Chemical Geology 456 (2017) 72–84

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Chemical Geology

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Impact of low denudation rates on soil chemical weathering intensity:

A multiproxy approach
Yolanda Ameijeiras-Mariño a, Sophie Opfergelt a,⁎, Jérôme Schoonejans b, Veerle Vanacker b, Philippe Sonnet a,
Jeroen de Jong c, Pierre Delmelle a
a
Université catholique de Louvain, Earth and Life Institute, ELIe, L7.05.10 1348 Louvain-la-Neuve, Belgium
b
Université catholique de Louvain, Earth and Life Institute, George Lemaître Center for Earth and Climate Research, L4.03.08 1348 Louvain-la-Neuve, Belgium
c
Université Libre de Bruxelles, Department of Earth and Environmental Sciences, CP160/02. Avenue F.D. Roosevelt 50, 1050 Brussels, Belgium

a r t i c l e i n f o a b s t r a c t

Article history: Quantifying the influence of denudation, i.e., physical erosion and chemical weathering, on soil weathering inten-
Received 18 August 2016 sity is an important component for a comprehensive understanding of element biogeochemical cycles. The rela-
Received in revised form 24 February 2017 tion between the weathering intensity and the denudation rate is not clear and requires further investigation in a
Accepted 4 March 2017
variety of climatic and erosional settings. Here, in the Betic Cordillera (southern Spain), we assess the soil chem-
Available online 8 March 2017
ical weathering intensity with a multiproxy approach combining different indicators of chemical weathering of
Keywords:
the soil: the Total Reserve in Bases (TRB), the content in Fe-oxides, the quartz and clay content, the soil cation
Chemical weathering exchange capacity (CEC), and the silicon (Si) isotope composition of the clay-sized fraction. Our multiproxy ap-
Soil weathering intensity proach demonstrates that in this semi-arid environment at low denudation rates, an increasing denudation rate
Low denudation rates decreases the soil weathering intensity, whereas Si mobility remains limited. Our results converge with previous
Semi-arid environment conclusions based on chemical mass balance methods in the same geological setting. Mass balance methods, and
Betic cordillera particularly Chemical Depletion Fractions (CDF), are based on the immobility of a refractory element (commonly
Silicon isotopes zirconium, Zr) relative to major cations in soils. Interestingly, our study suggests that a weathering index such as
the TRB may provide a useful complement to assess soil chemical weathering intensity in eroding landscapes
where the application of chemical mass balances may be hampered by potential Zr mobility in the soil or by het-
erogeneity of Zr concentrations in the bedrock.
© 2017 Elsevier B.V. All rights reserved.

1. Introduction
The Critical Zone is the uppermost part of Earth surface where chem-
ical, biological, physical and geological processes interact to support life
(National Research Council, 2001; Brantley et al., 2007). Soil cover influ-
ences the interactions occurring within this upper layer and it can be
thought of as a feed-through reactor, with a thickness controlled by
the balance between the removal of material by denudation processes,
i.e., the total loss of material from soils by both physical and chemical
processes, and the advance of the weathering front down to the bedrock
(e.g., Heimsath et al., 1997; Anderson et al., 2007). We can therefore ex-
pect denudation and weathering processes to be closely linked. Under-
standing the relationship between denudation and weathering
⁎ Corresponding author.
E-mail addresses: yolanda.ameijeiras@uclouvain.be (Y. Ameijeiras-Mariño),
sophie.opfergelt@uclouvain.be (S. Opfergelt), jerome.schoonejans@uclouvain.be
(J. Schoonejans), veerle.vanacker@uclouvain.be (V. Vanacker),
philippe.sonnet@uclouvain.be (P. Sonnet), jdejong@ulb.ac.be (J. de Jong),
pierre.delmelle@uclouvain.be (P. Delmelle).
processes is of great importance, as they control soil physical and chem-
ical properties. Moreover, weathering processes have important impli-
cations for the global carbon cycle and the climate through the
consumption of atmospheric CO2 by silicate weathering (review in
Goudie and Viles, 2012).
The relationship between denudation and weathering is traditional-
ly studied through mass-balance calculations using the chemical deple-
tion fraction (CDF, dimensionless) that represents the enrichment or
depletion of an immobile element within the soil column relative to
the parent material (e.g., Riebe et al., 2004). The relation between the
weathering intensity (CDF) and the denudation rate is not clear.
Previous work has tackled this relation (e.g., global compilations in
Dixon and von Blanckenburg, 2012 and in Ferrier et al., 2016) but the
conclusions remain diverse and highlight a controversy. While some
studies have shown a negative relation between CDF and denudation
rate (e.g., Dixon et al., 2012), others show no specific pattern (e.g.,
Riebe et al., 2004; Dixon et al., 2009). Thus, more work across all climatic
and erosional settings is needed to resolve the controversy.
The CDF estimations are commonly based on zirconium, which is
considered to be conservative in the soil. There are number of studies

http://dx.doi.org/10.1016/j.chemgeo.2017.03.007
0009-2541/© 2017 Elsevier B.V. All rights reserved.
 Y. Ameijeiras-Mariño et al. / Chemical Geology 456 (2017) 72–84
that have successfully used the CDF based on Zr concentrations to con-
strain the chemical weathering intensity (e.g., Riebe et al., 2004; Dixon
et al., 2009; Dixon et al., 2012; Ferrier et al., 2012; Schoonejans et al.,
2016a). In certain environments, such as shown by Kurtz et al. (2000)
for volcanic soils in Hawaii, Zr mobility can increase with rainfall, lead-
ing to potential underestimation of weathering losses (Hill et al., 2000;
Hodson, 2002). As such, other conservative elements (e.g. Hf, Ti, Nb)
have been used as an alternative (Kurtz et al., 2000; Little and Lee,
2010). In some areas, the heterogeneity in immobile element concen-
trations in the parent material might add uncertainty to the mass bal-
ance estimates (Ferrier et al., 2012).
Soil weathering indexes may provide complementary methods to
constrain the relationship between denudation and weathering. Chem-
ical weathering indexes such as the Chemical Index of Alteration (CIA)
or the Weathering Index of Parker (WIP) have been applied in the
past to study the relationship between weathering and soil production
(Burke et al., 2007; Larsen et al., 2014).
Here, we test a multiproxy approach to derive soil weathering in-
dexes in a semi-arid region where the mass balance approach based
on CDF was successfully applied, the Spanish Betic Cordillera
(Schoonejans et al., 2016a). The existence of a good correlation between
our approach and CDF estimates would generate complementary infor-
mation to quantify chemical weathering intensity in specific environ-
ments where the use of CDF might be prevented (i.e., mobility of the
reference elements and/or heterogeneity in the parent material). Our
approach combines physico-chemical soil properties, mineralogy and
isotope geochemistry to derive soil weathering indexes and estimate
the soil weathering intensity. Five weathering indexes classically used
in soil science are considered (the Total Reserve in Bases, TRB;
Herbillon, 1986), the amount of Fe-oxides, the amount of quartz, the
clay content (fraction b2 μm), the cation exchange capacity) and com-
bined with the silicon (Si) isotope composition of the clay-sized
fraction.
The Si isotope composition of the clay-sized fraction can be used as a
weathering index as Si isotopes respond to soil chemical weathering
and clay formation (Ziegler et al., 2005a; Ziegler et al., 2005b; Georg et
al., 2007; Opfergelt et al., 2009, 2010, 2011, 2012; Bern et al., 2010;
Pogge von Strandmann et al., 2012; Cornélis et al., 2014). The applica-
tion of Si isotopes to assessing the response of chemical weathering to
physical denudation has been suggested previously (Georg et al.,
2007; Opfergelt and Delmelle, 2012) although no publications have ex-
plored this application of Si isotopes so far.
2. Environmental setting
The study site is located in the Betic Cordillera in Southeast Spain,
Almería province, the southernmost extreme of the European Alpine
belt. The cordillera is subdivided in the External and Internal Zones.
This study focuses on the eastern part of the Internal Zone (Fig. 1).
Three catchments with comparable lithology and catchment size have
been selected along a gradient of denudation rates (Bellin et al.,
2014): from north-west to south-east, in the Sierra de las Estancias
(EST), Sierra de los Filabres (FIL-1) and Sierra Cabrera (CAB). The FIL-1
and CAB catchments belong to the Nevado-Filábride geological com-
plex, whereas the EST catchment is part of the Alpujárride complex.
Both complexes underwent similar metamorphic evolutions at different
geological times (López et al., 2001). According to Junta de Andalucía
(2004) the main lithology of these catchments is mica schist with a
local occurrence of quartzite and phyllite. In-situ produced 10Be denu-
dation rates for the eastern Betic Cordillera (Vanacker et al., 2014)
range from 34 ± 24 mm/kyr for Sierra de las Estancias (n = 5), 54 ±
25 mm/kyr for Sierra de los Filabres (n = 8) to 164 ± 74 mm/kyr for Si-
erra Cabrera (n = 3). The spatial pattern and magnitude of 10Be based
denudation rates are consistent with tectonic uplift constrained by
Braga et al. (2003) and Masana et al. (2005) based on marine deposits
and trenching observations (Table 1, Bellin et al., 2014).
73
Average annual precipitation ranges from 275 mm/yr in CAB to
425 mm/yr in EST, while mean annual temperature ranges from 17 °C
in CAB to 12 °C in EST (García, 2009). Evapotranspiration varies between
900 mm/yr for CAB and 794 mm/yr for EST (Junta de Andalucía, 2008).
Following the UNEP's aridity index (ratio evapotranspiration/rainfall;
Barrow, 1992) the study sites are characterized by a semi-arid climate
(Table 1). In the three catchments, the dominant vegetation type is
Mediterranean shrub characterized by a sclerophyllous and thorny veg-
etation (locally known as matorral), with some remnants of Quercus
trees at higher altitudes (Bellin et al., 2011; Table 2).
In each catchment (or its close vicinity), two profiles were sampled
on exposed ridgetops to avoid the complexities of soil-forming process-
es associated with lateral transport of chemical fluids and soil particles
along slope. The sampling sites have similar slope gradients, between
14 and 28°. The sampling sites were selected avoiding locations with
clear anthropogenic disturbances such as quarrying or terracing activi-
ties. These soil profiles present no evidences of strong anthropogenic
perturbations (Schoonejans et al., 2016a).
3. Materials and methods
3.1. Sampling and pre-treatments
Soil description and sampling was conducted in September 2013, as
part of a larger sampling campaign described in Schoonejans et al.
(2016a) and Schoonejans et al. (2016b). The soil profiles were sampled
in the Sierra de las Estancias, Sierra de los Filabres and Cabrera (Table 1).
The soil thickness was evaluated: EST-A is the deepest soil (47 cm) and
EST-B, CAB and FIL-1 (both A and B) have similar soil depth (20–30 cm).
The CAB and FIL-1 soil profiles are characterized by only one horizon,
while EST soils have two horizons.
Soil samples were air-dried and sieved through a 2 mm size mesh.
The b 2 mm fraction was analysed for the total element content, cation
exchange capacity (CEC), and Fe content following selective extractions.
The soil mineralogy, particle size distribution, pH and Si isotopic compo-
sition of the clay fraction (b 2 μm) were determined on a set of samples
selected as representative from the top and bottom horizons (eight
samples in total: EST-A-U1, EST-A-U3, EST-B-U1, EST-B-U3, FIL-1-A-
U1, FIL-1-B-U1, CAB-A-U2, CAB-B-U2).
Bedrock samples were collected below the soil-bedrock boundary,
right under the soil profile. The weathering rinds of rock samples were
removed via sawing in order to measure the most unweathered parent
material. The bedrock samples were analysed for their total element
content, mineralogy and Si isotopic composition.
3.2. Physico-chemical characterization of soils
The selected samples were characterized for their particle size distri-
bution; we applied the USDA Textural Soil Classification (1987). The
sand fraction (50 μm–2 mm) was recovered after dispersion of the
fine earth fraction with an ultrasonic disperser (Branson Sonifier 250)
and wet sieving. The separation of silt (2 μm–50 μm) and clay fractions
(b2 μm) was achieved by dispersion with Na+-resin (Rouiller et al.,
1972) and followed by 24 h cycles of decantation according to the
Stokes law. The separated sand-sized and clay-sized fractions were
then characterized for their mineralogy and Si isotopic composition.
The cation exchange capacity (CEC) of the soil was measured follow-
ing standard procedures (Page et al., 1982) through soil saturation with
ammonium acetate and posterior desorption and quantification of the
ammonia retained on the negative charges of soil, originating from
both organic matter and clay minerals.
The soil pH in DI-water was measured on the set of selected samples
(Section 3.1) using a ratio of 25 mL of water for 5 g of soil.
The total carbon content (CT) in soils was measured using a
Vario Max dry combustion CN analyser instrument (Elementar
Analysensysteme GmbH, Germany; uncertainty 0.1%). The inorganic
74 Y. Ameijeiras-Mariño et al. / Chemical Geology 456 (2017) 72–84

Fig. 1. Geological map of the internal zone of the Betic Cordillera with the three selected catchments and pictures of each catchment. The same colour code is used in all graphs: a) Sierra de
las Estancias (EST), in green, lies on the intermediate units of the Alpujárride complex. b) Sierra de los Filabres (FIL-1), in blue, lies on the Mulhacén unit of the Nevado-Filábride complex. c)
Sierra Cabrera (CAB), in red, lies on the Veleta unit of the Nevado-Filábride complex.

carbon content (Ci) was measured based on the modified-pressure
calcimeter method (Sherrod et al., 2002). This method consists in mea-
suring the pressure change produced by the release of CO2 in gaseous
phase when a known volume of HCl reacts with the fine earth fraction
of the soil sample. This method to measure Ci can only be applied to
samples presenting an observable chemical reaction at room
temperature after the addition of a few drops of HCl 10%, i.e., in this
case only in CAB soils.
The total element content was measured in our soil samples and bed-
rocks. The method consists in measuring the element content by ICP-AES
(b 3% uncertainty relative to standard material) after lithium metaborate
and tetraborate fusion of the sample at 1000 °C and dissolution of the

Table 1
Main characteristics of the studied catchments: code, uplift rates ([1] Masana et al., 2005; [2] Booth-Rea et al., 2004; [3] Braga et al., 2003), catchment denudation rates ([4] Bellin et al.,
2014), surface area, mean altitude of the catchment, annual mean temperature (T, [5] García, 2009), annual mean rainfall (P, [5] García, 2009), annual mean potential evapotranspiration
(PET, [6] Junta de Andalucía, 2008), aridity index calculated as the ratio between rainfall and potential evapotranspiration (Barrow, 1992). More information on the derivation of the cli-
matic variables can be found in Schoonejans et al. (2016a).

Sierra Catchment Uplift rate Catchment Area Catchment mean Annual Annual mean Annual Aridity
code (mm/kyr) denudation (km2) altitude (m) mean[5] P[5] (mm) mean PET[6] Index
rate[4] (mm/kyr) T(°C) (mm) (P/PET)

Sierra de las Estancias EST 10–40[1] 34 ± 24 0.21 1179 12.5 425 ± 25 794 0.54 (Semi-arid)
Sierra de los Filabres FIL-1 70–110[2],[3] 54 ± 25 0.26 811 15.5 375 ± 25 750 0.50 (Semi-arid)
Sierra Cabrera CAB 170[3] 164 ± 74 1.98 541 17 275 ± 25 900 0.31 (Semi-arid)
 Y. Ameijeiras-Mariño et al. / Chemical Geology 456 (2017) 72–84 75

Table 2 fractions (65% of the clay-sized fractions). Accuracy and reproducibility

Main characteristics of the studied soil profiles (side A and B of the catchment): altitude, (δ30Si) were checked over a period of 10 months on reference materials
soil depth, vegetation type and distribution of the soil horizons with depth.
for Si isotopes: Diatomite (+1.32 ± 0.20‰, 2SD, n = 25), Quartz Merck
Sierra Sampling site Altitude (m) Soil depth (cm) Horizons depth (−0.02 ± 0.12‰, 2SD, n = 18) and the USGS Hawaiian basalt BHVO-2
Sierra de las EST-A 1187 47 A (0–15 cm), B (−0.30 ± 0.11‰, 2SD, n = 9), which yielded isotope compositions in-
Estancias (15–47 cm) distinguishable from previously published values (Abraham et al.,
EST-B 1187 25 A (0–15 cm), B 2008; Reynolds et al., 2007).
(15–25 cm)
Sierra de los FIL-1-A 776 22 A (0–22 cm)
Filabres FIL-1-B 776 17 A (0–17 cm) 4. Results
Sierra Cabrera CAB-A 525 19 A (0–19 cm)
CAB-B 525 18 A (0–18 cm) 4.1. Soil general properties

fusion beads in HNO3 1 N (Chao and Sanzolone, 1992). The loss on igni-
tion (LOI) is assessed at 1000 °C and the total element content is
expressed in reference to the soil dry weight at 105 °C. The accuracy of
the measurement is checked by testing the method with the reference
material BHVO-2 (Basalt, Hawaiian Volcanic Observatory, USGS).
A selective extraction of Fe with Dithonite-Citrate-Bicarbonate
(DCB) was performed to quantify soil Fe-oxides (Mehra and Jackson,
1960) and the Fe extracted (Fed) was quantified by ICP-AES.
3.3. Mineralogical characterization by X-ray diffraction
The primary and secondary crystalline minerals in bedrock, bulk soil
(fine earth), and sand and clay-sized fractions were identified after X-
ray diffraction analysis (XRD, Cu Kα, Bruker, D8 Advance). Bulk soils,
sand-sized fractions and bedrock were analysed as finely milled powder
without pre-treatment. Clay-sized fractions were processed with hy-
drogen peroxide (H2O2) to remove organic matter, DCB to remove Fe
oxides and analysed after KCl and MgCl2 saturation. Samples saturated
with K+ were heated to 105, 300 and 550 °C and those saturated with
Mg2+ were solvated with ethylene glycol (Robert and Tessier, 1974).
The changes on the minerals structure (reflected on the XRD patterns)
following heating and saturation allow the identification of the clay
type (non-quantitative). The obtained bedrock and bulk soil diffraction
patterns were studied with the software Diffrac Plus (by Bruker; com-
posed of EVA 2.5 and TOPAS 2.0) for qualitative identification and
semi-quantitative analysis (uncertainty on mineral content b 1%).
3.4. Silicon isotopes analysis
The clay-sized and sand-sized fractions and the bedrock samples
were analysed for their Si isotopic composition. The soil fractions and
bedrock samples were dissolved by alkaline fusion at 750 °C with
NaOH in a silver crucible and recovered in 1% HNO3 suprapur. Silicon
was then purified using a cation exchange resin (Georg et al., 2006).
The Si isotope composition in solutions was measured with a Nu Plas-
ma II Multicollector Inductively Coupled Plasma Mass Spectrometer (MC-
ICP-MS) at the Université Libre de Bruxelles (ULB). Measurements were
performed in dry plasma mode using a Cetac Aridus-2 desolvating sample
introduction device and in medium resolution. The instrumental mass
bias was corrected for using Mg doping and the sample-standard
bracketing technique. Data are expressed in relative deviations of
30
Si/28Si ratios from NBS-28 standard using the common δ-notation (‰,
Eq. (1)):
0
30  1 (from 10 to 22%; Table 4), and the presence of biotite decreases from
Si
B 28 Si sample C CAB (14–15%; Table 4) to EST (from 2 to 6%; Table 4). Clinochlore is
δ Si ¼ @
30 
30
−1A∙1000
Si
28 Si
NBS−28
Each single δ-value (n) represents one sample run and two
bracketing standard runs. The total sample preparation, including disso-
lution by alkaline fusion, was replicated at least two times for two sand-
sized fractions (20% of the sand-sized fractions) and five clay-sized
The pH values of the set of selected soil samples (Section 3.1) are al-
kaline (7.6 to 9.1; Table 3). The Sierra Cabrera (CAB) soils display the
highest values (8.9 and 9.1; Table 3). The total carbon content in the
soils here studied is low, ranging from 0.2 to 1.6% (Table 3) and de-
creases with depth. CAB soils display higher total C content (1.1–1.6%)
than Sierra de los Filabres (FIL-1) and Sierra de las Estancias (EST)
soils (0.2–1.3%). The presence of inorganic carbon (Ci) was identified
in CAB soils: its content ranges from 0.1 to 0.9% and increases with
depth. The Ci content is slightly higher for CAB-A than for CAB-B.
The higher pH and Ci values in Sierra Cabrera (CAB) soils, together
with the higher Ca content in CAB soils (2.2 ± 0.8%; Electronic Annex,
Table A.1) than in Sierra de los Filabres (FIL-1) and Sierra de las
Estancias (EST) soils (0.4 ± 0.1%; Table 3) support the presence of sec-
ondary pedogenic carbonates in CAB soils. The amount of Ca associated
with secondary pedogenic carbonates is not related to the parent mate-
rial. Therefore, a correction is applied to the total Ca content in Sierra
Cabrera (CAB) soils before assessing the soil weathering degree with
the TRB (Electronic Annex A.1). A correction is also applied to the
amount of Fe selectively extracted by DCB (Fed) in the CAB-A soil
given that secondary carbonates including Fe are dissolved by the ex-
traction and affect the calculation of the Fed/Fet ratio for this soil
(Electronic Annex A.2).
4.2. Mineralogy of bedrock and soils
The four different bedrock samples (EST-A-UR, EST-C-R, FIL-1-A-R,
CAB-R) are characterized by a similar primary mineralogy composed
mainly of quartz, muscovite, biotite, clinochlore and plagioclase
(Table 4). This similarity in mineralogy is consistent with the chemical
composition of the four bedrock samples (Si content: 25.2–27.8%; Fe
content: 4.72–5.98%; Table 3), and supports the observation that the
lithology is similar across the three catchments. In addition to the
primary minerals, the presence of secondary minerals, i.e., kaolinite,
vermiculite (total of 5 to 8%, semi-quantitative; Table 4), has been
observed in the bedrock samples.
The primary minerals in bulk soils are dominated by quartz and
muscovite, with a lower proportion of biotite, clinochlore and minerals
from the plagioclase series (Table 4). This is consistent with the primary
mineral assemblage of the bedrock, supporting our hypothesis that the
bedrock samples can be considered as the parent material of the soils
studied. Quartz content increases from Sierra Cabrera (CAB, higher de-
nudation rates) to Sierra de las Estancias (EST, lower denudation
rates) soils (25 to 77%; Table 4). The abundance of muscovite is lower
in the EST catchment (from 3 to 14%; Table 4) compared to the FIL-1 (Si-
erra de los Filabres, intermediate denudation rates) and CAB catchments
ð1Þ
more abundant in CAB soils (from 7 to 10%; Table 4), which is associated
with a higher content of this mineral in the CAB bedrock (15%; Table 4).
The minerals of the plagioclase series are present in low abundance
(2.9 ± 1.2%, n = 7), except for FIL-1-B (14%; Table 4). The presence of
calcite in Sierra Cabrera (CAB) soils confirms the occurrence of pedo-
genic carbonates in this catchment (Section 4.1); that presence of calcite
is not considered to be of external origin. Dust deposition cannot be
 76
Table 3
Main characterization of the soil (b2 mm fraction; U samples) and bedrock samples (R samples): sampling depth; pHH20; major elements content (Al, Ca, Fe, K, Mg, Mn, Na, P, Si, Ti, expressed in element mass %; Zr expressed in mg/kg); loss on ignition
(LOI, %); cation exchange capacity (CEC, cmolc/kg); total carbon content (CT, %); inorganic carbon content (Ci, %); Fe extracted with DCB (Fed, g/kg). For bedrock and the separated sand-sized (50 μm–2 mm) and clay-sized (b2 μm) fractions: average Si
isotopic signature (δ30Si) with standard deviation (2SD) and number of replicates (n). For CAB soils, major element content and Fed values are corrected for the presence of secondary pedogenic carbonates (See Electronic Annex A.1 and A.2). *Bedrock
Si isotopic signature.

Sierra Sample Sampling depth pHH2O Al Ca Fe K Mg Mn Na P Si Ti Zr LOI CEC CT Ci Fed Sand-sized fraction Clay-sized fraction
30
cm % mg/kg % cmolc/kg % % g/kg δ Si (‰) 2SD n δ30Si (‰) 2SD n

Y. Ameijeiras-Mariño et al. / Chemical Geology 456 (2017) 72–84

Sierra de las Estancias EST-A-U1 6–8 7.59 4.73 0.25 2.19 0.99 0.39 0.03 0.33 0.01 37.4 0.37 305 4.35 6.91 1.29 8.13 −0.18 0.23 5 −0.53 0.18 5
EST-A-U2 12–14 5.53 0.28 2.64 1.04 0.48 0.02 0.26 0.01 36.6 0.44 284 3.71 6.25 0.48 9.15
EST-A-U3 20–22 7.83 7.87 0.49 4.01 1.57 0.74 0.02 0.29 0.01 32.5 0.46 264 4.65 10.5 0.41 12.5 0.04 0.11 2 −0.41 0.09 4
EST-A-U4 28–30 8.71 0.50 4.7 1.83 0.89 0.03 0.28 0.01 30.6 0.43 222 5.48 14.0 0.30 14.7
EST-A-U5 32–34 9.92 0.63 5.26 2.37 1.01 0.03 0.67 0.01 28.1 0.49 238 6.17 15.0 0.29 14.6
EST-B-U1 3–5 7.73 6.19 0.30 2.92 1.37 0.79 0.03 0.40 0.01 34.8 0.39 309 4.75 8.35 0.79 8.68 −0.01 0.11 2 −0.37 0.07 3
EST-B-U2 9–11 5.92 0.41 2.65 1.00 0.72 0.02 0.26 0.08 35.3 0.37 287 5.17 11.6 0.81 7.22
EST-B-U3 18–21 7.98 5.63 0.45 2.78 0.75 0.77 0.02 0.16 0.01 35.9 0.35 205 4.72 11.0 0.31 6.46 −0.14 0.12 5 −0.42 0.07 2
EST-B-U4 25–27 5.62 0.56 2.90 0.75 0.84 0.03 0.19 0.01 35.8 0.36 227 4.27 10.3 0.22 6.58
EST-A-UR 92.5 12.7 0.64 4.72 3.86 0.20 0.01 0.80 0.06 26.8 0.58 210 3.15 −0.32* 0.16 5
EST-C-R 82.5 13.2 0.67 5.19 3.90 0.22 0.01 1.05 0.07 25.8 0.65 232 3.50 −0.28* 0.04 2
Sierra de los Filabres FIL-1-A-U1 2–4 7.73 8.85 0.32 4.51 2.44 0.58 0.04 1.28 0.03 29.8 0.55 220 5.65 8.41 1.14 10.2 −0.14 0.15 10 −0.54 0.16 6
FIL-1-A-U2 6–8 9.51 0.31 4.83 2.56 0.62 0.04 1.28 0.03 29.1 0.56 208 5.30 6.57 0.96 10.8
FIL-1-A-U3 9–11 9.31 0.32 4.78 2.65 0.64 0.05 1.26 0.03 29.3 0.57 235 5.11 7.03 0.93 10.7
FIL-1-A-U4 11–13 9.55 0.30 4.76 2.62 0.61 0.04 1.28 0.03 29.1 0.58 218 5.17 6.95 0.93 11.6
FIL-1-B-U1 3–5 7.66 8.25 0.33 4.15 1.70 0.56 0.03 1.70 0.02 31.0 0.58 319 5.03 9.84 0.97 7.79 −0.08 0.08 2 −0.67 0.11 2
FIL-1-B-U2 6–8 8.30 0.31 3.96 1.73 0.56 0.03 1.67 0.02 31.3 0.55 332 4.76 9.19 0.88 7.62
FIL-1-B-U3 10–12 8.70 0.32 4.08 2.02 0.67 0.02 1.54 0.03 30.6 0.53 289 4.98 9.68 0.73 6.31
FIL-1-B-U4 15–16 9.20 0.28 4.14 2.25 0.84 0.02 1.13 0.03 30.4 0.52 277 4.50 8.30 0.46 7.13
FIL-1-A-R 43 12.3 0.60 5.97 3.31 0.88 0.03 1.79 0.12 25.2 0.57 204 3.89 −0.37* 0.08 6
Sierra Cabrera CAB-A-U1 1–2 12.6 0.87 6.54 2.61 1.06 0.07 0.55 0.06 23.9 0.84 213 8.43 4.98 1.18 0.455 12.9
CAB-A-U2 6 8.86 13 0.96 6.46 2.82 1 0.07 0.56 0.06 23.3 0.83 220 8.83 4.93 1.30 0.547 12.0 −0.25 0.14 3 −0.50 0.09 5
CAB-A-U3 11 12.9 0.66 6.82 2.83 0.95 0.09 0.54 0.06 23.2 0.79 220 10.42 4.62 1.57 0.868 7.11
CAB-A-U4 17–19 13 0.63 6.44 2.78 0.74 0.10 0.55 0.04 23.8 0.73 220 9.13 5.02 1.12 0.563
CAB-B-U1 4–6 12.3 0.33 6.05 2.75 1.03 0.05 0.67 0.08 24.9 0.78 266 7.09 1.94 1.23 0.132 10.6
CAB-B-U2 7–9 9.12 11.6 0.29 5.61 2.6 1.04 0.04 0.60 0.08 26.2 0.72 213 7.29 1.79 1.42 0.336 8.10 −0.22 0.14 3 −0.48 0.14 5
CAB-B-U3 10–11 11.6 0.37 5.85 2.56 1.08 0.04 0.59 0.08 25.9 0.68 208 8.19 1.70 1.62 0.530 10.2
CAB-B-U4 15–19 11.4 0.53 5.27 2.48 1.05 0.04 0.64 0.08 26.1 0.60 233 8.87 1.57 1.63 0.530 7.19
CAB-R 40 11.6 0.26 5.98 2.71 1.15 0.04 1.09 0.10 26.0 0.63 222 5.24 −0.39* 0.07 4
 Y. Ameijeiras-Mariño et al. / Chemical Geology 456 (2017) 72–84 77

Table 4
Additional characterization of eight selected soil samples (one horizon per profile for CAB and FIL-1, two horizons per profile for EST) and bedrock samples: sampling depth; particle size
distribution of the fine earth fraction (b2 mm); mineralogy of primary minerals ([1] Q = Quartz, M = Muscovite, B = biotite, Cl = clinochlore, P = plagioclase group), and mineralogy of
secondary minerals ([2] K = kaolinite, Z = zeolite, V = vermiculite, Ca = calcite, I = illite).

Type of sample Sierra Sample Sampling depth Particle size distribution Primary minerals [1] Secondary
minerals [2]

Sand (50 μm–2 mm) Silt (50 μm–2 μm) Clay (b2 μm) Q M B Cl P K Z V Ca I
cm % % %

Bulk soil Sierra de las Estancias EST-A-U1 6–8 52.1 39.5 8.4 77 8 4 2 4 5 – – –
EST-A-U3 20–22 32.3 47.5 20.3 65 14 6 4 2 4 2 3 –
EST-B-U1 3–5 40.1 46.1 13.8 66 10 4 6 3 6 3 2 –
EST-B-U3 18–21 25.4 59.7 14.9 69 3 2 8 2 9 3 4 –
Sierra de los Filabres FIL-1-A-U1 2–4 45.3 44.5 10.2 45 22 10 5 5 5 4 4 –
FIL-1-B-U1 3–5 53.6 32.5 13.9 60 10 4 3 14 4 2 3 –
Sierra Cabrera CAB-A-U2 6 21.5 67.9 10.6 25 17 14 10 2 16 3 4 4
CAB-B-U2 7–9 26.7 64.1 9.2 36 20 15 7 2 8 3 1 2
Bedrock Sierra de las Estancias EST-A-UR 92.5 – – – 37 25 12 2 5 4 3 2 – 5
EST-C-R 82.5 – – – 32 22 10 6 6 5 5 3 – 5
Sierra de los Filabres FIL-1-A-R 43 – – – 27 30 8 8 6 2 2 3 – 8
Sierra Cabrera CAB-R 40 – – – 32 23 10 15 3 5 3 2 – 3

completely ruled out in these soils, since the Betic Cordillera is exposed
to aeolian dust input from the Sahara and Sahel (Castillo et al., 2008;
Scheuvens et al., 2013). However, the influence of dust deposition is
considered as limited (Schoonejans et al., 2016b) since the soils have
been sampled in ridge tops typically exposed to wind and less
favourable for dust deposition, and since there is no evidence for Si- or
Al- enrichment at the top of the profiles as would be expected when
levels of mineral dust input are important (dust from northern Africa
and the Western Sahara: ~ 50–60% SiO2; Avila et al., 1998; Castillo et
al., 2008).
The sand-sized fractions mineral assemblage has been qualitatively
described. The X-ray patterns are dominated by quartz, with a relative
increase of the quartz presence from soils characterized by higher denu-
dation rates (CAB) to those characterized by lower denudation rates
(EST). Other primary minerals are also detected on the X-ray diffraction
pattern (muscovite, clinochlore, biotite and plagioclase).
The qualitative identification of the mineral assemblage (Section 3.3;
Table 4) from the clay-sized fractions indicates that they are dominated
by secondary minerals (chlorite, kaolinite, illite and vermiculite). Some
quartz is also observed. The semi-quantification in the bulk soil indi-
cates that the amount of kaolinite decreases from the soils with high de-
nudation rates (CAB) to soils with low denudation rates (EST) (16 to 4%;
except for EST-B-U3, 9%; Table 4). A qualitatively higher content of chlo-
rite in the clay fraction is noticed for CAB compared to the other sites.
This is directly associated with the occurrence of clinochlore (a mineral
of the chlorite group) in CAB rock (Table 4).
4.3. Indexes of chemical weathering
Six weathering indexes are used to characterize the weathering de-
gree of these soils: the Total Reserve in Bases (TRB), the ratio Fe-oxides
to total Fe (Fed/Fet), the quartz content, the clay content, the cation ex-
change capacity (CEC) and the silicon isotopic signature of the clay-
sized fraction (δ30Siclay-sized fraction). These indexes are expected to
evolve with weathering as follows:
- The TRB is the sum of the alkaline and alkaline-earth cations (Ca2+,
Mg2+, K+ and Na+, cmolc/kg) following Eq. (2) (Herbillon, 1986)
and is expected to decrease as cations are leached with increasing
weathering.
h i     h i Table 4).
TRBsoil ¼ Ca2þ þ Naþ þ K þ þ Mg 2þ ðcmolc =kgÞ
- The amount of iron oxides (Fed,) in reference to the total iron
content (Fet) is expected to increase with weathering, the ratio
Fed/Fet is, then, expected to increase as weathering increases.
- Quartz is a mineral highly resistant to weathering. As a consequence,
it can be expected that the quartz content in soil increase with in-
creasing weathering intensity.
- The clay content is expected to increase with increasing weathering
intensity.
- In this study case, given the low organic carbon content in these soils
(see Sections 4.1 and 4.3.5), the CEC is expected to increase with
weathering degree with increasing clay content.
- The δ30Siclay-sized fraction is expected to be more negative as
weathering and desilication increase.
4.3.1. Total Reserve in Bases (TRB)
Fig. 2a shows the evolution of TRB with depth for the study sites.
EST-A shows a clear evolution with depth, with increasing values of
TRB at higher depths. There is no clear trend with depth for the other
studied soil profiles. CAB (higher denudation rates) is the site present-
ing the higher TRB values although FIL-1 (intermediate denudation
rates) values are very close to them. EST (lower denudation rates) site
has the lower TRB values of all soil profiles studied, and present different
trends with depth between the A and B side. FIL-1 and CAB soils show
no significant differences between A and B sides.
4.3.2. Iron oxides content
The evolution of the Fed/Fet ratio in the soils is presented in Fig. 2b.
EST (lower denudation rates) site presents the highest Fed/Fet values
and the two EST profiles follow parallel evolutions of the Fed/Fet ratio,
decreasing with depth, although EST-A presents higher Fed/Fet ratio
than EST-B. In CAB and FIL-1 soils (higher and intermediate denudation
rates respectively), there is no observable pattern in the Fed/Fet ratio
with depth. FIL-1-A presents a higher Fed/Fet ratio than CAB-A, CAB-B,
and FIL-1-A.
4.3.3. Quartz content
The quartz content in EST (lower denudation rates) is up to three
times higher than in CAB (high denudation rates, 77% for EST-A-U1 ver-
sus 25% for CAB-A-U2; Table 4). The quartz content in EST (from 65% to
77%) is also higher than in FIL-1 soils (intermediate denudation rates,
FIL-1-A, 45%; FIL-1-B, 60%; Table 4). In FIL-1 and CAB catchments, the
side B presents higher quartz content than the side A. CAB is the catch-
ment presenting the lowest content on quartz (CAB-A, 25%; CAB-B, 36%;
ð2Þ
4.3.4. Clay content
The clay content is comparatively higher (Table 4) in EST-B (13.8 ±
0.4% and 14.9 ± 0.6%) and FIL-1-B (13.9 ± 0.3%) than in CAB (10.6 ±
0.7% and 9.2 ± 0.3%) and FIL-1-A (10.2 ± 0.3%). The clay content in
78 Y. Ameijeiras-Mariño et al. / Chemical Geology 456 (2017) 72–84
Fig. 2. Evolution of three weathering indexes with depth in the soil profiles of CAB, FIL-1
and EST catchments: a) the Total Reserve in Bases (TRB) or the sum of the total content
in Ca, Mg, Na, K; b) the Fe-oxides content expressed as the ratio between the iron
extracted by dithionite-citrate-bicarbonate (Fed) in reference to total Fe content (Fet); c)
the cation exchange capacity (CEC). Colours correspond to the intensity of the
denudation rates: red sites for higher (CAB), blue sites for medium (FIL-1) and green
sites for lower (EST) denudation rates. Open symbols stand for the profile on the A side
of each catchment and closed symbols for the profile on the B side. The error bars
represent the uncertainty on the measurement. Catchment code (CAB, FIL-1, EST) as in
Fig. 1.
EST-A is more variable, ranging from 8.4 ± 0.3% in the surface horizon to
20.3 ± 0.7% in the deepest horizon. This variation in EST-A is accompa-
nied by a decreasing content of the sand-sized fraction from the surface
to the deeper horizon (Table 4).
4.3.5. Cation exchange capacity (CEC)
The CEC is not directly a weathering index. This parameter reflects
the presence of negative charges in soil, due to the presence of
secondary clay minerals and organic matter. Since these soils are charac-
terized by low organic matter content (averages for soils of each catch-
ment: EST, 0.5% ± 0.4; FIL-1, 0.9% ± 0.2; CAB, 0.9% ± 0.2; for CAB, this is
the difference between the CT and the Ci; Table 3) the CEC is considered
to be mainly controlled by the clay presence, and is therefore compared
with other weathering indexes. The CEC values range from 1.6 cmolc/kg
in CAB-B soil up to 15 cmolc/kg in EST-A (Fig. 2c, Table 3). The CEC values
in CAB (higher denudation rates) soils are lower (1.6–5 cmolc/kg) than
in the other two catchments and they are homogenous with depth, al-
though the values for CAB-A (4.6–5 cmolc/kg) are significantly higher
than for CAB-B (1.6–1.9 cmolc/kg). FIL-1-A presents CEC values lower
(6.6–8.4 cmolc/kg) than FIL-1-B (8.3–9.8 cmolc/kg) and EST (lower
denudation rates) soils (except EST-A shallower horizon: samples EST-
A-U1 and U2). FIL-1-B and EST soils present similar CEC values, a com-
mon pattern which was also observed for the clay content (Table 4).
The horizons in EST-A soils are characterized by distinct CEC values,
with lower values in the shallowest horizon (EST-A-U1, 6.9 cmolc/kg,
EST-B-U2, 6.2 cmolc/kg) than in the deepest horizon (EST-A-U3,
10.5 cmolc/kg; EST-A-U4, 14.0 cmolc/kg; EST-A-U5, 15.0 cmolc/kg).
4.3.6. Silicon isotope composition of bedrock, and sand-sized and clay-sized
fractions of soils
The Si isotope compositions of the bedrock, the sand-sized and the
clay-sized fractions were determined (Table 3 and Fig. 3). The Si isotope
composition of the bedrock (from −0.39 to −0.28‰; Table 3; Fig. 3) is
consistent with values reported for schist and shale (e.g., between −1.1
and − 0.1‰, Ding et al., 1996; between − 0.5 and 0.0‰, André et al.,
2006; between −0.82 and 0.0‰, Savage et al., 2013). The four bedrock
samples present no significant differences in their δ30Si values: this is
consistent with the geochemical similarity of parent material across
sites (Section 4.2).
The Si isotope compositions of the sand-sized fractions
range from − 0.25 to 0.04‰ (Table 3; Fig. 3) and are not significantly
different between catchments. The sand fraction is dominated by
quartz but also contains other minerals such as micas, plagioclases
and chlorite (Table 4), which may explain the variability in δ 30 Si.
The presence of quartz is known to have a strong influence on δ30Si
in shales (Savage et al., 2013) due to the high variability of the quartz
isotopic signature across different geological settings (e.g., δ30Si in ‰
of − 0.09 in sandstone, Georg et al., 2009; − 0.33 in sandstone and
− 0.36 in paragneiss, Steinhoefel et al., 2011; − 0.2 in granites,
Savage et al., 2012).
The Si isotope composition of the clay-sized fractions (from −0.67
to − 0.37‰; Table 3; Fig. 3) is generally lighter than the δ30Si of the
sand-sized fractions of the corresponding soil profile, except the clay-
sized fraction of EST-A-U1 which cannot be distinguished from the cor-
responding sand fraction (given the large variability among the repli-
cates; Table 3). The average Si isotope composition of the clay-sized
fraction is not significantly different between the catchments (CAB:
− 0.49 ± 0.01‰, n = 2; FIL-1: − 0.61 ± 0.09‰, n = 2; EST: -0.43 ±
0.07‰, n = 4; where n is the number of samples considered for the
catchment). The only exception is FIL-1-B sample (− 0.67 ± 0.11‰,
2SD; Table 3; Fig. 3), which presents a significantly lighter δ30Si value
than samples from EST-B (− 0.37 ± 0.07‰, − 0.42 ± 0.07‰, 2SD;
Table 3; Fig. 3) and the deepest sample from EST-A (− 0.41 ± 0.09‰,
2SD; Table 3; Fig. 3).
5. Discussion
5.1. Multiproxy analysis of the soil weathering intensity
The six weathering indexes determined in the soils (TRB, Fed/Fet,
quartz content, clay content, CEC, δ30Siclay-sized fraction) are combined
and compared to assess the variation of the weathering intensity be-
tween catchments (Table 5). For the eight fully characterized samples
(EST-A-U1, EST-A-U3, EST-B-U1, EST-B-U3, FIL-1-A-U1, FIL-1-B-U1,
 Y. Ameijeiras-Mariño et al. / Chemical Geology 456 (2017) 72–84 79

denudation rates) is, according to one weathering index (CEC), similar

Fig. 3. Silicon isotopic compositions (δ30Si) of the: a) bedrock; b) sand-sized fraction; c)
clay-sized fraction. For bedrock (a), red symbols represent CAB sample, blue symbols
represent FIL-1 sample and green symbols (both open and closed) represent EST
samples. For sand-sized (b) and clay-sized fractions (c), colour code as in Fig. 2. In EST
profile (green), the diamonds represent the shallowest horizon (EST-A-U1, EST-B-U1)
and the triangles represent the deepest horizon (EST-A-U3, EST-B-U3). The error bars
represent the 2SD on the mean values of the different replicates. Catchment code (CAB,
FIL-1, EST) as in Fig. 1.
CAB-A-U2, CAB-B-U2), the multiproxy approach of the present study is
represented as a web graph (Fig. 4). Five weathering indexes (TRB, Fed/
Fet, quartz content, clay content and CEC) agree that the soils from the
catchment with the lowest denudation rates (EST) are more weathered
than the soils from the catchment with the highest denudation rates
(CAB). The weathering degree in FIL-1 catchment (intermediate
to the weathering degree of EST, and according to one weathering
index (TRB) similar to or close to the weathering degree of CAB. Accord-
ing to the three other weathering indexes (Fed/Fet, quartz content, clay
content), A and B sides of FIL-1 catchment present distinct weathering
degrees (Table 5). The weathering degree of the A side (FIL-1-A) is
close to EST according to Fed/Fet and close to CAB according to the
quartz and the clay content (Table 5). The weathering degree of the B
side (FIL-1-B) is close to CAB according to Fed/Fet and close to EST
soils according to the quartz and the clay content (Table 5). This sug-
gests that the FIL-1 catchment is an intermediate situation, a transition
between CAB and EST catchments. Overall, five weathering indexes
(TRB, Fed/Fet, quartz content, clay content and CEC) support that the
catchment characterized by the lowest denudation rate (EST; 34 ±
24 mm/yr; Bellin et al., 2014; Vanacker et al., 2014) is more intensely
weathered than the catchment with the highest denudation rate
(CAB; 164 ± 74 mm/yr; Bellin et al., 2014; Vanacker et al., 2014).
The EST-A profile is the most weathered profile (Table 5). This pro-
file presents two horizons well differentiated, with contrasted mineral-
ogical (Fed/Fet, quartz content), and physico-chemical (clay content,
TRB, CEC) characteristics (Table 5). Based on the differences observed
with depth in clay content (Section 4.3.4) and CEC (Section 4.3.5) it is
concluded that this profile is characterized by clay illuviation from the
upper A horizon and clay accumulation in the B horizon due to soil
development.
According to the web graph (Fig. 4), the δ30Siclay-sized fraction is not a
weathering index that allow differentiating weathering intensity be-
tween catchments. The lighter Si isotope composition of the clay-sized
fraction relative to the sand-sized fractions in all sites agrees with the
commonly accepted view that light Si isotopes are preferentially incor-
porated in secondary weathering phases (Ziegler et al., 2005a; Ziegler et
al., 2005b; Georg et al., 2007; Opfergelt et al., 2009, 2010, 2011, 2012;
Bern et al., 2010; Cornélis et al., 2014). The δ30Si of the clay-sized frac-
tion indicates no significant variation between catchments (Table 5).
As a consequence, there are no significant correlations between the δ-
30
Siclay-sized fraction values and the other weathering indexes (Fig. 5). Con-
sidering that Si isotopes are preferentially incorporated in secondary
phases with increasing weathering (Ziegler et al., 2005a; Ziegler et al.,
2005b; Georg et al., 2007; Opfergelt et al., 2009, 2010, 2011, 2012;
Bern et al., 2010; Cornélis et al., 2014), a difference of the δ30Siclay-sized
fraction between catchments of distinct weathering intensity could have
been expected. The clay-sized fraction (b2 μm) was physically separat-
ed and is not exclusively composed of secondary minerals. Micro-grains
of quartz (characterized by a δ30Si heavier than clay minerals; e.g.,
Savage et al., 2013) may partially contribute to reduce the differences
in Si isotope composition between catchments. An additional factor re-
ducing Si isotope fractionation with increasing weathering may be re-
lated to Si mobility in soils (Steinhoefel et al., 2011; Opfergelt et al.,
2012). Chemical weathering is characterized by element mobility and
element loss with mineral weathering, with the cations Ca, Mg, Na,
and K being the more mobile elements. The decrease in the soil TRB

Table 5
Qualitative comparison of the soil weathering intensity assessed using the different weathering indexes: Total Reserve in Bases (TRB); iron oxide content (ratio Fed/Fet); quartz content;
clay content; cation exchange capacity (CEC), and Si isotope composition of the clay fraction (δ30Siclay-sized fraction). The weathering intensity is evaluated for the eight selected soil horizons
(Section 3.1; two for EST-A and B profiles). For each weathering index, the relative intensity of weathering in one horizon is qualitatively assessed relative to the other horizons following a
scale of increasing weathering intensity: = very low; − low; + high; ++ very high; +++ the highest.

Sierra Code TRB Fed/Fet Quartz content Clay content CEC δ30Siclay-sized fraction

Sierra de las Estancias EST-A Horizon A +++ +++ +++ = + =

Horizon B + ++ ++ +++ +++ =
EST-B Horizon A ++ ++ ++ ++ ++ =
Horizon B ++ + ++ ++ ++ =
Sierra de los Filabres FIL-1-A − + − − + =
FIL-1-B − − + ++ ++ −
Sierra Cabrera CAB-A = − = − − =
CAB-B − − − = = =
80 Y. Ameijeiras-Mariño et al. / Chemical Geology 456 (2017) 72–84
Fig. 4. Web graph representing the multiproxy approach of this study, using six
weathering indexes (TRB, Fed/Fet, quartz content, clay content, CEC, δ30Siclay-sized fraction)
to assess the weathering intensity of eight fully characterized soil samples (EST-A-U1,
EST-A-U3, EST-B-U1, EST-B-U3, FIL-1-A-U1, FIL-1-B-U1, CAB-A-U2, CAB-B-U2). Each arm
of the web graph represents a weathering index, with increasing weathering intensity
from the center to the external part of the graph. For each weathering index, the sample
with the value corresponding to the highest weathering intensity is considered as 100%
of the weathering intensity, and the other samples are expressed as a percentage of
variation from 100%. Colour code: green for EST, blue for FIL-1, red for CAB. Catchment
code as in Fig. 1.
values from the catchment presenting higher denudation rates (CAB) to
the lowest denudated catchment (EST) supports cation loss (Ca, Mg, Na,
K) with increasing weathering (Fig. 2a). Silicon mobility in soils can be
assessed using the Tau Si index (τSi; Fig. 6, data published in
Schoonejans et al., 2016a). The Tau index expresses the relative gain
Fig. 5. Silicon isotope compositions (δ30Siclay-sized fractions) of the clay-sized fraction as a function of four of the studied weathering indexes: a) Total Reserve in Bases (TRB); b) proportion of
iron oxides relative to total iron (Fed/Fet); c) quartz content; d) cation exchange capacity (CEC) for the selected samples. Vertical error bars represent the 2SD on the mean δ30Si values.
Weathering indexes are single values for the corresponding depth with the horizontal error bars representing the uncertainty on the measurement. Colour code as in Fig. 2. Catchment
code (CAB, FIL-1, EST) as in Fig. 1.
(positive values) or loss (negative values) of an element with
weathering relative to an element considered chemically immobile, in
this case Zr (Brimhall and Dietrich, 1987). It appears that the studied
soils are characterized by a limited Si loss (generally b10%, except for
sample FIL-1-B-U1 up to 30%; Fig. 6), which suggests a low Si mobility
in soils likely due to the semi-arid climatic conditions in the area. Silicon
mobility is an important factor controlling Si isotope fractionation, with
lighter Si isotopes accumulating in soils with increasing Si mobility and
increasing Si loss (τSi increasingly negative) with increasing weathering
(Steinhoefel et al., 2011; Opfergelt et al., 2012). The only clay-sized frac-
tion presenting a significantly lighter δ30Si value than the other samples
(FIL-1-B-U1) is also characterized by a higher Si loss (more negative τSi
value; Fig. 6). This is consistent with observations on shales investigated
as part of the variability of Si isotopes in the upper continental crust
(Savage et al., 2013), and in which no correlation was observed between
δ30Si and weathering indexes such as CIA despite the presence of sec-
ondary minerals in the shales supporting the effect of weathering. The
lack of Si isotope fractionation in shales was explained by the authors
by the low desilication and the accumulation of detrital quartz that ob-
scured the influence of isotopically lighter secondary minerals. The low
Si mobility and limited Si loss in the soils from the Betic Cordillera are
suggested to be key factors to explain the limited difference in the
δ30Si clay-sized fraction between catchments despite the range in
weathering intensity (as indicated by the weathering indexes) observed
among the catchments.
5.2. Controls on soil weathering intensity
Soil weathering intensity in eroding landscapes is often assessed
using mass balance approaches based on chemical depletion fractions
(CDF). In the Betic Cordillera, Schoonejans et al. (2016a) investigated
the relationship between denudation rates and chemical weathering
intensity using the CDF (assuming Zr immobility). A significant
 Y. Ameijeiras-Mariño et al. / Chemical Geology 456 (2017) 72–84 81

Fig. 6. The Si isotopic signature of the clay-sized fraction (δ30Siclay-sized fraction) as a function
of the Si gain and loss expressed as a Tau index (τSi; data published in Schoonejans et al.
(2016a). Vertical error bars represent the 2SD on the mean δ30Si values and horizontal
bars represent the error associated to Tau calculation. Colour code as in Fig. 2.
Catchment code (CAB, FIL-1, EST) as in Fig. 1.

correlation exists between the CDF (calculated by Schoonejans et al.,

2016a) and three weathering indexes from this study: the TRB (Fig.
7a; R = − 0.81), the Fed/Fet (Fig. 7b; R = 0.81) and the quartz content
(Fig. 7c; R = 0.98). The relationship is less clear with the CEC (R = 0.42;
Fig. 7d), especially in EST due to clay illuviation (Section 5.1). The rela-
tion between the CDF and the clay content is not presented given the
bias induced by the identified pedogenic processes of clay illuviation af-
fecting the clay content (Section 5.1). The present study based on the
weathering indexes and the study based on the CDF (Schoonejans et
al., 2016a) converge to conclude that the soil weathering intensity in
the Betic Cordillera increases (from CAB to EST) with decreasing catch-
ment denudation rate (CAB = 164 ± 74 mm/kyr; EST = 34 ±
24 mm/kyr; Bellin et al., 2014; Vanacker et al., 2014).
The agreement between the conclusions from three weathering in-
dexes based on different soil constituents (TRB, Fed/Fet and quartz con-
tent) and the conclusions from the CDF in the Betic Cordillera has
important implications. First, it supports the validity of the mass balance
technique (CDF) in this environment to investigate weathering process-
es. Moreover, our study critically highlights that a multiproxy approach
can be a powerful complement to CDF to assess weathering intensity;
this might be useful in settings with mobilization of Ti and Zr within
weathered profiles (Du et al., 2012) or with heterogeneity in the bed-
rock of the concentration of the element used as reference. Finally, as
part of the controversy on the link between denudation rate and chem-
ical weathering intensities, the present study agrees with the observed
negative relation between CDF and denudation rate (e.g., Dixon et al.,
2012), and not with the hypothesis that there is no specific pattern to
relate CDF and denudation rate (e.g., Riebe et al., 2004; Dixon et al.,
Fig. 7. Comparison between the Chemical Depletion Fraction (CDF) as calculated in
2009). Further investigations considering more climatic and erosional
Schoonejans et al. (2016a) and four of the studied weathering indexes: a) Total Reserve
settings would be needed to resolve the controversy. in Bases (TRB); b) proportion of iron oxides relative to total iron (Fed/Fet); c) quartz
content; d) cation exchange capacity (CEC). The relation between the CDF and the clay
5.3. Implications for other eroding landscapes content is not presented given the bias induced by the identified pedogenic processes of
clay illuviation (Section 5.1). Error bars represent the uncertainty on the measurement.
Colour code as in Fig. 2. Catchment code (CAB, FIL-1, EST) as in Fig. 1.
Weathering indexes such as the TRB, independent from the Zr con-
tent, may provide a potential complement to quantify the relationship
between chemical weathering and denudation processes in landscapes from Swiss Alps (Norton and von Blanckenburg, 2010), and shale from
where the use of the CDF is questioned because of Zr mobility or hetero- Susquehanna/Shale Hills Critical Zone Observatory (Jin et al., 2010).
geneity of immobile elements in the parent material. The last study site has a lithology that is comparable to the mica schist
In order to evaluate the potential of the TRB to constrain weathering in our study sites in the Betic Cordillera.
intensity in eroding landscapes, we plotted the TRB (calculated from Eq. It appears that the slope of the correlation between the TRB and the
(2)) as a function of the CDF for a compilation of soil data from different CDF measured in soils depends on the lithology of the parent material
lithological settings: granite from San Gabriel Mountains (Dixon et al., (Fig. 8). In soils derived from mica schist (Betic Cordillera) and shale
2012) and Swiss Alps (Norton and von Blanckenburg, 2010), gneiss (Jin et al., 2010), the TRB decreases when the CDF increases, whereas
82 Y. Ameijeiras-Mariño et al. / Chemical Geology 456 (2017) 72–84

in soils derived from granite (Dixon et al., 2012; Norton and von
Blanckenburg, 2010) or gneiss (Norton and von Blanckenburg, 2010),
the TRB increases when the CDF increases. The Betic Cordillera and the
San Gabriel Mountains are both characterized by a semi-arid climate,
but display opposite trends in the relationship between CDF and TRB,
which suggests that climate likely has a limited control on the relation-
ship between CDF and TRB.
We hypothesize that the mineralogy of the parent material, and in
particular the amount of feldspar, exerts a strong control on the evolu-
tion of the TRB as a function of the CDF. In the data presented in Fig. 8,
the feldspar content ranges from ~0% in the shale (Jin et al., 2010), 3–
6% in the mica schist from the Betic Cordillera (Table 4), 59% in the gran-
ite from San Gabriel Mountains (Dixon et al., 2012), 62% in the granite
from the Swiss Alps (Norton and von Blanckenburg, 2010), and up to
70% in the gneiss (Norton and von Blanckenburg, 2010). Feldspars are
a group of primary weatherable minerals rich in cations. When the
amount of feldspar in the bedrock is low, chemical weathering removes
mobile elements (decreasing TRB) as they are released from the parent
material, leading to an enrichment in Zr (CDF increase). This behaviour
can be observed in soils that are derived from parent material with a
low content in feldspar minerals (having b 6% of feldspar minerals
such as shale and mica schist; negative slopes of the CDF-TRB relation;
Fig. 8). When the feldspar content in the parent material is higher, re-
lease of cations such as Ca or Na from feldspar weathering may be faster
than Ca or Na removal by leaching, leading to a relative enrichment in
these cations in the soil. Based on Eq. (2) (not corrected for mass losses),
an increase in cations such as Ca, Na, K, or Mg would lead to an increase
of the TRB in the soil, while the removal of other mobile elements would
lead to a Zr enrichment, and hence a CDF increase. This behaviour is ob-
served in soils that are derived from bedrock with high feldspar content
(59–70% feldspar; granite and gneiss; positive slopes of the CDF-TRB re-
lation; Fig. 8). Our data compilation suggests that the importance of
feldspar weathering for soil development, may explain differences in
the relationship between TRB and CDF. Exploring the potential of the
TRB as a complementary weathering index to the CDF in eroding land-
scapes requires further analyses.
An important caveat to consider is that the TRB should not be used as
a single weathering index but always as a complement to CDF. The TRB
is a sum of the moles of charge per gram of soil of Ca, Na, K and Mg (Eq.
(2)) and does not account for mass loss or gain occurring in the soil pro-
file relative to the parent material. This is mathematically different from
CDF which is an index normalized to an immobile element expressing
the mass loss or gain of an element relative to the parent material. The
TRB presents the advantage to complement the information from the
CDF in certain environments where the immobility of the element
used for the normalization in the CDF is questioned or when the concen-
tration in this element is considered as heterogeneous in the parent ma-
terial. This study highlights that in eroding landscapes, a weathering
index such as the TRB can provide a useful complementary approach
to the classically used CDF to investigate the relationship between denu-
dation rate and chemical weathering intensity.
6. Conclusions
This study investigated the impact of denudation rates on soil chem-
ical weathering intensity in a semi-arid environment characterized by
low denudation rates using physico-chemical soil properties, mineralo-
gy and Si isotopes as weathering indexes. More specifically, this
multiproxy approach uses the Total Reserve in Bases (TRB), the amount
of Fe-oxides (Fed/Fet), the quartz content, the clay content, the cation
exchange capacity (CEC), and the Si isotope composition of the clay-
sized fraction (δ30Siclay-sized fraction) as weathering indexes.
Five of the six weathering indexes (TRB, Fed/Fet, quartz content, clay
content, CEC) converge to demonstrate that differences in denudation
rates produce significant differences in the soil chemical weathering in-
tensity in this semi-arid environment with low denudation rates: the
higher the denudation rates, the lower the soil weathering intensity.
Using the sixth weathering index (δ30Siclay-sized fraction), there is no con-
trast in the soil weathering intensity between catchments. A limited Si
loss in these soils (generally b 10%) suggest a low Si mobility with
weathering in this semi-arid environment, and probably explains that
no difference in δ30Siclay-sized fraction between catchments is observed.

Fig. 8. The Total Reserve in Bases (TRB, the sum of the total content in Ca, Mg, Na, K) as a function of the Chemical Depletion Fraction (CDF) in different locations: Red diamonds for granitic
soils from Dixon et al. (2012); blue triangles for gneissic soils from Norton and von Blanckenburg (2010); green crosses for granitic soils from Norton and von Blanckenburg (2010); orange
stars for shale derived soils from Jin et al. (2010) (CDF values recalculated using the Zr content in the shale parent material); purple dashes for data from the present study for mica schist
derived soils from the Betic Cordillera (CDF data from Schoonejans et al., 2016a). The TRB values have been calculated according to Eq. (2) with the total element content. Samples from
Norton and von Blanckenburg (2010) have been separated in two groups according to the parent material. Different correlations are observed: Dixon et al. (2012; R = 0.75), Norton and
von Blanckenburg (2010; gneiss, R = 0.77), Norton and von Blanckenburg (2010; granite, R = 0.92), Jin et al. (2010; R = −0.90), this study (R = −0.81).
 Y. Ameijeiras-Mariño et al. / Chemical Geology 456 (2017) 72–84
Given the agreement between our multiproxy approach and the
mass balance methods (CDF) in the same study site, our data demon-
strate that a multiproxy approach based on physico-chemical soil prop-
erties and mineralogy provides a consistent way to assess soil
weathering intensity as a response to soil denudation. Weathering in-
dexes such as the TRB, which can be easily obtained from the total ele-
ment composition, may provide a potentially interesting complement
to assess chemical weathering intensity in certain regions where the
use of the CDF might be questioned by mobility of the reference element
(e.g., Zr) or when the concentration in the reference element in the bed-
rock is considered heterogeneous. This study calls for more investiga-
tions on the complementarity between CDF and TRB in settings with
contrasted lithology, climate, and denudation rates.
Acknowledgements
We thank A. Iserentant and C. Givron from UCL for their help with
soil characterization. We also want to thank R. Ortega for his help during
field work, M. Bravin (UCL) for his help with the quantification of the to-
tal and inorganic carbon, N. Mattielli for managing the MC-ICP-MS facil-
ities at ULB in Brussels, and A. Guevara (DEMEX, Escuela Politécnica
Nacional in Quito, Ecuador) for her help with mineral quantification
based on X-ray diffraction patterns. The manuscript benefited from
helpful discussions with J.T. Cornélis and G. Govers. We also want to
thank the editor, J. Gaillardet, and P. Savage and one anonymous review-
er for their constructive comments that greatly improved this manu-
script. Y.A.M. and J.S. are funded by the Belgian Science Policy Office
(BELSPO) in the framework of the Inter University Attraction Pole pro-
ject (P7/24): SOGLO – The soil system under global change, and S.O. is
funded by the FNRS (FC69480), Belgium.
Appendix A. Supplementary data
Supplementary data to this article can be found online at http://dx.
doi.org/10.1016/j.chemgeo.2017.03.007.
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