Chemie der Erde 73 (2013) 343–356
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Chemie der Erde
journal homepage: www.elsevier.de/chemer
Hydrochemical characteristics and controlling factors for waters’
chemical composition in the Tarim Basin, Western China
Ying Bo a,b , Chenglin Liu a,b,∗ , Pengcheng Jiao a , Yongzhi Chen a , Yangtong Cao a
a
MLR Key Laboratory of Metallogeny and Mineral Assessment, Institute of Mineral Resources, Chinese Academy of Geological Sciences, 100037 Beijing,
China
b
Institute of Mineral Resources, Chinese Academy of Geological Sciences, 100037 Beijing, China
a r t i c l e
i n f o
Article history:
Received 24 March 2012
Accepted 11 June 2013
Keywords:
Hydrochemical types
Controlling factors
Background value
Isotopic compositions
Hydrothermal Ca–Cl brines
Lop Nur
Tarim Basin
a b s t r a c t
This paper covers the chemical and isotopic composition of river water, groundwater from wells
(15–25 m), saline spring water and stagnant surface water providing evidence for controlling factors
of water composition and water evolution process in the Tarim Basin, Xinjiang, western China. Analytical
data for major and minor ions of totaling 537 water samples were obtained from both years of teamwork
and old reference materials. It is found that the ion background value ratio SO4 /Cl for river water (2.75)
of the Tarim Basin is two times higher than that of the Qaidam Basin (0.88) and 18 times higher than
seawater (0.14); K/Cl of these two basins (0.06 and 0.07) are all two times higher than seawater (0.02).
This reveals that material sources of Lop Nur are relatively richer in potassium and sulfate, while poorer
in chloride. Gradual changes of stable isotopic compositions in waters clearly indicate the effect of evaporation on water evolution of the basin. Besides evaporation and weathering of surrounding rocks, wide
distribution of chloride type water, which commonly exist in saline springs/brines and seldom exist in
other waters, indicates that hydrothermal Ca–Cl brines discharged from deep within the earth join water
evolution of the basin.
© 2013 Elsevier GmbH. All rights reserved.
1. Introduction
Hydrochemistry is of great importance to researching on water
evolution of arid regions. Hydrochemical characteristics such as
chemical composition, hydrochemical types and environmental
background value usually can help to understand the environmental and geological conditions in which waters are formed, i.e. the
controlling factors.
In recent years, hydrochemical researches usually focus on
recharge, mobilization, and evolution mechanism of groundwater. Shanyengana et al. (2004) studied major-ion chemistry and
groundwater salinization in ephemeral floodplains in arid regions
of Namibia. Tsujimura et al. (2007) researched stable isotopic and
geochemical characteristics of groundwater in a semi-arid regionKherlen River Basin in eastern Mongolia. Tweed et al. (2011) studied
recharge and salinization processes of groundwater in the Lake
Eyre Basin, Australia, through the study of major-ion chemistry,
stable isotope composition, etc. Vanderzalm et al. (2011) studied
recharge sources and hydrogeochemical evolution of groundwater
in alluvial basins in arid central Australia. In China, groundwater
∗ Corresponding author at: 26 Baiwanzhuang Street, Xicheng District, 100037
Beijing, China. Tel.: +86 010 68999067; fax: +86 010 68327263.
E-mail address: [email protected] (C. Liu).
0009-2819/$ – see front matter © 2013 Elsevier GmbH. All rights reserved.
http://dx.doi.org/10.1016/j.chemer.2013.06.003
hydrochemistry was studied in many regions, such as the Erdos
Basin (Dou et al., 2010), the Longdong Basin (Zhang et al., 2006b; Liu
et al., 2009), the Ejin Basin (Zhang et al., 2006a), the Hexi Corridor
(Bai and Yang, 2007), the Gongpoquan Basin (Chen et al., 2008), the
Tarim Basin (Li et al., 1995; Wu and Guo, 2004; Zhu and Yang, 2007;
Zeng et al., 2008; Dai et al., 2010) and so on. Besides, salt lakes, saline
springs and their evolution mechanism were also studied in arid
zones for sylvite exploration. For instance, in China, the QinghaiTibet Plateau (Zheng and Liu, 2009), the Qaidam Basin (lying to the
southeast of the Tarim Basin) (Fan et al., 2007a,b) and the Tarim
Basin (Tan et al., 2004; Ma and Ma, 2006) are the main research
areas. As for river water, formal references on river water hydrochemistry in arid zones in China are relatively fewer (Zhou and
Dong, 2002; Zhu and Yang, 2007).
Chemical composition and the content of different ions in natural water bodies may be controlled by many factors, such as
the surrounding geology, rock weathering, the climate, recharges
from precipitation, surface water or groundwater, so their material
sources and evolution processes are very complicated.
The Tarim basin, as the biggest enclosed inland basin of China
and being rich in mineral resources (especially oil, gas and salt
deposits), has caused interests of many scholars. However, few
hydrochemical evidences have been offered for research on its evolution process. Old hydrochemical materials can no longer meet the
demand of new research progress in this area.
344
Y. Bo et al. / Chemie der Erde 73 (2013) 343–356
In this research, based on analytical data of 537 natural water
samples obtained from years of teamwork (n = 302, 159 river water
samples, 62 saline spring/brine samples, 31 groundwater samples
and 50 stagnant surface water samples) and old geochemical results
(n = 235, 34 river water samples, 134 saline spring/brine samples,
51 groundwater samples, 16 stagnant surface water samples) (Guo,
1973; IOD & BGMR, 1977; Chen, 1978; Tan et al., 2004; Ma and Ma,
2006), hydrochemical composition, hydrochemical types, controlling factors of waters in the Tarim Basin, as well as environmental
background value for river water, are analyzed in order to help
to understand hydrochemical characteristics and evolution mechanisms of the basin. Besides, oxygen (␦18 O) and hydrogen (␦D)
isotopic compositions of 89 water samples are analyzed to offer
more information for this research.
Environmental background value is the content of chemical element in relatively clean (less influenced by human activities) areas
in studied regions under the present environmental conditions
(Chen, 2000). In the view of geochemistry, normal content of an element is called its background content, and its average value is called
the background value (Tao, 1981). Unusual data rejection is the
first step for determination of element environmental background
value (Huang and Xu, 2008). However, most criterions for rejection
of unusual values take data normal distribution as an assumption,
therefore there are some limitations in their application (Wei et al.,
2009). In this research, boxplot was used in unusual values rejection
for determination of element environmental background value.
2. Site description
2.1. Physical geography
The Tarim Basin of Xinjiang is a large 500,000 km2 closed basin,
located in China’s far west (Fig. 1). It is surrounded by the Tianshan
Mountains to the north, the Pamirs Plateau to the west, the Kunlun
Fig. 1. Lithologic sketch-map of the Tarim Basin. According to Zhang (1980), Li et al. (1991), Ma (2001) and Mao (1998).
Y. Bo et al. / Chemie der Erde 73 (2013) 343–356
345
Table 1
Annual runoff volumes of main river systems in the Tarim River Basin (from He, 1998).
River system
Hotan river
Yarkant river
Aksu river
Weigan river
Kaidu river, Kongque
river
River name
Monitoring station
Annual runoff volume (108 m3 )
Yurungkax river
Karakax river
Yarkant river
Tiznap river
Toxkan river
Kumalake river
Tailanhe river
Muzat river
Kabusilanghe river
Tailewaiqiukehe river
Kalasuhe river
Heizihe river
Kuqa river
Kaidu river
Dina river
Tongguziluoke
Wuluwati
Kajun
Yuzimenleke
Shaliguilanke
Xiehela
Tailan
Ahebulong
Kamuluke
Teerweiqike
Kalasu
Heizi
Lanqian
Dashankou
Dina river
22.23
21.63
64.33
8.17
25.76
46.04
7.35
14.54
27.08
Mountains to the south, the Karakoram Mountains to the southwest
and the Altun Mountains to the southeast. At the east end of the
basin lies a saline depression-Lop Nur. Since the Late Pliocene-early
Pleistocene, the west of the Tarim Basin has been uplifted, and Lop
Nur has sunk and become the final confluence of waters in the basin
(Liu et al., 2002), with an altitude of 780 m. The famous Taklimakan
Desert (the second biggest desert in the world) dominates much of
the central basin. Between two big mountain systems-the Tianshan
and the Kunlun Mountains, there are plains or sub-basins of the
Tarim Basin (Lv, 1993). Being in the warm temperate zone with dry
continental climate, the annual mean temperature of the basin is
between 10 ◦ C and 12 ◦ C, while annual mean precipitation ranges
from 15 mm to 60 mm (Zhu and Yang, 2007).
2.2. Hydrology
As water flows into the basin plain, it includes 144 rivers, which
bring meteoric waters from the surrounding mountains. These
rivers belong to nine inland river systems, among which the annual
runoff volume of Yarkant River (more than 5 × 109 m3 ) is the largest
(Table 1, He, 1998). A second major source of inflow is derived from
active fault zones-saline springs/brines. Saline spring waters are
often exposed around salt domes, two wings of anticlines, gullies
and valleys, with low flow rate. This can be interpreted as subsurface brines that have risen to the surface along deep faults.
Groundwater of the basin usually comes out at the mountain passes
and join into river runoff, with a small part penetrating aside into
the plain groundwater. The annual groundwater inflow volume to
the plain area is 4.455 × 109 m3 (He, 1998), including pore phreatic
water and confined water stored in loose Quaternary sediments.
Stagnant surface water in the Tarim Basin includes long-term stagnant surface water (lake water, reservoir water) and pond water
and short-term stagnant surface water (ditch water and puddle
water).
2.3. Geology
The basin is a big and stable Craton in China, with gypsum-salt
deposited in the Cambrian system, the carboniferous system, the
Permian system, the Cretaceous system, the Paleogene system, the
Neogene system and the Quaternary system (Zheng et al., 2006). It
is a superimposition of several small marine basins (Liu et al., 2006,
2008). As the sub-basins in the Tarim Basin, the Kuqa Basin (north
of the Tarim Basin) and the Shache Basin (southwest of the Tarim
Basin) were formed in marine or marine continental evaporation
sedimentary environment from the Cretaceous to Early Tertiary,
with evaporite deposit layer thickly and widely distributed. In the
alpine zone of the basin, though crystalline rocks like granite and
2.13
3.15
3.34
36.46
3.41
metamorphic rocks contain high content of Na,K, Ca, etc., they are
not easy to be dissolved, so bicarbonate is the main soluble salt,
and partially exist marble and limestone. However, lower mountain
zones are composed of salt-bearing rock of the Tertiary, so soluble
salts dominate (Zhu and Yang, 2007).
On the basis of geographical (distribution of rivers and mountains) and geological conditions, the Tarim Basin is divided into
five regions (Figs. 1 and 2). Region 1 contains the southern and
southeastern Tarim Basin, i.e. the north of the Kunlun Mountains
and the Altun Mountains, from the Yurungkax River to the east of
the Milanhe River; Region 2 is the southwestern Tarim Basin, i.e.
the north of the Karokoram Mountains, from the Yarkant River to
the Karakax River; Region 3 is western Tarim Basin, including the
Kashigaer River and the surrounding rivers that originate from the
Pamirs Plateau; Region 4 is the northern Tarim Basin, i.e. the south
of the Tianshan Mountains; central Tarim Basin-hinterland of the
Taklimakan desert is Region 5.
Region 1 is dominated by granite which mainly formed in
middle-late Proterozoic era, Devonian, Carboniferous and Permian
period; Paleogene (E1–2 ), Neogene (N1 ) gypsum or gypsum-bearing
rocks exist in few areas. In Region 2, granites are extensively
developed, which were formed during the Yanshanian age, the
Indosinian age, the middle-late Proterozoic era and the Permian
period; late Cretaceous and Paleogene evaporate rocks, including
gypsum and halite, can be seen on the western Kunlun piedmont
zone (the Yigeyazi-Aertashi and Pishan-Sangzhu areas) and few
upper Cretaceous and upper Triassic gypsum and gypsum-bearing
rocks can be found in marginal zones of the basin; carbonatites
or carbonate-bearing rocks seldom exist in this region. Region 3
is characterized by great development of late Cretaceous, Paleogene and Neogene evaporate rocks such as gypsum, halite or other
gypsum-bearing rocks; few carbonatites only occur in Early Paleozoic strata; small amounts of granite can only be seen at the south
edge of this region. In region 4, carbonatites occurred in Early Paleozoic strata (O1 , O1+2 ) are mainly distributed in Aheqi-Keping area;
the Paleogene and Neogene evaporites including halite, gypsum
and gypsum-bearing rocks are distributed in Baicheng-Kuqa area,
while the granite seldom exist. The Quaternary deposit mostly covers region 5, some Paleogene and Neogene gypsum rocks can only
be seen between the Yarkant River and the Hotan River.
3. Material and methods
3.1. Sample collection and determination
A total of 302 water samples were collected from the Tarim Basin
from 2002 to 2010:
346
Y. Bo et al. / Chemie der Erde 73 (2013) 343–356
Fig. 2. Distribution of sampling spots of the Tarim Basin. 1–5 stands for river water, saline spring/brine, groundwater, short-term stagnant surface water and long-term
stagnant surface water, respectively; base map is according to Li (1991) and Mao (1998).
• 46 samples in 2002 (mainly river water),
• 27 in 2003 (river water and stagnant surface water),
• 15 in 2004 (river water, surface stagnant water and saline
spring/brine),
• 24 in 2005 (mainly river water and stagnant surface water),
• 35 in 2006 (mainly river water, and few saline spring/brine),
• 86 in 2007 (mainly river water and groundwater),
• 7 in 2008 (saline spring/brine),
• 60 in 2010 (mainly saline spring/brine, groundwater and stagnant
surface water).
Saline spring samples are mainly from the Kuqa Basin-north of
the Tarim Basin in region 4.
Sampling was done in accordance to the concerned operation
guides (MGMR, 1987; EPA, 2004). Groundwater samples were collected from wells (the depth range is 15–25 m) of local villages:
After 1–2 h pumping, filtered through 0.45 ␮m filter paper and
transferred to two low-density polyethylene bottles. One bottle
of sample was for anion analysis and the other for cation analysis
(acidified with HNO3 at a final concentration of 5%). Water samples for oxygen and hydrogen isotope analysis were also collected
in inclosed high-density polyethylene bottles without adding any
reagent. Samples of other water bodies were also processed in the
same way. During sampling, pH values for part of these samples
were measured with portable pH meter.
Each batch of samples were sent to the National Research Center for Geoanalysis (NRCGA, PRC) for chemical analysis. Standard
quality control methods were used to ensure accuracy in lab processes, according to the guideline DZ/T 0130-2006 (Ministry of Land
and Resources of the People’s Republic of China, 2006). Standard
solutions parallel samples and blank samples were used during
the process of sample analyzing. Besides, 20% of each batch of
samples was rechecked in other certified laboratories with the
same method to assure the reliability of analytical results. K+ , Ca2+ ,
Na+ , Mg2+ were detected according to the guideline JY/T 015-1996
(Education Commission of the People’s Republic of China, 1996)
by Inductively Coupled Plasma and Atomic Emission Spectrometry (ICP-AES,IRIS Advantage, Thermo Jarrell Ash, USA); Cl− was
titrated using the silver nitrate volumetric method with potassium
chromate as an indicator (DZG20.01-1991); SO4 2− was measured
by barium chloride titration with methyl orange as an indicator;
HCO3 − and CO3 2− were measured by hydrochloric acid titration
with phenolphthalein and mixed solution of methylene blue and
methyl red as indicators (CO3 2− was undetected). Minor ions Sr2+ ,
Li+ , B3+ , Br− and I− were measured by Inductively Coupled Plasma
and Mass Spectrometry (ICP-MS, Agilent 7500a, Agilent, USA). Cl−
and SO4 2− content in water samples with lower TDS (<1 g/L) were
also detected by Ion Chromatography (Dionex ICS900, USA). Br− ,
I− and B3+ (expressed as B2 O3 ) were also detected using colorimetry. TDS contents were estimated based on the conductivity
measurements and the sum of total analyzed dissolved solids: after
filtration, the filtrate was evaporated to dryness by water bath,
then the solids left was processed with hydrogen dioxide solution
to remove organic substances; after being dried at 105–110 ◦ C in
the oven for 2 h, the residue was cooled in desiccators to the constant weight (Editorial Board of Environmental Protection, 2002;
The Ministry of Water Resources of the People’s Republic of China,
1995; General Administration of Quality Supervision, Inspection
and Quarantine of the People’s Republic of China & Standardization
Administration of the People’s Republic of China, 2008).
The oxygen and hydrogen isotope compositions were determined using standard methods for waters (Epstein and Mayeda,
1953; Coleman et al., 1982). The analytical precision for oxygen and
hydrogen determinations is ±0.2‰ and 2‰ (MAT 253 stable isotope
ratio mass spectrometer, Thermo Scientific, USA), respectively.
3.2. Data processing and analysis
Data on 537 samples were collected and analyzed, which were
divided into four groups-river water (n = 193), saline spring/brine
(n = 196), groundwater (well water, n = 82) and stagnant surface
water (short-term, n = 57; long-term, n = 9). Gibbs plot, Piper diagram (Piper, 1953), ration graphs of ions (in meq/L) were used to
study hydrochemical characteristics and controlling factors of different waters in the Tarim Basin. Environmental background values
of major and minor ions and TDS values in river water were calculated with the SPSS 17.0 statistics software.
Y. Bo et al. / Chemie der Erde 73 (2013) 343–356
347
Table 2
Statistical result of different waters of the Tarim Basin.
Water bodies
Items
a
River water
Saline spring/brine
Groundwater
Short-term
stagnant surface
water
Long-term
stagnant surface
water
Water bodies
River water
Saline spring
Groundwater
Short-term
stagnant surface
water
Long-term
stagnant surface
water
a
n
Maximum
Median
Mean
Minimum
n
Maximum
Median
Mean
Minimum
n
Maximum
Median
Mean
Minimum
n
Maximum
Median
Mean
Minimum
n
Maximum
Median
Mean
Minimum
K+ (mg/L)
Na+ (g/L)
Ca2+ (mg/L)
Mg2+ (mg/L)
Cl− (g/L)
SO4 2− (g/L)
HCO3 − (mg/L)
TDS (g/L)
163
213.512
4.649
10.386
1.472
184
2135.000
107.000
169.000
5.000
32
127.593
6.271
18.921
0.972
41
726.123
25.468
70.114
0.166
9
2218.964
18.203
284.064
2.490
140
7.663
0.084
0.353
0.002
192
133.104
81.063
70.135
0.817
28
19.735
0.137
1.418
0.006
34
25.148
0.751
3.006
0.008
7
22.371
0.650
4.294
0.306
193
515.370
58.605
75.305
0.000
196
14,890.000
1808.000
2940.000
4.000
53
1567.830
90.298
167.078
9.900
57
1073.846
276.462
341.935
0.054
9
940.000
50.743
188.867
0.046
193
411.273
22.195
33.385
0.000
196
10,113.000
556.000
1166.000
0.000
53
838.400
67.630
153.743
2.393
57
4437.602
230.000
532.377
0.003
9
3828.831
373.821
656.428
0.003
193
5.632
0.089
0.264
0.000
196
196.942
129.869
111.692
0.668
53
31.049
0.380
1.886
0.033
57
30.328
1.640
4.042
0.033
9
13.667
0.325
2.584
0.100
193
4.922
0.198
0.386
0.008
196
76.660
3.429
4.697
0.062
53
4.895
0.523
1.094
0.086
57
31.822
1.495
3.083
0.041
9
45.499
0.601
6.349
0.154
186
537.289
113.778
110.144
0.086
185
882.637
48.260
99.162
0.000
53
813.000
73.224
107.120
0.086
57
675.100
134.244
159.011
0.089
9
970.900
153.236
272.584
18.388
166
17.894
0.596
1.284
0.163
191
371.057
227.678
190.176
4.003
30
57.862
0.908
4.479
0.239
50
92.168
5.593
11.784
0.309
9
88.560
1.682
13.674
0.822
Items
Sr2+ (mg/L)
Li+ (mg/L)
I− (mg/L)
Br− (mg/L)
B2 O3 (mg/L)
pH
n
Maximum
Median
Mean
Minimum
n
Maximum
Median
Mean
Minimum
n
Maximum
Median
Mean
Minimum
n
Maximum
Median
Mean
Minimum
n
Maximum
Median
Mean
Minimum
158
12.177
0.568
1.203
0.000
122
455.440
18.285
73.248
0.457
30
23.035
1.213
2.91
0.248
41
26.806
5.953
5.633
0.001
9
14.490
0.846
4.167
0.001
158
1.257
0.05
0.084
0.000
122
46.450
2.79
11.272
0.000
31
0.795
0.036
0.09
0.000
41
1.663
0.083
0.213
0.000
9
16.575
0.070
2.010
0.020
158
0.149
0.034
0.034
0.000
58
13.950
0.122
1.447
0.000
31
0.102
0.031
0.032
0.000
41
1.038
0.02
0.076
0.000
9
0.342
0.056
0.077
0.000
158
7.738
0.235
1.303
0.000
177
147.430
2.16
11.842
0.000
32
7.738
0.461
2.038
0.065
41
41.265
2.381
3.468
0.001
9
7.530
2.381
3.089
0.225
147
30.821
0.445
1.602
0.000
141
115.172
5.004
12.408
0.000
23
18.648
0.46
3.388
0.218
24
29.286
0.631
3.099
0.139
6
40.880
1.054
7.828
0.528
72
5.55
7.72
7.67
8.52
15
8.39
7.00
6.97
5.22
12
8.01
7.51
7.56
7.16
–
–
–
–
–
–
–
–
–
–
n – the sample size of each item; this is the same in statistical result of TDS and ions’ contents of other water bodies.
In this study, boxplot was used for rejection of unusual values,
which has its own superiority in the recognition of unusual values
(Zhuang, 2003; Wang, 2011), especially for large amounts of geochemical data processing. After the unusual values were rejected
by boxplot with SPSS 17.0 software step by step till each value was
in the normal scope and achieved the normal analytical conditions
(Chang et al., 2005), then the arithmetic mean value of the data
left was calculated, i.e. the background value. The lower limit of
unusual values can be obtained by adding two times of the corresponding standard deviation (SD) to the arithmetic mean value
(Li, 1983, 1991; Qiu and Huang, 1994; Huang and Xu, 2008; Zhang
et al., 2011), which has greatly saved the computing time.
Gibbs plot (Gibbs, 1970) is a useful tool for surface water
evolution mechanism study, and through plots of total dissolved
solids (TDS) versus the sodium to sodium plus calcium ratio and
the chloride to chloride plus bicarbonate ratio, i.e. Na/(Na + Ca)
and Cl/(Cl + HCO3 ), material sources of natural waters can be
effectively distinguished: atmospheric precipitation, rock dominance and the evaporation-fractional crystallization process. This
study has shown proof positive why many scholars have used this
model to study relationships between chemical composition of
waters and regional climate, geological features, etc. (Larsen et al.,
2011; Edet and Okereke, 2005; Min et al., 2007; Zhu and Yang, 2007;
Al-Shaibani, 2008; Hou et al., 2009; Bonotto and De Lima, 2010;
Song et al., 2010; Ye et al., 2010). So, in this research, Gibbs plot
also takes a great role in data analysis.
4. Results
4.1. General characteristics and isotopic compositions of waters
Chemical and isotopic analyses of waters were undertaken as a
basis for investigating the hydrochemical characteristics and controlling factors in the Tarim Basin. Statistical results of major and
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Y. Bo et al. / Chemie der Erde 73 (2013) 343–356
Fig. 3 is: ␦D = 9.2593␦18 O + 26.033 (r = 0.9921) and that for saline
spring/bring is: ␦D = 2.8764␦18 O + 49.668 (r = 0.8455).
4.2. Environmental background values of river water
Element background value reflects the basic geochemical conditions of element distribution in a region. Background values of
major and minor ions and TDS in river water of four regions are
shown in Table 3 (sample size of Region 5 is too small to be
involved). TDS background values are:
•
•
•
•
Fig. 3. Plot of ␦18 O-␦D for waters from the Tarim Basin only water samples from
Region 3 and Region 4, as well as two subsurface brine samples from the Lop Nur
were collected and analyzed; most data for subsurface brine of Lop Nur are from
Wang et al. (2001).
minor ions’ content and TDS value of different waters are shown in
Table 2. Saline spring/brine shows much higher level of TDS, than
other water bodies with a median TDS value of 227.678 g/L, and
the maximum is 371.057 g/L. Besides, some phreatic groundwater and stagnant surface water (ditch water and salt lake water)
samples, as well as river water flowing through salt-rock bearing areas, also have relatively higher TDS values. TDS range of
groundwater, short-term stagnant surface water and long-term
stagnant surface water is 0.239–57.862 g/L, 0.309–92.168 g/L, and
0.822–88.560 g/L, respectively. While for river water, TDS ranges
from 0.163 g/L to 17.894 g/L, and the median is 0.596 g/L; these are
all higher than those of the Qaidam Basin river water (ranges from
0.126 to 0.778 g/L) (Zhou and Dong, 2002). Among all the159 river
water samples, 11 show TDS values higher than 3 g/L.
Saline spring/brine and other water samples with higher TDS
level contain higher content of K+ , Na+ , Ca2+ , Mg2+ , Cl− , SO4 2− , Sr2+ ,
Li+ , Br− , I− , and B (B2 O3 ), while HCO3 − content in different water
bodies show small differences. Besides, saline spring/brine show
lower pH value (Table 2) than river water and groundwater, with a
median pH value of 7.00, and that of river water and groundwater
is 7.72 and 7.51, respectively. pH value for the same water body in
different regions show small differences.
On a global average, the general relation between ␦18 O
and ␦D for natural waters can be expressed by the equation:
␦D = 8␦18 O + 10 (Craig, 1961), i.e. the Global Meteoric Water Line
(GMWL). As shown in Fig. 3, isotopic compositions of different water types show great differences. Isotopic compositions
of river water, groundwater and some stagnant surface water
(from both region 3 and region 4), as well one meteoric water
from Lop Nur, fall very close to the GMWL on the left, which
clearly prove that they originate from regional precipitation. However, isotopic compositions of subsurface brine from Lop Nur
and a part of saline spring/brine from region 4 fall far away
from the GMWL on the right, revealing strong evaporation the
brine suffered during their evolution. Data points of other saline
spring/brine and other stagnant surface water fall just between
the two groups mentioned above, indicating both the source of
meteoric water and the effect of evaporation. Besides, oxygen
and hydrogen isotopic compositions for groundwater (from region
3) and saline spring/brine (from region 4) show good positive
correlations. The regression line for groundwater data plotted in
Region 1 (the south and southeast, 0.923 g/L) and
Region 2 (the southwest, 0.824 g/L) are higher than
Region 3 (the northwest, 0.446 g/L) and
Region 4 (the north, 0.444 g/L). This is related to the climate of
the basin-the north is wetter and the south is drier (Lv, 1993).
Background value range of K+ , Na+ , Cl− , Ca2+ is
0.042–0.244 g/L,
0.039–0.164 g/L
and
3.823–8.895 mg/L,
51.174–65.247 mg/L respectively; there are small differences
among background values of Mg2+ in these four regions, the range
is 22.077–26.003 mg/L; background value range of HCO3 − and
SO4 2− is 35.573–165.023 mg/L and 0.206–0.282 g/L, respectively.
In addition, based on background value (bij ) of each analytical
item (i) in the four regions and its corresponding valid sample size
(nij ), background value of each item in river water in the Tarim Basin
(Bi ) has been calculated (Table 4), according to Eqs. (A.1) and (A.2).
Bi =
4
bij × kij
(A.1)
i=1
ki =
nij
4
(A.2)
nij
j=1
Background values listed in Table 4 above can help to understand the overall characteristics of river water in the Tarim Basin.
However, in future practical work, background values of each
region may be referred more often in regional studies, and lower
limit of unusual values for each item (mij ) can be calculated based
on its standard deviation (SD) value (ıij ) and background value (bij ),
i.e. mij = bij + 2ıij .
In comparison with river water of the Qaidam Basin (Zhou and
Dong, 2002), background values of major ions (K+ , Na+ , Mg2+ , Cl−
and SO4 2− ) for river water of the Tarim Basin are higher than those
of the Qaidam Basin (3.666 mg/L, 0.084 g/L, 19.119 mg/L, 0.051 g/L,
0.045 g/L, respectively), while the Qaidam Basin river water contains higher level of Ca2+ (65.316 mg/L) and HCO3 − (141.115 mg/L)
because of its local marble, dolomite, limestone, etc. Besides, background value ratio of SO4 2− to Cl− (SO4 /Cl) of river water in the
Tarim Basin (2.75) is much higher than that of river water in the
Qaidam Basin (0.88) and seawater (0.14)-8 times higher than seawater and two times higher than river water of the Qaidam Basin;
the K+ to Cl− ratio (K/Cl) of river water in the Tarim Basin is two
times higher than seawater, and slightly lower than that in the
Qaidam Basin (Table 5).
4.3. Hydrochemical types of waters
According to Valyashko’s classification (Valyashko, 1965), water
samples in the Tarim Basin are divided into the chloride type, magnesium sulfate subtype, sodium sulfate subtype and carbonate type.
Hydrochemical type of waters in the Tarim Basin shows zonal distribution (Fig. 4).
Y. Bo et al. / Chemie der Erde 73 (2013) 343–356
349
Table 3
Statistical result of environmental background values in river water of different regions in the Tarim Basin.
Nb
Region 1 (n = 37)
K+ (mg/L)
Na+ (g/L)
Ca2+ (mg/L)
Mg2+ (mg/L)
Sr2+ (mg/L)
Li+ (mg/L)
Cl− (g/L)
SO4 2− (g/L)
I− (mg/L)
Br− (mg/L)
B2 O3 (mg/L)
HCO3 − (mg/L)
TDS (g/L)
Region 3 (n = 35)
K+ (mg/L)
Na+ (g/L)
Ca2+ (mg/L)
Mg2+ (mg/L)
Sr2+ (mg/L)
Li+ (mg/L)
Cl− (g/L)
SO4 2− (g/L)
I− (mg/L)
Br− (mg/L)
B2 O3 (mg/L)
HCO3 − (mg/L)
TDS (g/L)
b
Minimum
Maximum
Mean
SD
18
19
36
36
8
12
31
33
19
17
18
33
33
4.563
0.042
0.026
0.001
0.001
0.032
0.055
0.064
0.044
2.024
0.646
22.066
0.351
15.614
0.659
212.978
67.540
0.002
0.064
0.325
0.757
0.067
3.393
9.234
309.109
1.864
8.895
0.244
57.854
24.279
0.001
0.042
0.164
0.272
0.059
2.475
3.043
165.023
0.923
3.067
0.182
61.570
20.077
0.000
0.009
0.073
0.206
0.006
0.384
2.933
61.071
0.422
28
28
31
28
32
23
28
34
33
32
27
34
23
1.494
0.016
0.044
0.002
0.001
0.035
0.014
0.008
0.002
0.000
0.000
49.035
0.240
9.713
0.170
146.014
69.953
4.143
0.070
0.152
0.975
0.082
4.819
1.470
269.500
0.667
4.464
0.066
63.867
26.003
1.323
0.054
0.061
0.282
0.024
1.062
0.448
155.101
0.446
1.494
0.016
0.044
0.002
0.001
0.035
0.014
0.008
0.002
0.000
0.000
49.035
0.240
Region 2 (n = 25)
K+ (mg/L)
Na+ (g/L)
Ca2+ (mg/L)
Mg2+ (mg/L)
Sr2+ (mg/L)
Li+ (mg/L)
Cl− (g/L)
SO4 2− (g/L)
I− (mg/L)
Br− (mg/L)
B2 O3 (mg/L)
HCO3 − (mg/L)
TDS (g/L)
Region 4 (n = 94)
K+ (mg/L)
Na+ (g/L)
Ca2+ (mg/L)
Mg2+ (mg/L)
Sr2+ (mg/L)
Li+ (mg/L)
Cl− (g/L)
SO4 2− (g/L)
I− (mg/L)
Br− (mg/L)
B2 O3 (mg/L)
HCO3 − (mg/L)
TDS (g/L)
N
Minimum
Maximum
Mean
SD
16
13
25
25
15
17
21
22
17
7
13
23
22
2.021
0.036
0.048
0.001
0.000
0.008
0.037
0.090
0.047
2.381
0.220
98.071
0.412
13.199
0.340
155.088
72.968
1.099
0.141
0.254
0.513
0.073
2.381
1.081
232.800
1.675
6.127
0.141
51.174
22.077
0.294
0.052
0.113
0.225
0.058
2.381
0.541
144.374
0.824
2.827
0.088
50.073
24.003
0.393
0.041
0.065
0.127
0.009
0.000
0.261
36.558
0.404
77
44
87
88
65
79
56
86
86
66
68
85
48
1.472
0.000
0.000
0.000
0.010
0.000
0.009
0.045
0.000
0.000
0.056
0.086
0.163
7.951
0.101
125.071
64.947
1.216
0.087
0.067
0.489
0.092
0.369
0.733
173.900
0.900
3.823
0.042
65.247
24.637
0.511
0.039
0.039
0.206
0.025
0.103
0.320
35.373
0.444
1.625
0.027
26.074
15.182
0.223
0.023
0.016
0.107
0.023
0.097
0.163
55.609
0.160
N – the valid sample size involved in background value calculation.
• In Region 1 and Region 2, the carbonate type and the sodium sulfate subtype dominate, and seldom exists the magnesium sulfate
subtype;
• In Region 3, waters mainly belong to the sodium sulfate subtype, and partially belong to the magnesium sulfate subtype and
chloride type;
• In Region 4, the sulfate types (the magnesium sulfate subtype and
the sodium sulfate subtype) dominate, with a small part belonging to the chloride type.
Besides, hydrochemical types of different waters also show
zonal distribution.
• River waters in Region 1 and Region 2 mainly belong to the carbonate type and the sodium sulfate subtype;
• River waters in Region 3 mainly belong to the sodium sulfate
subtype;
• River waters in Region 4 mainly belong to the sulfate types, with
a small part belonging to the chloride type;
Fig. 4. Distribution of hydrochemical types in the Tarim Basin.
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Y. Bo et al. / Chemie der Erde 73 (2013) 343–356
Fig. 5. Piper plots of chemical compositions for different types of water in the Tarim Basin. (a) River water; (b) saline spring/brine; (c) ground water; (d) surface water. Group
1 to group 5 in Fig. 4 represents Region 1 to Region 5, respectively; the apex of Na means the sum of Na+ and K+ .
• The only one river water sample from Region 5 belongs to the
magnesium subtype.
• Groundwaters in Region 1, Region 2, Region 3 and Region 5 mainly
belong to the sodium sulfate subtype, with a few belonging to the
magnesium subtype or the carbonate type;
• Groundwaters in Region 4 mainly belong to the sulfate types, and
few belong to the chloride type.
• Saline springs/brines in Region 1, Region 2 and Region 3 mainly
belong to the sulfate types, and few belong to the chloride type;
Table 4
Statistical result of environmental background values in river water of the Tarim
Basin.
Table 5
Comparision of main ions’ contents and ratios for river water of the Tarim Basin and
the Qaidam Basin with seawater.
Items
Background value
Items
Background value
Water
K+ (mg/L)
Na+ (g/L)
Ca2+ (mg/L)
Mg2+ (mg/L)
Sr2+ (mg/L)
Li+ (mg/L)
Cl− (g/L)
4.924
0.102
60.778
24.640
0.669
0.044
0.088
SO4 2− (g/L)
I− (mg/L)
Br− (mg/L)
B2 O3 (mg/L)
HCO3 − (mg/L)
TDS (g/L)
0.242
0.033
0.834
0.767
89.249
0.685
River water in the
Tarim Basin
Sea watera
River water in the
Qaidam Basinb
a
b
K+ (mg/L)
4.92
429
3.67
From Drever (1988).
From Zhou and Dong (2002).
Cl− (mg/L)
88
20,057
51
SO4 2− (mg/L)
K/Cl
SO4 /Cl
242
0.06
2.75
2784
45
0.02
0.07
0.14
0.88
Y. Bo et al. / Chemie der Erde 73 (2013) 343–356
351
Fig. 6. Relation graphs of ions (in meq/L) in river water of the Tarim Basin. 1–5 stands for Region 1 to Region 5, respectively; (a) the plot of (Cl− + SO4 2− ) versus HCO3 − ; (b) the
plot of HCO3 − versus (Ca2+ + Mg2+ ); (c) the plot of (Na+ + K+ ) versus Cl− ; (d) the plot of Na+ versus SO4 2− ; (e) the plot of (Ca2+ + Mg2+ ) versus SO4 2− ; (f) the plot of (Ca2+ + Mg2+ )
versus Cl− .
• Saline springs/brines in Region 4 mainly belong to the chloride,
followed by the sulfate types.
Chloride type water usually reveals recharge of hydrothermal
Ca–Cl brine, which means fluids from the deep join the hydrochemical evolution of the Tarim Basin (Lei and Xu, 1999; Yang et al., 1993;
Lowenstein and Risacher, 2009). Stagnant surface waters in Region
1 and Region 2 belong to the magnesium sulfate subtype and the
carbonate type; in Region 3 the sodium sulfate subtype dominates,
with few belonging to the magnesium sulfate subtype; stagnant
surface waters in Region 4 mainly belong to the sulfate types, and
few belong to the chloride type.
Additionally, in Lop Nur playa, there exists plenty of underground potassium-rich brine, which belongs to magnesium sulfate
subtype (Wang et al., 2001).
4.4. Water chemical composition and controlling factors
4.4.1. River water
Chemical compositions for river water in different regions of the
Tarim Basin can be seen in Fig. 5a. HCO3 − contents are mostly less
than 40% of the total anions, except several data points of Region
3 (40–80%). Cl− and SO4 2− are the main anions in Region 4, with
quite a few projection points of anions falling on the SO4 2− –Cl−
line. As for cations, Mg2+ contents in most river water samples are
below 40% and Ca2+ are mostly 20–80%. Besides, more than ten data
points of Region 1 and Region 2 fall on the (Na+ + K+ ) apex, and this
is greatly relevant to the weathering of rocks (granite, gneiss and
other metamorphic rocks, etc.) of the surrounding mountains.
Furthermore, ration graphs of ions can also help to understand
material source of river water in different regions of the basin.
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Y. Bo et al. / Chemie der Erde 73 (2013) 343–356
Fig. 7. Gibbs plots indicating the mechanisms that determine major-ion composition of river water in the Tarim Basin.
Fig. 6a reveals that the evaporite is a more important material
source of most river waters than the carbonatite in the basin, for
most data points are projected below the equivalence line except
a small part of Region 3. Fig. 6c implies that Na+ , K+ and Cl− in
river water of the Tarim Basin primarily come from the solution
of halite and sylvine, and Fig. 6d shows that the sulfate is also an
important source of Na+ . From Fig. 6e, combined with Fig. 6b and
Fig. 6f, the sulfate is the main source of Ca2+ and Mg2+ in Region
3 and Region 4, while Ca2+ and Mg2+ in Region 1 and Region 2 are
less relevant to the evaporite or the carbonatite, so they may have
something to do with the silicate. For the only one sample of Region
5, Ca2+ , Mg2+ and SO4 2− mostly come from the solution of the sulfate, and Na+ , K+ and Cl− come from the solution of halite and
sylvine.
Gibbs plots of TDS versus the ion ratios Na/(Na + Ca) and
Cl/(Cl + HCO3 ) of river water in the Tarim Basin are shown in
Fig. 7. Most data points fall on the intermediate area between the
rock dominance end member and the evaporation/precipitation
dominance end member. This indicates that rock weathering and
evaporation are the dominant processes controlling the majorion composition of river water in the Tarim Basin. Besides, some
data points approaching to the Na/(Na + Ca) = 1 or Cl/(Cl + HCO3 ) = 1
line reveal the evaporation of atmospheric precipitation dominated
water.
Totally, besides evaporation, chemical composition of river
water in the Tarim Basin is greatly influenced by rocks and minerals
of the surrounding mountains. In Region 1 and Region 2, chemical composition of river water is mainly influenced by the granite,
gneiss and other metamorphic rocks, etc., while in Region 3 and
Region 4, it is mainly influenced by the dissolution of evaporite,
such as gypsum and halite rocks, and chemical composition of river
water in Region 3 is partially influenced by the carbonatite.
4.4.2. Saline spring/brine
Chemical compositions for saline spring/brine in different
regions are shown in Fig. 5b. For anions, most data points fall on
the SO4 2− –Cl− line, and approach the Cl− apex in the anions’ triangular plot, with Cl− accounting for more than 60%. Besides, most
data points approach the (Na+ + K+ ) apex in the cations’ triangular plot, and contents of Mg2+ and Ca 2+ , are lower than 30% of
the total anions. All the saline spring samples are characterized by
the major anion pattern Cl− > SO4 2− > HCO3 − . From the Gibbs plot
(Fig. 8a), chemical compositions of saline spring in the Tarim basin
are mainly controlled by evaporation, for all data points fall on the
evaporation/precipitation end member, similar with the composition of seawater.
4.4.3. Groundwater
From the Piper plot (Fig. 5c), groundwater in Region 1 and
Region 2 have similar compositions, the data points of cations
are close to the (Na+ + K+ ) apex, and SO4 2− and Cl− dominate in
the anions. Data points of anions of Region 3 approach to the
SO4 2− apex, and the compositions of cations are similar with
those of Region 1, Region 2 and Region 5. In Region 4, Ca2+ and
Mg2+ are the main cations, while SO4 2− is the main anion, with
most data points falling on the SO4 2− –Cl− line. Groundwater in
Region 5 (n = 13) has stable chemical composition. The Gibbs plot
(Fig. 8b) reveals that chemical compositions of groundwater in different regions are different. Groundwater composition of Region
3 is controlled by evaporation and rock weathering, and that of
Region 4 is controlled by evaporation of atmospheric precipitation
dominated water, while chemical composition of groundwater in
Region 5-the central desert area, is mainly controlled by evaporation.
Y. Bo et al. / Chemie der Erde 73 (2013) 343–356
353
Fig. 8. Gibbs plots indicating the mechanisms that determine major-anion composition of saline spring (a), groundwater (b) and stagnant surface water (c) in the Tarim
Basin.
4.4.4. Stagnant surface water
As shown in Fig. 5d, most data points of anions in stagnant surface water fall on or approach the SO4 2− –Cl− line. The chemical
composition of stagnant surface water in Region 5 is quite stable,
with Cl− accounting for more than 60% and (Na+ + K+ ) accounting for more than 40%. Chemical compositions of stagnant surface
water in the other four regions are less stable, especially cations’
composition of Region 4. From the Gibbs plot (Fig. 8c), chemical
composition of stagnant surface water is primarily controlled by
evaporation, and partially (in Region 4) influenced by rock weathering and evaporation of atmospheric precipitation dominated water.
5. Discussion
5.1. Recharge of hydrothermal Ca–Cl brines
Lowenstein and Risacher (2009) studied closed basin brine evolution and the influence of Ca–Cl inflow waters (Death Valley
and Bristol Dry Lake California, Qaidam Basin, China, and Salar
de Atacama, Chile). They called those brines hydrothermal Ca–Cl
brines. Diagenetic-hydrothermal waters are typically brines (rich in
Na–Ca–Cl) that contain little SO4 or HCO3 , which reflects the interactions between heated groundwaters and sediments or rocks at
elevated temperatures, commonly 100 ◦ C to >300 ◦ C (Hardie, 1990).
They have Ca equivalents > SO4 + HCO3 + CO3 and are commonly
discharged as springs or seeps at low temperatures (Lowenstein
and Risacher, 2009). Hydrothermal Ca–Cl brines can reach the
surface by convection-driven circulation associated with thermal anomalies or by topographically driven circulation (Hardie,
1990).
In this study, chloride type of waters are widely distributed in
saline springs/brines of Region 4-the Kuqa Basin, where two big
tectonic fault belts (Qiulitage in the south and Kelasu in the north)
are distributed from the east to the west. These waters have Ca
Fig. 9. Ternary Ca–SO4 –Cl phase diagrama for saline springs/brines in the Tarim
Basin.
Modified from Lowenstein and Risacher (2009).
equivalents > SO4 + HCO3 + CO3 and here they are also called
hydrothermal Ca–Cl brines. From Fig. 9, they are chemically distinct from meteoric weathering water because they fall within the
Ca–Cl field. Besides, some data points of river water, groundwater
and stagnant surface water also fall in the Ca–Cl field (the chloride
type of water referred in Section 4.3) in Region 4. Hydrothermal
Ca–Cl brines reflect interactions between groundwaters and rocks
or sediments at elevated temperature (Lowenstein and Risacher,
2009). Therefore, in the Tarim Basin, hydrothermal Ca–Cl brines
from the deep within the earth not only are the main recharge for
saline springs/brines but also join the evolution of other waters
(river water, groundwater and stagnant surface water).
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Y. Bo et al. / Chemie der Erde 73 (2013) 343–356
Fig. 10. Water circulation and evolution of the Tarim Basin.
5.2. Material sources of Lop Nur
In Lop Nur, a huge liquid potash ore deposit (a great deal of
potassium-rich brine reserved in pores of glauberite) was found in
1995. However, till now the formation mechanism of the brine and
glauberite is not quite clear (Liu et al., 2007; Ma, 2010). The sources
of Ca2+ , K+ and SO4 2− , as well as the reason that the brine contains
much higher level of SO4 2− than Cl− , are still unknown.
In this study, some very important clues have been found.
Because of strong evaporation and weathering of the surrounding
rocks, river waters in the Tarim Basin mostly belong to the sulfate
types, which are greatly different from river waters in other areas
of the world (the carbonate type dominates). Besides, higher level
of background value ratios SO4 /Cl (2.75) and K/Cl (0.06) make it
more reasonable that the inflow waters of Lop Nur are relatively
richer in K+ and SO4 2− , while relatively poorer in Cl− . Furthermore, recharge of hydrothermal Ca-Cl brines from deep within the
earth bring abundant Ca2+ to the Tarim Basin and finally become an
important material source for glauberite accumulation in Lop Nur.
5.3. Water evolution in the Tarim Basin
Water evolution is a very complicated process in the Tarim
Basin. River water plays an important role in water evolution of
the Tarim Basin, however, the participation of other waters is not
negligible, especially saline springs/brines. As for the influence of
evaporation, oxygen and hydrogen isotopic compositions in river
water, groundwater, stagnant surface water, saline spring and subsurface brine in Lop Nur show water evolution process of the Tarim
Basin stage by stage: river water, groundwater and part of stagnant
surface water show recharge from meteoric water with weaker
evaporation, other stagnant surface water and saline spring reveal
strong evaporation, and subsurface brine in Lop Nur represents the
highest stage of water evolution in the Tarim Basin.
Based on closure and one-way incline of the Tarim Basin, water
circulation and evolution are suggested as shown in Fig. 10: since
the uplift of the western Tarim Basin, a great deal of waters (surface waters and groundwater, as well as brine from deep within the
earth) had been forced to lower places and finally gathered in Lop
Nur Lake; because of high temperature and aridness, waters suffered from strong evaporation and the salts began to precipitate;
over a long period of time, the lake dried up with plenty of salts and
other minerals accumulated.
6. Conclusions
Determination of element background value for river water
can offer essential data information for research on basic
hydrogeochemical characteristics of the Tarim Basin. In comparison with river water of the Qaidam Basin and seawater, background
value ratio SO4 /Cl for river water of the Tarim Basin is 18 times
higher than seawater and two times higher that river water of the
Qaidam Basin; the ratio K/Cl for river water of the Tarim Basin and
the Qaidam Basin are two times higher than seawater. This reveals
that the material source of Lop Nur is relatively richer in SO4 2−
and K+ and poorer in Cl− , which may give a reasonable explanation
for the accumulation of abundant glauberite and potassium in Lop
Nur.
Hydrochemical types and chemical compositions of different
water bodies in the Tarim Basin show zonal distribution. River
water compositions of the Tarim Basin are greatly related to the
surrounding rock types and strong evaporation. As for effect of rock
weathering, chemical compositions of river water in the north and
the northwest of the basin are greatly influenced by the dissolution
of evaporite (halite and gypsum, etc.), so the sulfate types water
dominate. While water compositions in the south and southeast are
greatly influenced by the granite, the gneiss and other metamorphic
rocks, etc., so the carbonate type and the sodium sulfate subtype
water dominate. Groundwater, saline spring, as well as stagnant
surface water in the Tarim basin also suffer strong evaporation,
and compositions of these waters are also more or less controlled
by rock weathering. Moreover, the wide distribution of chloride
type water proves that hydrothermal Ca-Cl brines from the deep
play an important role in the hydrochemical evolution of the Tarim
Basin.
Acknowledgements
National Key Basic Research and Development Program (973
program, No. 2011CB403007) and National Natural Science Foundation of China (No. 40830420) from the Chinese government
provided the funding for this study. We are grateful to graduate
students Chao Gao and Xianfu Zhao of Chinese Geology University (Beijing) for their help in sample collecting. We also would
like to kindly acknowledge the NRCGA (National Research Center for Geoanalysis), Yingsu Wang, Meifang Dai et al., for their
hard work in water sample analysis. Besides, Ph.D. student Hua
Zhang of Chinese Academy of Geological Sciences is thanked for
his help in part of graph drawing and Ph.D. student Wenxiang
Wang of Chinese Geology University (Beijing) is thanked for his
help in data collection from literatures. Mr. Tim Swanson is thanked
for his revision of English. Prof. Liqiang Luo and two anonymous
reviewers are thanked for their constructive comments on the
manuscript.
Y. Bo et al. / Chemie der Erde 73 (2013) 343–356
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