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Hao 2011 Organic-Geochemistry
Hao 2011 Organic-Geochemistry
Organic Geochemistry
journal homepage: www.elsevier.com/locate/orggeochem
State Key Laboratory of Petroleum Resources and Prospecting, China University of Petroleum, Fuxue Road No. 18, Changping, Beijing 102249, China
Key Laboratory of Tectonics and Petroleum Resources, Ministry of Education, China University of Geosciences, Wuhan 430074, China
Department of Earth Sciences, Zhejiang University, Hangzhou, Zhejiang 310027, China
d
Tianjin Branch of China National Offshore Oil Company Ltd., Tianjin 300452, China
b
c
a r t i c l e
i n f o
Article history:
Received 15 September 2010
Received in revised form 15 November 2010
Accepted 27 January 2011
Available online 2 February 2011
a b s t r a c t
Three Paleogene syn-rift intervals from the Bohai Bay Basin, the most petroliferous basin in China, were
analyzed with sedimentological and geochemical techniques to characterize the lateral source rock heterogeneities, to reveal the environmental and ecological changes through geologic time and to construct
depositional models for lacustrine source rocks under different tectonic and climatic conditions. The third
(Es3) and rst (Es1) members of the Eocene Shahejie Formation and the Oligocene Dongying Formation
(Ed) display widely variable total organic carbon contents, hydrogen indices and visual kerogen compositions, suggesting changes in organic facies from deep to marginal sediments. Carefully selected deeplake facies samples from any interval, however, display fairly uniform biomarker composition. These
three intervals have distinctly different biomarker assemblages, which indicate weakly alkaline, freshwater lakes with a moderately deep thermocline during Es3 deposition, alkaline-saline lakes with shallow
chemocline during Es1 deposition and acidic, freshwater lakes with deep, unstable thermocline during
the deposition of the Dongying Formation. Such environmental changes corresponded to changes in subsidence rate and paleoclimate, from rapid subsidence and wet climate during Es3 deposition, through
slow subsidence and arid climate during Es1 deposition to rapid subsidence and wet climate during Ed
deposition and resulted in synchronous changes in terrigenous organic matter input, phytoplankton community and primary productivity. The co-evolution of environments and organisms controlled by tectonic subsidence and climate accounted for the deposition and distribution of high quality lacustrine
source rocks with distinctly different geochemical characteristics. Most rift basins experienced changes
in subsidence rates and possibly changes in climates during their syn-rift evolutions. The models constructed in this paper may have important implications for source rock prediction in other lacustrine rift
basins.
2011 Elsevier Ltd. All rights reserved.
1. Introduction
Lakes and lake deposits are important to understand and
predict because they host signicant petroleum resources (e.g.,
Kelts, 1988; Katz, 1990, 1995), are used to address climate change
and paleoclimate questions (e.g., Meyers, 1997, 2003; Fan et al.,
2007) and are signicant sources of biodiversity (Carroll and
Bohacs, 1999). Modern and ancient lakes displayed a wide variation in hydrogeology and water chemistry (e.g., Carroll and Bohacs,
Corresponding author at: State Key Laboratory of Petroleum Resources and
Prospecting, China University of Petroleum, Fuxue Road No. 18, Changping, Beijing
102249, China.
E-mail addresses: haofang@cup.edu.cn (F. Hao), zhouxh3@cnooc.com.cn
(X. Zhou), zyming@zju.edu.cn (Y. Zhu), yangyuanyuan3@foxmail.com (Y. Yang).
0146-6380/$ - see front matter 2011 Elsevier Ltd. All rights reserved.
doi:10.1016/j.orggeochem.2011.01.010
324
variations in hydrocarbon potentials and geochemical characteristics (e.g., Follows and Tyson, 1998; Justwan et al., 2006; Keym
et al., 2006; Hao et al., 2009a). Several case studies have been
examined to explain the horizontal (Follows and Tyson, 1998)
and vertical (Carroll and Bohacs, 1999, 2001; Bohacs et al., 2000;
Gonalves, 2002; Harris et al., 2004) heterogeneities of lacustrine
source rocks. Carroll and Bohacs (1999, 2001) and Bohacs et al.
(2000) emphasize the controls of lake types (balance lled lakes,
underlled lakes and overlled lakes) on source rock properties.
Fig. 1. (A) Sub-basins of the Bohai Bay Basin (sub-basin classication from Allen et al. (1997)). (B) The Bozhong sub-basin showing wells from which samples were taken.
YRM = Yellow River Mouth.
325
BOZHONG SUB-BASIN
JIYANG SUB-BASIN
Anz
N+Q
Es
Depth (km)
Es
Ed
Ed
Pz
10
Mz
20
Mz
Post-rift Sediments
Syn-rift Sediments
Mz
10
Ek
12
15
Ek
Mz
8
Es
Ek
Pz
Ek
Ed
Pz
Es
Ek
Es
6 Mz
Pz
Es
25
Pz
0
25
50 km
Ed
N+Q
30
35
Fig. 2. Cross section showing the structural framework of the Bohai Bay Basin. Note the thick Oligocene syn-rift sediments (the Dongying Formation, Ed) and Miocene to
Quaternary post-rift sediments and strong faulting in the Bozhong sub-basin. Section location in Fig. 1A.
Miocene
15
Neogene
10
20
Oligocene
25
30
Mingmuazhen
Pliocene
5
TECTONIC
EVOLUTION
Nmu
NmL
post-rift
Guantao
Quaternary
STRATA
LITHOLOGY
Form. Symbol
Qp
PY
Dongying
GEOLOGICAL
AGE (Ma)
35
Ng
Ed1
Ed2
Ed3
Es1
Shahejie
45
Eocene
40
Paleogene
Es2
Es3
S
syn-rift
Es4
2.5 109 tons (18.3 109 barrels) (Hao et al., 2009b; Gong et al.,
2010), is one of the most petroliferous sub-basins of the Bohai
Bay Basin. While the most important source rock interval in other
Bohai Bay sub-basins is the fourth member of the Eocene Shahejie
Formation (Es4, 50.543.0 Ma, Fig. 3) (e.g., Fuhrmann et al., 2004;
Zhang et al., 2005), Es4 has made no signicant contribution to
oil reserves so far found in the Bozhong sub-basin (Gong, 1997;
Hao et al., 2007, 2009b,c) and factors controlling the deposition
of lacustrine source rocks in the Bozhong sub-basin are not clearly
understood. All syn-rift intervals in the Bozhong sub-basin are
dominated by sandstones and mudstones/shales. The relatively
monotonous lithologic composition and paleoenvironments restrict the application of a conventional sedimentological approach
to reveal the environmental and ecological changes through geologic time (Gonalves, 2002). On the other hand, the Bozhong
sub-basin experienced multiple rifting events (Hao et al., 2009b),
and paleoclimate changed considerably during the syn-rift evolution (Wang et al., 2010). Therefore, the Bozhong sub-basin provides
an excellent natural laboratory for investigating the environmental
and ecological changes induced by changes in tectonic subsidence
and paleoclimate and for revealing the mechanisms for high quality source rock deposition under different tectonic and climatic
conditions. The purpose of our study is to assess the geochemical
variability of the Eocene and Oligocene lacustrine rift sequences
of the Bozhong sub-basin, Bohai Bay Basin, to reveal environmental
and ecological changes and to construct models for high quality
lacustrine source rocks under different tectonic and climatic conditions by integrating geological and geochemical data.
2. Geological setting
60
Paleocene
55
65
Kongdian
50
Ek
Basement
Conglomerate
Pre-Tertiary
Rocks
Sandstone
Mudstone
Potential
Source Rock
Major Oil
Reservoir
Fig. 3. Generalized stratigraphy of the Bozhong sub-basin, Bohai Bay Basin. Possible
source rock and major reservoir intervals are marked. Form. = Formation;
PY = Pingyuan.
The Bohai Bay Basin, also known as the North China Basin (Ye
et al., 1985; Hsiao et al., 2004) or the Bohai Basin (Chang, 1991;
Allen et al., 1997), is a Cenozoic lacustrine basin located on the
eastern coast of China (Fig. 1A). The Bohai Bay Basin formed on
the North China Craton (Wang and Qian, 1992; Ge and Chen,
1993) and has an area of about 200,000 km2. The mechanisms for
the formation of the Bohai Bay Basin are still controversial. Ye
et al. (1985) explained the formation of the Bohai Bay Basin with
McKenzies (1978) two stage extension model proposing Paleogene
rifting and Neogene to Quaternary thermal subsidence stages.
Allen et al. (1997, 1998), in view of the prominence of the Tan-Lu
fault, proposed a composite pull-apart basin model to explain the
formation of the Bohai Bay Basin. In recent years, more and more
workers tend to explain the Bohai Bay Basin as a Cenozoic rift basin
modied by synchronous strike slip faulting (e.g., Hsiao et al.,
2010; Qi and Yang, 2010).
326
The Bohai Bay Basin experienced two major tectonic evolutionary stages (Wang and Qian, 1992; Ge and Chen, 1993; Allen et al.,
1997; Hsiao et al., 2004, 2010) (Figs. 2 and 3). The basin consists of
Paleogene rifts, which were lled by a thick non-marine clastic
succession. An unconformity at the top of the syn-rift sediments
separates them from MioceneRecent strata, which were deposited during post-rift thermal subsidence (Allen et al., 1997). During
the syn-rift stage (65.024.6 Ma), a series of grabens and halfgrabens (Fig. 2) developed along major NW and NE trending fault
sets (Lu and Qi, 1997; Yang and Xu, 2004; Qi and Yang, 2010).
Table 1
Biomarker parameters for rock samples from different intervals in the Bozhong sub-basin, Bohai Bay Basin.
SN
Well
Depth (m)
Lithology
Interval
Pr/Ph
C35/C34
G/H
ETR
C27/C27
C19/C23
C20/C23
C24/C26
C23/C30
4MSI
C27/C29
C28/C29
S/H
1
2
3
4
5
6
7
8
9
10
11
12
13
14
15
16
17
18
19
20
21
22
23
BZ-2
BZ-2
BZ-2
BZ-2
BZ-2
BZ-2
BZ-2
BZ-2
BZ-2
BZ-2
BZ-7
BZ-6
BZ-8
BZ-8
BZ-9
BZ-3
BZ-3
BZ-8
BZ-9
BZ-3
BZ-3
BZ-3
BZ-3
3777.5
3805
3825
3860
3905
3925
3975
4010
4122.5
4155
3205
3084.5
3171.8
3177.5
2928.5
2781
3289.5
3290
3037.5
3318
3505.5
3595.5
3691.5
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Mudstone
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Ed
Ed
Ed
Ed
Ed
Ed
Ed
Ed
Ed
Ed
Ed
Ed
Ed
Ed
Ed
Ed
Ed
Ed
Ed
Ed
Ed
Ed
Ed
2.46
2.32
2.38
2.63
2.67
2.75
2.63
2.68
1.79
1.66
3.04
2.66
2.75
2.11
2.88
1.93
2.19
1.9
1.82
2.07
2.12
1.58
1.33
0.38
0.41
0.34
0.33
0.4
0.38
0.55
0.49
0.5
0.47
0.36
0.32
0.51
0.43
0.46
0.37
0.37
0.43
0.48
0.37
0.49
0.64
0.58
0.05
0.05
0.06
0.05
0.04
0.05
0.04
0.05
0.03
0.04
0.04
0.05
0.06
0.05
0.05
0.05
0.04
0.05
0.07
0.04
0.03
0.03
0.05
0.28
0.28
0.28
0.23
0.24
0.24
0.27
0.29
0.24
0.26
0.22
0.17
0.22
0.23
0.26
0.38
0.25
0.25
0.25
0.28
0.25
0.28
0.28
0.78
0.76
0.83
0.83
0.77
0.76
0.77
0.69
0.81
0.58
0.68
0.96
0.56
0.84
0.96
1.12
1.02
0.72
0.58
1.11
0.9
0.66
0.58
0.87
0.79
0.72
0.89
1.02
1.05
1.27
1.11
0.86
1.26
1.71
1.21
1.33
0.99
1.9
1.56
1.22
0.83
0.59
1.25
0.86
1.34
1.12
1.44
1.34
1.23
1.45
1.43
1.68
1.68
1.6
1.1
1.14
1.44
1.27
1.06
0.96
1.95
1.79
1.5
0.95
0.82
1.59
1.08
1.19
1.1
2.75
2.56
2.4
3.2
3.84
3.78
5.01
3.87
3.64
4.74
6.24
3.29
4.14
4.19
5.44
2.33
2.98
4.3
3.62
2.89
2.8
4.66
3.52
0.01
0.01
0.01
0.01
0.01
0.01
0.01
0.02
0.01
0.01
0.01
0.01
0.01
0.01
0.01
0.03
0.01
0.01
0.02
0.02
0.01
0.01
0.03
0.08
0.09
0.08
0.07
0.06
0.07
0.08
0.07
0.09
0.09
0.05
0.08
0.11
0.06
0.06
0.06
0.05
0.06
0.12
0.06
0.05
0.05
0.08
0.71
0.68
0.7
0.7
0.64
0.61
0.57
0.6
0.64
0.48
0.85
0.94
0.59
0.92
0.74
0.84
1
0.88
0.93
0.96
0.88
0.59
0.75
0.4
0.4
0.43
0.43
0.44
0.43
0.39
0.44
0.58
0.52
0.47
0.51
0.57
0.69
0.3
0.43
0.6
0.66
0.84
0.59
0.58
0.52
0.64
0.08
0.07
0.07
0.07
0.06
0.06
0.07
0.08
0.08
0.08
0.13
0.18
0.09
0.19
0.14
0.18
0.11
0.15
0.24
0.11
0.08
0.08
0.14
24
25
26
27
28
29
30
31
32
33
34
35
36
37
38
39
40
BZ-5
BZ-5
BZ-5
BZ-5
BZ-5
BZ-5
BZ-5
BZ-7
BZ-6
BZ-8
BZ-9
BZ-11
BZ-11
BZ-8
BZ-9
BZ-10
BZ-4
4401
4407
4423.5
4449
4459.5
4476
4492.5
3287.5
3264
3417.5
3185
3033
3039
3450
3240
3250
3646
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Es1
Es1
Es1
Es1
Es1
Es1
Es1
Es1
Es1
Es1
Es1
Es1
Es1
Es1
Es1
Es1
Es1
1.21
1.26
1.3
1.69
1.38
1.22
1.35
1.27
1.48
1.3
1.92
1.39
1.81
1.16
1.49
1.33
1.47
0.79
0.62
0.68
0.54
0.57
0.58
1.02
0.47
0.54
0.46
0.48
0.67
0.56
0.49
0.5
0.57
0.6
0.4
0.46
0.41
0.26
0.44
0.41
0.42
0.53
0.07
0.14
0.08
0.2
0.24
0.31
0.22
0.64
0.16
0.67
0.65
0.62
0.43
0.59
0.62
0.64
0.45
0.36
0.35
0.25
0.62
0.43
0.42
0.39
0.52
0.51
0.28
0.22
0.29
0.51
0.25
0.25
0.24
0.29
0.61
0.49
0.74
0.53
0.99
0.46
0.61
0.6
0.47
0.24
0.34
0.27
0.65
0.43
0.22
0.31
0.17
0.3
0.34
0.53
0.15
0.53
0.24
0.26
0.18
0.47
0.69
0.8
0.78
1.04
1.06
0.75
1.08
0.5
0.49
0.57
0.72
0.43
1.06
0.5
0.54
0.45
1.09
0.59
0.59
0.55
0.73
0.61
0.59
0.55
0.92
1.23
1.75
2.31
0.53
1.23
1.06
1.05
0.77
0.8
0.29
0.14
0.15
0.09
0.12
0.18
0.18
0.05
0.03
0.02
0.02
0.14
0.08
0.04
0.04
0.06
0.22
0.19
0.23
0.22
0.17
0.23
0.23
0.22
0.34
0.18
0.11
0.1
0.23
0.25
0.16
0.13
0.21
0.18
0.98
0.86
1.02
0.89
0.83
0.9
0.99
0.86
0.85
0.91
0.93
1.1
1.41
0.98
1.11
1.09
0.97
0.88
0.91
0.88
0.85
0.84
0.84
0.85
0.74
0.57
0.7
0.8
0.57
0.42
0.79
0.92
0.92
0.7
0.44
0.39
0.39
0.31
0.33
0.41
0.42
0.18
0.16
0.18
0.2
0.57
0.28
0.22
0.24
0.31
0.2
41
42
43
44
45
46
47
48
49
50
51
52
53
54
55
56
57
BZ-8
BZ-8
BZ-8
BZ-9
BZ-9
BZ-9
BZ-4
BZ-4
BZ-4
BZ-1
BZ-1
BZ-1
BZ-7
BZ-7
BZ-7
BZ-1
BZ-1
3555
3570
3585
3537.5
3587.5
3637.5
3745
3764.5
3775
3632.5
3662.5
3687.5
3335
3598.5
3997.3
3945
3985
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Shale
Es3
Es3
Es3
Es3
Es3
Es3
Es3
Es3
Es3
Es3
Es3
Es3
Es3
Es3
Es3
Es3
Es3
1.64
1.57
1.47
1.44
1.62
1.37
1.55
1.59
1.48
2.05
1.87
1.7
1.51
1.67
1.71
1.81
1.55
0.54
0.55
0.6
0.54
0.56
0.53
0.53
0.52
0.53
0.46
0.43
0.4
0.54
0.62
0.42
0.48
0.43
0.07
0.07
0.08
0.07
0.07
0.1
0.04
0.05
0.06
0.06
0.06
0.06
0.05
0.07
0.14
0.08
0.09
0.26
0.26
0.31
0.28
0.29
0.3
0.5
0.43
0.39
0.16
0.29
0.31
0.33
0.32
0.54
0.37
0.4
0.67
0.69
0.64
0.72
0.54
0.55
0.2
0.26
0.29
0.95
0.95
0.94
0.53
0.66
0.81
0.84
0.83
0.54
0.54
0.42
0.64
0.67
0.39
0.37
0.36
0.37
0.65
0.56
0.38
0.42
1.01
0.24
0.5
0.48
0.69
0.66
0.56
0.74
0.79
0.6
0.82
0.83
0.79
0.83
0.75
0.64
0.64
0.62
0.44
0.77
0.9
1.59
1.24
1.05
1.55
1.35
0.7
1.14
1.27
1.08
2.74
2.46
1.91
1.24
1.53
0.09
1.71
1.46
0.03
0.03
0.04
0.03
0.05
0.08
0.03
0.03
0.03
0.02
0.02
0.03
0.03
0.02
0.15
0.2
0.39
0.09
0.16
0.52
0.16
0.56
0.45
0.09
0.12
0.13
0.34
0.29
0.15
0.13
0.13
0.81
0.74
0.71
0.81
0.8
0.61
0.73
0.71
0.67
0.9
0.99
0.96
0.97
0.42
0.52
0.83
0.75
0.64
0.63
0.7
0.69
0.7
0.82
0.51
0.57
0.56
0.52
0.74
0.71
0.62
0.5
0.57
0.58
0.49
0.11
0.11
0.11
0.11
0.13
0.16
0.1
0.1
0.11
0.19
0.16
0.16
0.16
0.13
0.37
0.22
0.23
0.08
0.07
Note: SN = sample number; Pr/Ph = pristane/phytane; C35/C34 = C35 22S/C34 22S hopane; G/H = gammacerane/ C30 hopane; ETR = (C28 + C29)/(C28 + C29 + Ts); C27/C27 = C27
(20R + 20S) diasteranes/C27 (20R + 20S) steranes; C19/C23 = C19 tricyclic terpane/C23 tricyclic terpane; C20/C23 = C20 tricyclic terpane/C23 tricyclic terpane; C24/C26 = C24 tetracyclic terpane/C26 tricyclic terpane; C23/C30 = C23 tricyclic terpane/ C30 hopane; 4MSI = 4-methylsterane index (4-methylsteranes/C29 steranes); C27/C29 = C27/C29 steranes;
C28/C29 = C28/C29 steranes; S/H = steranes/hopanes (C27 C29 steranes/C27 C35 hopanes).
327
4. Results
4.1. RockEval pyrolysis
RockEval pyrolysis is a commonly used technique to classify
organic matter (OM) types and to assess hydrocarbon generating
potentials (e.g., Peters, 1986). The third member of the Eocene
Shahejie Formation (Es3, 43.038.0 Ma) has total organic carbon
(TOC) contents of 0.19.19% and RockEval S2 values of 0.02
63.08 mg HC/g rock. Hydrogen indices for Es3 samples range from
<50 to 1115 mg HC/g TOC, suggesting different organic matter
types (Fig. 4A). The rst member of the Shahejie Formation (Es1,
35.832.8 Ma) displays TOC contents of 0.226.80%, RockEval S2
values of 0.2550 mg HC/g rock, and hydrogen indices of 15
777 mg HC/g TOC (Fig. 4B). The Oligocene Dongying Formation
(Ed, 32.824.6 Ma) has TOC contents ranging from 0.35% to
3.91%, RockEval S2 values from 0.126.3 mg HC/g rock and hydrogen indices from <50 to 716 mg HC/g TOC (Fig. 4C). Most samples
have RockEval Tmax lower than 445 C, suggesting thermal maturity from immature to early oil generation (Peters, 1986).
1000
1000
1000
Hydrogen Index (mg HC/g TOC)
(B) Es1
(A) Es3
I
800
Ro=0.5%
(C) Ed
800
Ro=0.5%
II
600
600
600
400
400
400
200
Ro=1.0%
III
420
Ro=0.5%
II
II
0
400
800
440
460
Tmax (C)
480
500
200
Ro=1.0%
III
0
400
420
440
460
Tmax (C)
480
500
200
Ro=1.0%
III
0
400
420
440
460
480
500
Tmax (C)
Fig. 4. Variation of hydrogen index as a function of Tmax for samples from different possible source rock intervals in the Bozhong sub-basin, Bohai Bay Basin.
328
1000
(A)
800
1000
Ed
Ed Rock
Rock
Es
Rock
Es11Rock
Es
Es33Rock
Rock
600
400
200
0
10
20
30
40
Woody Organic Matter (%)
800
600
400
200
0
50
10
20
30
40
50
60
Amorphous Organic Matter (%)
70
80
800
Hydrogen Index (mg HC/g TOC)
800
Hydrogen Index (mg HC/g TOC)
(B)
(C)
700
600
500
400
300
200
100
0
0.0
0.5
1.0
1.5
2.0
2.5
3.0
Pristane/Phytane (Pr/Ph)
3.5
(D)
700
600
500
Phytane from
methanogenic archaea?
400
300
200
100
0
4.0
3
4
Phytane/nC18
Fig. 5. Variation of hydrogen indices as a function of woody organic matter contents (A), amorphous organic matter contents (B), Pristane/Phytane ratios (C) and Phytane/nC18 ratios (D), showing source rock heterogeneities in the Bozhong sub-basin, Bohai Bay Basin.
(B)
Ed
Ed Rock
Rock
Es
Es11Rock
Rock
Rock
Es
3
Es3 Rock
Phytane/n-C18
Pristane/n-C17
(A)
0
400
410
420
430
Tmax (C)
440
450
0
400
460
410
420
430
Tmax (C)
440
10
10
(C)
(D)
Ox
Pristane/n-C17
s t
ce e n
ur nm
t
so iro
en
v
OM n OM nm
d le
o
xe ona lgal vir
i
M it i
A en
g
ns
c in
t ra
du
e
r
g
in
10
1.0
460
c
du
Re
1.0
Phytane/n-C18
0.1
0.1
Te
n
izi
Pristane/Phytane
id
1.0
sO
ou
en
g
i
rr
450
0.1
0.1
1.0
Phytane/n-C18
10
Fig. 6. Variation of pristane/phytane (A) and Pristane/n-C17 (B) as a function of Phytane/n-C18, and variation of Pristane/n-C17 (C) and Phytane/n-C18 (D) as a function of Tmax
for rock samples from the Bozhong sub-basin, Bohai Bay Basin.
329
m/z 191
m/z 217
C24 Tet
C30 hopane
C20
C19
C27
C29
C27 RA
steranes
C21
C23
C28
4-MS
C24
C22
Gam
C25 C26
C23
C21
C28
C24
C20
C19
C25 C26
C22
C29
C24 Tet
4-MS
Gam
C23
C20
C19
C27
C24 Tet
C22
C25 C26
4-MS
C28
C24
Gam
Fig. 7. Representative mass chromatograms of terpane (m/z = 191) and sterane (m/z = 217) series of saturate fractions for different stratigraphic intervals in the Bozhong subbasin, Bohai Bay Basin. Peaks marked by solid dots are tricyclic terpanes (C19C26). C24 Tet = C24 tetracyclic terpane; Gam = gammacerane; RA = re-arranged; C27, C28 and C29
represent C27 sterane 20R, C28 sterane 20R and C29 sterane 20R, respectively; 4-MS = 4-methylsteranes. Note the abundant C19, C20 tricyclic terpanes, C24 tetracyclic terpane
and C27 re-arranged steranes for Ed sample (A), abundant gammacerane for Es1 sample (B), and abundant 4-methylsteranes for the Es3 sample (C).
330
0.3 0.6
0.5 1.0 0
C28/C29
C27/C29
0.8 1.6 0
0.4 0.8 0
4MSI
C27/C27
4
1
1
0.6 1.2 0
0.4 0.8 0
ETR
G/H
C35/C34
0.4 0.8 0
2
4600
4400
4200
4000
3800
3600
3400
3200
3000
2800
2600
Pr/Ph
0.6 1.2 0
C19/C23
C20/C23
C24/C26
C23/C30
0.2 0.4 0
S/H
Depth (m)
Fig. 8. Variations of major biomarker parameters reecting depositional conditions and/or organic matter input as a function of burial depth. Open triangles: Ed samples;
Crosses: Es1 samples; solid dots: Es3 samples. Abbreviations for biomarker parameters are explained in Table 1.
is therefore not applicable. Contribution from eukaryotic phytoplankton may simultaneously lead to high abundances of both
pristane and phytane, as is the case in the Levant Platform of
central Jordan (Seplveda et al., 2009). Yet in the Bozhong subbasin Pr/Ph ratios decrease as Ph/n-C18 increases (Fig. 6C) and
samples with Ph/n-C18 greater than 2.0 display Pr/n-C17 ratios
obviously lower than the Pr/n-C17 ratios for many Dongying
Formation samples that have Ph/n-C18 < 1.0 (Fig. 6D). Therefore,
contribution from eukaryotic phytoplankton could not be the main
cause of the high phytane abundance observed in the Bozhong subbasin. In the Bozhong sub-basin, samples with high Ph/n-C18 ratios
have a large isotopic difference between saturate and aromatic
fractions and plot above the best t line (d13CAro = 1.14d13CSat + 5.46) on the so called Sofer-plot (Sofer, 1984) (Guo, 2009,
personal communication). The 13C depleted saturate fractions resulted from input from methanotrophic bacteria (Collister and
Wavrek, 1996). Methanotrophic bacteria thrive at the chemocline
of stratied lakes (Collister and Wavrek, 1996). The 13C depleted
saturate fractions as a result of methanotrophic input of isotopically depleted lipids imply that a considerable amount of methane
should have been generated below the chemocline. Therefore, we
explain the high Ph/n-C18 ratios for samples with high hydrogen
indices as reecting a contribution from methanogenic archaea.
Based on RockEval hydrogen indices (Fig. 4), elemental compositions of kerogens (not shown), visual kerogen compositions
(Fig. 5A and B) and redox conditions reected by isoprenoid hydrocarbon distributions (Figs. 5C, D and 6), four types of organic facies
(Jones, 1987) can be recognized. Organic facies A has hydrogen
indices >700 mg HC/g TOC and is dominated by uorescent AOM
and well preserved algal materials usually with low Pr/Ph (<1.0)
and high Ph/n-C18 (>1.0 to 1.5) ratios. Organic facies B usually displays hydrogen indices between 500 and 700 mg HC/g TOC. Organic
facies B is also dominated by AOM but may have woody organic
matter contents up to 15%. Organic facies BC has hydrogen indices
between 200 and 500 mg HC/g TOC and woody organic matter
contents of 1045%. Organic facies C has hydrogen indices
<200 mg HC/g TOC and is dominated by woody organic matter.
AOM in organic facies C is ne grained and is red in color in transmitted light and shows no uorescence in ultraviolet light, which is
distinctly different from AOM in organic facies A and B.
Both Es3 and Es1 contain organic facies AC. The Dongying Formation contains organic facies B to C without well developed organic facies A. The wide, successive variations in hydrogen
indices (Fig. 4) and visual kerogen composition (Fig. 5A and B) suggest strong heterogeneities of all the three intervals, from hydrogen rich organic facies in the deep lake sediments to hydrogen
poor facies in lake marginal sediments. Such heterogeneities may
be explained as reecting varying redox conditions from anoxic
through transitional to oxic (Fig. 6D). It should be pointed out that,
in the Bozhong sub-basin, organic facies BC and C usually have total organic carbon (TOC) contents <1.0% (Hao et al., 2010). The relatively low hydrogen indices and TOC contents mean that the
hydrocarbon generating potential of organic facies BC and C is
much lower than that of organic facies A and B. In addition, organic
facies BC and C might contribute to condensates and hydrocarbon
gases, but are of minor signicance for normal oils due to the
oxygen rich nature of the organic matter (Price, 1989). Therefore,
to understand the mechanisms for the deposition of organic facies
A and B and to predict their distribution are of great signicance
for petroleum exploration in lacustrine basins.
5.2. Changes in lake water chemistry
Primary productivity and redox conditions are among the most
important factors controlling high quality source rock (organic facies A and B) deposition (e.g., Kelts, 1988; Huc et al., 1992; Katz,
331
1990, 2005; Tyson, 2005). The primary productivity and redox conditions in a lake are largely controlled by lake water chemistry,
such as salinity and acidity/alkalinity. Rapid progress in organic
geochemistry in the last 20 years makes it possible to qualitatively
estimate changes in lake water chemistry from biomarker parameters (e.g., Volkman et al., 1998; Peters et al., 2005, p. 483580).
The great thickness of the syn-rift succession in the Bozhong
sub-basin (cf. Fig. 2) makes it impossible to construct a biomarker
prole in a single well. In order to reveal changes in lake water
chemistry and the resultant changes in biota through geologic
time, 57 samples of deep-lake facies from different intervals were
analyzed (Table 1) and a composite biomarker prole (Figs. 8 and
9) was constructed. Hao et al. (2010) showed that no terpane
and sterane parameters for these samples displayed any obvious
correlation with the C29 bb/(bb + aa) sterane ratio (an effective
maturity parameter believed to be independent of organic matter
input; Peters et al., 2005, p. 625630). In addition, although the
selected sample set covers a relatively wide depth range (2781
4492.5 m), most parameters show no obvious correlation with
burial depth (Fig. 8), and the variation trends of several parameters
are even opposite to those caused by thermal maturity. For
instance, if Pr/Ph and C19/C23 TT had been intensively inuenced
by thermal maturity, they would have had to increase with
increasing depth. Yet, exactly the opposite is observed (Fig. 8). It
appears that all parameters displayed in Figs. 8 and 9 are not intensively inuenced by thermal maturity and therefore can be used to
reect organic matter input and/or depositional conditions. Carefully selecting deep-lake facies samples based on the result of
sedimentological analysis from different wells and constructing a
composite biomarker prole could minimize the inuence of local
water inow and/or sediment input. Despite the fact that samples
for any interval were from different wells and cover a relatively
wide depth range (Table 1), all three intervals display relatively
narrow variation ranges for most parameters (Fig. 9). This on one
hand suggests that the inuence of local water inow and/or sediment input, if any, is minor, and on the other hand implies that
these parameters have not been signicantly affected by thermal
maturity.
Pr/Ph and C35 22S/C34 22S hopane are effective oxicity parameters (see Peters et al., 2005, p. 499502, 566569 and references
therein). Es1 has the lowest Pr/Ph ratios and the highest C35 22S/
C34 22S hopane ratios (Table 1, Fig. 9A and B). In contrast, the
Dongying Formation displays the highest Pr/Ph ratios and the
lowest C35 22S/C34 22S hopane ratios. The relatively low Pr/Ph
ratios and high C35 22S/C34 22S hopane ratios for Es3 and Es1 samples suggest that anoxic conditions prevailed in the bottom water
during Es3 and Es1 deposition, whereas less reducing conditions
dominated in the bottom water in lakes during Ed deposition. This
is consistent with the result of bulk geochemistry analysis. On the
Pr/n-C17 vs Ph/n-C18 plot, many Es3 and Es1 samples plot in areas
suggesting euxinic, anoxic conditions, whereas most Ed samples
fall in the transitional to oxic elds (Fig. 6D).
The gammacerane index (gammacerane/ab C30 hopane), extended tricyclic terpane ratio [ETR = (C28 + C29)/(C28 + C29 + Ts)]
and C27 ba (20R + 20S) diasteranes/C27 abb (20R + 20S) sterane
(C27 Dia/C27 ST) were used to reect changes in water salinity/alkalinity through geologic time (Fig. 9CE).
Gammacerane is believed to form by reduction of tetrahymanol
(e.g., Venkatesan, 1989; ten Haven et al., 1989). The principal
source of tetrahymanol appears to be bacterivorous ciliates, which
occur at the interface between oxic and anoxic zones in stratied
water columns (Sinninghe Damst et al., 1995). Therefore, abundant gammacerane is usually believed to indicate the presence of
a stratied water column (e.g., Sinninghe Damst et al., 1995;
Peters et al., 2005, p. 576; Seplveda et al., 2009). Although a
stratied water column can result from either hypersalinity or a
(L)
0.5
(K)
0.8 1.6 0
(J)
0.3 0.6 0
(I)
0.2 0.4 0
(H)
(G)
(F)
(E)
0.6 1.2 0
(D)
0.4 0.8 0
(C)
0.4 0.8 0
(B)
0.6 1.2 0
(A)
55
50
40
35
30
20
15
10
25
45
SN
Pr/Ph
4 0
C35/C34
G/H
ETR
C27/C27
C19/C23
2 0
C20/C23
2 0
C24/C26
C23/C30
4MSI
C27/C29
C28/C29
1 0
(M)
0.3 0.6
S/H
332
E3 (32.824.6 Ma)
Fig. 9. Composite organic geochemistry prole showing changes in major biomarker parameters reecting depositional conditions and/or organic matter input from Es3
through Es1 to Ed3. Vertical lines represent the average values for the interval. SN = sample number. Abbreviations for biomarker parameters are explained in Table 1.
Holba et al. (2001) used ETR to differentiate crude oils generated from Triassic, Lower Jurassic and MiddleUpper Jurassic
marine source rocks. They observed a sharp drop in ETR at the
end of the Triassic that corresponds to a major mass extinction
and implied that the mass extinction may have had an impact on
333
the principal biological sources of tricyclic terpanes. The effectiveness of ETR as an age related parameter was questioned by Ohm
et al. (2008). In the Bozhong sub-basin, ETR increases with increasing gammacerane/ab C30 hopane and sterane/hopane ratios and
decreases with increasing Pr/Ph ratios (Fig. 10AC). Similar trends
were also observed in lacustrine oils and source rocks in the
Junggar Basin where high ETR occurs in crude oils and source rocks
with abundant b-carotane and ETR increases as gammacerane/ab
C30 hopane increases (Hao et al., in press). Our observations in
the Junggar and Bohai Bay basins are consistent with those of
Kruge et al. (1990a,b) and De Grande et al. (1993) who concluded
that fossil lipids of prokaryotes in saline, alkaline lakes are rich in
precursors of extended tricyclic terpanes. The close correlation of
ETR with Pr/Ph, sterane/hopane and gammacerane/ab C30 hopane
ratios indicate that in lacustrine environments, ETR is an effective
0.8
0.8
(A)
0.6
0.4
Ed
Ed Rock
Rock
Es
Es11Rock
Rock
Es
Es33Rock
Rock
0.2
0.0
0.03
0.1
0.4
0.2
0.0
0.0
1 .0
(C)
0.6
ETR
ETR
ETR
0.8
(B)
0.6
0.4
0.2
0.1
0.2
0.3
0.4
0.5
0.0
1.0
0.6
1.5
2.0
S/H
G/H
1.5
(D)
C27/C27
1.0
0.5
2.5
3.0
3.5
Pr/Ph
7.0
(E)
(F)
6.0
5.0
1.0
C24/C26
1.5
C27/C27
0.5
4.0
3.0
2.0
1.0
0.0
1.0
1.5
2.0
2.5
3.0
0.0
0.0
3.5
0.2
0.4
Pr/Ph
60
3.0
2.0
1.0
2.5
3.0
50
40
30
20
0.0
3.5
4.0
2.0
1.0
0.5
1.0
Pr/Ph
1.5
50
40
30
20
0.0
2.0
2.0
4.0
6.0
8.0
C24/C26
0.6
(J)
2.0
(I)
C19/C23
1.0
1.5
60
(H)
C29 Steranes (%)
5.0
1.5
0.5
C19/C23
(G)
6.0
C24/C26
0.0
0.0
0.8
G/H
7.0
0.0
1.0
0.6
0.6
(K)
(L)
0.4
S/H
0.4
S/H
C28/C29
0.8
0.6
0.2
0.2
0.4
0.2
0.4
0.6
0.8
1.0
C27/C29
1.2
1.4
1.6
0.0
0.1
0.2
0.3
0.4
0.0
0.3
0.4
0.5
0.6
Fig. 10. Correlation between various biomarker parameters reecting organic matter input and/or depositional environments in the Bozhong sub-basin, showing the
differences in biomarker compositions among the three source rock intervals. Abbreviations for biomarker parameters are explained in Table 1.
334
are presumed to be 4-methyl sterols. Apart from compounds specically identied as originating from methane oxidizing bacteria
(Jahnke et al., 1999), 4-methyl steroids are mostly algal in origin
(e.g. de Leeuw et al., 1983), and dinoagellates are believed to be
their main source (De Leeuw et al., 1983; Summons et al., 1987).
In the Bohai Bay Basin, abundant 4-methylsteranes appear to be
associated with abundant dinoagellates Bohaidina and Parabohaidina (e.g., Chen et al., 1996, 1998; Zhang et al., 2005). The 4methylsterane index (4-methylsteranes/RC29 steranes) exhibits a
general decrease up section (Fig. 9J), suggesting decreasing contributions from dinoagellates Bohaidina and Parabohaidina. The fact
that Es3 has higher 4-methylsterane abundances than Es1 (Figs. 7
and 9J) supports our interpretation that freshwater lakes
dominated during Es3 deposition whereas saline lakes dominated
during Es1 deposition, since dinoagellates Bohaidina and
Parabohaidina thrive in freshwater settings (Fu et al., 1990; Peters
et al., 2005, p. 531).
It is usually believed that C27 steranes derive mainly from phytoplankton and metazoa, whereas C29 steranes mainly originate
from terrigenous higher plants (e.g., Huang and Meinschein,
1979; Volkman, 1986). C27/C29 sterane ratios range between 0.42
and 0.99 (average 0.76) for Es3 samples, increase to the highest values in the Bozhong sub-basin for Es1 samples (0.821.41, average
0.98), and then decrease to low values (0.481.0, average 0.75)
for the Dongying samples (Fig. 9K). As discussed earlier, C19/C23
TT, C20/C23 TT and C24 Tet/C26 TT are effective parameters reecting
organic matter input from terrigenous higher plants. The Es3 and
Ed have quite similar C27/C29 sterane ratios (Figs. 7, 9K), which appears to be inconsistent with the fact that the Dongying Formation
has much higher C19/C23 TT, C20/C23 TT and C24 Tet/C26 TT ratios
(Table 1, Figs. 7, 9FH) and therefore has signicant contribution
from terrigenous higher plants whereas Es3 was dominated by algal organic matter. The relative C29 sterane abundances show a
general increase with increasing C19/C23 TT and C24 Tet/C26 TT ratios (Fig. 10H, I). The Es3 and Ed have quite different C19/C23 TT
(0.241.01 and 0.591.90 for Es3 and Ed, respectively) and C24
Tet/C26 TT (0.092.74 and 1.366.24 for Es3 and Ed, respectively)
ratios. Yet they have quite similar relative abundances of C29 steranes (36.1450.85% and 36.6251.89% for Es3 and Ed, respectively,
Figs. 7, 10H and I). The elevated C29 sterane abundances for the Es3
that has been conrmed to have minor terrigenous organic matter
input indicate that an additional source for C29 steranes existed.
Volkman et al. (1999) and Kodner et al. (2008) conrmed that
freshwater microalgae may be an important source for C29 steranes. Since freshwater lakes dominated during Es3 deposition, a
plausible explanation for the enhanced C29 sterane abundances relative to the low C19/C23 TT and C24 Tet/C26 TT ratios in Es3 is the
contribution of freshwater microalgae.
C28 steranes are associated with specic phytoplankton types
(e.g., diatoms, Grantham and Wakeeld, 1988; Volkman et al.,
1998) that contain chlorophyll-c (Knoll et al., 2007). In the Bozhong
sub-basin, an overall trend of increasing C28/C29 sterane ratio with
increasing C27/C29 sterane ratio (Fig. 10J) was observed. C28/C29
sterane ratios show moderate values for Es3 (0.490.82, average
0.62), increase to relatively high values between 0.42 and 0.92
(average 0.77) for Es1 and then decrease to low values for the
Dongying Formation (0.300.84, average 0.51) (Table 1, Fig. 9L).
This suggests an enhanced contribution from chlorophyll-c
containing phytoplankton relative to C29 producing organisms
(Knoll et al., 2007) in Es1.
The sterane/hopane ratios reect input of eukaryotic (mainly algae and higher plants) versus prokaryotic (bacteria) organisms to
the source rocks (e.g., Peters and Moldowan, 1993; Gonalves,
2002; Peters et al., 2005, p. 524; Seplveda et al., 2009). In the
Bozhong sub-basin, sterane/hopane ratios increase as C28 sterane
abundances increase and decrease as C29 sterane abundances
335
336
(A)
Moderate to High Productivity
TOM
Freshwater, Oxic
TOM
MB
Ciliates
CH4
(B)
evaporation
High Productivity
Saline
water,
oxic
Saline, anoxic
Carbonate
CH4
Organic Facies
BC and C
Organic Facies A and B
Low water inflow and sediment supply, intensive evaporation, abundant carbonate
deposition, regressional or aggradational basin-fill.
Shallow, stable chemocline, euxinic bottom conditions (methanogenesis).
Very low terrigenous organic matter input, high primary productivity, blooming of
chlorophyll-c containing phytoplankton.
High Water Inflow and
Efficient Sediment Supply
(C)
Moderate to High Productivity?
TOM
Freshwater, oxic
Dysoxic to anoxic
Organic Facies BC and C
Organic Facies
B + BC
from the very low gammacerane indices (Fig. 9C). The dysoxic
bottom water conditions are indicated by the relatively high Pr/Ph,
low C35 22S/C34 22S hopane and low ETR (Fig. 9B, D), and can
6. Conclusions
Based on our bulk geochemical study of more than 300 samples
and molecular geochemical observation on 57 samples, the following conclusions can be drawn.
(1) The third (Es3) and rst (Es1) members of the Eocene Shahejie
Formation and the Oligocene Dongying Formation (Ed) all
display widely variable total organic carbon contents,
RockEval hydrogen indices, woody and amorphous organic
matter contents, Pr/Ph and Ph/n-C18 ratios, suggesting strong
lateral heterogeneities in organic facies from deep water to
marginal lake sediments. Amorphous organic matter, which
is usually believed to originate mainly from algal organic
matter in reducing environments, may be complex in origin
and therefore may be either rich or poor in hydrogen.
(2) Despite the strong lateral heterogeneities indicated by bulk
geochemical analyses, the deep-lake facies samples from
any interval display fairly narrow variation ranges for most
molecular parameters reecting organic matter origins
and/or depositional environments. This implies that effective oil source rocks (high quality source rocks that have
generated and expelled a considerable amount of oil and
made a considerable contribution to commercial oil
accumulations) in different intervals might not be as
heterogeneous as that reected by the wide variation in
TOC contents, visual kerogen composition and hydrogen
indices, which is particularly important for oil-source rock
correlation. The deep-lake facies from the three intervals,
although all are dominated by shales/mudstones, have
distinctly different biomarker associations, suggesting that
molecular geochemical analysis is a powerful tool to construct the basin ll history.
(3) The distinctly different biomarker assemblages for the three
syn-rift intervals indicate weakly alkaline, freshwater lakes
with moderately deep thermocline during Es3 deposition,
alkaline-saline lakes with shallow chemocline during Es1
deposition and acidic, freshwater lakes with deep, unstable
thermocline during the deposition of the Dongying Formation. Such environmental changes corresponded to changes
337
338
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