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Environ Earth Sci (2016)75:309

DOI 10.1007/s12665-015-5187-8

ORIGINAL ARTICLE

Further evidence for magnetic susceptibility as a proxy


for the evaluation of heavy metals in mining wastes: case study
of Tlalpujahua and El Oro Mining Districts
Juan Morales1 • Marı́a del Sol Hernández-Bernal2 • Pedro Corona-Chávez3 •

Avto Gogichaishvili1 • Francisco Bautista4

Received: 18 May 2015 / Accepted: 22 October 2015


Ó Springer-Verlag Berlin Heidelberg 2016

Abstract Magnetic susceptibility is nowadays used in Keywords Mining tailings  Magnetic susceptibility 
most areas of environmental research as a proxy for heavy Potentially toxic elements  Proxy
metal pollution in industrial and urban areas. Although the
relationship between magnetic susceptibility and concen-
tration of toxic elements in different environments has been Introduction
pointed out in several studies, mining wastes (tailings) have
hardly been investigated by magnetic methods. We report Industrial mining in Mexico has been developed since 1550
the relationships between magnetic susceptibility and and consequently there are abundant mining districts
potentially toxic elements monitored at 12 vertical ground associated with several billion tons of waste mining (tail-
profiles of the Tlalpujahua and El Oro mining districts, ings) scattered around the country (Corona et al. 2010).
western Mexico. Specific bulk magnetic susceptibility Nowadays, the study of the distribution and concentra-
(k) measurements, percentage frequency-dependent sus- tion of potentially toxic elements (PTE) contained in the
ceptibility (%XFD) determinations as well as the identifi- mining tailings acquires great relevance since it has been
cation of the magnetic carriers within the samples were recognized that such elements may cause serious environ-
accomplished using standard rock-magnetic techniques on mental and health problems to populations established in
geochemically well characterized sister samples. Magnetite their vicinity (Monroy et al. 2002; Armienta et al. 2003;
and/or Ti-poor titanomagnetite seem to be the main mag- Talavera et al. 2005; Ramos-Arroyo et al. 2004; Canet
netic carriers in the samples. Tight correspondence et al. 2008 and references therein). Moreover, due to social
between k and Fe concentrations, as well as Pb and As with and demographic aspects, among other reasons, tailings of
the iron content were found. This association seems to hold abandoned mining districts in Mexico are now occupied
also for pH variations. and serve as settlements for various inhabitant groups.
These studies are carried out traditionally by means of
geochemical analysis, which are expensive, laborious and
& Juan Morales time-consuming. The need for fast and inexpensive moni-
jjulio1962@yahoo.com.mx; jmorales@geofisica.unam.mx toring tools of heavy metal pollution has led to the search
1
of other methods of determination (Morton-Bermea et al.
Laboratorio Universitario de Geofı́sica Ambiental (LUGA),
Unidad Michoacán del Instituto de Geofı́sica, UNAM
2009). The correlation between magnetic susceptibility and
Campus Morelia, Mich, Mexico heavy metal content has been reported in numerous works
2
Escuela Nacional de Estudios Superiores (ENES), Unidad
(Petrovsky et al. 1998, 2001; Durza 1999; Shu et al. 2001).
Morelia, UNAM Campus Morelia, Mich, Mexico This correlation could be due to the fact that heavy metal
3 elements are incorporated into the lattice structure of the
Instituto de Investigaciones en Ciencias de la Tierra,
UMSNH, Morelia, Mich, Mexico ferrimagnetics during combustion process or are adsorbed
4 onto the surface of ferrimagnetics already present in the
Laboratorio Universitario de Geofı́sica Ambiental (LUGA),
Centro de Investigaciones en Geografı́a Ambiental, UNAM environments (Petrovsky et al. 1998; El Baghdadi et al.
Campus Morelia, Mich, Mexico 2012).

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However, except by the study by Matasova et al. (2005)


carried out in wastes of the mining industry in Western
Siberia, Russia and very recently that of Pérez et al. (2014)
accomplished in a metallurgical area in the San Luis Potosi
State, Mexico; magnetic methods have not been applied
systematically to the study of tailings in spite of the fact
that magnetic measurements are sufficiently sensible to
detect the magnetic signal of the minor fraction of ferro-
magnetic materials, in most of the cases with concentra-
tions less than 1 % (Chaparro 2006). Their results remain
scarce.
Because of the more than 60 years of abandon, the
Tlalpuhajua and El Oro mining districts, western Mexico
(see below for details), represent a potentially pollution
problem due to the more than 60 tons of wastes dispersed
on the area estimated by Uribe Salas (2008).
Fig. 1 Location map of the Tlapujahua-El Oro Mining District
Aimed to overcome this situation, we focused on eval-
(TOMD)
uating the potentiality of magnetic methods to reliably
determine PTE concentrations in tailings in a faster and an
economical way; magnetic susceptibility determinations Corona-Chávez 2006 and references therein) and is
(the key magnetic parameter used in this study) are low- emplaced over a Jurassic-Early Cretaceous rock basement
cost, easy and fast to obtain. (Centeno-Garcı́a et al. 2003), Fig. 2. The surface covered
We report the relationships between magnetic suscep- by the tailings dams was estimated by Martı́nez-Medina
tibility and pH with PTEs, monitored at 12 different ver- (2009) in approximately 62 ha.
tical ground profiles in tailings of the Tlalpujahua and El
Oro mining districts, western Mexico.
Samples

Study area Samples were taken from tailings belonging to two mining
localities: Tlalpuhajua and El Oro, Michoacán and Estado
Historical background de Mexico states, respectively.

It is widely recognized that the extraction of metals in Tlalpujahua


Mexico began since pre-Hispanic times (e.g. Horcasitas de
Barros 1981; Maldonado 2005; Martı́nez-Medina 2009), At the Tlalpujahua District thickness of tailings varies from
while the formal mining activity until the XVI century, 2 up to 48 m (Fig. 3a). According to Martı́nez-Medina
during the colonial era. In this time, a series of exposed (2009) textures are diverse, but using soil texture triangle
silver and gold veins were located and exploited for more recognizable horizons are classified as silty loam, sandy
than five centuries in the heart of the modern cities of loam, loam sand, silty clay loam, silt, silty clay, medium
Tlalpujahua and El Oro (hereafter referred to as TOMD); loam and sand.
which was known as the ‘‘Real de Minas of Tlalpujahua’’
(Corona et al. 2010) and where more than 60 tons of wastes El Oro
were generated and disposed of, as estimated by Uribe
Salas (2008). Thickness of tailings at El Oro District varies from 1 up to
The TOMD is located at the boundaries of the 20 m (Fig. 3b). Textures of the tails correspond to loamy
Michoacán and Estado de Mexico states (Fig. 1) and is part sand, silt, silty loam, clay loam and silty clay loam. In both
of the hydrological basin ‘‘Lerma Santiago River’’ (Corona cases, the textures are different and there is no predomi-
et al. 2010). Although the TOMD is recognized essentially nance of any, except in the profile of El Carmen (Tlalpu-
as a gold-deposit, the mineralization in this district is jahua), where certain homogeneity is observed,
considered as a part of the big-silver metallogenic province predominantly silty loam, because the deposit is the result
(Ostrooumov and Corona Chávez 1999; Albinson et al. of the overflow of the dam tailings Los Cedros in 1937.
2001). The TOMD is located within the Miocene-Pliocene At both mining localities, samples of 1.5–2 kg in
Trans-Mexican Volcanic Belt (Morales-Gámez and weight were taken within each profile every 20 cm,

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Environ Earth Sci (2016)75:309 Page 3 of 10 309

Fig. 2 Simplified geological


map of TOMD. Modified from
‘El Oro de Hidalgo E14-A16’
chart of ‘Servicio Geológico
Mexicano 2000’

Fig. 3 Current view of Cedros tailings dam at Tlalpujahua (a) and Tiro México at El Oro (b)

packed into plastic bags and identified sequentially quartering. Finally, they were stored in hermetic
accordingly to the corresponding profile (S) and horizon cylindrical PVC containers.
(H). Particular attention of sampling was taken when
clear evidence of different horizons was evident. Some
isolated samples, when profile excavation was not Methodology
possible, were also taken. In total, 12 profiles were
sampled (Fig. 4); eight from Tlalpujahua and four from Background
El Oro, yielding 57 samples. Samples were dried by
placing them in an oven at a temperature \40 °C for a Based on the results of a geochemical and mineralogical
period of 12 h, and were then homogenized by study on the variations within Au-tailings from

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Fig. 4 Location of sampled


sites

XRF methodology

The procedure for pressed-pellet sample-preparation and


XRF analysis are widely described elsewhere (e.g. Lozano
and Bernal 2005). Chemical composition of samples was
determined by X-ray fluorescence using a Xenemetrix
energy dispersion spectrometer (EDXRF X-Calibur, with
Rh tube and a Beryllium detector) at Laboratorio Univer-
sitario de Geofı́sica Ambiental (LUGA) facilities.

Fig. 5 SiO2 vs Fe2O3tot plot from the mining district Tlalpujahua-El Magnetic methodology
Oro
Magnetic susceptibility is directly proportional to the
quantity and grain size of the ferromagnetic or ferrimag-
Tlalpujahua-El Oro mining district, Corona et al. (in netic materials in a sample (Verosub and Roberts 1995).
preparation) noted certain linear variation between some Therefore, among other information, magnetic suscepti-
mayor element (ME) oxides (CaO, MgO, Al2O3, Fetot) bility measurements provide a straightforward and rapid
when plotted against the corresponding SiO2 and pH val- estimation of the iron content (Fe concentration) in a
ues. Worth of noting for the aim of the present study is the sample. Powdered samples were packed into standard
inverse linear relationship between SiO2 (the oxide nor- 10 cc cubic plastic containers for the magnetic analysis.
mally used in geochemical studies as an evolution param- These specific bulk magnetic susceptibility (k) and per-
eter, depending on the mineral phases that crystallize) and centage frequency-dependent susceptibility (%XFD) mea-
Fetot (Fig. 5). Based on this observation, it seems natural to surements were carried out using a Bartington MS2
follow a symmetrical approach to that employed in geo- susceptibility meter at LUGA facilities. Alternatively, the
chemical analysis but using the Fe concentration (or identification of the magnetic carriers within the samples
alternatively magnetic susceptibility, which is the key was accomplished by means of continuous low-field high-
parameter used as a proxy in magnetic studies) as the basis temperature susceptibility (k–T) curves or saturation-mag-
for an alternatively magnetic methodology for the study of netization curves (thermomagnetic curves) using standard
PTEs, see below. techniques at LUGA.

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Environ Earth Sci (2016)75:309 Page 5 of 10 309

Physical–chemical analysis

Electric conductivity and pH measurements were done at


the chemistry lab of the ENES facilities using a multi-
parametric kit HI 2020.

Results

Most samples present null and/or very low frequency


dependence of k (%XFD % 0), except those situated at the
very upper part of the profiles (10 % B %XFD B 15 %). Fig. 7 k values of tailing samples vs their corresponding XRF-
This fact reflects a considerable amount of superparamag- determined Fe concentrations (FeXRF). Tight correspondence between
netic particles (SP) within the particulate matter (PM) k and Fe concentrations variations is observed
\0.03 lm. In most of the cases, magnetite or Ti-poor
titanomagnetite seem to be the main magnetic minerals corresponding volume susceptibility j. Figure 11 shows
within the samples, with variable proportions of other the obtained correlations.
weaker phases (Fig. 6).
Magnetic susceptibility values of tailing samples were
plotted against their corresponding XRF-determined Fe Discussion and concluding remarks
concentrations (FeXRF) values. The results of such corre-
lation are presented in Fig. 7. Note the tight correspon- In a study carried out in lake sediments of lake Nechranice,
dence between k and Fe concentrations variations. This the captive area being typical for intensive industrial and
correspondence seems to hold also for pH variations mining activity from Northern Bohemia, Petrovsky et al.
(Fig. 8). It is also worth noting the predominantly alkaline (1998) found no positive correlation with magnetic sus-
character of most of the tailings (7.5 \ pH \ 8.5), asso- ceptibility of toxic elements present in the samples, except
ciated to very low conductivity values (EC \80 lS/cm), for Mn; arguing that the practically random observation of
which suggests an active leaching processes within the magnetic susceptibility data could be caused by complex
tailings. effects of various pollution sources.
Following this approach, the plots of different trace On the contrary, Matasova et al. (2005) found an inverse
elements (TE) present in the tailing samples make evident correlation between Pb and Zn content in the upper ground
the correlation between these elements and the iron content layer and magnetic susceptibility in an environmental study
(Fe concentration) (Fig. 9). Figure 10 shows the individual of areas polluted with wastes of the mining industry in
regression that best represents the correlation between Western Siberia. The authors concluded that the mecha-
some TE concentrations with the corresponding FeXRF nisms responsible for the relationships between magnetic
within the samples. characteristics of the deposit and the degree and charac-
In order to verify the above presented correlations, TE teristic of its pollution should be quite different from those
concentrations of tailing samples were plotted against in industrial and urban areas.

Fig. 6 Representative
thermomagnetic curves. Both
curves show similar single
ferrimagnetic phases (Ti-poor
titanomagnetite). Curie
temperatures (Tc) of the
ferrimagnetic phases are quite
similar

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Fig. 8 pH vs k within the


tailing samples. A close
correspondence variation is also
observed. Abbreviations on the
horizontal axis are as follows:
S stands for profile while H for
horizon, so that S5H1
corresponds to sample taken
from horizon 1 at profile 5

As properly pointed out by Matasova et al. (2005),


mining wastes seems to belong to a special class of objects
that has not been sufficiently investigated by magnetic
methods, in which an inverse correlation between PTE and
magnetic susceptibility exists.
Such an inverse correlation could be explained in terms
of the combined results of the active leaching processes
and significant differences in atomic weight between Fe
(*55.8) and some PTEs (e.g. As: *74.9; Pb: *207.2).
Samples at the bottom show low (high) Fe(Pb) concen-
trations. This relationship varies inversely through the
profile so that at the upper part of the tailings higher Fe
concentrations and lower Pb concentrations are observed
(Fig. 12). In the case of elements with similar atomic
weights to that of Fe (Cr: *52.0; V *51.0), direct linear
Fig. 9 Overview of trends followed by different trace elements (TE) correlations between them are observed (Fig. 13).
with the iron content (Fe concentration) On the other hand, recent environmental investigations
include a series of rock-magnetic measurements (e.g.
NRM, IRM, SIRM ARM, etc.), and the calculation of
Sarris et al. (2009) also confirm that magnetic suscep- different ratios (e.g. S, XLF/SIRM, FD/ARM, etc.) as
tibility measurements provide the basis for an environ- indicators of pollution in addition to magnetic suscepti-
mental study in polluted areas with the results they bility determinations. Their use is widely employed and
obtained in an environmental study for pollution in the area represents a comprehensive way to fully characterize the
of Megalopolis power plant (Peloponnesos, Greece) where magnetic mineralogy. However, their inclusion in any
a very high correlation among magnetic properties; spe- environmental study protocol would make magnetic
cially between v and Fe was observed. investigations lose some of their distinctive characteristics
Likewise the former study, some other recent investi- which make them nowadays an alternative to traditional
gation (e.g. Zhang et al. 2012; Pérez et al. 2014) relates the techniques as a proxy for heavy metal pollution investi-
enhancement of magnetic susceptibility values with gations; namely, speediness, easiness and economy.
increased concentration of PTEs based on the high positive Furthermore, pH measurements seem to be also an
correlation coefficients between these elements and mag- indirect and complementary sign of variation in Fe con-
netic susceptibility. It is worth noting, however, that the centration and, consequently, of potentially polluted areas.
outcomes and conclusions of these studies are the result of Among the analyzed elements, Pb and As versus j plots
investigations carried out mainly on surface soils collected show the highest correlation coefficients. Magnetic sus-
in the vicinity of the tailings and on farmland soil irrigated ceptibility, along with k–T curves, can be used as a pre-
with polluted river water in the vicinity of a steel plant, liminary fast and inexpensive method in the evaluation of
respectively. PTE content in mining wastes.

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Fig. 10 Trends followed by different trace elements (TE) plotted against SiO2 content (left part) and against the iron content (Fe concentration,
right part). Note the higher R2 value for plots on the right side, compared to the corresponding value for plots on the left part

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Fig. 11 a, b Trends followed by different trace elements (TE) with magnetic susceptibility (k)

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Fig. 12 Pb vs v plots along a single profile. Samples at the bottom of the profile show low v values that gradually increase, up to higher values at
the top of the profile. The situation for Pb is the opposite; gradually decreasing values from bottom to top of the profile

Fig. 13 Cr and V (atomic weights close to that of Fe) vs Fe concentration plots. Note the direct linear correlations with Fe followed by these
elements

A detailed and quantitative identification of polluted Armienta MA, Talavera O, Morton O, Barrera M (2003) Geochem-
areas should be based on a comprehensive study, focused istry of metals from mine tailings in Taxco, Mexico. Bull
Environ Contam Toxic 71:387–393
on those areas highlighted by the magnetic results as the Canet C, Corona-Chávez P, Lozano-Santa Cruz R (2008) Geologı́a,
most probable contaminated areas. geoquı́mica e impacto ambiental de residuos mineros en México;
e Historia de la minerı́a en México: Sesiones especiales del. XI
Acknowledgments The authors are grateful to Doris A. Dı́az and Coloquio de Mineralogı́a de la Sociedad Mexicana de Miner-
Julio C. Gómez, undergraduate students who actively participated in alogı́a, 7–9 de mayo, Centro de Ciencias de la Tierra de la
this project. Neftali Razo is acknowledged for the supervision of Universidad Veracruzana, Boletı́n de Mineralogı́a 18, p 98
physical–chemical analysis. Gabriela Solis-Pichardo is greatly Centeno-Garcı́a E, Corona-Chávez P, Talavera-Mendoza O, Iriondo
acknowledged for her careful review of the manuscript for an A (2003) Geology and tectonic evolution of the western
appropriate grammatical style. This study was supported by UNAM- Guerrero terrane—a transect from Puerto Vallarta to Zihu-
PAPIIT project IA102413. atanejo, Mexico. In: Geologic transects across Cordilleran
Mexico, Guidebook for the field trips of the 99th Geological
Society of America Cordilleran Section Annual Meeting, Puerto
Vallarta, Jalisco, Mexico, April 4–6, 2003: México, D.F.,
Universidad Nacional Autónoma de México, Instituto de
References Geologı́a, Publicación Especial 1, Field trip 9, p 201–228
Chaparro MAE (2006) Estudios de parámetros magnéticos de
Albinson T, Norman DI, Cole D, Chomiak BA (2001) Controls on distintos ambientes relativamente contaminados en Argentina y
formation of low-sulfidation epithermal deposits in Mexico: Antártica. Monografı́as del Instituto de Geofı́sica, UNAM, p 107
constraints from fluid inclusion and stable isotope data. Soc Econ Corona Chávez P, Uribe Salas JA, Razo Pérez N, Martı́nez Medina
Geol Spec Pub 8:1–32 M, Maldonado Villanueva R, Ramos Arroyo YR, Robles

123
309 Page 10 of 10 Environ Earth Sci (2016)75:309

Camacho J (2010) The impact of mining in the regional Pérez I, Romero FM, Zamora O, Gutiérrez-Ruiz ME (2014) Magnetic
ecosystem: the Mining District of El Oro and Tlalpujahua, susceptibility and electrical conductivity as a proxy for evalu-
Mexico. De Re Metallica 15:21–34 ating soil contaminated with arsenic, cadmium and lead in a
Durza O (1999) Heavy metals contamination and magnetic suscep- metallurgical area in the San Luis Potosi State, Mexico. Environ
tibility in soils around metallurgical plant. Phys Chem Earth Earth Sci 72:1521–1531
24:541–543 Petrovsky E, Kapicka A, Zapletal K, Sebestova E, Spanila T, Dekkers
El Baghdadi M, Barakat A, Sajieddine M, Nadem S (2012) Heavy MJ, Rochette P (1998) Correlation between magnetic parameters
metal pollution and soil magnetic susceptibility in urban soil of and chemical composition of lake sediments from Northern
Beni Mellal City (Morocco). Environ Earth Sci 66:141–155 Bohemia—preliminary study. Phys Chem Earth 23:1123–1126
Horcasitas de Barros ML (1981) Una Artesanı́a con Raı́ces Pre- Petrovsky E, Kapicka A, Jordanova N, Boruvka L (2001) Magnetic
hispánicas en Santa Clara del Cobre. Colección Etnologı́a. properties of alluvial soils contaminated with lead, zinc and
INAH, México cadmium. J Appl Geophys 48:127–136
Lozano R, Bernal JP (2005) Characterization of a new set of eight Ramos-Arroyo YR, Prol-Ledesma RM, Siebe-Grabach C (2004)
geochemical reference materials for XRF major and trace Caracterı́sticas geológicas y mineralógicas e historia de extrac-
element analysis. Revista Mexicana de Ciencias Geológicas ción del Distrito de Guanajuato, México. Posibles escenarios
22(3):329–344 geoquı́micos para los residuos mineros. Rev Mex Cienc Geol
Maldonado BE (2005) Metalurgia Tarasca del Cobre en el Sitio de 21:268–284
Itziparátzico, Michoacán. FAMSI, México Sarris A, Kokinou E, Aidona E, Kallithrakas-Kontos N, Koulouri-
Martı́nez-Medina M (2009) Diagnóstico de impacto ambiental dakis P, Kakoulaki G, Droulia K, Damianovits O (2009)
causado por la minerı́a en el Distrito Minero El Oro-Tlalpujahua Environmental study for pollution in the area of Megalopolis
mediante el uso de un sistema de Información Geográfica (SIG). power plant (Peloponnesos, Greece). Environ Geol
Msc Thesis, Universidad Michoacana de San Nicolás de 58:1769–1783
Hidalgo, Morelia, Mich. México Shu J, Dearing JA, Morse AP, Yu LZ, Yuan N (2001) Determining
Matasova GG, Kazansky AY, Bortnikova SB, Airijant AA (2005) The the sources of atmospheric particles in Shanghai, China, from
use of magnetic methods in an environmental study of areas magnetic and geochemical properties. Atmos Environ
polluted with non-magnetic wastes of the mining industry (Salair 35:2615–2625
region, Western Siberia, Russia). Geochem Explor Environ Anal Talavera O, Yta M, Moreno R, Dótor A, Flores N, Duarte C (2005)
5:75–89 Mineralogy and geochemistry of sulfidebearing tailings from
Monroy M, Dı́az-Barriga F, Razo I, Carrizales L (2002) Evaluación silver mines in the Taxco, Mexico area to evaluate their potential
de la contaminación por arsénico y metales pesados (Pb, Cu, Zn) environmental impact. Geofis Int 44:49–64
y análisis de riesgo en salud en Villa de la Paz-Matehuala, S. Uribe Salas JA (2008) Historia de la Minerı́a en Michoacán. Morelia,
L. P., Universidad Autónoma de San Luis Potosı́, Instituto de Universidad Michoacana de San Nicolás de Hidalgo, Sociedad
Metalurgia, Nota Informativa, p 7 Mexicana de Mineralogı́a, Museo Tecnológico del Siglo XIX
Morales-Gámez M, Corona-Chávez P (2006) Geotecnia y prob- ‘‘Las Dos Estrellas’’, 2 vols. Morevallado Editores, Morelia,
lemática de extracción en los bancos de rocas ornamentales de la Michoacán
región de Tlalpujahua. Ciencia Nicolaı́ta 43:113–130 Verosub KL, Roberts AP (1995) Environmental magnetism: past,
Morton-Bermea O, Hernandez E, Martı́nez-Pichardo E, Soler- present and future. J Geophys Res 100:2175–2192
Arechalde AM, Lozano Santa-Cruz R, González-Hernández G, Zhang C, Appel E, Qiao Q (2012) Heavy metal pollution in farmland
Beramendi-Orosco L, Urrutia-Fucugauchi J (2009) Mexico City irrigated with river water near a steel plant—magnetic and
topsoils: heavy metals vs. magnetic susceptibility. Geoderma geochemical signature. Geophys J Int 192(3):963–974. doi:10.
151:121–125 1093/gji/ggs079
Ostrooumov M, Corona Chávez P (1999) Ensayo metalogénetico del
Estado de Michoacán. In: Universidad Michoacana de San
Nicolás de Hidalgo y Gob (Ed) Carta Geológica de Michoacán
Escala 1:25000. del Edo. de Mich, pp 91–107

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