Hydrogeology Journal

https://doi.org/10.1007/s10040-018-1763-9

PAPER

Influences of groundwater extraction on flow dynamics

and arsenic levels in the western Hetao Basin, Inner Mongolia, China
Zhuo Zhang 1,2 & Huaming Guo 1,2 & Weiguang Zhao 2 & Shuai Liu 2 & Yongsheng Cao 2 & Yongfeng Jia 2

Received: 16 November 2017 / Accepted: 15 March 2018

# Springer-Verlag GmbH Germany, part of Springer Nature 2018

Abstract
Data on spatiotemporal variations in groundwater levels are crucial for understanding arsenic (As) behavior and dynamics in
groundwater systems. Little is known about the influences of groundwater extraction on the transport and mobilization of As in
the Hetao Basin, Inner Mongolia (China), so groundwater levels were recorded in five monitoring wells from 2011 to 2016 and in
57 irrigation wells and two multilevel wells in 2016. Results showed that groundwater level in the groundwater irrigation area had
two troughs each year, induced by extensive groundwater extraction, while groundwater levels in the river-diverted (Yellow
River) water irrigation area had two peaks each year, resulting from surface-water irrigation. From 2011 to 2016, groundwater
levels in the groundwater irrigation area presented a decreasing trend due to the overextraction. Groundwater samples were taken
for geochemical analysis each year in July from 2011 to 2016. Increasing trends were observed in groundwater total dissolved
solids (TDS) and As. Owing to the reverse groundwater flow direction, the Shahai Lake acts as a new groundwater recharge
source. Lake water had flushed the near-surface sediments, which contain abundant soluble components, and increased ground-
water salinity. In addition, groundwater extraction induced strong downward hydraulic gradients, which led to leakage recharge
from shallow high-TDS groundwater to the deep semiconfined aquifer. The most plausible explanation for similar variations
among As, Fe(II) and total organic carbon (TOC) concentrations is the expected dissimilatory reduction of Fe(III) oxyhydroxides.

Keywords Arsenic . Groundwater extraction . Spatiotemporal trends . Salinization . China

Introduction and Kinniburgh 2002). Reducing aquifers that host high-As

High concentrations of arsenic (As) have been found in
groundwater worldwide (Ravenscroft et al. 2009), and occur
under both oxic conditions and reducing conditions (Smedley
Published in the special issue BGroundwater sustainability in fast-
developing China^
Electronic supplementary material The online version of this article
(https://doi.org/10.1007/s10040-018-1763-9) contains supplementary
material, which is available to authorized users.
* Huaming Guo
hmguo@cugb.edu.cn
1
State Key Laboratory of Biogeology and Environmental Geology,
China University of Geosciences, Beijing 100083, People’s Republic
of China
2 phologic characteristics and superimposing anthropogenic ef-
MOE Key Laboratory of Groundwater Circulation & Environment
Evolution & School of Water Resources and Environment, China
University of Geosciences (Beijing), Beijing 100083, People’s
Republic of China
groundwater have been reported in various river deltas
(including deltas of the Ganges, Mekong, and Red River in
Asia, and Pearl River, Yangtze River and Yellow River in
China; Polizzotto et al. 2008; Eiche et al. 2008; Norrman
et al. 2008; Fendorf et al. 2010; Radloff et al. 2011; Wang
et al. 2012; Guo et al. 2014a; Erban et al. 2014; Stuckey
et al. 2016) and inland basins (including the Datong basin,
Hetao basin, west Songnen basin, Yinchuan basin, and
Zhunger basin in China, and the Pannonian basin and
Danube basin in Europe; Luo et al. 2012; Guo et al. 2003,
2014a, b, c; Rowland et al. 2011; Ujević et al. 2010). It is well
known that reductive dissolution of Fe(III) oxyhydroxides
leads to As release from aquifer sediments under anoxic con-
ditions (Islam et al. 2004; Mladenov et al. 2009; Fendorf et al.
2010; Guo et al. 2013a, b), which depends in turn on the
quality and quantity of available organic matter, local geomor-
fects (Harvey et al. 2002, 2006; Neumann et al. 2010; Lawson
et al. 2013; Neidhardt et al. 2013; Desbarats et al. 2014;
Schaefer et al. 2016; Postma et al. 2016).

Many studies have been done concerning the effects of
groundwater extraction on groundwater As in river deltas. In
the Bengal Basin (India and Bangladesh), around 10 million
irrigation and potable-water wells had been installed during the
past four decades (Harvey et al. 2005). At a site in Bangladesh,
the recharge from surface water, induced by intensive ground-
water extraction, which can be rich in labile organic matter, was
thought to cause the release of As by fueling reductive dissolu-
tion of Fe(III) oxyhydroxides (Harvey et al. 2002); however, in
the Yangtze River Basin, owing to extensive groundwater ex-
traction in the dry season, the surface water seasonally supplied
oxidizing water to the anoxic aquifer, which promoted a transient
drop in As concentrations (Schaefer et al. 2016). Massive extrac-
tion of deep groundwater also created local depression cones in
the aquifers in the Bengal Basin, causing subsequent drawdown
of As-rich shallow groundwater into deep pumping wells
(Michael et al. 2009; Burgess et al. 2010). In addition, Stahl
et al. (2016) showed that the Hanoi (Vietnam) aquifers adjacent
to the Red River were susceptible to further As contamination
where riverine recharge is drawn into aquifers by extensive
groundwater pumping, with the water flowing through recently
deposited river sediments before entering the aquifer. Hence,
diverse temporal changes in As concentrations have been attrib-
uted to variations in local groundwater flow patterns caused by
excessive water extraction in river deltas; however, few studies
have been carried to investigate the response of As concentra-
tions to variations in groundwater flow patterns in inland basins.
The Hetao basin is a typical inland basin in northwest
China, where the prevalence of endemic arsenicosis was up
to 25% of the population in 2002 (Jin et al. 2003). There are
more than 5,000 deep wells that extract groundwater for irri-
gation and drinking at the mountain fronts along the margin of
the basin (Guo et al. 2016a). Among these deep wells, ground-
water As concentration has been found up to 390 μg/L (Jia
et al. 2017). Dissimilatory and bacterial sulfate reduction
(BSR)-induced reduction of Fe(III) oxides were demonstrated
to be the important mechanisms for As mobilization based on
Fe and S isotope signatures (Guo et al. 2013a, b, 2016b), and
hydrogeological and biogeochemical investigation (Guo et al.
2011; Jia et al. 2017).
Nevertheless, little is known regarding the influences of
groundwater extraction on groundwater flow dynamics and As
distribution in the Hetao basin, although reverse variation pat-
terns of shallow groundwater levels are observed in the ground-
water irrigation area (GIA) and diverted Yellow River water
irrigation area (YIA; Guo et al. 2013a, b). Owing to the flat
topography, extremely low flow rates provoke a high vulnerabil-
ity toward the effects of groundwater extraction, which can lead
to severe disturbances of the naturally established hydrochemical
conditions and possibly As distribution. Therefore, it is crucial to
characterize the relationship between temporal variations in
groundwater flow pattern and groundwater chemistry and to
understand the effects of groundwater extraction on groundwater
Hydrogeol J
As dynamics for developing effective strategies for sustainable
usage of low-As groundwater in As-affected areas.
The objectives of this study are to (1) investigate the spa-
tiotemporal variations of groundwater levels at the mountain
fronts that are subject to intensive groundwater extraction, (2)
characterize temporal trends in groundwater chemistry and As
concentration on an interannual time scale, and (3) evaluate
the influences of groundwater extraction on groundwater As
distribution.
Materials and methods
The study area
The Hetao basin, as one of the Cenozoic rift basins, is located
between Yinshan uplift and Erdos platform in western Inner
Mongolia. Active faults, inactive faults and insidious faults
bound the northwest, the east, and the south of the basin,
respectively. The Langshan Mountains, to the north of the
basin, are mainly composed of Mesoproterozoic deeply meta-
morphic rocks and intrusive rocks and Jurassic to Cretaceous
metamorphic rocks. The basin is a SW–NE tilting flat plain,
with increasing sediment thickness from 500 to 1,500 m in the
east to 4,000–8,000 m in the west. The basin, located in an
arid-semiarid climate zone, has an average annual precipita-
tion of 130–220 mm (mainly during July to September) and
annual evaporation rate of about 2,000–2,500 mm (Guo et al.
2008a).
The study area is located in the northwest of the Hetao
basin with ground elevations between 980 and 1,050 m
above sea level (asl), including alluvial fans and a flat plain
(Fig. 1b). Pluvial sediments occurring in the alluvial fans
are normally composed of gravel, coarse sand, and medium
sand, while fluvial and lacustrine sediments mainly ob-
served in the flat plain consist of Quaternary silt and fine
sand. Groundwater mainly occurs in the Quaternary alluvi-
al, alluvial-pluvial, and alluvial-lacustrine aquifers (Guo
et al. 2008a). The alluvial-pluvial unconfined aquifers are
generally observed in the belt of alluvial fans, while fluvial-
lacustrine leaky-confined aquifers are common in the flat
plain. According to borehole logs and a previous
hydrogeologic report (Inner Mongolia Institute of
Hydrogeology 1982), shallow groundwater is considered
to be hosted in aquifers overlying the clay layers around
40 m below land surface (bls), while aquifers underlying
the clay layers, being regarded as semiconfined, host deep
groundwater.
The groundwater level generally rises from around 20 m
below land surface (bls) in the alluvial fans to around 2.0 m bls
in the flat plain for both shallow groundwater and deep
groundwater. Groundwater is mainly recharged by fracture
water along the mountain front in the alluvial fans, and by
Hydrogeol J

E107° E108° E109°

(a)
Wulatehouqi Wuyuan

N41°0'
Hangjinhouqi
GIA Linhe N

(b) 0 15 30 60km
N40°30'
Lake Flat plain City/county
Dengkou Yellow River Alluvial fans Irrigation channel
Desert Alluvial fan plain Drainage channel
Steep massif Tectonic terrace The study area
I22 I21
I20 Hetao basin
Russia
Kazakhstan
K2

a
zone I

re
I5
(b) lia

Ko
Kyrgyzstan go
on

rth
I10 Tajikistan M

No
I9 Inner

tan n
Beijing

kis sta

So
uth
Pa hani
I3 China

Ko
g
Af

rea
N
ep
I1
YIA

al
Bhutan
K1

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nma
Bangladesh
India
zone II

Mya
I14

Vi
Laos
etn
1-3 I15

am
5-2
Shahai Lake 2-4
Drainage channel
Boundary of zones
3-4
Spring water
Surface
water Lake water
Diverted Yellow River water 4-5
Continuous sampling well
of groundwater (n=10)
Regular monitoring well of N
groundwater level(n=57)
Irrigation
well @2011(n=80) @2014(n=25)
@2012(n=16) @2015(n=29)
@2013(n=13) @2016(n=18) 1km
Multilevel well (n=2)
Long-term monitoring well of
groundwater level (n=5)
Fig. 1 Locations of a the study area and b the sampling sites. GIA means the groundwater irrigation area and YIA is the diverted Yellow River water
irrigation area

vertically infiltrating precipitation, ditch water (irrigation
channels), and irrigation water in the flat plain, and discharged
mainly via evapotranspiration, drainage, and extraction. As a
natural boundary between the two geomorphic units (the pied-
mont alluvial plain in the north and the alluvial lacustrine plain
in the south), the drainage channel is regarded as the discharge
route of shallow groundwater, where groundwater flows from
the piedmont area in the north and from the flat plain in the
south (Zhang et al. 2013). The general direction of groundwa-
ter flow is from the alluvial fans, through the transition area, to
the flat plain, but the flow rate has been recorded as relatively
slow, with the range between 0.002 and 0.2 m/day due to the
gentle topography and low permeability of the aquifer sedi-
ments (Inner Mongolia Institute of Hydrogeology 1982).
For more than 50 years, the diverted water from the Yellow
River has been predominately used for agricultural irrigation
in the basin (Guo et al. 2011). Since the diverted Yellow River
water is unavailable near the mountains due to the high eleva-
tion and overuse of the water in the upstream of the irrigation
channels, groundwater has recently been used for both irriga-
tion and drinking to the north of the drainage channel. Reverse
variation patterns of groundwater levels are observed in GIA
and YIA (Guo et al. 2013a, b). During irrigation seasons, high
groundwater levels occur in YIA, while low levels occur in
GIA; therefore, irrigation activities, including the overextrac-
tion of groundwater and the diverted Yellow River water irri-
gation, may change groundwater flow patterns and potentially
affect the chemistry of groundwater.

According to monitoring data of groundwater levels/heads
in GIA in this study, the GIA may be divided into two zones:
the northwestern groundwater recharge area (zone I) near the
piedmont, and the southeastern surface water recharge area
(zone II) close to the Shahai Lake. During irrigation seasons,
groundwater flows from northwest to southeast in zone I,
while it flows from southeast to northwest in zone II.
Monitoring of groundwater levels
Five monitoring wells were installed in Shahai town; two of
them were located in GIA (Nos. 1-3 and 5-2) and three in YIA
(Nos. 2-4, 3-4, and 4-5; Fig. 1b). Groundwater levels were
monitored every 30 min from 2011 to 2016 using water level
data loggers (HOBO U20, Onset) and local atmospheric pres-
sure was also monitored in the same way. Water levels of the
Shahai Lake were monitored every 30 min from May 2016 to
May 2017. Groundwater heads of 45 irrigation wells (Fig. 1b)
were measured using an electronic water sensor (Model 101B,
Solinst) in July 2016 (irrigation season), while water heads of
57 irrigation wells were measured in October 2016 and
March 2017 which are in the nonirrigation seasons; addition-
ally, two multilevel wells (Nos. K1 and K2) were installed in
zone II and zone I, respectively. Each multilevel well had
seven piezometers at seven different depths. Piezometers
No. K2-3 (41 m) and No. K2-6 (65 m) in zone I, and No.
K1-3 (38 m) and No. K1-6 (74 m) in zone II, were selected
to regularly measure groundwater levels/heads of shallow
groundwater and deep groundwater, in April 2016,
May 2016, August 2016, November 2016 and March 2017.
The real-time kinematic difference global positioning system
(RTK-GPS) was used to measure the elevations of all well
heads and to calibrate water level/head depth measurements
to water level/head elevations above mean sea level (amsl).
Sample collection and analysis
Groundwater samples were collected in 2011 (n = 80), 2012
(n = 16), 2013 (n = 13), 2014 (n = 25), 2015 (n = 29), and
2016 (n = 18) from irrigation wells (in GIA), and yearly from
two monitoring wells (in YIA) from 2012 to 2015 (Fig. 1b). In
particular, from the piedmont area to the Shahai Lake, ground-
water samples of 10 typical irrigation wells (five wells: Nos. I22,
I21, I20, I5 and I9 in zone I; five wells: Nos. I10, I3, I1, I14 and
I15 in zone II, in GIA) were collected yearly from 2011 to 2016.
The depths of these irrigation wells mostly ranged between 60
and 110 m. The monitoring wells have depths of around 20 m
bls. In addition, spring water, Shahai Lake water and diverted
Yellow River water were collected in July 2016 (Fig. 1b).
Before groundwater sampling, wells were pumped at least
20 min until water temperature, EC, pH, and Eh kept stable.
All samples were filtered through 0.22-μm membrane filters
in the field. Water samples for major cation and trace element
Hydrogeol J
analysis were acidified with ultrapure 6 M HNO3 to pH <2.0.
Those for analysis of As species were preserved with 0.25 M
EDTA in amber bottles. Samples for anion analysis were fil-
tered but unacidified. All samples were kept and transported to
the laboratory at 4 °C, and kept in a refrigerator at 4 °C.
At the time of sampling, parameters including water tem-
perature, EC, pH, and Eh were measured using a multiparam-
eter portable meter (HI9828, HANNA), while Fe(II) concen-
tration was determined by using a portable spectrophotometer
(DR2800, HACH) and alkalinity using a Model 16,900 digital
titrator (HACH) using bromocresol green-methyl red indica-
tor. Eh readings were normalized with reference to a hydrogen
electrode.
Concentrations of major cations and trace elements were
determined by ICP-AES and ICP-MS, respectively. The ana-
lytical precision of ICP-AES and ICP-MS was 3.0%, whereas
the detection limit for As was 0.01 μg/L. Unacidified aliquots
were analyzed for major anions by ion chromatography (DX-
120, Dionex), with the analytical precision less than 5.0%;
however, for most samples, ion charge imbalances were less
than 5%. Arsenic species in groundwater samples were ana-
lyzed by HPLC-HG-AFS and detection limits of As(III) and
As(V) were 2 and 4 μg/L, respectively.
Results
Variations in groundwater levels/heads
In the study area, groundwater levels/heads fluctuated from
2011 to 2016. During irrigation seasons, groundwater levels/
heads decreased in GIA. Water level elevations in well Nos. 1-
3 and 5-2 declined to the minimum during May and August
(spring irrigation; Fig. 2a), which were caused by the intense
extraction of groundwater for irrigation. As soon as the spring
irrigation ceased, the groundwater level of well No. 1-3 rose
from September to October and then presented a trough in
November, while the groundwater level of well No. 5-2 rose
from September to October and then reached a peak in
November. Generally, the water level elevations in well No.
5-2 were higher than in well No. 1-3 and there were decreas-
ing trends in groundwater levels from 2012 to 2016 in GIA.
In addition to shallow groundwater, deep groundwater
heads were lower in irrigation seasons relative to nonirrigation
seasons. The groundwater levels of piezometer Nos. K1-6 and
K2-6 in August (irrigation season) were around 1,025.5 and
1,023.6 m amsl, respectively, which are around 4–5 m lower
than those in March (nonirrigation season; Fig. 3). It indicated
that groundwater irrigation decreased groundwater levels/
heads in both the shallow aquifer and deep aquifer.
Although water levels/heads varied, higher water levels/
heads were generally observed in zone II than those in zone
I. Groundwater levels/heads of well No. K1 in zone II were
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Fig. 2 Variations of groundwater levels in a YIA and b GIA. Green-shaded area means spring irrigation season and gray-shaded area means winter
irrigation season. Date format is mm/dd/yyyy

higher than those of well No. K2 in zone I of both shallow
groundwater and deep groundwater during April 2016 and
March 2017 (Fig. 3). It indicated that groundwater would flow
from zone II to zone I, which is opposite to the groundwater
flow direction reported before by Zhang et al. (2013).
Water heads of the 57 irrigation wells, which showed that a
depression cone had occurred in GIA in July (Fig. 4a), are
consistent with those of the piezometers. Water heads dropped
2.5 m from the top of the alluvial fans to the depression cone
and 9 m from the Shahai Lake to the depression cone (Fig. 4).
Three months after summer irrigation, an obvious increase in
groundwater levels was observed in GIA, especially in the de-
pression cone with an increase in water levels around 3 m,
which resulted from the recharge of groundwater from both
the piedmont area and the Shahai Lake (Fig. 4b) and the de-
crease in groundwater extraction. Groundwater levels kept a
rising trend during winter due to no irrigation from November
to March (Fig. 4c). Groundwater level elevations in the top of
the alluvial fans increased from 1,026.5 to 1,029 m from
July 2016 to March 2017. The water head difference between

Fig. 3 Variations of groundwater levels/heads in a piezometer Nos. K2-3 and K2-6 in zone I and b piezometer Nos. K1-3 and K1-6 in zone II from GIA.
Green-shaded area means spring irrigation season, and gray-shaded area means winter irrigation season

Fig. 4 Contour maps of groundwater levels/heads of the 57 irrigation wells in GIA in a July 2016, b October 2016, and c March 2017. Yellow solid dots
mean locations of irrigation wells for monitoring groundwater levels
the Shahai Lake and the depression cone reduced to 5 m
(Fig. 4c); therefore, during the spring irrigation, groundwater
mainly flowed from both southeast and the northwest of GIA to
the depression cone, while groundwater flowed to the northeast
after pooling in the depression cone at other times of the year.
In GIA, hydraulic connection between the shallow aquifer
and deep aquifer may exist. Groundwater levels/heads were sim-
ilar in both the shallow aquifer and deep aquifer in nonirrigation
seasons (Fig. 3); however, groundwater heads of the deep
groundwater (Nos. K1-6 and K2-6) declined faster than those
of the shallow groundwater (Nos. K1-3 and K2-3; Fig. 3) in
irrigation seasons, indicating that the hydraulic connection would
be weak. Accordingly, the lower water heads in the deep aquifer
increased hydraulic gradients between the shallow groundwater
and deep groundwater, and therefore recharged from the shallow
groundwater into the deep groundwater in irrigation seasons.
In YIA, the shallow groundwater levels increased during
irrigation seasons. For well Nos. 2-4, 3-4, and 4-5, water level
elevations had two peaks in each year. One peak was observed
in May–August and the other in November, both of which
were caused by the extensive irrigation using the diverted
Yellow River water. A slight decline was observed from
August to October because of the decrease in the recharge of
irrigation water and evaporation. During winter, the shallow
groundwater levels decreased by 2 m, possibly due to strong
evaporation and freezing. There was no obvious interannual
change of water levels in those three wells from 2011 to 2016
(Fig. 2b). A similar trend in water level was observed in the
lake water and well No. 2-4, both of which had two water level
peaks within 1 year. Generally, the lake-water levels were
higher than those of well Nos. 1-3 and 5-2 and lower than those
of well Nos. 3-4 and 4-5 (Fig. 2). The groundwater levels of
well No. 4-5 were generally higher than the other two wells
(Nos. 2-4 and 3-4), indicating that groundwater flow direction
was from the flat plain region to the drainage channel, which is
consistent with the observation of Zhang et al. (2013) in YIA.
Hydrogeol J
Interannual variations in groundwater chemistry
In GIA, the groundwater in zone I was mainly of Ca-HCO3-
SO4 type and did not change over time, while the groundwater
in zone II changed from Na-SO4-HCO3 type and partly Na-
Cl-HCO3 type to Na-Cl-SO4 type from 2011 to 2016 (Fig. 5).
Groundwater in zone I usually had a lower TDS than that in
zone II, which kept relatively stable, with an average value
ranging from 555 to 591 mg/L from 2011 to 2016—Fig. 6;
Table S1 of the electronic supplementary material (ESM);
however, a significantly rising trend in groundwater TDS
was observed in zone II, increasing from 1,024 to 1,715 mg/
L between 2011 and 2016.
Those trends in major ions were also supported by the repre-
sentative 10 irrigation wells. Mean values of TDS of five wells in
zone I kept relatively constant from 2011 to 2016. Similarly,
concentrations of major ions stayed at almost the same level
(Fig. 7). However, there were statistically long-term increasing
trends in TDS for five wells (r > 0.7) in zone II (Table S1 of the
ESM). The largest increase (45%) was observed in well No. I15,
which was nearest to the lake (Fig. 7). Accordingly, concentra-
tions of major ions had obvious increasing trends except for
HCO3−, with the mean values of Ca2+, Na+, Mg2+, SO42− and
Cl− increasing from 114 to 149, 309–396, 66–105, 410–583 and
423–547 mg/L from 2011 to 2016, respectively.
Groundwater in YIA was mainly of Na-Cl-HCO3 type,
which witnessed a slight decrease in TDS within 6 years
(Fig. 5). There were statistically long-term declining trends
of TDS for well Nos. 2-4 and 3-4 from 2012 to 2015 (r =
0.69 and 0.96, respectively). Especially, the decreasing trend
in TDS of well No. 3-4 (12%) was more evident than that of
well No. 2-4 (2.1%). The decrease in groundwater TDS was
undoubtedly accompanied by decreases in some major ions,
mainly Cl−, SO42− and Na+ (12, 0.8 and 2.7% for well No. 2-4;
19.6, 37.3 and 9.7% for well No. 2-4, respectively; Fig. 7;
Table S1 of the ESM). In addition, the spring water was of
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Fig. 5 Piper plot of groundwater

and surface-water samples in the
study area

Fig. 6 Contour maps of groundwater total dissolved solids (TDS) in GIA in a 2011 (n = 80), b 2012 (n = 16), c 2013 (n = 13), d 2014 (n = 25), e 2015
(n = 29), and f 2016 (n = 18). Cyan solid dots mean sampling sites

Fig. 7 Spatiotemporal variations
of major ions and TDS: five wells
(Nos. I22, I21, I20, I5 and I9) in
zone I of GIA; five wells (Nos.
I10, I3, I1, I14 and I15) in zone II
of GIA; and two monitoring wells
in YIA (Nos. 2-4 and 3-4)
Ca-HCO3-SO4 type, while both the lake water and the
diverted Yellow River water were of Na-Cl-SO4 type.
Accordingly, the former had a lower TDS (438 mg/L) than
both of the latter (1,050 and 657 mg/L, respectively).
Interannual variations in groundwater
as and redox-sensitive components
Total As concentrations ranged between <2 and 400 μg/L,
generally showing increasing trends from the alluvial fans to
the flat plain (Fig. 8). The trends are consistent with a previous
investigation (Guo et al. 2016a). From 2011 to 2016, the geo-
graphical area with groundwater As less than 50 μg/L de-
creased, while the area with groundwater As higher than
300 μg/L increased (Fig. 8). Especially in 2016, an area with
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groundwater As concentrations higher than 350 μg/L gradu-
ally emerged (Fig. 8f). In zone I, the mean values of ground-
water As concentration kept nearly unchanged from 2011 to
2016; however, there was an obvious rising trend in the mean
values of groundwater As concentration in zone II from 191 to
252 μg/L from 2011 to 2016 (Fig. 9). In addition, the concen-
tration of As(III), as the major species, spanned a comparable
range, from <2 to 343 μg/L, which mostly accounted for 22–
96% of total As (average 79%). Groundwater samples had
As(V) concentrations ranging between <3 and 88 μg/L.
Similarly, these ten irrigation wells in GIA witnessed a
rising trend in groundwater As concentrations from zone I to
zone II. In zone I, four (well Nos. I22, I21, I20 and 5) out of
five wells met the Chinese drinking water standard (<
50 μg/L), and well No. I9 did not meet the standard with As
Hydrogeol J
Fig. 8 Contour maps of groundwater As in GIA in a 2011 (n = 80), b 2012 (n = 16), c 2013 (n = 13), d 2014 (n = 25), e 2015 (n = 29) and f 2016 (n = 18).
Cyan solid dots mean sampling sites
concentrations increasing from 97.7 to 123 μg/L between
2011 and 2016 (Fig. 10). However, in zone II, groundwater
As concentrations in well Nos. I10, I3, I1, I14 and I15 were
much higher than the standard, ranging from 103 to 400 μg/L.
Liner regression of As concentration as a function of time
indicated that there were statistically long-term increasing
trends for these five wells (r > 0.6; Table S1 of the ESM) with
the largest increases from 4.37 to 10.5 μg/L/year (Fig. 10).
Moderate groundwater As concentrations were observed in
YIA. Two monitoring wells (Nos. 2-4 and 3-4) had As concen-
trations between 48.2 and 106 μg/L, whereby well No. 3-4, which
had As concentrations lower than 50 μg/L between 2012 and
2014, especially did not meet the standard in 2015, while well
No. 2-4 remained relatively stable during 2012–2015. The tem-
poral variations in As(III) were comparable to those of total As,
whereby arsenic concentrations of spring water, lake water and
the diverted Yellow River water were lower than 10 μg/L.
From the piedmont to the flat plain, groundwater Eh pre-
sented decreasing trends. Concentrations of redox-sensitive
components Fe(II) in groundwater displayed rising trends. In
GIA, the groundwater Fe(II) concentrations of five irrigation
wells in zone I ranged from <0.01 to 0.66 mg/L and from 0.02
to 0.55 mg/L, which were lower than those of another five
irrigation wells in zone II, varying from 0.59 to 2.48 mg/L and
0.90 to 6.40 mg/L, respectively (Table S1 of the ESM).
From 2011 to 2016, the fluctuation (% RSD, relative stan-
dard deviation) of Fe(II) concentration of the five irrigation
wells in zone I remained <20.6%, excluding the wells with
Fe(II) concentrations <0.05 mg/L (Table S1 of the ESM). In
addition, slight rising trends in Fe(II) concentrations were ob-
served in well Nos. I5 and I9 of zone I, increasing by 0.04 and
0.03 mg/L/year respectively. In zone II, five irrigation wells
showed obvious long-term increases in Fe(II) concentrations
between 0.03 and 0.19 mg/L/year (r > 0.7; Table S1 of the
ESM); however, in YIA, no temporal change was observed
concerning Fe(II) concentrations in well Nos. 2-4 and 3-4.
Discussion
Influences of extraction on groundwater flow fields
Pre-extraction
Before 2006, the diverted Yellow River water irrigation was
widely applied in the study area and almost no groundwater

Fig. 9 Mean values of groundwater As in zone I and zone II of the GIA
from 2011 to 2016
was used for agriculture irrigation (Li et al. 2011).
Groundwater mainly flowed from the alluvial fans to the flat
plain, and partly discharged into the drainage channel (Zhang
et al. 2013; Fig. 11a). There were scattered wetlands and tarns
in zone I, which gradually shrunk with groundwater extraction
for irrigation after 2006 (Li et al. 2016). Under the natural
groundwater flow conditions, a large area of saline land was
observed in zone II near the drainage channel, which resulted
from the intense evaporation concentration due to flat terrain
and shallower groundwater depth (Shanafield et al. 2015; Jia
et al. 2017). However, in YIA, the groundwater flowed from
southeast to northwest (Fig. 11a), with the dominant discharge
areas being around Shahai Lake and the drainage channel.
Post-extraction
Irrigation wells have been gradually installed in GIA owing to
the improvement of electric power facilities and difficulties in
diverting the Yellow River water to the piedmont since 2006.
A total of 127 irrigation wells, each with a flow rate of
0.027 m3/s have been used for irrigation in the studied area
until 2016. Around 15.5 million m3 of groundwater has been
extracted for irrigation in the spring of each year. Although the
groundwater levels/heads fluctuated due to the irrigation ac-
tivities, the Shahai Lake generally kept higher water levels
than the northwestern groundwater levels/heads, which acted
as a recharge area throughout the year (Fig. 11b). Therefore,
groundwater flowed from the Shahai Lake to the northwest in
zone II, which is opposite to the observation by Zhang et al.
(2013), although it flowed from the alluvial fans to the south-
east in zone I. During the spring irrigation, pumping caused
sharp drops in the water levels of well Nos. 1-3 and 5-2
(Fig. 2b) and also induced a depression cone in GIA
(Fig. 4). As the pumping continued, the water level difference
Hydrogeol J
Fig. 10 Spatiotemporal variations of As, Fe(II), Eh and SO42−/Cl− in
groundwater of ten representative irrigation wells in GIA and two
monitoring wells YIA. Red dot line means the Chinese drinking water
standard for As
between the center of the depression cone and the Shahai Lake
gradually increased, which resulted in the increase of hydraulic
gradient and the flow rate of groundwater recharge from the
Shahai Lake (around twice as fast as normal). Accordingly,
the lake water level presented a decreasing trend. When the
spring irrigation ended, the groundwater levels/heads rose again
and the depression cone subsequently shrunk (Figs. 2b and 4b).
In the period of winter irrigation, relatively less groundwater
(2.1 million m3) was needed for irrigation, which caused a slight
drop in groundwater levels. Before the drop, a slight peak was
also observed due to the influence of the diverted Yellow River
water irrigation which occurred earlier than the groundwater
irrigation. During winter irrigation, the diverted Yellow River
water irrigation affected groundwater levels near well No. 5-2.
As soon as the winter irrigation ceased, the water levels recov-
ered. Before the next irrigation season, the area of the depres-
sion cone decreased to the minimum. The lake-water recharge
continuously introduced chemicals into the groundwater be-
tween the depression cone and the Shahai Lake in zone II,
which may affect groundwater As variations.
For the whole year, well No. 5-2 had higher water levels
than well No. 1-3, showing that the flow direction was from the
west to the east of the depression cone. Additionally, from
2012 to 2016, significant downward trends of water levels
were observed in well Nos. 1-3 and 5-2, with the decrease rates
Hydrogeol J
Fig. 11 Conceptual models of
groundwater flow for a pre-
extraction and b post-extraction
of 0.25 and 0.2 m/year, respectively (Fig. 2b). It indicated that
groundwater extraction led to the continuous decrease in
groundwater levels/heads, and the previous groundwater flow
conditions had been broken in the study area (Fig. 11).
Nevertheless, in YIA, the diverted Yellow River water irriga-
tion was still the predominant irrigation method. Groundwater
levels had two peaks each year, which corresponded to the
spring irrigation season and the winter irrigation season, indicat-
ing that the diverted Yellow River water irrigation was the main
recharge source for groundwater. No obvious interannual varia-
tions in groundwater levels were observed, suggesting that the
recharge and discharge of groundwater maintain a long-term
stable state. Therefore, the groundwater flow conditions
remained unchanged in YIA, which is consistent with the ob-
servation by Zhang et al. (2013).
Spatiotemporal variations of groundwater chemistry
Although the groundwater flow field in zone I was disturbed
by the depression cone due to the intensive extraction (Fig. 4),
the groundwater recharge source did not change. Owing to the
deep water table, ranging between 10 and 20 m bls (Fig. 4),
groundwater evaporation was relatively weak; consequently,
groundwater TDS or major ions concentrations kept relatively
stable from 2011 to 2016 (Fig. 8).
However, in zone II, groundwater TDS increased significant-
ly over time, which was accompanied by increases in the major
ions. This phenomenon was governed by the change of ground-
water flow conditions. The shift of the groundwater recharge
source from the low-TDS piedmont groundwater to the high-
TDS lake water, which was induced by the depression cone,
increased groundwater salinity in zone II (Figs. 6 and 7). Since
zone II was the local discharge area of shallow groundwater
before 2006, near-surface sediments in this zone contained a
lot of soluble components (Yuan et al. 2017). The lake-water
recharge flushed those sediments and carried a large amount of
soluble components into the groundwater. Moreover, intensive
extraction of deep groundwater increased the hydraulic gradient
between the shallow groundwater and deep groundwater (Fig.
3b) and might induce recharge of shallow highly saline ground-
water into the deep low-salinity groundwater. Hence, the TDS of
the deep semiconfined groundwater tended to gradually increase
over time with the intensive extraction. Although shallow
groundwater levels in YIA would lead to intensive evaporation
(Fig. 2a), the dilution by the diverted Yellow River water (with
low TDS 657 mg/L) counteracted the evaporation, resulting in
the relatively constant TDS (Fig. 7).
Influences of groundwater flow changes
on groundwater As
High-As groundwater (> 50 μg/L; Figs. 8 and 9) was
observed in zone II and the YIA with high concentra-
tions of Fe(II) and TOC and lower Eh (Fig. 10).

Obvious increases in groundwater As concentrations
were observed in zone II from 2011 to 2016 (Fig. 10).
Temporal variations in As concentrations were well correlated
to temporal variations in Fe(II) (r > 0.7) for five irrigation wells
(Fig. 10). Increases in groundwater TOC were also obvious in
zone II (Table S1 of the ESM). The increases in groundwater
As may be associated with the increases in groundwater TOC
and may indicate that reductive dissolution of Fe(III) oxides
played a dominant role in As mobilization. This process was
usually fueled by natural organic matter (Islam et al. 2004;
McArthur et al. 2004); however, in addition, higher As ground-
water generally had lower concentrations of SO42−/Cl− in the
study area (Fig. 10). The bacterial sulfate reduction (BSR) was
verified by S and O isotopes of groundwater SO42− and chem-
ical analysis in the study area, and by the abundant distribution
of sulfate-reducing bacteria (Guo et al. 2008b; Li et al. 2014a, b;
Guo et al. 2016b), which would induce reduction of As-bearing
Fe(III)-oxyhydroxides and lead to the release of As into
groundwater.
The shift of the groundwater recharge source from the
piedmont groundwater to the lake water would be related
to the increase in groundwater As concentrations in zone
II. The Shahai Lake water had higher TOC contents than
the piedmont groundwater. The shift of the groundwater
recharge source introduced more dissolved organic matter
(DOM) into the aquifers, and the recharge source DOM
was believed to be more labile in comparison with the
resident groundwater DOM. The labile DOM readily
fueled dissimilatory reduction of Fe(III) oxides and
BSR-induced reduction of Fe(III) oxyhydroxides. In addi-
tion, pumping-induced fluctuations of groundwater levels/
heads could physically disturb the sediment matrix, which
would destabilize the mineral-associated sedimentary or-
ganic matter (Eusterhues et al. 2003). The destabilized
sedimentary organic matter is believed to be bioavailable
for microbes (Neumann et al. 2014) and may also con-
tribute to the increase in groundwater As concentrations in
zone II; however, in YIA, no obvious changes of ground-
water As were observed, which is consistent with the
previous observation (Guo et al. 2013a, b). No significant
variations in As concentrations are attributed to the rela-
tively steady groundwater flow direction and recharge
source (Fig. 10).
It is noteworthy that groundwater in zone I has the po-
tential to be contaminated by As, although relatively low As
concentrations are currently observed. With the intensive
groundwater extraction, the depression cone will be moved
northwestwards, and high-As groundwater will flow north-
westward. In this case, groundwater As in zone I is likely to
increase (Fig. 9); therefore, the extent of the groundwater
depression cone must be restrained or decreased to protect
the low-As groundwater in zone I via regulation of ground-
water extraction in zones I and II.
Hydrogeol J
Conclusion
Groundwater levels temporally fluctuated during the 6 years
of observation. The fluctuation patterns of groundwater level
were different between the GIA and YIA, as they were affect-
ed by groundwater extraction, the diverted Yellow River water
irrigation and evaporation. In GIA, groundwater was extracted
for irrigation during April–August and in November, resulting
in two troughs in groundwater levels each year. From 2011 to
2016, groundwater level presented a decreasing trend due to
the overextraction. However, in YIA, surface water was uti-
lized for spring irrigation and winter irrigation, resulting in
two peaks in groundwater levels each year. In GIA, the inten-
sive groundwater extraction caused a depression cone, which
reversed the groundwater flow direction and changed the re-
charge source in zone II. From 2011 to 2016, groundwater
TDS of zone II showed an obvious increase, which could be
explained by the fact that the recharge from the lake water
flushed near-surface sediments, which contained soluble com-
ponents, and finally carried shallow high-TDS groundwater
into the deep aquifer. Furthermore, a rising trend of ground-
water As was also observed, which was accompanied by the
increases in groundwater Fe(II) and TOC and the decrease in
SO42−/Cl−, implying that the biologically degradable organic
carbon introduced by the lake water promoted dissimilatory
reduction of Fe(III) oxides and BSR-induced reduction of
Fe(III) oxyhydroxides; besides, the low-As groundwater in
zone I would be potentially affected by the high-As ground-
water from zone II due to the reverse groundwater flow direc-
tion. Slight decreases in groundwater TDS occurred in YIA
due to the dilution effect of surface water, and temporal vari-
ation in groundwater As was slight. The groundwater extrac-
tion, altering recharge sources of groundwater and conse-
quently providing labile organic matter for biogeochemical
processes of As release, should be restrained in terms of ef-
fective protection of groundwater quality.
Funding Information The study was financially supported by the
National Natural Science Foundation of China (grant Nos. 41672225
and 41222020), the program of China Geology Survey (grant No.
12120113103700), the Fundamental Research Funds for the Central
Universities (grant No. 2652013028), and the Fok Ying-Tung
Education Foundation, China (grant No. 131017).
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