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Article history: Clean and safe groundwater is the basic guarantee for social and human sustainable development. With
Received 13 August 2019 the increasing groundwater pollution, it is essential to characterize hydrogeochemistry and assess
Received in revised form groundwater quality accurately for water supply purpose. In this study, investigation of groundwater was
21 January 2020
conducted in the urban area of Xi’an, which has a more than 3100 years glorious city history. 97
Accepted 7 March 2020
Available online 11 March 2020
groundwater samples were collected from domestic tube wells for physical and chemical analysis. Re-
sults showed that groundwater in the study area was predominantly the HCO3eCa and HCO3eCa$Mg
Handling Editor: Lincoln C. Wood type, which were controlled by multiple processes of water-rock interaction, evaporation, cation ex-
change etc. Some samples fall in Zone 4 (mixed type) and Zone 2 (SO4eNa type) in Piper diagram,
Keywords: indicating the complex influence of both rock-water interactions and anthropogenic activities. To assess
Groundwater groundwater quality reasonably, an innovative integrated-weight water quality index (IWQI) was pro-
IWQI posed by combining objective and subjective weights through additive model. The calculated weights
Hydrogeochemistry showed that integrated weights balanced the relationship between subjective expertise about impacts of
Order relation analysis method
chemical components on human health risk and objective entropy information of ion concentration. The
Entropy weight method
high integrated weight for F (0.237), NO2eN (0.104) and HCO 3 (0.103) indicated their significant in-
Ancient pollution
fluences on groundwater quality. According to the IWQI, overall situation of groundwater in the study
area was described as good, while only 9.4% of groundwater samples was of medium to poor quality and
unsuitable for drinking. Investigation and historical documents data showed that this poor groundwater
quality in the city centre can be attributed to the low terrain, special characteristics of loess deposit,
modern pollution in recent decades and the migration of ancient pollutants over one millennia. The
sensitive analysis of IWQI indicated the innovative IWQI could describe the overall water quality reliably,
stably and correctly, and have the potential suitability for extensive application.
© 2020 Elsevier Ltd. All rights reserved.
https://doi.org/10.1016/j.jclepro.2020.121006
0959-6526/© 2020 Elsevier Ltd. All rights reserved.
2 Y. Gao et al. / Journal of Cleaner Production 260 (2020) 121006
cities, groundwater is bound to be polluted by frequent and intensive according to their practical experiences and local hydrogeological
human activities (Wang et al., 2019), and the no longer clean condition, and different experts may have different preferences,
groundwater in turn threatens the health of thousands of people. which lead to subjective final WQI scores with multiple un-
Therefore, safe and hygienic drinking water has been a primary focus certainties (Chen et al., 2019; Kamrani et al., 2016; Du et al.,
of water resource management and related researches (An et al., 2020)). To avoid the subjectivity of traditional weights, entropy-
2016; Cai et al., 2019). To ensure safe water supply and solve or weighted water quality index (EWQI) was developed, which
reduce the severity of groundwater quality degradation, it is essen- determined the weights based on the amount of useful informa-
tial to identify the status of groundwater quality and assess the tion with the provided data (Shannon, 1948; Castellano et al.,
suitability of groundwater for drinking (Edmunds et al., 2003; 2013; Kamrani et al., 2016; Li et al., 2015; Piplani and Wetjens,
Mattos et al., 2018; Wang et al., 2017). 2007; Amiri et al., 2014). Although the advantages of the en-
Xi’an, being the capital city of Shaanxi Province, is a modern tropy theory’s application have been observed, many of its limits
mega city with a population over ten million. The city is located in still need to be improved, which include: 1) entropy-weights re-
a semi-arid area of northwest China. Historically, thirteen Dy- lies excessively on the objective data that cannot reflect the
nasties had set their capitals in Xi’an. Xi’an represents an impor- practical experience of experts (Xu et al., 2018); 2) entropy-
tant birthplace of Chinese civilization and is the starting point of weights have instable characteristics, which are easy to change
the ancient Silk Road. Being the political, economic and cultural with sample sizes and values; 3) the relationship between in-
centre of ancient China for thousands years, large numbers of dicators and objective are often neglected when calculating the
people once lived here, and groundwater pollution had been a weights, resulting in confusing and unexplainable evaluations (Liu
serious problem from ancient time. For example, after the West- et al., 2019b). Another common method to determine index
ern Han Dynasty (8 A.D.), the groundwater pollution in Xi’an weight is the order relation analysis (G1 method), which is an
forced the city center to be moved to southeast many times. In this improved analytic hierarchy process and subjectively takes into
semi-arid loess region, owing to the weak renewable ability of full account of the relationships between indices and objective. In
groundwater and high adsorption ability of loess to pollutants, this study, an integrated-weight water quality index (IWQI) is
groundwater pollution is hard to control and remove once it developed by incorporating subjective weights (determined by G1
occurred. Therefore, groundwater quality in this ancient capital method) and objective weights (determined by entropy weight
can typically represent the comprehensive effects of natural method) to assess the suitability of groundwater for drinking
evolution, modern and historical human activity. To our best purpose.
knowledge, the effects of ancient pollution on modern or current The present study took Xi’an as an example to conduct integrated
groundwater quality are scarcely considered in most studies. investigation of groundwater environment and quality assessment.
Chemical components in groundwater, as the “Gene Bank” that Our objectives are to (1) identify the hydrogeochemical character-
marks the evolution of water environment, are generally used to istics and sources of major ions using multiple statistical analysis and
elucidate the sources of major ions and distinguish the effects of hydrogeochemical methods; (2) assess suitability of groundwater for
natural and anthropogenic factors (Khalid et al., 2018). Due to the drinking purpose based on an improved integrated-weight water
weak renewable ability of groundwater in some areas, hydro- quality index (IWQI). The results are expected to provide scientific
chemical characteristic is also a main approach to acquire infor- information on groundwater resource management and sustainable
mation about ancient pollution. Moreover, knowledge of development in Xi’an, and be a reference for cities with similar sit-
hydrochemical characteristics is the prerequisite for assessing uation in the world.
suitability of groundwater for drinking purpose.
Protection of groundwater quality, which plays a key role in 2. Materials and methods
providing cleaner and safer drinking water for people, requires the
combined efforts of many partners such as water resource man- 2.1. Study area
agers, water suppliers, lawmakers and public (Abtahi et al., 2015).
Considering the different professional backgrounds of the public, Xi’an, located in the centre of the Guanzhong Basin, is the capital
information about groundwater quality needs to be reported in a of Shaanxi province and is one a key central city in northwest China
concise manner (Nasirian, 2007). Therefore, traditional methods (He et al., 2008). Xi’an stretches from longitude 107400 e109 490
such as individual parameter assessment of water quality were and latitudes 33 420 e34 450 , with a concentrated urban area of
replaced by water quality index (WQI), which was firstly developed 824.7 km2. The main urban area consists of six regions: Baqiao,
by Horton (1965). WQI integrates large numbers of individual Beilin, Lianhu, Weiyang, Yanta and Xincheng. Population in these
groundwater chemical component into an easily expressible and regions is approximately 4.46 million, which represents around
understood format (a single score) through selecting and weighting fifty percent of the population in Xi’an. As seen from Fig. 1, ~60% of
the water quality parameters and applying an aggregation function the study area has been urbanized.
(Abtahi et al., 2015). Moreover, it has been an effective approach to Xi’an is bound by the Qinling Mountains in the south and the
communicate water quality information to decision makers, and is Wei River to the north. The climate of the study area is dominated
widely used in numerous water quality assessment works (Batabyal by a warm sub-humid continental climate, with average annual
and Chakraborty, 2015; Chen et al., 2019; Das Kangabam et al., evaporation (852.7 mm/year) exceeding average annual precipita-
2017; Molekoa et al., 2019; Nath et al., 2018; Vasanthavigar et al., tion (650 mm/year). Eight rivers, namely the Wei River, Jing River,
2010). Feng River, Lao River, Jue Rive, Hao River, Chan River and Ba River
Despite the widespread application of WQI, its drawbacks such constitute the river network of Xi’an, which is famous for “Eight
as subjective weights, inflexible structure and inadequate input rivers around Chang’an” (Xi’an is called Chang’an in ancient time).
parameters are obvious, and the efforts to develop improved WQI The topography of the study area shows the ladder-like distribution
have been continued (Abtahi et al., 2015; Mohebbi et al., 2013). from the Qinling Mountains to the Wei River, turning from the al-
The weights in WQI determine the relative importance of each luvial fan of mountains to loess tablelands and river terraces. Loess
parameter in the overall water quality, so reasonable weights have tableland is mainly distributed in the southeast of Xi’an. An alluvial
critical influence on the accuracy of those results (Liang et al., plain with a thick, overlying Quaternary sediment is widely
2019). However, weights are traditionally assigned by experts distributed along rivers.
Y. Gao et al. / Journal of Cleaner Production 260 (2020) 121006 3
2.2. Geology and hydrogeology consists of Archean - Proterozoic metamorphic rocks and Yan-
shannian intrusive rocks. The Quaternary stratum is composed
Xi’an is located in the Guanzhong Basin, between the Ordos primarily of sands, gravels, silty clay, clay and loess. The tertiary
block and the Qinling fault uplift. With the intense geotectonic sandstones are dominated by quartz, feldspars, calcite, dolomite
movement, several active faults of different periods, scale and di- and plagioclase (Chen et al., 2019). The phreatic aquifer is generally
rections are developed. Xi’an fault depression has a very thick less than 100 m thick. Due to the developed water system, the
Cenozoic strata deposited (4000e5000 m), and its basement depth of groundwater in the alluvial plain is very shallow, less than
4 Y. Gao et al. / Journal of Cleaner Production 260 (2020) 121006
10 m. Therefore, local residents living in the suburbs drilled wells in 2.4. Water quality assessment method
their homesteads and farmlands for domestic or irrigation water
supplies. In the loess tableland, due to the low-permeability of the 2.4.1. Overall framework of IWQI
thick loess deposit, the groundwater table is deep and shallow The calculation of IWQI includes four steps: subjective weight
wells are ~30e80 m deep. calculation, objective weight calculation, calculation of integrated
weight, and groundwater quality assessment based on IWQI. The
overall framework of IWQI is shown in Fig. 2.
(iii) Calculate index weight. The weights wi of each parameter are Table 2
calculated as follows: Groundwater quality classifications for drinking based on
IWQI values.
!1
X
n Y
n IWQI values Water quality
wn ¼ 1 þ ri (2) <50 Excellent
k¼2 i¼k 50e100 Good
100e150 Medium
wi1 ¼ ri wi ; i ¼ 2; 3; 4; …; n (3) 150e200 Poor
>200 Extremely poor
L1 X
L1
L XL2
Lm X
Lm where ej is the information entropy of the jth parameter. 104 is
wsi ¼ w*ki þ 2 w*kj þ… þ w*kp (4) used to ensure the formula is meaningful.
L L L
k¼1 k¼1 k¼1
(iii) Calculate the entropy weight (objective weight: woj) with Eq.
where, wki* is the relative weight of parameter xi calculated ac-
(9):
cording to the kth of the L1 experts. L ¼ L1þL2þL3þ … þLm.
1 ej
2.4.3. Step 2: objective weight based on entropy-weighted method woj ¼ n
(9)
P
Information entropy proposed by Shannon objectively reflects 1 ej
useful information because it is based on original data (Shannon, j¼1
ri Description
1.0 Parameter xi-1 is important as parameter xi 2.4.5. Step 4: groundwater quality assessment based on IWQI
1.2 Parameter xi-1 is slightly more important than parameter xi The Water Quality Index (WQI) is an efficient technique to assess
1.4 Parameter xi-1 is obviously more important than parameter xi the suitability of groundwater for drinking purposes (Tian et al.,
1.6 Parameter xi-1 is strongly more important than parameter xi 2019). The quality rating scale (qj) of each parameter is calculated
1.8 Parameter xi-1 is extremely more important than parameter xi
using Eq. (13) (Talib et al., 2019):
6 Y. Gao et al. / Journal of Cleaner Production 260 (2020) 121006
Parameters Mean Max Min SD CV(%) WHO (2011) % of SEL PCA is a powerful technique to reveal the interrelationship of
pH 7.60 9.1 7.1 0.33 4.28 6.5e8.5 3.09 geochemical variables by reducing the dimensionality of a large
TDS 806.80 4415 117 571.46 70.83 1000 17.53 number of parameters (Hu et al., 2013). In this study, PCA analysis
Kþ 8.54 150 0.59 24.31 284.69 e e was applied to the concentrations of TH, TDS, F, NH4eN, NO2eN,
Naþ 106.32 580 13.3 82.56 77.65 200 8.25 NO3eN and the major ions, to identify the dominant factors con-
Ca2þ 95.90 481 5.01 66.35 69.19 200 2.06
Mg2þ 48.01 159 0 32.58 67.86 150 1.03
trolling the chemical components of groundwater. Three principal
Cl 80.39 436 3.5 70.80 88.07 250 4.12 components (PCs) with eigenvalues above 1 were retained, which
SO2-4 157.32 1633 2.78 196.13 124.67 250 11.34 explained 69.15% of the total variance. PC1 explained 45.95% of total
HCO 3 438.35 906 42.7 177.11 40.40 250 86.60 variance and had strong loadings on Naþ, Cl, Mg2þ, SO2 4 , TH, TDS,
TH
402.33 1007 19.5 192.28 47.79 450 38.14
NO3eN and HCO 3 (Fig. 3). The results of PC1 indicate that multiple
F 0.54 1.99 0.03 0.37 69.00 1.5 12.37
NH4eN 0.17 8.56 0 0.87 502.5 0.5 4.12 processes including silicate, carbonate weathering and evaporite
NO3eN 10.44 135.48 0 18.48 176.9 20.0 12.37 dissolution may be the dominant sources of these ions. PC2 ac-
NO2eN 0.05 2.26 0 0.23 497.6 1.0 1.03 counts for 14.17% of the total variance, with strong loadings on Ca2þ,
SD, standard deviation; CV (%), coefficient of variation; % of SEL, % of samples F and pH. The collection of these parameters reflects geogenic
exceeding acceptable limit. contamination such as fluorite dissolution. PC3 accounts for 9.04%
Y. Gao et al. / Journal of Cleaner Production 260 (2020) 121006 7
Fig. 6. Plots of (a) Naþ vs. Cl, (b)Naþ vs. TZþ, (c) CAI-I vs. CAI-II, (d) (Ca2þþMg2þ)-(SO2- þ þ -
4 þ HCO3 ) vs. (Na þK -Cl ), (e) Ca
2þ
vs. SO2
4 , and (f) Mg
2þ
vs. SO2-
4
10 Y. Gao et al. / Journal of Cleaner Production 260 (2020) 121006
KAl2 ½AlSi3 O10 F2 þ2OH /KAl2 ½AlSi3 O10 ½OH2 þ2F (19) integrated weights were 0.237, 0.104 and 0.103, respectively. Naþ
had the lowest integrated weight (0.038), indicating the minimum
influence on water quality.
CaF2 /Ca2þ þ2F (20)
CaF2 þ2HCO
3 /CaCO3 þ2H2 O þ CO2 þ2F
(21) Table 5
Index weights determined by different methods.
Table 4
Relative importance and weight determined by four experts.
Relative importance Index weight Relative importance Index weight Relative importance Index weight Relative importance Index weight
ri W1i ri W2i ri W3i ri W4i
Table 6 3.5.3.2. Modern pollution. The area inside the city wall, as the most
Classification of groundwater quality according to IWQI values. famous tourist attraction and the business center, produces a great
IWQI values Water Quality Number of Samples Percentage of Samples amount of municipal domestic waste, wastewater and exhaust
<50 Excellent 36 37.5%
gases. According to Li (2014), the moat around the city wall had
50e100 Good 52 54.7% been seriously polluted by municipal sewage for approximately
100e150 Medium 6 6.3% fifty years (from the 1950s to the 2000s). Groundwater in nearby
150e200 Poor 3 3.1% areas was also polluted to some extent and difficult to restore and
200 Extremely poor 0 0%
improve in the short term. Cl and NO 3 , which are the main ions
indicating the influences of domestic sewage (Fulazzaky et al.,
2015), are both high and coincide with IWQI in this area (Fig. 9).
3.5.2. Groundwater suitability for drinking Therefore, modern pollution combined with natural factor jointly
Based on integrated weights, IWQI was used to assess water lead to poor groundwater quality in this area.
quality for drinking purposes. The calculated WQI values of
groundwater ranged from 11.62 to 174.32, with an average of 63.24. 3.5.3.3. Ancient pollution. Ancient pollution may be also an
As shown in Table 6, of 97 groundwater samples, no samples had an important factor affecting groundwater quality in the area. In
extremely poor quality and only three samples showed poor 200 B.C (Han dynasty), the Emperor Gao of the Han established the
quality. Overall, only 9.4% of groundwater samples were unsuitable capital in Xi’an and Hanchenghu was the moat of his palaces. Since
for drinking, while 54.7% of samples had good quality and even then, Hanchenghu had been the moats of the capital for different
37.5% of samples were of excellent quality. The spatial variation of dynasties until the Sui dynasty (~800 years), the long-term, heavy
groundwater quality is shown in Fig. 8. Groundwater in most urban burden of dense population seriously polluted the groundwater.
areas of Xi’an was of good to excellent quality. However, ground- Hence, in 600 A.D (Sui dynasty), the capital moved southeastward
water around the north-west corner of city wall was not good to Zhonglou due to the bitter and salty groundwater around Han-
enough or even poor, which may be attributed to three factors: chenghu. However, groundwater drawn from wells around Zhon-
natural factors, modern pollution and ancient pollution. glou also became salty and undrinkable in 1014 A.D (Song dynasty)
(http://xadfz.xa.gov.cn/). Due to the limited self-purification ca-
3.5.3. Controlling factors analysis of poor groundwater quality pacity and the adsorption capacity of loess, groundwater in this
3.5.3.1. Natural factors. According to the topography of ground loess area was very difficult to restore once polluted. According to
surface, the most polluted area is a low-lying area. In this area, the permeability test in the field and parameter calibration by
urban surface runoff gathers and recharges groundwater. Since model, horizontal permeability coefficient and porosity of loess are
surface runoff is easily influenced or polluted in large and 1.2 m/d and 0.08, respectively (Peng et al., 2012). Additionally,
concentrated cities like Xi’an, groundwater recharged by these based on the topographic map of Xi’an, the hydraulic gradient and
waters could be of poor quality. distance from the city center (Zhonglou) to the center of pollution
Moreover, this area is covered with thick loess deposits, which is are 0.449‰ and 2272 m, respectively. By Darcy’s law, the flow ve-
characterized by high vertical permeability but poor horizonal locity is 0.0067 m/d, and it needs about 929 years for pollutants to
permeability. Thus, pollutants in the surface are hard to migrate migrate from the city center to the center of pollution. Considering
horizontally but relatively easy to infiltrate into groundwater with the effect of hydrodynamic dispersion, the estimated time for so-
precipitation. lute transport (929 years) is generally in correspondence with the
Fig. 9. (a) Spatial distribution of NO3eN; (b) Spatial distribution of Cl; (c) Conceptual model of factors leading to poor groundwater quality in Xi’an (natural factor, modern
pollution and ancient pollution).
actual time (from 1014 to 2018). the more instable the assessment results are (Lodwick et al., 1990).
In conclusion, influenced by natural factors such as topography Sensitivity analysis was conducted to investigate the influence of
and sediment, modern pollution coupled with the accumulation of each input parameter on the IWQI score according to Eq. (22).
ancient pollutants jointly led to the poor groundwater quality at the
city center (Fig. 9). jðVi =NÞ ðvi =nÞj
Si ¼ 100% (22)
Vi
3.6. Sensitivity analysis
Where, Si is the sensitivity of ith evaluating unit, Vi is the IWQI score
Sensitivity analysis is an effective method to identify the effects of ith evaluating unit, vi is the IWQI score after removing ith input
of each input parameter on assessment results and test the index (chemical component), N and n are the number of parameters
reasonability of selected index system. The larger the sensitivity, when calculating Vi and vi, respectively.
Y. Gao et al. / Journal of Cleaner Production 260 (2020) 121006 13
The effects of removing each input index (chemical component) correlation with Ca2þ, indicates the coupling effects of exchange
on the IWQI score (Fig. 10) show that the average sensitivity of each between OH and F, fluorite dissolution and hydrolysis of F-
parameter is generally small, which ranges from 0.049e1.79%. bearing silicates.
Removing HCO 3 has the most positive effect on the IWQI score, An innovative method (integrated-weight water quality index-
followed by fluoride with an average sensitivity of 1.07%. The IWQI) was proposed and applied to assess the suitability of
smallest change was pH with an average sensitivity of 0.049%. The groundwater for drinking purpose. Assignment of weight factors
effects of removing parameters on the IWQI score showed a good for input parameters was the main modification carried out in
relationship with index weights (e.g. integrated weights of HCO 3, IWQI. Considering the subjectivity of traditional WQI and blind
F and NO2eN are 0.103, 0.237 and 0.104, respectively (Table 5)). objectivity of EWQI, the integrated weights in IWQI were calculated
According to the sensitivity analysis, the IWQI was not par- by combining objective weights (G1 method) with subjective
ticularity sensitive to any one parameter, indicating that the sta- weights (entropy-weighted method) through additive model. The
bility of water quality assessment (IWQI) is not affected by integrated weights avoided the exaggerated weight of HCO 3 caused
removing any one parameter. In the other word, the IWQI does not by high concentrations effectively, and balanced the too small
rely excessively on one or a few parameters, and all parameters weights of toxicological indexes caused by the small order of
play a role in the water quality assessment (Abtahi et al., 2015). magnitude. The integrated weighted showed that F, NO2eN and
The sensitivity analysis also indicated that the IWQI was devel- HCO 3 had more important effects on groundwater quality, while
oped correctly. Naþ had the lowest integrated weight. The IWQI values, which
were calculated with thirteen available input parameters, show
that overall situation of groundwater quality was described as good,
4. Conclusions while only 9.4% of samples was unsuitable for drinking. The me-
dium and poor groundwater quality are primarily located in the
Groundwater is an essential and strategic resource for social and low-lying area around the north-west corner of city wall. Based on
human sustainable development, especially in arid and semi-arid the field investigation, historical documents review and solute
areas. However, Xi’an, as a modern mega city and historical capi- transport estimation, the poor quality in this area can be attributed
tal city of China, has suffered from groundwater quality degrada- to natural factors, modern pollution in recent decades and the
tion for over one millennia. To ensure water supply security, the accumulation and migration of ancient pollutants over one
hydrogeochemical characteristics and suitability for drinking of millennia.
groundwater in the concentrated area of Xi’an was investigated and Sensitivity analysis indicated that the IWQI did not rely exces-
studied. sively on one or a few parameters and could be used as a suitable
Statistics showed that the abundance of major ions in ground- method to evaluate groundwater quality for drinking purpose.
water of Xi’an was in the following order: HCO 2
3 > SO4 > Cl and Finally, based on this study, we recommend the city environ-
Naþ z Ca2þ> Mg2þ> Kþ. Hydrochemical facies were predominantly mental departments to adopt comprehensive treatment of surface
HCO3eCa, HCO3eCa$Mg type, which were controlled water-rock water, soil and groundwater according to the local natural con-
interaction, evaporation, cation exchange etc. Some samples fall ditions. Moreover, due to the long-term effects of pollutants
in Zone 4 (mixed type) and Zone 2 (SO4eNa type) in the Piper di- migration, it is necessary to stringently monitor poor groundwater
agram, indicating the complex influence of both rock-water in- quality regions and to carry out groundwater vulnerability studies
teractions and anthropogenic activities. PCA revealed that multiple in Xi’an to define the fragile areas for groundwater protection, so
water-rock weathering processes had strong loadings for Naþ, Cl, as to ensure the sustainable water security.
Mg2þ, SO2 4 , TH, TDS and HCO3 ; PC2 had strong loadings for Ca ,
2þ
pH and F; while PC3 had strong loadings on NH4eN. The strong Declaration of competing interest
positive correlation between pH and F as well as negative
We declare that all authors have no any actual or potential
conflict of interest including and financial, personal or other re-
lationships with other people or organizations.
Acknowledgments
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