Soil Pollution and Remediation in Zimapán, México

SOIL POLLUTION AND REMEDIATION
Arsenic and metals mobility in soils impacted by tailings
at Zimapán, México
María Aurora Armienta1
& Violeta Mugica2
& Isabel Reséndiz3
&
Mirella Gutierrez Arzaluz2
Received: 28 January 2015 /Accepted: 14 August 2015 /Published online: 27 August 2015
# Springer-Verlag Berlin Heidelberg 2015
Abstract
Purpose Mining wastes may cause important environmental
impacts in soil, water, and air due to their high metals and
arsenic contents. The aim of this work was the assessment of
the mobility of arsenic and several heavy metals in soils lo-
cated near different types of tailing heaps in the town of
Zimapán, México.
Materials and methods One hundred twenty soil samples
were collected nearby to three tailing heaps, one oxidized
presenting a red color (RT), and two with gray wastes (OSM
and NSM) but with different age, during the dry and rainy
seasons at the surface and to 40 cm depth, as well as to differ-
ent distances from the deposits. Arsenic, Cd, Cu, Fe, Mn, Pb,
V, and Zn total concentrations were determined; in addition,
geochemical phase distribution of As, Cu, Mn, and Zn in
selected samples was determined by sequential extraction.
Concentrations were measured by graphite furnace atomic
absorption spectrometry and inductively coupled plasma. To
interpret the results, statistical analyses were performed.
Results and discussion All samples presented high As con-
centrations reaching more than 50,000 mg kg−1
close to OSM
tailings, although the highest concentrations in the available
fractions were measured in NSM impacted soils. Arsenic and
metals concentrations exceeded the screening limits recom-
mended for industrial sites. In samples influenced by OSM
tailings, most of the elements analyzed were in the residual
fraction, whereas in NSM and RT they were mostly in the
organic and sulfide fractions and in the Fe and Mn oxides
fractions, respectively. Larger concentrations of As and metals
than those allowed by the screening values in Canada and the
Netherlands were measured in the residential area
representing a health threat for the inhabitants and the
environment.
Conclusions Acid mine drainage, water, and wind erosion of
tailings have polluted nearby soils. Higher concentrations of
As and metals were measured during the rainy season in gray
tailings impacted soils and during the dry season in red tail-
ings, showing both deposit types’ different mobility. Elements
fractionation in soils depends mainly on tailings characteris-
tics. Low metals and As proportions were found in the fraction
with the highest mobility. Metals and arsenic are more stable
in soils impacted by gray tailings, mainly in the organic and
sulfides and residual fractions, while in RT, most are linked to
Fe and Mn oxyhydroxides. Polluted soils in residential areas
constitute a health hazard. Remedial actions must be taken to
stop the population exposure.
Keywords México . Mining wastes . Sequential extraction .
Soil pollution
1 Introduction
Soil pollution by mining activities is a worldwide problem.
High concentrations of toxic elements produced by mining
wastes have been reported in Europe, Asia, Africa,
Australia, and America (Hutchinson and Whitby 1974; Bech
et al. 1997, 2012; Razo et al. 2004; Archer and Caldwell 2004;
Responsible editor: Saulo Rodrigues-Filho
* María Aurora Armienta
victoria@geofisica.unam.mx
1
Instituto de Geofísica, Universidad Nacional Autónoma de México,
Circuito Exterior, C.U., México 04510, D.F., México
2
Universidad Autónoma Metropolitana, Azcapotzalco, Av. San Pablo
180 Col. Reynoza, Azcapotzalco, Mexico 02200, D.F., México
3
Secretaría de Medio Ambiente y Recursos Naturales (SEMARNAT),
Blvd. Adolfo Ruiz Cortines, México 14210, D.F., México
J Soils Sediments (2016) 16:1267–1278
DOI 10.1007/s11368-015-1244-x

Osher et al. 2006; Teršič et al. 2009; Stefanowicz et al. 2014;
Teng et al. 2014; Ngure et al. 2014; Bačeva et al. 2014;
Morales et al. 2015). At Zimapán, a historical mining zone
in central Mexico, groundwater arsenic contamination has
been a concern for almost 20 years (Armienta et al. 1997,
2001; Ongley et al. 2001; Rodriguez et al. 2004; Romero
et al. 2004; Sracek et al. 2010). Natural (mineralization in
the fractured deep limestone aquifer) and anthropogenic (tail-
ings leaching) were identified as arsenic sources. However,
drinking water was polluted by the natural source. Currently,
the construction of three treatment plants has decreased arse-
nic population exposure. Further, a general overview of As
content in soils was provided by Ongley et al. (2007).
Importance of tailings as a potential source of As to nearby
soils was highlighted in this study. These wastes have also
impacted the sediments of the nearby Tolimán River with high
As, Pb, Cd, and Zn concentrations (Espinosa et al. 2009).
Sequential fractionation was also used to assess the environ-
mental availability of those toxic elements in sediments col-
lected along the river (García et al. 2001; Espinosa et al.
2009). Abundance of limestones in the area proved to be a
major factor in the geochemical behavior of the elements stud-
ied. Presence of tailings impoundments with contrasting ap-
pearance and mineralogical variations in the town skirts may
represent different environmental hazards to soils close by
according to the As and heavy metals availability in each
deposit. In addition to tailing particulates, As and heavy
metals-polluted soils constitute an important exposure route
to plants, animals, and population. Besides, some corn fields
and shallow wells (used for irrigation) are located next to the
studied zone.
The aim of this study was to determine the environmental
mobility of As and heavy metals (Cd, Cu, Fe, Mn, V, Pb, Zn)
in soils potentially impacted by tailings impoundments at
Zimapán town. To achieve this goal, samples were collected
at increasing distances from two apparently low-oxidized
(gray) and one oxidized (red) deposits. In addition, sequential
fractionation of As, Cu, Mn, and Zn was carried out in select-
ed samples.
2 Materials and methods
2.1 Site description
Zimapán mining zone is located in Central Mexico about
150 km from Mexico City (Fig. 1). Climate is semi-arid
with average temperatures between 16 and 18 °C and pre-
cipitation from 400 to 500 mm3
mainly occurring as heavy
storms (INEGI 1994, 2010). Geology is composed of
Upper Jurassic calcareous shales of Las Trancas
Formation, overlaid by the Cretaceous limestones
Tamaulipas, Abra, and Soyatal Formations. Tertiary Age
continental and volcanic rocks El Morro Fanglomerate
and Las Espinas Formation are also present in the area.
Late Tertiary and Quaternary alluvial fans cover the lower
zones (Simons and Mapes-Vazquez 1956; García and
Querol 1991).
Ore comprises sphalerite, galena, chalcopyrite, and
tetrahedrite-tennantite, while calcite, pyrite, arsenopyrite,
pyrrothite, and silicates are the main gangue minerals
(Simons and Mapes-Vazquez 1956; Villaseñor et al.
1996). Ore processing by selective flotation has pro-
duced tailing heaps, most of them located in the town
outskirts. Soils close to three of the several tailing heaps
at Zimapán town outskirts were sampled in this study.
Of the six deposits settled in that zone, three of them
with different characteristics were selected in order to
have an overview about the influence of tailings on
soils: the first one is New San Miguel (NSM) that is
a gray deposit, which is still active and close to resi-
dential areas; the second one is Old San Miguel (OSM)
which is a 30-year-old abandoned deposit with gray
tailings similar to NSM; and the third one corresponds
to oxidized tailings which are here named Red Tailings
(RT) (Fig. 1). In addition, NSM and OSM are the largest
deposits in Zimapán town outskirts.
2.2 Sampling and analysis
One hundred twenty soil samples were collected in eight
transects at increasing distances from the basements of
the three selected tailing heaps (Fig. 2). Within each
transect, a soil sample was collected every 20 m, from
the surface and at 40 cm depth. In addition, three dupli-
cate samples were taken close to NSM tailings during the
dry season, two of them marked as 13 and 15 sited in a
residential area at the back of the NSM deposit uphill
and upwind, and the other one around 700 m at the
Eastern of NSM marked as 16 and located at the front
of a high school. These areas were selected to have a
first approach to population exposure.
Location was determined with a GPS II Plus Garmin
Personal Navigator. Sampling was carried out in the dry and
in the rainy seasons. About 1.5 kg was taken with a shovel and
placed in a pre-washed plastic bag for their transport to the
laboratory where the samples were air-dried, quartered,
ground, and sieved through a 230 mesh (<62 μm). One gram
of the quartered sample was taken for As analyses and another
for heavy metals determinations.
The pH was measured in a 1:1 (water/soil) slurry
following the 9045 C USEPA method (USEPA U.S.
Environmental Protection Agency 1995) measuring with
a Beckman model ф720 potentiometer. Mineralogy of
1268 J Soils Sediments (2016) 16:1267–1278

tailing samples was determined with an XRD Siemens
D5000.
Samples for As analysis were digested following
USEPA 3051A (USEPA U.S. Environmental Protection
Agency 2007) in a microwave oven MDS 2000 at
90 psi during 30 min and 100 % power with an acid
solution. Sequential extraction of selected samples was
carried out following the method established by Tessier
et al. (1979) and modified by Dold (2003). Arsenic was
measured by atomic absorption spectrometry with a
graphite furnace in a Perkin Elmer AAnalyst 100 and
HGA 850.
Inductively coupled plasma-atomic emission spec-
trometry (ICP-AES; Atom Advantage Thermo Jarrel
Ash) was used to analyze total metals contained in the
soils after digestion in the microwave oven (OI-
Analytical) using high-pressure Teflon digestion vessels
with HCl and HNO3, following also USEPA method
3051A (USEPA U.S. Environmental Protection Agency
2007).
The sequential extraction procedure described in detail
by Ure et al. (1993) was used to determine Cu, Mn, Pb, and
Zn fractionation in the samples. In addition, the soluble
fraction suggested by Tessier et al. (1979) was also
obtained.
Analytical quality was assessed measuring 20 % duplicates
and analyzing the NIST standard 2710 Montana soil highly
elevated trace element concentration.
3 Results and discussion
3.1 Tailings impoundments
Main mineralogy, physical characteristics, and covered area
are shown in Table 1. An important difference between OSM
and NSM deposits relies on their consolidation degree since
most of the surface of NSM is composed of loose material
while OSM is more compacted and welded (Fig. 1). Calcite,
quartz, and arsenopyrite were identified in gray tailings; in
addition, pyrite was also present in the New San Miguel
deposit.
Presence of gypsum and K-jarosite in red tailings (Fig. 1)
indicates the occurrence of important oxidation processes that
have produced these secondary minerals (Méndez and
Armienta 2003). Gypsum is formed by the reaction of sulfate
with calcium which are released by pyrite oxidation produc-
ing acid mine drainage which in turn promotes calcite disso-
lution. Though this process goes to a series of reactions, it
may be simplified as (Seal and Hammarstrom 2003):
Fig. 1 Location of Zimapán in México, and Google view of the tailing heaps: NSM New San Miguel, OSM Old San Miguel, RT red tailings
J Soils Sediments (2016) 16:1267–1278 1269

FeS2 þ 7
.
2 O2 þ H2O→ Fe2þ
þ 2SO4
2−
þ 2Hþ
Fe2þ
þ 1=4 O2 þ 5
.
2 H2O → Fe OH
ð Þ3 þ 2Hþ
CaCO3 þ Hþ
→ Ca2þ
þ HCO3
−
Calcium and sulfate may then react to form anhydrite and/
or gypsum; jarosite (KFe(SO4)2(OH)6) is also formed in the
paragenesis of mine wastes containing pyrite (Jambor 2003).
Goethite, which is also a characteristic secondary mineral, has
also been identified by optical microscopy in RT (Romero
et al. 2006).
3.2 Total concentrations
Medians and ranges of the measured metals and arsenic in the
transects for the dry and rainy seasons and for superficial and
at 40 cm depth samples are displayed in Table 2, while
Spearman correlations between concentrations at different
depths and measured species during the two seasons are
shown in Table 3. In general, the highest concentrations were
Fe>Zn>As for all the sites, depths, and seasons, whereas the
lowest concentrations were found for V. With pyrite being one
of the main minerals at Zimapán mineralization, it is not sur-
prising that Fe was the most abundant element in the sampled
Fig. 2 Location of sampling points
Table 1 Mineralogy, visual
characteristics, and area of
tailings impoundments
Tailings Mineralogy Physical characteristics Covered area (m2
)
New San Miguel Calcite, gypsum, arsenopyrite,
pyrite, quartz
Gray, silt-clayey particles 100,855
Old San Miguel Calcite, gypsum, arsenopyrite,
quartz, pyrite
5688
30,126
Red tailings Gypsum, quartz, K-jarosite Brown-reddish 9178
26,281
14,415

soils, reaching a value of 94.7 % in the RT transects during the
dry season. Presence of Fe oxides in RT is responsible for the
color in these heaps. Iron was also the most abundant metal
measured in Zimapán tailings, but higher concentrations of As
than Zn were determined in gray and red tailings by Romero
et al. (2006) (Table 2). The sequence of the other metals in
Table 2 Concentrations of arsenic and heavy metals at the three sites (mg kg−1
)
Old San Miguel gray tailings (OSM)
Dry season surface Dry season 40 cm depth Rainy season surface Rainy season 40 cm depth
Median Range Median Range Median Range Median Range
As 5312 479–51,534 3692 124–19,166 7752 275–22,681 7278 159–23,570
Cd 100 2–3160 18 1–905 1763 22–3060 991 6–3404
Cu 165 12–2215 146 6–1818 6405 3923–11,062 7190 5084–8292
Fe (%) 17.9 7.3–54.7 11.8 29.2–74.6 39.6 6.6–58.7 36.4 7.9–62.8
Mn 751 288–13,011 738 156–10,909 2962 772–8474 1609 718–11,788
Pb 760 64–7503 546 30–3696 3468 408–4787 2890 83–4912
V 113 24–145 98 13–123 134 81–169 137 111–168
Zn 1285 152–58,648 973 56–70,159 25,683 254–32,430 13,879 99–50,233
pH 7.3 7.1–8.0 7.4 6.9–8.2 6 5.5–6.3 5.8 5.6–6.3
New San Miguel gray tailings (NSM)
As 1069 15–3468 313 0–1172 6492 459–16,666 7449 2343–14,331
Cd 277 106–411 46 5–285 1031 63–2628 1096 153–2016
Cu 994 223–1211 97 8–701 1154 55–2310 910 587–1520
Fe (%) 13.6 6.2–16.2 9.6 19.4–15.6 23.9 10.4–50.8 29.3 8.5–66.7
Mn 3139 605–5361 668 428–2683 5126 831–8417 3035.5 1012–11,623
Pb 3457 1307–4763 1374 237–6569 3093 190–5970 3194.5 1831–9758
V 68 59–219 64 34–132 126 91–181 84.5 44–140
Zn 2012 1375–14,631 870 130–1922 3052 364–29,464 3799 1698–53,348
pH 7.6 7.3–8.3 7.6 7.2–8.4 6 5.4–6.2 6.1 5.5–6.4
Red tailings (RT)
As 8426 1189–11,737 7585 3336–23,821 3910 407–7965 478 95–10,600
Cd 165 6–405 161 4–219 102 17–293 81 11–438
Cu 494 43–1252 447 2–856 194 45–718 132 34–1154
Fe (%) 54.6 17.6–94.7 29 12.1–70.9 24.8 13.2–40.6 13 7.4–45.7
Mn 881 629–8141 745 410–7592 1352 423–3311 975 342–3348
Pb 4685 419–12,526 4584 135–6587 2451 250–5814 1359 330–13,932
V 54 34–100 47 21–115 102 0–189 121 63–157
Zn 11,965 777–98,040 3312 94–74,819 1326 348–22,562 1388 138–33,752
pH 2.4 2.0–7.4 2.3 2.0–7.6 4.6 2.3–6.1 5.6 2.2–6.0
Tailing heapsa
Gray (total) Red (total) Gray (soluble mg/L) Red (soluble mg/L)
As 39,500 6200–82,500 17,500 3800–40,900 – 0.03–0.15 14.14 0.41–48.68
Cu 1600 300–4900 1300 500–3500 – Bdl 7.9 2.5–25.5
Fe 7.88 % 5.26–9.73 % 17.86 % 14–24.44 % – Bdl 114.5 71.3–897.5
Mn 3560 3300–3872 460 310–852 – – – –
Pb 9300 700–21,100 2400 1400–4100 – Bdl 0.7 <1.0–1.8
Zn 32,600 4100–21,100 6400 2200–17,400 – 0.2–1.0 114.3 22.5–400
Bdl below detection level
a
Data from Romero et al. (2006)

soils showed variations depending on the different sites,
depths, and seasons. Manganese and Pb exhibited overall
greater concentrations than Cu, with the exception of OSM
during the rainy season at both depths, where some Cu con-
centrations had values 2.5 times higher than Mn and Pb.
During the dry season, the RT transects displayed the greater
As medians at both depths, with sample concentrations from
1189 to 23,821 mg kg−1
, although the highest As value (51,
534 mg kg−1
) was measured at the base of OSM tailings. In
this season, the greatest median concentrations of Fe, Pb, and
Zn at the two depths were determined also in RT with sample
concentrations reaching 94.7 %, 12,526 mg kg−1
, and 98,
040 mg kg−1
respectively, whereas the highest Cu, Mn, and
Cd median concentrations were measured at NSM. However,
the largest values of Cu, Mn, Cd, and V were reported at OSM
impacted soils with 2215, 13,011, 3160, and 145 mg kg−1
,
respectively.
Metals and As concentrations had important increments
during the rainy season at OSM and NSM possibly due to
the decrease of pH (Table 2) with the consequence of acid
drainage of elements from the heaps to the land. In addition,
washout of tailings during the rainy season may have mobi-
lized As and heavy metals to the surrounding soils, as ob-
served in sediments close to tailings in the Xochula river by
Espinosa and Armienta (2007). Besides, many correlations
among As and metals were found for these sites in both sea-
sons (Table 3), reflecting their similar source. Differences be-
tween soils close to the two gray tailings may have resulted
from the fact that NSM is still in operation and OSM is an old
heap with a longest exposure time to atmospheric oxygen and
rain.
Cadmium, Cu, and Zn presented the highest median con-
centrations increasing at OSM during the rainy season with up
to 18, 39, and 20 times, respectively, in comparison to the dry
season in the surface samples, but up to 55, 49, and 14 times,
respectively, in the 40 cm depth samples showing the occur-
rence of important vertical transport of the elements, mainly of
those present as soluble species. For NSM, the increase of
median concentrations in the rainy season compared to the
dry season was 3.7 and 1.2 times higher for Cd and Cu, re-
spectively, whereas increases at 40 cm depth were around 24
and 9 times for those metals. Arsenic was higher in the rainy
season at OSM, with 1.5 and 2 times for surface and 40 cm
depth samples, respectively, than in the dry season, while at
NSM the increases of As for the rainy season were 6 and 24
times in average, showing also an important leaching due to
the rain.
An opposite situation occurred at RT where As and metal
concentrations had important decrements during the rainy sea-
son with the exception of Mn and V. This behavior, only at RT,
could be related with the low values of soil pH during the dry
season (close to 2) in comparison with the high values of 6.9–
8.3 at OSM and NSM. Besides, the hard cover formed by Fe
oxides may prevent the occurrence of wash-off processes in
RT heaps.
The As, Cd, Cu, Pb, V, and Zn measured concentrations in
both seasons presented greater values than those recommend-
ed for agriculture and industrial sites by the Canadian Council
of Ministers of the Environment (CSQG 2007).
Rodríguez et al. (2009) reported metal concentrations at the
tailings of a Spanish abandoned Pb-Zn mine in Ciudad Real
where Cd, Cu, and Pb concentrations had values of 2.9–54.5,
44.1–716.6, and 1243.2–93,900.9 mg kg−1
, respectively,
which, with the exception of Pb, were lower than the metal
concentrations measured at Zimapan’s soils, with values of 2–
3404, 12–11,062, and 30–13,932 mg kg−1
for Cd, Cu, and Pb,
respectively. Barrutia et al. (2011) reported metal contents also
in an abandoned Pb-Zn mine at Cantabria, Spain, finding Cd,
Pb, and Zn concentrations of 3–84, 340–32,600, and 1220–
61,300 mg kg−1
, respectively, which, as the other case with the
Table 3 Significant Spearman correlation at p ≤0.05 between superficial and 40 cm depth samples and between metals and As at the three tailings sites
>0.6
OSMS dry FeS–Fe40; As–Cd–Mn–Zn, Cd–Cu–Fe–Mn–Zn, Cu–Fe–Mn–Pb–Zn, Fe–Mn–Pb–Zn
OSM40 dry As–Cu, Cd–Cu–Mn–Pb–Zn, Fe–Mn, Mn–Pb–Zn
OSMS rainy CdS–Cd40, CuS–Cu40, FeS–Fe40, PbS–Pb40, ZnS–Zn40; As–V, Cd–Fe–Pb–Zn, Fe–Mn, Fe–Pb, Fe–Zn, Mn–Zn, Pb–Zn
OSM40 rainy As–Cd, Cd–Fe, Cd–Pb, Cd–Zn, Fe–Mn–Pb–Zn
NSMS dry ZnS–Zn40; As–Cd–Cu–Pb, Cd–Fe, Cd–Pb, Cu–Mn, Cu–Pb, Mn–Zn
NSM40 dry As–Cu, Cd–Zn
NSMS rainy ZnS–Zn40; As–Cd–Mn, As–Zn, Cd–Cu–Mn, Cu–Mn–Pb, Fe–Zn
NSM40 rainy As–Cu, Cd–Cu, Cd–Fe–Mn–V–Zn
RTS dry CdS–Cd40, FeS–Fe40, MnS–Mn40, VS–V40; Cd–Cu–Mn, Cd–Pb, Cu–Pb, Mn–Zn
RT40 dry Cd–Cu–Pb, Mn–Zn
RTS rainy VS–V40, As–Fe–Pb, Cd–Cu–Fe–Pb–Zn, Mn–V
RT40 rainy As–Mn, As–Zn, Cd–Cu–Fe–Pb–Zn
MS–M40 correlation of species concentrations between surface and 40 cm depth

exception of Pb, are lower than the concentrations found in
this study. The Bureau of Land Management of Arizona re-
ported that in an abandoned mine in Saginaw Hill, concentra-
tions of As in the tailings had values of 5348 to 30,
426 mg kg−1
(LaBerge et al. 2008), which are lower than the
reported concentrations of this study with concentrations up to
51,534 mg kg−1
although the concentration of Pb was 21,373–
49,539 mg kg−1
that is higher than the values found at
Zimapán (30–13,932 mg kg−1
).
In comparison with other studies carried out in Mexico,
Cortés-Jiménez et al. (2013) reported average concentrations
of Cu, Mn, Pb, and Zn of 254±26, 4520±225, 3291±358, and
3735±143 mg kg−1
in tailings at La Concha-Guerrero, which
are lower than those measured in this study. Talavera et al.
(2005) reported also lower concentrations of As and all the
metals determined in this study in tailings of six Mexican
mines located in Guerrero.
Romero et al. (2006) reported strong differences between
gray and red heaps in aqueous leachates obtained from gray
and red tailings at Zimapán (Table 2), with Fe and Cu concen-
trations below detection levels and As and Zn from 0.03 to
1 mg L−1
in solutions from gray samples, while median con-
centrations for Fe, Cu, As, and Zn were 114.5, 7.9, 14.1, and
114.3 mg L−1
, respectively, in leachates from red samples.
Lead was below detection level in gray tailings leachates
and up to 1.8 mg L−1
in red ones. The presence of limestone
plays an important role on gray tailings composition since
calcite is one of the main neutralizing minerals of acid mine
drainage (Blowes et al. 1998), which is characterized by high
concentrations of As and heavy metals. Calcite also promotes
the formation of secondary minerals as stated above.
Furthermore, an important decrease in water-soluble concen-
trations of As, Cd, Pb, and Fe with increasing CaCO3 was
observed in another tailings deposit located about 9 km NE
of Zimapán town (Armienta et al. 2012). However, as reported
in Table 2, soils influenced by red and gray tailings did not
have such strong concentration differences. Thus, heavy
metals and As presence in soils may mainly be due to
tailings particulates deposition, either carried by wind or rain
but less to their transport as soluble species. Similarly, Reza
et al. (2014) found low association of Pb and Zn with second-
ary Fe and Mn oxyhydroxides in soils impacted by mining,
and related this behavior with their transport as dust.
Regarding differences between concentrations at both
depths, most of the samples at the three sites presented lower
concentrations at 40 cm depth. In OSM, these differences
ranged from 5 to 85 % with the exception of Cd that presented
a median five times higher at the surface than at 40 cm depth
during the dry season. At this site, only Fe had a high corre-
lation between the two depths during the dry season, while
during the rainy season the correlation was higher between
both depths in the cases of Cd, Cu, Fe, Pb, and Zn suggesting
a similar vertical mobility of these elements. The
concentrations of As, Cd, Cu, Mn, Pb, and Zn measured dur-
ing the dry season at the NSM tailings transect were 4, 6, 10,
5, 2.5, and 2 times higher, respectively, at the surface than at
40 cm depth, whereas Fe and V were no more than 1.4 times
higher. Contrariwise, most of the median concentrations of As
and metals during the rainy season were lower at the surface
(although not with the maximum values). During the two sea-
sons, only Zn showed high correlation at the two depths at
NSM.
At RT, high Spearman correlations (>0.6 at p ≤0.05) were
found for Cd, Fe, Mn, and V between the two depths during
the dry season, and the concentrations of most species were
from 3 to 18 % higher at the surface than at 40 cm depth, but
Fe and Zn had concentrations 1.9 and 3.6 times higher at the
surface.
During the rainy season, no correlations were found at RT
between the two depths, with the exception of V which seems
to be very stable in these tailings; in addition, the differences
between surface and 40 cm depth concentrations were quite
higher than in the dry season, and As was eight times higher at
the surface, whereas the median concentrations for Cd, Cu, Fe,
Mn, and Pb in the dry season were from 30 to 90 % higher at
the surface suggesting a poor vertical transport probably due
to the nature of this stabilized soil.
Exceptions during the rainy season were V and Zn, which
presented slightly lower concentrations at the surface. The
observed behavior in the correlations probably results from
the settling of tailings particulates carried by the wind in the
dry season and leaching of As and most metals in the rainy
season.
Concerning the variation in the concentrations registered
for the species at different distances, no pattern was found
for any of the elements. In some cases, the concentrations
increased with distance and sometimes decreased. This can
be due to the irregular geography and that the three deposits
are uphill compared to the other points, which are close to the
river or to canyons, and then the transport by water or wind
can occur and vary throughout the year.
3.3 Sequential fractionation
Sequential fractionation (Fig. 3) shows that the lowest propor-
tion of all elements at the three tailings transects was contained
in the soluble fraction with up to 3.57 % for Cu, 2.39 % for
Mn, 3.61 % for Pb, 4.12 % for Zn, and 2.81 % for As. It was
followed by the interchangeable fraction in almost all samples.
Clear differences were observed in the proportion of elements
linked to the Fe and Mn oxyhydroxides (FeMnOOH) between
the soil transects starting from red (RT) with respect to those
starting from gray Old San Miguel (OSM) and New San
Miguel (NSM) tailings. While Pb, Cu, Mn, Zn, and As (except
the farthest sample) were mostly present in the FeMnOOH
fraction in RT impacted soils (from 39.48 to 91.87 %), they

comprised lower proportions (up to 26.43 %) in soil samples
influenced by the gray ones. In addition, the analyzed ele-
ments were mostly associated to the residual and organic
and sulfide fractions in all of the gray impacted samples with
up to 56.2 % for Cu, 49.1 % for Mn, 69.3 % for Pb, 61.2 % for
Zn, and 70.5 % for As. Predominance of the association with
the residual fraction was also observed by Arenas-Lago et al.
(2014), reporting even higher proportions, up to 70 % for Cu,
96 % of Mn, 68 % for Pb, and 97 % for Zn in soil samples
collected at a copper mine site in Touro, NW Spain.
Presence of elements mostly on the sulfide and organic and
residual fractions in soils close to the gray tailings indicates a
low influence of sulfide oxidation processes, whereas those
soils influenced by RT displayed a higher degree of oxidation.
It is well known that iron oxides possess a high capacity to
retain heavy metals and arsenic. Thus, the observed differ-
ences between red and gray tailings’ transects regarding the
proportion associated with Fe and Mn oxyhydroxides reflect
the importance of oxidation processes taking place at the tail-
ings, along with limestone presence that have increased the
formation of iron oxyhydroxides in RT with respect to OSM
and NSM. It is thus not surprising that the predominance of
this fraction in the elements distribution in soil samples is
influenced by RT. In addition, goethite has been reported in
RT (Romero et al. 2006). Differences in elements fraction-
ation may be ascribed mainly to the tailings characteristics
and oxidation degree since similar distributions of the ana-
lyzed elements were determined in samples influenced by a
certain tailing deposit.
Sequential fractionation is a proxy to the environmental
mobility of toxic metals and metalloids (Tessier et al. 1979;
Salomons 1995; Cai et al. 2002; Garcia et al. 2008;
Marabottini et al. 2013); in the applied scheme, the soluble
fraction contains the most mobile proportion of elements and
in decreasing mobility order: soluble>interchangeable>
FeMnOOH>sulfide and organic>residual. Results showed
that low proportions of all the analyzed elements are in the
highest mobile fraction in soils surrounding tailings impound-
ments. However, the following labile interchangeable fraction
may deliver important amounts of those contaminants present
in high concentrations (mainly As, Pb, Zn, and Mn) to the
environment. On the other hand, due to their prevalence in
the organic and sulfide and residual fractions, metals and ar-
senic are more stable in soils impacted by gray tailings, with
respect to those influenced by red ones where they are mostly
linked to iron and manganese oxyhydroxides. In addition, acid
pH in soils close to RT (Table 2) also enhance As and heavy
metals mobility (González-Corrochano et al. 2014).
Figure 3 also shows variations in the fractionation be-
havior with distance. A slightly higher proportion of solu-
ble As was observed in samples collected at the base of the
three tailings with respect to farther ones. The organic and
sulfide fraction of As decreased and the residual fraction
increased with distance in OSM transect, while an opposite
trend was observed in NSM. Most of the As was contained
in the FeMnOOH fraction in RT at the base and 60 m far,
but it represented less than 20 % in the sample collected at
80 m from RT, where it was mostly in the organic and
sulfide fraction. Relevance of iron oxyhydroxides on As
retention has been highlighted in many publications
(Dzombak and Morel 1990; Bowell 1994; Dold and
Fontboté 2001; Patinha et al. 2004). Its presence in the base
of RT may thus have played an important role on the de-
crease of As mobilization. The observed decrease in the
soluble fraction in the three transects and the increase in
the organic and sulfide fraction in the farthest sample of RT
transect indicate lowering of the As environmental mobility
upon moving away from tailings.
0%
20%
40%
60%
80%
100%
Old San Miguel
Sol Int Fe-Mn O-OH Org Res
0%
20%
40%
60%
80%
100%
New San Miguel
0%
20%
40%
60%
80%
100%
Red Tailings
Fig. 3 Sequential fractionation in soils collected at various distances
from OSM, NSM, and RT

Copper did not have a fractionation trend with distance
with most of the metal in the organic and sulfide, and re-
sidual fractions (29.78 to 49.62 % and 25.86 to 56.2 %,
respectively) at gray tailings transects, and in the iron and
manganese oxyhydroxides fraction (40.55 to 54.24 %) at
red tailings transect. High Cu association with iron oxides
was also observed by Ramos and Siebe (2007) in oxidized
tailings. An increase in the proportion of Mn in the residual
fraction with distance from tailings was observed from
OSM deposit, while it decreased in NSM and RT. Soluble
Mn decreased with distance in RT transect. These differ-
ences in the behavior of Mn among the three deposits main-
ly indicate less environmental mobility with distance from
RT and OSM with respect to NSM.
Soluble Pb decreased from OSM and RT, while it de-
creased and increased slightly from NSM. On the other hand,
the residual fraction decreased from NSM while it decreased
and increased in OSM and RT.
These variations with distance show an overall Pb mobility
decrease coming from OSM and RT, and an increase of that
supplied by NSM when moving away from tailings. Zinc
associated to the organic and sulfide fraction in OSM and in
the soluble fraction in the RT transects showed a clear de-
crease with distance. Conversely, Zn in the residual fraction
increased with distance in OSM and RT. Zinc fractionation did
not show a clear trend in NSM transect. These changes indi-
cate less Zn mobility in the farthest soils from OSM and RT
heaps.
Influence of limestone presence on soils pH was mostly
observed in RT transect since pH increased from about 2 in
the dry season at the tailings base to between 4 and 5 at 60 m
and about 7.5 in the 70 m far samples. This is also related to
the calcisol soil type present in this area. Low development of
oxidation processes along with calcite presence in gray tail-
ings and calcisol soil type have contributed to the fractionation
and relatively low mobility of As and metals provided by
these deposits to soils.
Differences in fractionation with distance result mainly
from tailings characteristics (mineralogy and oxidation de-
gree) and from the geochemistry of each element. Sequential
fractionation showed that environmental potential mobility of
As, Mn, Pb, and Zn decreased with distance from RT and
OSM, while Cu did not have a clear trend. In addition, the
analyzed elements did not show a tendency in the NSM tran-
sect. This lack of a pattern may be due to the fact that NSM are
still active and thus the nearby soils may receive influence of
tailings with diverse composition with time.
3.4 Concentrations in residential areas
With the aim to have an approach of the exposure levels to As
and metals by the population, samples were collected in two
residential areas surrounding the NSM tailings. Table 4 shows
the average concentrations of As and metals, where, surpris-
ingly, it is possible to observe that in a waste land located at
the back of NSM deposits at 100 m of a small residential area,
the concentration of As is more than five times higher than in
the tailings, and Cd, Fe, V, and Zn levels are also higher,
suggesting accumulation, although the concentrations de-
creased substantially with depth. The samples collected inside
the soils of a house in front of the previous site showed con-
centrations from 3 to 16 times lower than at the base of NSM
tailings, with the exception of As and V which presented con-
centrations around 3 times higher.
Regarding the concentrations close to a high school, with
the exception of V, the concentrations of the measured species
were lower than at the base of the NSM tailings from 30 % for
As to 23 times for Cd. According to the screening values for
residential soil recommended in Canada and the Netherlands,
there is a risk potential mainly for the high values of As and
Table 4 Concentrations of As and metals in residential areas close to New San Miguel (mg kg−1
)
Waste land located at the back of NSM (13) House in front of the waste land (15) Front of high school (16) CSQG NDL
Surface Sol+Int fraction 40 cm depth Surface 40 cm depth Surface Sol+Int fraction 40 cm depth
As 17,724 451 624 3416 18 732 73 480 12 55
Cd 693 n.a. 15 33 2 12 n.a. 8 10 12
Cu 837 100 99 61 6 190 6.5 136 63 190
Fe (%) 25.3 n.a. 7.2 9.1 1.1 n.a. n.a. 7.7 n.a. n.a.
Mn 1329 231 706 925 190 n.a. 109 856 n.a. n.a.
Pb 2719 309 688 362 355 530 48 1889 140 530
V 72 n.a. 130 191 16 250 n.a. 106 130 250
Zn 5931 664 154 177 150 720 94 1903 200 720
pH 7.4 7.7 7.8 8.2 7.8 8.1
n.a. not available, Sol+Int sum of soluble and interchangeable fractions, CSQG Canadian Soil Quality Guidelines (2007), NDL screening values for
potentially unacceptable risk (residential soil-use) for metals and metalloids in the Netherlands (Carlon 2007)

Cd which exceeded in the three sites the recommended screen-
ing values. For the other metals, Cu exceeded in the high
school the proposed value by the Canadian Guidelines, but
the values of the other metals were not exceeded. In the case
of the other two sites close to the NSM tailings, with the
exception of Cu, all the values are exceeded. This represents
a concern since the population is exposed to high concentra-
tions of metals in residential areas. On the other hand, as
shown in Table 4, the most available fractions (soluble and
interchangeable) in the waste ground in front of the residential
area are 2.6, 3.6, 11.4, and 11.2 % of the total concentration for
As, Cu, Pb, and Zn, respectively, whereas in the high school
the available concentration represents 10, 9.3, 10.7, and
11.5 % for As, Cu, Pb, and Zn, respectively. According to
the Risk Assessment Code, when the available fraction is be-
tween 1 and 10 %, there is a low environmental risk, which
was the situation for As and Cu at the high school.
4 Conclusions
This study reveals that acid mine drainage, water, and wind
erosion of tailings have polluted nearby soils with As, Cd, Cu,
Mn, Pb, V, and Zn in different grades.
Soils impacted by gray tailings presented higher concentra-
tions of As and metals during the rainy season, probably due
to the pH decrease, that is opposite to those close to red tail-
ings that presented higher concentrations during the dry sea-
son. This shows a different mobility of the species from both
types of deposits.
Arsenic and metal median concentrations were higher in
the surface than at 40 cm depth during the dry and rainy
seasons, with the exception of NSM in the rainy season where
most of the median concentrations were higher at 40 cm
depth.
Acid mine drainage is clearly occurring in red tailings and
impacting the soils mainly due to the low pH. Limestone
presence favors oxyhydroxide formation and arsenic and
metals sorption, but they may be released upon interaction
with acid water.
Highest As concentrations were found in RT impacted soils
during the dry season, representing the most important envi-
ronmental hazard. Arsenic is mostly present in the less mobile
residual and organic matter and sulfide fractions, in soils close
to gray tailings, and in the more mobile Fe-Mn oxide fraction
in soils close to red tailings.
The observed decrease in the soluble fraction in the three
transects and the increase in the organic and sulfide fraction in
the farthest sample of RT transect indicate lowering of the
environmental mobility of As upon moving away from
tailings.
Arsenic mobility through soils constitutes also an impor-
tant pollution source to shallow groundwater.
Concentration decreasing trends of the analyzed elements
with distance from tailings were not observed at the sampled
sites. Concentrations of As and metals in the residential areas
showed an important transportation in the whole studied zone,
which represents a threat to the health of the population of
Zimapán, which means that it is fundamentally important that
policy makers implement remedial actions to protect the
health of inhabitants and the surrounding environment.
Acknowledgments The authors acknowledge A. Aguayo, N.
Ceniceros, and O. Cruz for their participation in arsenic determinations,
and to Adolfo Hernández for drawing the maps. We also thank the anon-
ymous reviewers for valuable suggestions that greatly improved the
manuscript.
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