Seasonal Interaction of River Water-Groundwater-Salt Lake Brine and Its Influence on Water-Salt Balance in the Nalenggele River Catchment in Qaidam Basin, NW China

Jibin Han; Jianxin Xu; Lei Yi; Zheng Chang; Jianping Wang; Haizhou Ma; Baoyun Zhang; Hongchen Jiang

doi:10.1007/s12583-022-1731-0

Volume 33 Issue 5

Oct 2022

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Article Contents

Abstract

0. INTRODUCTION

1. MATERIALS AND METHODS

2. RESULTS

3. DISCUSSIONS

4. CONCLUSION

References

Journal of Earth Science > 2022 > 33(5): 1298-1308.

Jibin Han, Jianxin Xu, Lei Yi, Zheng Chang, Jianping Wang, Haizhou Ma, Baoyun Zhang, Hongchen Jiang. Seasonal Interaction of River Water-Groundwater-Salt Lake Brine and Its Influence on Water-Salt Balance in the Nalenggele River Catchment in Qaidam Basin, NW China. Journal of Earth Science, 2022, 33(5): 1298-1308. doi: 10.1007/s12583-022-1731-0

Citation:

Jibin Han, Jianxin Xu, Lei Yi, Zheng Chang, Jianping Wang, Haizhou Ma, Baoyun Zhang, Hongchen Jiang. Seasonal Interaction of River Water-Groundwater-Salt Lake Brine and Its Influence on Water-Salt Balance in the Nalenggele River Catchment in Qaidam Basin, NW China. Journal of Earth Science, 2022, 33(5): 1298-1308. doi: 10.1007/s12583-022-1731-0

Citation:

Jibin Han, Jianxin Xu, Lei Yi, Zheng Chang, Jianping Wang, Haizhou Ma, Baoyun Zhang, Hongchen Jiang. Seasonal Interaction of River Water-Groundwater-Salt Lake Brine and Its Influence on Water-Salt Balance in the Nalenggele River Catchment in Qaidam Basin, NW China. Journal of Earth Science, 2022, 33(5): 1298-1308. doi: 10.1007/s12583-022-1731-0

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Seasonal Interaction of River Water-Groundwater-Salt Lake Brine and Its Influence on Water-Salt Balance in the Nalenggele River Catchment in Qaidam Basin, NW China

doi: 10.1007/s12583-022-1731-0

Jibin Han^{1
,
,
,},
Jianxin Xu¹,
Lei Yi¹,
Zheng Chang^{1, 2},
Jianping Wang¹,
Haizhou Ma¹,
Baoyun Zhang³,
Hongchen Jiang^{1, 4
,
,
,}

1.
Qinghai Provincial Key Laboratory of Geology and Environment of Salt Lakes, Qinghai Institute of Salt Lakes, Chinese Academy of Sciences, Xining 810008, China
2.
University of Chinese Academy of Sciences, Beijing 100049, China
3.
Haixi Water Resources Bureau of Qinghai Province, Delingha 817200, China
4.
State Key Laboratory of Biogeology and Environmental Geology, China University of Geosciences, Wuhan 430074, China

More Information

Corresponding author: Jibin Han, jbhan@isl.ac.cn; Hongchen Jiang, jiangh@cug.edu.cn
Received Date: 10 Nov 2021
Accepted Date: 06 Aug 2022

Available Online: 19 Oct 2022

Issue Publish Date: 30 Oct 2022

Abstract

Abstract

Identifying interactions among river water, groundwater and salt lake brine is important for sustainable exploitation of brine mineral resources. In this study, we investigated the water exchange rate in dry and wet seasons, and assessed the influence of seasonal water exchange on brine concentration and crystallization process in the Nalenggele (NLGL) catchment of Qaidam Basin, China. The results show that the surface water infiltration and groundwater recharge rates in the wet season were 2.81 × 10^-3 and 1.15 × 10^-3 m³/(s·m) in upstream, 1.63 × 10^-2 and 1.53 × 10^-2 m³/(s·m) in midstream, and 2.83 × 10^-4 and 6.82 × 10^-5 m³/(s·m) in downstream, respectively; while their counterparts in the dry season were 9.81 × 10^-4 and 5.05 × 10^-4 m³/(s·m) in upstream, and 8.34 × 10^-3 and 7.78 × 10^-3 m³/(s·m) in midstream, respectively. The water exchange strongly influenced brine concentration and crystallinzation process, with brine chemistry belonging to 3K₂SO₄·Na₂SO₄ and KCl types in wet and dry seasons, respectively. The strong water exchange in wet season destroyed the water-salt balance, while the low water exchange rate in dry season facilitated preparation of KCl products.
- river water-groundwater-salt lake interactions,
- ²²²Rn isotope,
- δ¹⁸O-δD isotope,
- seasonal variation,
- Nalenggele River catchment,
- hydrogeology

Electronic Supplementary Materials: Supplementary materials (Figs. S1, S2, Table S1) are available in the online version of this article at https://doi.org/10.1007/s12583-022-1731-0.

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0. INTRODUCTION

Interactions between river water and groundwater are common in river basins (Bouchez et al., 2021; Wang et al., 2021; Yang et al., 2021). Study of this interaction is of great significance to assessing groundwater budget and water resources allocation (Xu et al., 2017; Wang et al., 2016; Su et al., 2015; Cook et al., 2006; Batelaan et al., 2003). In arid and semi-arid regions, the characteristics of river water and groundwater vary greatly between wet season (WS) and dry season (DS) (Jia et al., 2021; Yang et al., 2021). Groundwater and river water support fragile ecosystems and human activities in arid and semi-arid regions (Wang et al., 2021; Yin et al., 2021; Zhang et al., 2021; Xu et al., 2017). Modern salt lakes are located in the catchment basin. The inflowing river water and the groundwater in the catchment area are finally supplied to the salt lake. They not only provide the water source for the salt lake, but also (Zhang, 1987). In the salt lake plain, there is usually interactions among river water, groundwater and salt lake brine, which are significantly different between wet season and dry season. This interaction maintains the water-salt balance in the salt lake area (Bischoff et al., 2004; Yu, 1995), and is necessary for sustainable brine mining of the salt industry.

Qaidam Basin, located in northwestern China, is a super arid basin with an area of 121 × 10³ km² (Yu et al., 2013). There are 25 salt lakes in Qaidam Basin, and these salt lakes possess abundant brine deposits, such as KCl and LiCl (Han et al., 2021; Wei et al., 2014; Tan et al., 2012). Among these salt lakes, Dong-Xi Taijinaer Salt Lake (DXTSL), with an average elevation of 2 860 m above sea level (m.a.s.l.) is the largest LiCl mine in China. The DXTSL is fed by Nalenggele (NLGL) River that originates from the east of Kunlun Mountain with an average elevation of 4 500 m.a.s.l. The annual water supply of the NLGL River is about 10.0 × 10⁸ m³, which can be used for local ecology, agriculture and animal husbandry, domestic water, and salt chemical industry. The DXTSL area needs about 5.95×10⁸ and 2.4×10⁸ m³/a water resources to sustain the salt lake area and water-salt balance, respectively (Shi et al., 2021). The amount of brine used for the production of LiCl is up to 2.0×10⁸ m³/a (Han et al., 2020). However, the water consumption and brine extraction of salt chemical industry are increasing in recent years, resulting in the intensification of contradiction between supply and demand of water resources (Han et al., 2020; Guo et al., 2012). Besides, the runoff of the NLGL River varies greatly between wet (June, July, August) and dry seasons (January, February, December): in the wet season, floods often occur and discharge into salt lakes, leading to the destruction of water-salt balance. In recent years, climate warming leads to increase of atmospheric precipitation (Liu et al., 2021; Lu, 2014; Fu et al., 2011), so that floods in summer have seriously destroyed salt minerals (dissolution, decreasing grade, the ground collapsed) in the Qaidam Basin. However, so far limited is known about the interactions among river water, groundwater and the DXTSL, the quantity of river water and groundwater inflowing fluxes to the DXTSL in wet and dry seasons, and its influence for the salt lake brine concentration and brine crystallization process. Such knowledge is of great importance for understanding of water-salt balance and sustainable exploitation of brine in the DXTSL.

Various methods and techniques have been developed to study water source identification, hydrologic dynamics, and water quality and water exchange characteristics (Qin et al., 2021; Zhang et al., 2021a, b; Wu et al., 2020; Liao et al., 2018; Zhao et al., 2018; Xu et al., 2017; Stellato et al., 2008). Among these methods and techniques, radioactive isotope ²²²Rn is a natural conservative tracer, which has recently been widely employed to investigate exchange between groundwater and river water (Oh et al., 2021; Dimova et al., 2013; Santos et al., 2010; Cook et al., 2003), especially in arid and semi-arid areas (Yang et al., 2021; Zhao et al., 2018; Xu et al., 2017; Su et al., 2015). The concentration of ²²²Rn in groundwater is higher than that in river water (Ortega et al., 2015; Dimova and Burnett, 2011). This distinct difference enables researchers to identify the interaction between groundwater and river water during wet and dry seasons. Stable isotopes of hydrogen (D) and oxygen (¹⁸O) carry the information of water circulation, and thus can be used to determine the rate of supply to discharge, which makes these two common stable isotopes very useful for determining the sources of different types of water. Such methods have been widely used in hydrological and hydrogeological studies in recent decades (Zhao et al., 2018; Xu et al., 2017; Gu et al., 2011; Gat 2010; Kendall and McDonnell, 1998; Clark and Fritz, 1997).

In this study, we investigated the contributions of groundwater, river water to the brine of DXTSL along the NLGL River from upstream to downstream in wet and dry seasons, and their impacts on salt minerals. The aims of this study were to 1) quantitatively identify the interactions among the groundwater, river water and salt lake in wet and dry seasons; and 2) assess the influence of water exchange on brine concentration and brine crystallization process.

1. MATERIALS AND METHODS

1.1 Study Site

The NLGL River is the largest river in Qaidam Basin, northeasten Tibetan Plateau (Fig. 1a), and its runoff is 528.0 and 4.03 m³/s in wet and dry seasons, respectively, with an average of 13.66×10⁸ m³/year; the runoff of the NLGL River in wet season accounted for 74% of annual average runoff (Xu, 2015). In the DXTSL region, rainfall mainly occurs in summer, with average precipitation of less than 30 mm/a and average evaporation of larger than 2 700 mm/a (Xu and Su, 2019; Yu et al., 2013). The average temperature is approximately 3.0 ℃/year, with maximum and minimum temperature of 35.3 and -29.5 ℃, respectively (Xu et al., 2017).

Figure 1. Location of the study area on the Tibetan Plateau (a); and sampling sites in the wet season and dry season (b).

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The main bedrock types in the source area (upstream) of the NLGL River mainly consists of granodiorite, plagioclase granite and quartz diorite (Tan et al., 2012), which mainly contain bedrock fissure water (Rong et al., 2002). In the middle reaches, the NLGL River widens sharply after flowing out of the Kunlun Mountains, forming a huge foreland alluvial fan (I), which is rich in sedimentary sand, sandy clay and gravel. From the root to the edge of the fan I, the aquifer medium changes from single-layer to multi-layer, with the aquifer thickness changing from 20 to 165 m, the phreatic depth changing from about 100 to 3 m, and the permeability coefficient changing from 54.95 to 98.49 m/d. At the fan root, the aquifer is thick and widely distributed, with abundant groundwater (Tai, 2015; Xu, 2015); while at the edge of the fan there is confined aquifer, with a thickness of 10–50 m and less groundwater (Xu, 2015; Rong et al., 2002). In the midstream, the river water exchanges frequently with groundwater. In the downstream (fan II), river water disappears in winter and is remained at a high level in summer; the DXTSL is mainly recharged by groundwater. The sedimentary lithology of the aquifers is sand, sand with salt, and salt for the fan root, fan front, and the salt plain, respectively (Han et al., 2020). From the root to the edge of the fan II, the aquifer also changes from single-layer to multi- layer, which is filled with pore water (brine). In the salt lake plain area, the phreatic aquifer dominates, and its thickness gradually increases from the fan root (south) to the fan edge (north) (the thickness range is 2.0–8.2 m), and the water outflow from single wells increases from south to north, with the maximum value of 1 108.51 m³/d. This indicates that the salt lake plain area is rich in intergranular brine. The confined aquifer is only distributed in the center of the salt lake basin, with a depth of 7.0–9.0 m from the surface, a thickness of 10.0–25.0 m and a maximum water outflow of 182.47 m³/d from single wells. This suggests that there is less intercrystalline brine in the center of the salt lake basin (Rong et al., 2002).

1.2 Field Measurements and Sampling

Sampling cruises were performed along the NLGL River from upstream to downstream in July (wet season) and December (dry season) (Fig. 1b) of 2020. River water and brine samples were directly collected in the NLGL River and DXTSL, respectively; and groundwater samples were collected from phreatic water wells (15–25 m) and artesian wells (80–150 m) (Fig. 1b). In the field, the ²²²Rn activity of the water samples were measured by using a portable radon instrumentation RAD7-H₂O (Durridge, USA) via α-decay accounts. After field measurements, river water samples and salt lake brine samples were collected at the depth of about 10–20 cm below the water surface. The groundwater samples of artesian wells were directly collected into 500 mL bottles. The groundwater samples were collected from phreatic wells after pumping out at least five times the volume of stagnant water in the borehole. The spring water samples were extracted by using a peristaltic pump and air bubbles were removed as much as possible to ensure that the pumped water was representative. Intercrystalline brine samples were collected from the salt layer at the depth of about 50–150 cm below the lakebed. A total of 68 water samples were collected in July 2020, including 8 from the upstream NLGL River, 10 from branches in the mid-downstream, 41 from groundwater, 2 from salt lake brine, and 7 from intercrystalline brine (Fig. 1b); A total of 73 water samples were collected in Dec. 2020, including 1 from the upper stream of NLGL River, 11 from branches in the mid-lower stream, 31 from groundwater in alluvial fan I, 5 from salt lake brine, and 15 from intercrystalline brine in alluvial fan II (Fig. 1b).

1.3 Lab Analysis

Chemistry measurements of the collected water samples were carried out at the Qinghai Institute of Salt Lakes, Chinese Academy of Sciences. The contents of Ca²⁺, Mg²⁺, Na⁺, and K⁺ were determined by inductively coupled plasma optical emission spectrometry (ICP-OES) (IRIS Intrepid II XSP, Thermo Elemental, Madison, WI, USA) (error < ±1%), and the concentrations of SO₄^2- and Cl^- were determined by ion chromatography (IC) (Dionex 120, Dionex, Sunnyvale, CA, USA) (error < ±5%) (Han et al., 2018). The contents of HCO₃^- and CO₃^2- were analyzed by using hydrochloric acid titration with phenolphthalein and the mixed solution of methylene blue and methyl red as indicators (error < ±1%) (Han et al., 2018). The δ²H, δ¹⁸O isotopes of water samples were analyzed at the Institute of Hydrogeology and Environmental Geology, Shijiazhuang. The isotopes of δ²H (Zn reduction method) and δ¹⁸O (CO₂-H₂O method) were measured with Picarro L2130-i Isotope Analyzer, the measurement resolution of δ²H and δ¹⁸O isotopes is δD- VSMOW (Vienna Standard Mean Ocean Water) (‰) ≤ ±1.0‰ and δ¹⁸O-VSMOW(‰) ≤ ±0.2‰, respectively.

2. RESULTS

2.1 Hydrochemical Characteristics

The hydrochemistry data were shown in Table 1. During wet season (WS), in the upstream, Na⁺ and Ca²⁺ were the dominant cations in river water, with concentration ranging 35.7–148.2 and 119.9–258.4 mg/L (average: 55.8 and 165.5 mg/L), respectively; Cl^- and SO₄^2- were the major anions in river water, with concentration ranging 192.5–373.2 and 65.41–424.3 mg/L (average: 251.1 and 129.79 mg/L), respectively. In the midstream, Na⁺ was the dominant cation in river water, with concentration ranging 143.8–459.2 mg/L (average: 233.4 mg/L); and Cl^- was the major anion in river water, with concentration ranging 205.5–668.8 mg/L (average: 348.1 mg/L). Na⁺ was the dominant cation in groundwater, with concentration ranging 137.4–615.0 mg/L (average: 202.3 mg/L); and Cl^- was the major anion in groundwater, with concentration ranging 212.6–992.2 mg/L (average: 308.1 mg/L). In the downstream, Na⁺ and Cl^- were the dominant ions in the salt lake brine, with concentration ranging 2 141.0–115 106.0 mg/L (average: 58 623.0 mg/L) and 3 375.0–180 818.0 mg/L (average: 92 097.0 mg/L), respectively. Na⁺, Mg²⁺ and Cl^- were dominant ions in the intercrystalline brine, with concentration ranging 1 620.0–88 506.0 mg/L (average: 34 033.0 mg/L), 137.0–119 829.0 mg/L (average: 55 691.0 mg/L), 2 550.0–328 149.0 mg/L (average: 197 712.0 mg/L), respectively. The hydrochemical type was Na-Ca·Cl-SO₄ for the upstream river water, Na·Cl for the midstream river water and groundwater and the salt lake brine, and Na-Mg·Cl for the intercrystalline brine (Fig. S1).

Table 1. Concentrations of major cations and anions in the studied waters of the NLGL River catchment, Qaidam Basin

Season	Regions	Ca²⁺ (mg/L)		Mg²⁺ (mg/L)		Na⁺ (mg/L)		K⁺ (mg/L)		HCO₃^- (mg/L)		CO₃^2- (mg/L)		Cl^- (mg/L)		SO₄^2- (mg/L)
Season	Regions	Ave.	Range	Ave.	Range	Ave/	Range	Ave.	Range	Ave.	Range	Ave.	Range	Ave.	Range	Ave.	Range
Wet season	Upstream river water	55.8	35.7-148.2	24.9	20.7-39.28	165. 5	119.9-258.4	14.6	12.5-19.4	155.7	131.3-175.7	7.9	3.9-13.4	251.1	192.5-373.2	129.8	65.4-424.3
	Midstream groundwater	37.3	18.9-79.8	25.2	11.6-84.6	202.3	137.4-615.0	15.5	6.33-31.54	143.4	104.78-224.82	9.1	4.2-28.1	308.1	212.6-992.2	97.0	66.0-334.5
	Midstream river water	60.0	44.9-93.0	36.2	25.4-63.1	233.4	143.8-459.2	17.9	12.60-29.84	222.8	181.05-250.02	11.6	7.5-17.0	348.1	205.5-6 68.8	145.0	86.9-327.0
	Downstream salt lake brine	281.7	105.9-457.4	3 057.0	157.1- 5957.0	58 623.0	2 141.0- 115 106.0	2 158.0	72.0- 4 246.0	412.2	155.8-668.5	23.7	17.3-30.0	92 097.0	3 375.0- 180 818.0	13 187.0	739.6- 25 635.0
	Downstream intercrystalline brine	249.7	79.0-443.3	55 691.0	137.0- 119 829.0	34 033.0	1 620.0- 88 506.0	4574.0	62.0- 23 995.0	3108.0	143.0-9 895.0	28.4	0.4-28.4	197 712.0	2 550.0- 328 149.0	34 829.0	655.0- 58 364.0
Dry season	Upstream river water	54.2	-	27.4	-	160.0	-	10.4	-	157.0	-	11.6	-	240.6	-	102.1	-
	Midstream groundwater	59.7	24.4-126.4	35.0	20.8-80.0	267.5	140.0-830.0	17.8	9.0-58.0	403.2	211.0-1 080.0	8.6	0-38.7	124.1	66.9-1 84.9	226.1	58.5-477.5
	Midstream river water	73.5	48.6-84.9	47.2	28.0-63.5	300.0	165.0-520.0	20.1	14.0-27.0	269.1	165.2-397.3	16.3	11.6-23.2	433.0	257.4-709.0	204.2	86.4-359.7
	Downstream salt lake brine	509.4	88.1-812.5	2 244.8	104.2- 4 566.0	36 668.8	1 300.0- 110 000.0	916.1	42.5- 2 700.0	265.6	125.9-590.1	33.8	0-108.3	62 113.3	1 992.0- 183 158.0	5 797.7	522.7- 16 618.0
	Downstream intercrystalline brine	1561. 8	902.8- 2 347.0	16 222.4	4 161.0- 86 505.0	75 650.0	9 000.0- 105 000.0	4 420.0	900.0- 22 500.0	925.7	137.7-6 806.0	0	0	161 888.6	82 717.0- 243 930.0	12 937.2	5 299.0- 52 479.0

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During the dry season, Na⁺ and Cl^- were dominant ions in the upstream river water, with concentration ranging 160.0 and 240.6 mg/L, respectively (Table 1). In the midstream, Na⁺ and Cl^- were also dominant ions in river water, with concentration ranging 165.0–520.0 and 257.4–709.0 mg/L with average concentrations of 300.0 and 433.0 mg/L, respectively (Table 1); Na⁺ was the dominant cation in groundwater, with concentration ranging 140.0–830.0 mg/L (average: 267.5 mg/L); and Cl^- and SO₄^2- were dominant anions in groundwater, with concentration ranging 66.9–184.9 mg/L (average: 124.1 mg/L) and 58.5–477.5 mg/L (average: 226.1 mg/L), respectively (Table 1). In the downstream, Na⁺ and Cl^- were dominant ions in the salt lake brine, with concentration ranging 1 300.0–110 000.0 mg/L (average: 36 668.8 mg/L) and 1 992.0–18 3158.0 mg/L (average: 62 113.3 mg/L), respectively; and Na⁺, Mg²⁺, and Cl^- were dominant ions in the intercrystalline brine, with concentration ranging 9 000.0–105 000.0 (average: 75 650.0 mg/L), 4 161.0–86 505.0 (average: 16 222.4 mg/L), 82 717.0– 243 930.0 mg/L (average: 161 888.6 mg/L), respectively (Table 1). The hydrochemical type was Na·Cl for the upstream and midstream river water and salt lake brine, and Na·Cl-SO₄ for the midstream groundwater and intercrystalline brine (Fig. S1). The element concentration of the surface water and groundwater in dry season (especially in the midstream reaches) is higher than that in wet season, suggesting that water exchange is limited in the dry season.

2.2 Stable Isotopic Compositions of Hydrogen and Oxygen

In the wet season, the averaged δD values were -55.7‰, -53.9‰, +26.0‰ for the river waters of the upstream and midstream NLGL River and salt lake brine, respectively (Table 2); and the corresponding δ¹⁸O values were -7.82‰, -7.73‰, +8.4‰, respectively (Table 2). The δD values were -57.0‰ and +4.0‰ for the groundwater and intercrystalline brine of the midstream NLGL River, respectively; and the corresponding δ¹⁸O values were -8.56‰ and +5.9‰, respectively (Table 2).

Table 2. Isotopic compositions (δD, δ¹⁸O, ²²²Rn) in the studied waters of the NLGL River catchment, Qaidam Basin

Season	Regions	δ²H_vsmow (‰)		δ¹⁸O_vsmow (‰)		References	²²²Rn Bq/L
Season	Regions	Average	Range	Average	Range	References	Average	Range
Wet season	Upstream river water	-55.7	--	-7.82	--	Tan et al. (2012)	136.72	22.50-450.99
	Midstream groundwater	-57.0	--	-8.56	--	Kong et al. (2014)	1641.12	20.76-3975.0
	Midstream river water	-53.9	--	-7.73	--	Tan et al. (2012)	982.73	194.34-2600.0
	Downstream salt lake brine	+26.0	--	+8.4	--	This study	198.62	88.23-309.01
	Downstream intercrystalline brine	+4.0	+3.0- +5.0	+5.9	+5.7- +6.0	This study	2 029.87	1 501.16-2 546.18
Dry season	Upstream river water	-77.0	--	-11.9	--	Li et al. (2007)	110.8	76.0-145.6
	Midstream groundwater	-56.8	-64.0- -45.0	-8.70	-9.60- -4.50	This study	206.04	0.89-424.0
	Midstream river water	-53.1	--	-7.32	--	Wei et al. (1983) Tan et al. (2012)	214.00	162.4-279.2
	Downstream salt lake brine	-6.0	--	+9.0	--	This study	27.52	-
	Downstream intercrystalline brine	-12.3	-20.0- -6.0	+7.1	+4.3- +9.6	This study	8.12	0.48-23.4
"--" indicates not available.

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In the dry season, the average δD values were -77.0‰, -53.1‰, -6.0‰ for the river water of the upstream and midstream NLGL River and salt lake brine, respectively; and the corresponding average δD values were -11.9‰, -7.32‰, and +9.0‰ for δ¹⁸O, respectively (Table 2). The average δD values were -56.8‰ and -12.3‰ for the groundwater and intercrystalline brine of the midstream NLGL River, respectively; and the corresponding average δ¹⁸O values were -8.7‰ and +7.1‰, respectively (Table 2).

2.3 ²²²Rn Concentrations in the River Water and Groundwater

In the wet season, the concentration of ²²²Rn ranged 22.50–450.99, 194.34–2 600.0, and 88.23–309.01 Bq/L for the upstream and midstream river water and salt lake brine, with an average of 136.72, 982.73, and 198.62 Bq/L, respectively (Table 2). The concentration of ²²²Rn ranged 20.76–3 975.0 and 1 501.16–2 546.18 Bq/L in the midstream groundwater and intercrystalline brine, with average concentration of 1 641.12 and 2 029.87 Bq/L, respectively (Table 2).

In the dry season, the concentration of ²²²Rn ranged 76.00–145.60, 162.40–279.20, and 0–27.52 Bq/L the upstream and midstream river water and salt lake brine, with an average of 110.80, 214.00, and 27.52 Bq/L, respectively (Table 2). The concentration of ²²²Rn ranged 0.89–424.00 and 0.48–23.40 Bq/L in the midstream groundwater and intercrystalline brine, with an average value of 206.04 and 8.12 Bq/L, respectively (Table 2).

3. DISCUSSIONS

3.1 River Water and Groundwater Interactions in the NLGL River Catchment

The δD and δ¹⁸O isotopic compositions of the river water and groundwater in the upstream and midstream of this study followed the global meteoric water line (abbreviated as GWML: δ²H = 8δ¹⁸O + 10) (Craig, 1961) and local meteoric water line (abbreviated as LMWL: δ²H = 7.86δ¹⁸O + 11.05) (Zhao et al., 2018; Xu et al., 2017) (Fig.2). Such consistency suggested that the mountain precipitation and snow melt water were the recharge sources of the NLGL River. Moreover, the upstream river water, midstream surface water and groundwater were highly mixed (Fig. 2), while the downstream samples were plotted at the lower right of the LMWL, indicating the characteristics of residual water after secondary evaporation (Gu et al., 2011).

Figure 2. The δ²H-δ¹⁸O relationship of different waters of the NLGL River catchment from upstream to downstream in wet and dry seasons.

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The initial water is considered as the intersection of the Nalenggele local evaporation line (abbreviated as NLEL) and the local meteoric water line (abbreviated as LMWL), and the residual water refers to the water left after evaporation from atmospheric precipitation (Gu et al., 2011; Clark and Fritz, 1997). The NLEL was obtained by fitting the initial water and residual water samples using the least square method. The NLEL was greatly different between the wet and dry seasons, with slopes 4.68 and 2.93, respectively (Fig. 2). The slopes of the evaporation lines in Fig. 2 showed the evaporation intensity in the dry season is stronger than in the wet season. The samples from salt lake plain showed small variation of δ¹⁸O values (ranging +4.3‰– +9.6‰) between the wet and dry seasons, but the δD values in the wet season were higher than in the dry season (Fig. 2), which is related to the water from liquid phase to gaseous phase during evaporation. It is reported that "light water" (¹H₂¹⁶O) evaporates preferentially than "heavy water" (¹H₂¹⁸O, ²H₂¹⁶O, ²H₂¹⁸O), resulting in the enrichment of ²H and ¹⁸O in water (Gu et al., 2011). In this study, the temperature of salt lake plain in summer is higher (max: 35.3 ℃) than in winter (min: -29.5 ℃), which easily leads to the escape of "light water" in summer, thus enriching "heavy water" in brine or intercrystalline brine. Therefore, the evaporation intensity is actually stronger in summer (wet season) than in winter.

There were two obvious water exchanges between groundwater and river water from the upstream to downstream of the NLGL River catchment, as indicated in Fig. 3. At the distance about 53 km, most groundwater samples and a few of river water samples showed a high concentration of ²²²Rn, indicating that river water interacted strongly with groundwater in the overflowing region (alluvial fan I); from 110 to 180 km, there was also water interaction between river brine and intercrystalline brine (underground; Fig. 3).

Figure 3. The ²²²Rn concentration of the studied samples collected in wet season (a) and dry season (b).

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The difference of ²²²Rn concentration indicated that the water exchange was different in the water samples between wet and dry seasons (Fig. 3). In the wet season, most of the groundwater samples in overflowing region and intercrystalline brine samples had high concentration of ²²²Rn in salt lake plain, suggesting that water recharge was obvious in salt lake plain (Fig. 3a). In contrast, in the dry season, the concentration of ²²²Rn in most of the surface water and groundwater samples from midstream was higher than that in the salt lake plain (Fig. 3b), suggesting that there was no obvious water drainage in the salt lake plain.

Along the NLGL River, river water and groundwater had quite distinct concentration of ²²²Rn. River water had low concentration of ²²²Rn (22.50–450.99 Bq/L, with an average of 136.72 Bq/L), which was considered as background concentration of ²²²Rn in natural river water in the NLGL catchment. However, at the distance about 53 km, the ²²²Rn concentration of both river water and groundwater increased (194.34–2 600.0 and 20.76–3 975.0 Bq/L, with an average value of 982.73 and 1641.12 Bq/L, respectively) (Fig. 3a). The ²²²Rn concentration of the groundwater and river water in the midstream was much higher than that of the upstream of the NLGL River, indicating that the midstream river water mainly originated from groundwater discharge. At the distance of about 130 km, the ²²²Rn concentration of the river water (salt lake brine) and groundwater (intercrystalline brine) ranged 88.23–309.01 and 1 501.16– 2 546.18 Bq/L, with an average of 198.62 and 2 029.87 Bq/L, respectively. The ²²²Rn concentration of the salt lake brine was similar to that of the upstream NLGL River, indicating that the gas exchange with the atmosphere led to the low ²²²Rn concentration in the salt lake brine. Previous studies showed that sinks of ²²²Rn in the river water included decay (half-life of ²²²Rn: 3.8 days) and atmospheric losses (Oh et al., 2021; Zhao et al., 2018; Ellins et al., 1990). The ²²²Rn concentration of the intercrystalline brine was about fifteen times higher than the background concentration in the river, suggesting that the midstream groundwater was discharged into intercrystalline brine in the downstream through the flow path. Our field investigation showed that the original source of the upstream NLGL River is atmospheric precipitation or snow melt water from the Kunlun Mountains, and the spring water at the root of alluvial fan I. Moreover, the NLGL River maintains continuous flow during the wet season. Therefore, the river infiltration recharge and groundwater recharge may lead to the high concentration of ²²²Rn in the intercrystalline brine.

In contrast with the wet season, the ²²²Rn concentration in the dry season (110.80 Bq/L) may be regarded as the background concentration. In the midstream, the ²²²Rn concentration of river water and groundwater ranged 162.40–279.20 and 0.89–424.00 Bq/L, with an average of 214.00 and 206.04 Bq/L, respectively, indicating that a large amount of river water was recharged into the groundwater, or no obvious groundwater was discharged into river water. Field investigation showed the number of springs in the alluvial fan I was significantly reduced in the dry season (Fig. 3b). In the downstream, the ²²²Rn concentration of the salt lake brine and intercrystalline brine ranged 27.52 (one sample) and 0.48–23.40 Bq/L, with an average of 27.52 and 8.12 Bq/L, respectively. The concentration of ²²²Rn in the downstream samples was about several to hundred times lower than that of the downstream in the wet season, and about several to ten times lower than that of the background concentration in the dry season, suggesting that the recharge of surface water and groundwater from the midstream to the downstream is very limited.

3.2 Quantity of River Water and Groundwater Inflow to the DXTSL

The ²²²Rn is an inert radioisotope derived from the ²²⁶Ra decay process in aquifers (Cook et al., 2003). In general, groundwater and surface water are frequently exchanged when the river water from mountains area is recharged into the basin. In this process, the ²²²Rn concentration in the river water was also changed. The ²²²Rn concentration in groundwater is much higher than in river water. Most of ²²²Rn in river water comes from groundwater recharge, and its concentration is limited by riverbed sediments, which is insignificant and often neglected (Dimova et al., 2013; Wu et al., 2004; Cook et al., 2003). When groundwater is discharged into river water, the ²²²Rn concentration in the river water increases significantly, but it decreases repidly because of radioactive decay (from ²²⁶Ra to ²²²Rn) and atmospheric loss (Ellins et al., 1990). Based on the ²²²Rn isotope characteristics and its concentration, the exchange flux between groundwater and river water can be identified. To estimate the groundwater flow discharged into the NLGL River, a model based on ²²²Rn mass balance was constructed in the reach between the river sampling sites in the midstream and downstream of the NLGL River according to the ²²²Rn mass conservation theory. In the model, the gas exchange and radioactive decay of ²²²Rn in river and groundwater discharge were taken into account. The model can be expressed as follows (Su et al., 2015; Xu, 2015): q_r and q_g represented surface water infiltration and groundwater recharge rates, respectively (m³/(s·m)); α is ²²²Rn loss coefficient caused by both radioactive decay and gas exchange, and it was explained by surface renewal theory for the gas exchange part (Su et al., 2015; Stellato et al., 2008; Cook et al., 2006); L is the distance between two sampling sites (m), which measured from GoogleEarth; C_d: concentration of ²²²Rn in river water at downstream section (Bq/L); C_u: concentration of ²²²Rn in river water at upstream section (Bq/L); C_g: concentration of ²²²Rn in the groundwater (Bq/L); Q_d: river flow at downstream section (m³/s); Q_u: river flow at upstream section (m³/s); v was the average stream velocity between two sampling sites (m/s), which was measured by portable flow rate meter (LS1206B); h was the stream depth (m), which was measured by portable sounders; λ was ²²²Rn radioactive decay coefficient (2.08 × 10^-6 s^-1); D was radon molecular diffusivity (cm²/s), -logD=(980/T) + 1.59, and T was absolute water temperature (K) (Peng et al., 1974). All the parameters (v, h, L, W. The "W" means the width (m) of the river, which was measured by a diastimeter) of the sections were manually measured. Thus the groundwater recharge and its proportion in surface water infiltration can be calculated by solving the equation (Zhao et al., 2018). For calculation, D was calculated to be 1.32 × 10^-5 and 7.76 × 10^-6 cm²/s at 298.15 and 278.15 K (5 ℃) in the wet and dry season, respectively; α was calculated from Eq. (1) in the wet and dry season, respectively.

$\alpha =\frac{\lambda }{v}+\frac{{D}^{0.5}}{{v}^{0.5}· {h}^{1.5}}$

(1)

${q}_{r}=\frac{{C}_{d}{Q}_{d}–{C}_{u}{e}^{(-\alpha L)}{Q}_{u}}{{C}_{u}}· \frac{\alpha }{{e}^{(-\alpha L)}–\mathrm{ }1}$

(2)

${q}_{r}=\frac{2\alpha ({C}_{d}{Q}_{d}–{C}_{u}{Q}_{u}{e}^{-\alpha L})}{\left(1\mathrm{ }–{e}^{-\alpha L}\right)(2{C}_{g}–{C}_{u}–{C}_{d})}–\frac{2{C}_{g}({Q}_{d}–{Q}_{u})}{L(2{C}_{g}–{C}_{u}–{C}_{d})}$

(3)

${q}_{g}=\frac{2\alpha ({C}_{d}{Q}_{d}–{C}_{u}{Q}_{u}{e}^{-\alpha L})}{\left(1\mathrm{ }–{e}^{-\alpha L}\right)(2{C}_{g}–{C}_{u}–{C}_{d})}–\frac{({C}_{u}+{C}_{d})({Q}_{d}–{Q}_{u})}{L(2{C}_{g}–{C}_{u}–{C}_{d})}$

(4)

${q}_{g}=\frac{{C}_{d}{Q}_{d}–{C}_{u}{e}^{(-\alpha L)}{Q}_{u}}{{C}_{g}}· \frac{\alpha }{1\mathrm{ }–{e}^{(-\alpha L)}}$

(5)

The water exchange between river water and groundwater can be calculated respectively according to the following three cases (Su et al., 2015): (1) C_d< C_u and Q_d< Q_u indicate that river water is recharged into groundwater, and thus Eq. (2) should be employed; (2) C_d > C_u and Q_d < Q_u indicate that these two water exchange processes occurred simultaneously, that is, groundwater discharged into surface water, and river water was recharged into groundwater, and thus Eqs. (3) or (4) should be used; (3) C_d > C_u, Q_d > Q_u indicate that groundwater is discharged into surface water, and thus Eq. (5) should be used. The ²²²Rn mass balance method is usually applicable when the values of C_d, C_u, Q_d and Q_u exhibited great difference with each other. However, when they show less difference, it is necessary to choose reasonable formula (Li, 2020).

The field monitoring data was presented in Table S1. In the wet season, in the upstream, C_d < C_u and Q_d < Q_u. However, field investigation revealed that spring water and fracture water in bedrock were discharged into river water, meaning that river water exchanged with groundwater in this section. Eqs. (3) and (4) showed that the resulting surface water infiltration and groundwater discharge rates were 2.86×10^-3 and 1.15×10^-3 m³/(s·m), respectively. This surface water infiltration rate was consistent with the water balance theory (Xu, 2015). Accordingly, the recharge flux (Flux(river water) = q_r × L and Flux(groundwater) = q_g × L) of river water and groundwater at the distance (< 53 km) were 151.58 and 60.95 m³/s, respectively. In the midstream (C_d > C_u and Q_d < Q_u), groundwater discharged into the river, and river water was recharged into groundwater, which was ever reported in the same river section (Su et al., 2015). So based on Eqs. (3) and (4), the surface water infiltration and groundwater recharge rates were 1.63×10^-2 and 1.53×10^-2 m³/(s·m), and the corresponding recharge fluxes were 358.6 and 336.6 m³/s, respectively. These calculated water exchange rates were consistent with previous studies based on pumping experiments in the same region (Chen et al., 2018; Rong et al., 2002). In the downstream, C_d < C_u, Q_d < Q_u. Salt lake brine and intercrystlline brine exchanged in different seasons. So Eqs. (3) and (4) were employed for calculating recharge rates. The resulting surface water infiltration and groundwater recharge rates were 2.83×10^-4 and 6.82×10^-5 m³/(s·m), respectively; and the corresponding recharge fluxes of the river water and groundwater were 16.98 and 4.09 m³/s, respectively.

In the dry season, C_d < C_u and Q_d < Q_u were shown in the upstream, while the ²²²Rn concentration of river water was higher than that of groundwater, meaning that groundwater was discharged into river water. So Eqs. (3) and (4) were used for the calculation of recharge rates. The resulting q_r and q_g values were 9.81×10^-4 and 5.05×10^-4 m³/(s·m), respectively; and the corresponding recharge fluxes were 51.99 and 26.77 m³/s, respectively. In the midstream, C_d > C_u and Q_d < Q_u, Eqs. (3) and (4) were used for the calculation of recharge rates, with the production of q_r and q_g being 8.34 × 10^-3 and 7.78 × 10^-3 m³/(s·m), respectively; the corresponding recharge fluxes of the river water and groundwater were 183.48 and 171.16 m³/s, respectively (Table S1). However, in the downstream, river water disappeared and the water exchange rate was considered as zero. The concept map of the water exchange was shown in Fig. 4.

Figure 4. The quantification of the interaction between surface water and groundwater in wet season (a) and dry season (b).

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In summary, the intensity of exchange between surface water and groundwater varies greatly between wet and dry seasons, which is manifested in strong water exchange in wet season and weak water exchange in dry season. This can be attributed to the changing runoff of NLGL River. In the wet season, the runoff increase of NLGL River increases the runoff area, resulting in a significant increase in river recharge, especially in the extensively developed alluvial fan zone composed of sand. The increase of river recharge leads to an increase in the discharge of groundwater systems such as springs and lakes. One previous study has also shown that the increase of watershed runoff leads to a significant increase in infiltration recharge and groundwater discharge (Xiao et al., 2017). In addition, the obvious difference of water exchange between wet and dry seasons may also be related to the circulation of groundwater. Due to the rise of groundwater level during the wet season, the overflow area of groundwater in the alluvial fans I and II extends to the fan root, increasing the area of overflow zone and thus promoting the local circulating water flow. In contrast, the reduction of river runoff during dry season decreases the river recharge and groundwater level, resulting in the weakening of local circulating water flow, so the water exchange between surface water and groundwater is significantly reduced. Therefore, the river runoff and groundwater circulation have important impacts on the water exchange between surface water, groundwater and salt lake brine, which should be paid special attention when regulating the water resources of the river basin or assessing water-salt balance.

3.3 The Influence of Brine Concentration and Brine Crystallization

The interaction between river water and groundwater had great effects on the brine concentration. Although the recharge rates of river water and groundwater in the wet season was much higher than that in the dry season, the brine concentration (especially Na⁺, K⁺, Mg²⁺, CO₃^2-, Cl^- and TDS) in the wet season was still higher than that in the dry season (Fig. 5a). This finding may be due to the large surface area of the lake and its evaporation in summer is higher than in winter. Previous studies showed that the larger the water surface area of a lake, the higher its evaporation in summer (Han et al., 2020). In addition, high ion concentration in summer indicates that there may be ionic dissolution of salt minerals in the studied area. The concentrations of most elements (except CO₃^2-) in the DXTSL brine in dry season were higher than in wet season (Fig. 5b), suggesting water supply was limited in winter. In wet season, the contents of TDS and K⁺ in brine were basically similar to those in dry season, but the content of Mg²⁺ in brine is significantly increased in wet season. This situation led to a high ratio of Mg²⁺/Li⁺, which is not conducive to the separation and extraction of lithium from brine (Zhao et al., 2020). In contrast with surface water (yahu lake (Fig. 5a) and salt lake brine (Fig. 5b)), the intercrystalline brine (> 1.2 m) may not be affected by evaporation, but only by river water and groundwater recharge (Fig. 5c). In contrast in the dry season, the contents of Na⁺, Cl^- and TDS of the intercrystalline brine were similar to that in the wet season (Fig. 5c), while the contents of Mg²⁺, SO₄^2- and HCO₃^- decreased. This situation resulted in a low ratio of Mg²⁺/Li⁺, which is conducive to the separation and extraction of lithium from intercrystalline brine.

Figure 5. Comparison of ion concentration of the studied water samples. (a) Yahu lake; (b) salt lake brine; (c) intercrystalline brine in wet season and dry season.

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In salt lake chemical industry, potassium fertilizers were produced through crystallization of original intercrystalline brine. The crystallization sequence of brine is usually the evaporation from initial mineral (mirabilite), intermediate mineral (sodium salt) to terminal mineral (sylvine) (Zhang, 1987). The crystallization path of DXTSL brine is as follows: mirabilite, hydrohalite, halite, sylvinite, epsom salt, hexahydrite, carnallite, bischofite and lithium salt (Wen et al., 2011). The phase diagram of Na⁺, K⁺, Mg²⁺//Cl^-, SO₄^2--H₂O (25 ℃) revealed that most samples in the wet season were in the stage of 3K₂SO₄·Na₂SO₄, while most samples in the dry season were in the KCl stage, suggesting that water supply in the wet season had great influences on the crystallization sequence of salt minerals (Supplementary Fig. S2).

In summary, the interaction between river water and groundwater in wet and dry seasons will significantly affect brine concentration and crystallization sequence. Comparatively, in dry season, the ionic conditions (e.g., suitable brine concentration, in the KCl mineral phase) of the brine were suitable for extraction of LiCl and KCl.

4. CONCLUSION

Interactions between the surface water (river water and lake brine) and groundwater (groundwater and intercrystalline brine) were significantly different between dry and wet seasons in the NLGL River catchment. In wet season, the river water and groundwater from midstream recharged the intercrystalline brine, while no obvious water from midstream was recharged into salt lake plain in dry season. Such strong water exchange in wet season influenced the brine concentration and intercrystalline process in DXTSL. Seasonal variations of water supply had great influences on the crystallization sequence of salt minerals, making the chemistry of the DXTSL water be in the 3K₂SO₄·Na₂SO₄ and KCl stage in wet and dry seasons, respectively. The condition of recharge rate in the dry season was beneficial for water-salt balance and utilization of salt minerals in DXTSL. In addition, the intercrystalline brine of DXTSL contained low concentration of Mg²⁺, SO₄^2- and HCO₃^- and low ratio of Mg²⁺/Li⁺ in dry season, which was beneficial for separation of lithium. This study demonstrated that the combination of various tracers is helpful to make rational utilization of water resource and reveal the water-salt balance in salt lake area and other salt lake areas.

ACKNOWLEDGMENTS: The authors would like to thank the editors and anonymous reviewers for their helpful comments, which improved the quality of the final manuscript. This study was supported by the Key Deployment projects of the Chinese academy of sciences (No. ZDRW-ZS-2020-3), the Funds for the Qinghai Province (Nos. 2020-ZJ-932Q; 2020-ZJ-732), the National Natural Science Foundation of China (No. 42007169), the "Western Light" of Chinese Academy of Sciences, the Fourth Batch of Qinghai Province "Thousand Talents Program for High-end Innovative Talents" (No. 2020000051) and supported by the Second Tibetan Plateau Scientific Expedition and Research Program (No. 2019QZKK0805). The final publication is available at Springer via https://doi.org/10.1007/s12583-022-1731-0.

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