenclature
486
Fault 2
487
Fault 25
488
Fault 27
489
Fault 30
M AN U
Fault 1
TE D
485
SC
481
F-F Fracture-Filling gas hydrate reservoir
491
P-F Pore-Filling gas hydrate reservoir
492
NA No data
AC C
493
EP
490
Formation temperature (℃)
494
Annual average surface temperature (℃)
495
Temperature of the bottom of permafrost (℃)
496
Geothermal gradient of permafrost (℃/m)
497
Geothermal gradient below permafrost (℃/m)
498
Depth of formation (m) 29
ACCEPTED MANUSCRIPT !
Depth of the bottom of permafrost (m)
500
"#
Initial water saturation
501
References
502
Bily C, Dick J W L, 1974. Naturally occurring gas hydrates in the Mackenzie Delta, NWT. Bulletin
503
of Canadian Petroleum Geology. 22(3), 340-352.
RI PT
499
Cao DY, Li J, Wang D, et al, 2013. Study of the gas hydrate stability zone in Muri Coalfield,
505
Qinghai Province, China. Journal of China University of Mining & Technology. 42(1), 76-82[in
506
Chinese with English abstract].
SC
504
Chen LM, Cao DY, Jiang AL, et al, 2015a. Structural control of reservoir forming for natural gas
508
hydrate in Sanlutian well field, Qinghai. Science & Technology Review. 33(6), 91-96 [in
509
Chinese with English abstract].
M AN U
507
Chen LM, Qin RF, Jiang AL, et al, 2015b. Structural fracture characteristics of cores from gas
511
hydrate drillholes in Sanlutian of Muli Coalfield, Qinghai. Geoscience. 29(5), 1087-1095 [in
512
Chinese with English abstract].
TE D
510
Cheng B, Xu JB, Lu ZQ, et al, 2017. Hydrocarbon source for oil and gas indication associated with
514
gas hydrate and its significance in the Qilian Mountain permafrost, Qinghai, Northwest China.
515
Marine and Petroleum Geology (2017), https://doi.org/10.1016/j.marpetgeo.2017.02.019.
517 518 519 520 521 522 523
Collett TS, 2002. Energy resource potential of natural gas hydrates. AAPG bulletin. 86(11),
AC C
516
EP
513
1971-1992.
Collett TS, 1993. Natural gas hydrates of the Prudhoe Bay and Kuparuk River area, North Slope, Alaska. AAPG bulletin. 77(5), 793-812. Collett TS, Dallimore SR, 2000. Permafrost-associated gas hydrate//Natural Gas Hydrate. Springer Netherlands. 43-60. Collett TS, Lee MW, Agena WF, et al, 2011. Permafrost-associated natural gas hydrate occurrences on the Alaska North Slope. Marine and Petroleum Geology. 28(2), 279-294. 30
ACCEPTED MANUSCRIPT 524 525
Collet TS, Johnson A, Knapp C, et al, 2009. Natural gas hydrates: Energy resource potential and associated geologic hazards. Am Assoc Pet Geol Mem. 89, 137. Herri JM, Bouchemoua A, Kwaterski M, et al, 2011. Gas hydrate equilibria for CO2-N2 and
527
CO2-CH4 gas mixtures, experiments and modelling[C]//7th International Conference on Gas
528
Hydrates. 435.
RI PT
526
He XL, Liu CL, Meng QG, et al, 2015. Gas composition of hydrate-bearing cores in juhugeng
530
drilling area in Qinghai and its indicative significance. Geoscience. 29(5), 1194-1200 [in
531
Chinese with English abstract].
SC
529
Huang X, Zhu YH, Wang PK, et al, 2011. Hydrocarbon gas composition and origin of core gas from
533
the gas hydrate reservoir in Qilian Mountain permafrost. Geological Bulletin of China. 30(12),
534
1851-1856 [in Chinese with English abstract].
M AN U
532
Hou J, Zou CC, Qu L, et al, 2015. Classification and identification of gas hydrate reservoirs from
536
well log data in Sanlutian, Muli Coalfield, Qinghai. Geoscience. 29(5), 1110-1121 [in Chinese
537
with English abstract].
538 539
TE D
535
Jiang AL, Chen LM, Qin RF, et al, 2015. Tectonic subsidence history of Sanlutian mining field in Muli, Qinghai. Geomechanics. 21(3), 1096-1102[in Chinese with English abstract]. Jin CS, Qiao DW, Lu ZQ, et al, 2011. Study on the characteristics of gas hydrate stability zone in the
541
Muli permafrost, Qinghai - comparison between the modeling and drilling results. Chinese
542
J.Geophys. 54(1), 173- 181[in Chinese with English abstract].
AC C
EP
540
543
Li CF, Liu CL, Meng QG, et al, 2015. CT image characterization of pores and fissures in rock core
544
from Juhugeng gas hydrate area in Qinghai. Geomechanics. 21(3), 1189-1193[in Chinese with
545
English abstract].
546
Li J, Cao DY, Chen LM, et al, 2014. Studies on occurrence and controlling factors of natural gas
547
hydrate in Muli coalfield, Qinghai province. Annual Joint Annual Meeting of Chinese Earth
548
Sciences. 2475-2477 [in Chinese]. 31
ACCEPTED MANUSCRIPT 549
Li J, Cao DY, Dou XQ, et al, 2012. Accumulation model of natural gas hydrate in Muli area. Journal
550
of Liaoning Technical University (Nature Science). 31(4), 484-488[in Chinese with English
551
abstract]. Li YH, Ji CW, Shao LY, et al, 2013. Characteristics and accumulating model of gas hydrates in the
553
Muli coalfield of Qinghai province. Xinjiang Geology. 31(2), 223-227 [in Chinese with English
554
abstract].
556
Li YH, Wang WC, Lu ZQ, et al, 2015. Preliminary evaluation on gas hydrate resources in Sanlutian of Muli Qinghai. Geoscience. 29(5), 1251-1258 [in Chinese with English abstract].
SC
555
RI PT
552
Lu ZQ, Li YH, Wang WC, et al, 2015a. Study on the accumulation pattern for permafrost-associated
558
gas hydrate in Sanlutian of Muli,Qinghai. Geoscience. 29(5), 1014-1023 [in Chinese with
559
English abstract].
M AN U
557
Lu ZQ, Tang SQ, Wang WC, et al, 2015b. Study on the nature of gas source for
561
permafrost-associated gas hydrate in Sanlutian of Muli, Qinghai. Geomechanics. 21(3),
562
995-1001[in Chinese with English abstract].
563 564
TE D
560
Lu ZQ, Zhu YH, Zhang YQ, et al, 2010a. Study on genesis of gases from gas hydrate in the Qilian Mountain permafrost, Qinghai. Geoscience, 24(3), 581-588 [in Chinese with English abstract]. Lu ZQ, Zhu YH, Zhang YQ, et al, 2010b. Basic geological characteristics of gas hydrates in Qilian
566
Mountain permafrost area, Qinghai Province. Mineral Deposits. 29(1), 182-191 [in Chinese
567
with English abstract].
AC C
EP
565
568
Lu ZQ, Zhu YH, Zhang YQ, et al, 2010c. Estimation method of gas hydrate resource in the Qilian
569
Mountain permafrost area, Qinghai, China—a case of the drilling area. Geological Bulletin of
570
China. 29(9), 1310-1318[in Chinese with English abstract].
571 572
Lu ZQ, Zhu YH, Zhang YQ, et al, 2013a. Accumulation system of gas hydrate in the Qilian Mountains permafrost. Chinese Academy of Geological Sciences. 486-487 [in Chinese].
32
ACCEPTED MANUSCRIPT 573 574 575 576
Lu ZQ, Zhu YH, Liu H, et al, 2013b. Gas source for gas hydrate and its significance in the Qilian Mountain permafrost, Qinghai. Marine and Petroleum Geology. 43, 341-348. Majorowicz JA, Osadetz KG, 2001. Gas hydrate distribution and volume in Canada. AAPG bulletin. 85(7), 1211-1230. Meng QG, Liu CL, Li CF, et al, 2015. Reman spectroscopic characteristics of natural gas hydrates
578
from Juhugeng drilling area, Qinghai. Geoscience. 29(5), 1180-1188 [in Chinese with English
579
abstract].
RI PT
577
Pang SJ, 2012. Relationship between tectonic, sedimentation characteristics and distribution of gas
581
hydrate in Muli coalfield of Qilian Mountain, China. China University of Geosciences (Beijing)
582
[in Chinese with English abstract]
M AN U
SC
580
583
Pang SJ, Su X, He H, et al, 2013. Geological controlling factors of gas hydrate occurrence in Qilian
584
Mountain permafrost, China. Earth Science Frontiers. 20(1), 223-239 [in Chinese with English
585
abstract].
Tang SQ, Lu ZQ, Rao Z, et al, 2015a. The indicative significance of gas composition and isotopes of
587
headspace gases from the gas hydrate drilling core in the Qilian Mountain permafrost: A case
588
study of well DK-9. Geological Bulletin of China. 34(5), 961-971 [in Chinese with English
589
abstract].
EP
TE D
586
Tang SQ, Lu ZQ, Wang WC, et al, 2015b. Organic geochemical characteristics of gas source rocks
591
in the Sanlutian mine of the Muli mining area, Qinghai. Geomechanics. 21(3), 1214-1222[in
592
Chinese with English abstract].
AC C
590
593
Tang SQ, Lu ZQ, Wang WC, et al, 2015c. The indicative significance of gas composition of
594
headspace gases from the gas hydrate drilling holes in the Sanlutian mine of the Muli mining
595
area, Qinghai. Geomechanics. 21(3), 1201-1213[in Chinese with English abstract].
596
Sloan Jr E D, Koh C, 2007. Clathrate hydrates of natural gases. CRC press.
33
ACCEPTED MANUSCRIPT 597 598
Wang WC, Lu ZQ, Li YH, et al, 2015. Distribution and reservoir characteristics of gas hydrates in Sanlutian of Muli,Qinghai. Geoscience. 29(5), 1035-1046 [in Chinese with English abstract]. Wang PK, Zhu YH, Lu ZQ, et al, 2011. Gas hydrate in the Qilian Mountain permafrost and its
600
distribution characteristics. Geological Bulletin of China. 30(12), 1839-1850 [in Chinese with
601
English abstract]
RI PT
599
Wang PK, Zhu YH, Lu ZQ, et al, 2014. Geochemistry and genesis of authigenic pyrite from gas
603
hydrate accumulation system in the Qilian Mountain permafrost, Qinghai, northwest China.
604
Science China: Earth Sciences. 44(6), 1283 ~ 1297 [in Chinese with English abstract].
SC
602
Wang SL, 1989. Formation and evolution of permafrost on the Qinghai-Xizang Plateau since the
606
Late Pleistocene. Journal of Glaciology and Geocryology. 11(1), 69-75[in Chinese with English
607
abstract].
M AN U
605
Wang Y, Liu JB, Wang WQ, et al, 2012. The research on the determination of the porosity limitation
609
of the low permeability sandstone reservoirs by the water film thickness. Petrochemical
610
Industry Application. 31(6), 13-16[in Chinese with English abstract].
611 612
TE D
608
Wen HJ, Lu ZQ, Li YH, et al., 2015. New advance on gas hydrate survey and research in Sanlutian of Muli,Qinghai. Geoscience. 29(5), 983-994 [in Chinese with English abstract]. Xu JS, Wen ZG, Hu DG, et al, 2015. Evaluation of the hydrocarbon generation potential of source
614
rocks of the Jurassic Yaojie formation in Muli depression of Qilian Mountains. Journal of
615
Geomechanics. 21(3), 446-452[in Chinese with English abstract].
617
AC C
616
EP
613
Yakushev VS, Chuvilin EM, 2000. Natural gas and gas hydrate accumulations within permafrost in Russia. Cold Regions Science and Technology. 31(3), 189-197.
618
Yang ZY, Wang WC, Shao LY, et al, 2015. Deposition environment of the middle Jurassic in the
619
Sanlutian mining field of the Juhugeng mining area in Qinghai Province. Geoscience. 29(5),
620
1073-1086 [in Chinese with English abstract].
34
ACCEPTED MANUSCRIPT 621
Zhai GY, Lu ZQ, Lu HL, et al, 2014. Gas hydrate geological system in the Qilian Mountain
622
permafrost. Journal of Mineralogy and Petrology. 34(4), 79-92 [in Chinese with English
623
abstract]. Zhang JH, Wei W, Wei XH, et al, 2013. Discussion about natural gas hydrate formation conditions
625
and accumulation pattern in China’s major permafrost regions. China Petroleum Exploration.
626
18(5), 74-78 [in Chinese with English abstract].
RI PT
624
Zhu YH, Liu YL, Zhang YQ, 2006. Formation conditions of gas hydrates in permafrost of the Qilian
628
Mountains, Northwest China. Geological Bulletin of China. 25(1-2), 28-63[in Chinese with
629
English abstract].
M AN U
633
Zhu YH, Zhang YQ, Wen HJ, et al, 2010b. Gas hydrates in the Qilian Mountain permafrost and their basic characteristics. Acta Geoscientica Sinica. 31(1), 7-16 [in Chinese with English abstract].
TE D
632
Qinghai, Northwest China. Acta Geologica Sinica (English Edition). 84(1), 1-10.
EP
631
Zhu YH, Zhang YQ, WEN HJ, et al, 2010a. Gas hydrates in the Qilian Mountain permafrost,
AC C
630
SC
627
35
ACCEPTED MANUSCRIPT Highlights The mechanism of gas hydrate formation in the Qilian Mountain permafrost was inferred in detail.
numerical analysis and laboratory experiments.
RI PT
Some control factors of gas hydrate formation were analysed and validated through
The gas hydrate stability zone in the Qilian Mountain permafrost was at the depth of
SC
100-400 m.
M AN U
The low-porosity and low-permeability formation with high water saturation can effectively seal gas and form gas accumulation zone.
AC C
EP
TE D
The occurrence of gas hydrate was controlled by lithology and the fractured system.