Processes that control the dissolution of loess sediments and contribution of arsenic release in the Chaco-Pampean plain, Argentina

Groundwaters of the Chaco-Pampean Plain in Argentina are contaminated by arsenic released from weathered volcaniclastic loess sediments. To better understand As release, the dissolution of three loessial materials (loess, volcanic glass shards (VGS) and volcanic ash) that make up the sediments was studied at pH 2–12 and 10–50 °C using flow-through experiments. The variation in the output concentrations was reproduced by 1D reactive transport simulations, enabling us to infer that the reactivity of the phases controlling the overall dissolution of the loessial materials varies as a function of pH. Oligoclase dissolves faster than K-feldspar and the Al–Si-amorphous phase at acid pH whereas the K-feldspar and Al–Si-amorphous phases dissolve more rapidly at basic pH. The steady-state output Si concentrations attributed to the main dissolving phases at different pH were used to calculate the dissolution rates of the loessial materials, yielding faster rates at acid pH than at the circumneutral to basic pH. The variation in the dissolution rate (mol m−2 s−1) of the Al–Si-material making up the loess sediments in the shallow aquifers in the Chaco-Pampean Plain as a function of pH and temperature is expressed as Rdiss=10−2.25·aH+0.20±0.01·e[Formula presented]+10−8.51·e[Formula presented] Simulations indicate that an initially high release of cations is due to rapid dissolution of fine particles and cation exchange between the exchangeable cations (Na, Ca, K and Mg) of the Al–Si-amorphous phase and those of the electrolyte solution. At steady state, dissolution of the coarse fraction was responsible for the cations release. The variation in the output As concentrations was simulated by considering two arsenic sources: (i) the arsenic from the As-rich fluorapatite and Fe-(hydr)oxides (e.g. ferrihydrite) that dissolve at acid pH and desorb As at basic pH, releasing arsenic into the solution, and (ii) Al–Si phases (e.g. volcanic glass), the dissolution of which releases the arsenic from the solid structure into the solution at any pH. At the start of the experiments, fluorapatite, ferrihydrite, glass an aluminosilicates contributed arsenic to the solution. At steady state, As was mainly released from the glass and the aluminosilicates, and the rate of As release from the loessial materials that constitute the Chaco-Pampean loess sediments was calculated using the aqueous As/Si ratios ((9.2 ± 8.8)·10−5 and (7.4 ± 2.2)·10−5 at acidic and basic pH, respectively).

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Main Authors: Cacciabue, Lucía, Ceballos, Elina, Sierra, Leonardo, Soler, Josep M., Cama, Jordi
Other Authors: Ministerio de Ciencia e Innovación (España)
Format: artículo biblioteca
Language:English
Published: Elsevier 2022-05-01
Subjects:Reactive transport modeling, Arsenic, Dissolution kinetics, Flow-through experiments, Loess,
Online Access:http://hdl.handle.net/10261/268420
http://dx.doi.org/10.13039/501100004837
https://api.elsevier.com/content/abstract/scopus_id/85127853490
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id dig-idaea-es-10261-268420
record_format koha
institution IDAEA ES
collection DSpace
country España
countrycode ES
component Bibliográfico
access En linea
databasecode dig-idaea-es
tag biblioteca
region Europa del Sur
libraryname Biblioteca del IDAEA España
language English
topic Reactive transport modeling
Arsenic
Dissolution kinetics
Flow-through experiments
Loess
Reactive transport modeling
Arsenic
Dissolution kinetics
Flow-through experiments
Loess
spellingShingle Reactive transport modeling
Arsenic
Dissolution kinetics
Flow-through experiments
Loess
Reactive transport modeling
Arsenic
Dissolution kinetics
Flow-through experiments
Loess
Cacciabue, Lucía
Ceballos, Elina
Sierra, Leonardo
Soler, Josep M.
Cama, Jordi
Processes that control the dissolution of loess sediments and contribution of arsenic release in the Chaco-Pampean plain, Argentina
description Groundwaters of the Chaco-Pampean Plain in Argentina are contaminated by arsenic released from weathered volcaniclastic loess sediments. To better understand As release, the dissolution of three loessial materials (loess, volcanic glass shards (VGS) and volcanic ash) that make up the sediments was studied at pH 2–12 and 10–50 °C using flow-through experiments. The variation in the output concentrations was reproduced by 1D reactive transport simulations, enabling us to infer that the reactivity of the phases controlling the overall dissolution of the loessial materials varies as a function of pH. Oligoclase dissolves faster than K-feldspar and the Al–Si-amorphous phase at acid pH whereas the K-feldspar and Al–Si-amorphous phases dissolve more rapidly at basic pH. The steady-state output Si concentrations attributed to the main dissolving phases at different pH were used to calculate the dissolution rates of the loessial materials, yielding faster rates at acid pH than at the circumneutral to basic pH. The variation in the dissolution rate (mol m−2 s−1) of the Al–Si-material making up the loess sediments in the shallow aquifers in the Chaco-Pampean Plain as a function of pH and temperature is expressed as Rdiss=10−2.25·aH+0.20±0.01·e[Formula presented]+10−8.51·e[Formula presented] Simulations indicate that an initially high release of cations is due to rapid dissolution of fine particles and cation exchange between the exchangeable cations (Na, Ca, K and Mg) of the Al–Si-amorphous phase and those of the electrolyte solution. At steady state, dissolution of the coarse fraction was responsible for the cations release. The variation in the output As concentrations was simulated by considering two arsenic sources: (i) the arsenic from the As-rich fluorapatite and Fe-(hydr)oxides (e.g. ferrihydrite) that dissolve at acid pH and desorb As at basic pH, releasing arsenic into the solution, and (ii) Al–Si phases (e.g. volcanic glass), the dissolution of which releases the arsenic from the solid structure into the solution at any pH. At the start of the experiments, fluorapatite, ferrihydrite, glass an aluminosilicates contributed arsenic to the solution. At steady state, As was mainly released from the glass and the aluminosilicates, and the rate of As release from the loessial materials that constitute the Chaco-Pampean loess sediments was calculated using the aqueous As/Si ratios ((9.2 ± 8.8)·10−5 and (7.4 ± 2.2)·10−5 at acidic and basic pH, respectively).
author2 Ministerio de Ciencia e Innovación (España)
author_facet Ministerio de Ciencia e Innovación (España)
Cacciabue, Lucía
Ceballos, Elina
Sierra, Leonardo
Soler, Josep M.
Cama, Jordi
format artículo
topic_facet Reactive transport modeling
Arsenic
Dissolution kinetics
Flow-through experiments
Loess
author Cacciabue, Lucía
Ceballos, Elina
Sierra, Leonardo
Soler, Josep M.
Cama, Jordi
author_sort Cacciabue, Lucía
title Processes that control the dissolution of loess sediments and contribution of arsenic release in the Chaco-Pampean plain, Argentina
title_short Processes that control the dissolution of loess sediments and contribution of arsenic release in the Chaco-Pampean plain, Argentina
title_full Processes that control the dissolution of loess sediments and contribution of arsenic release in the Chaco-Pampean plain, Argentina
title_fullStr Processes that control the dissolution of loess sediments and contribution of arsenic release in the Chaco-Pampean plain, Argentina
title_full_unstemmed Processes that control the dissolution of loess sediments and contribution of arsenic release in the Chaco-Pampean plain, Argentina
title_sort processes that control the dissolution of loess sediments and contribution of arsenic release in the chaco-pampean plain, argentina
publisher Elsevier
publishDate 2022-05-01
url http://hdl.handle.net/10261/268420
http://dx.doi.org/10.13039/501100004837
https://api.elsevier.com/content/abstract/scopus_id/85127853490
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spelling dig-idaea-es-10261-2684202023-02-03T21:51:27Z Processes that control the dissolution of loess sediments and contribution of arsenic release in the Chaco-Pampean plain, Argentina Cacciabue, Lucía Ceballos, Elina Sierra, Leonardo Soler, Josep M. Cama, Jordi Ministerio de Ciencia e Innovación (España) 0000-0001-6623-8116 Reactive transport modeling Arsenic Dissolution kinetics Flow-through experiments Loess Groundwaters of the Chaco-Pampean Plain in Argentina are contaminated by arsenic released from weathered volcaniclastic loess sediments. To better understand As release, the dissolution of three loessial materials (loess, volcanic glass shards (VGS) and volcanic ash) that make up the sediments was studied at pH 2–12 and 10–50 °C using flow-through experiments. The variation in the output concentrations was reproduced by 1D reactive transport simulations, enabling us to infer that the reactivity of the phases controlling the overall dissolution of the loessial materials varies as a function of pH. Oligoclase dissolves faster than K-feldspar and the Al–Si-amorphous phase at acid pH whereas the K-feldspar and Al–Si-amorphous phases dissolve more rapidly at basic pH. The steady-state output Si concentrations attributed to the main dissolving phases at different pH were used to calculate the dissolution rates of the loessial materials, yielding faster rates at acid pH than at the circumneutral to basic pH. The variation in the dissolution rate (mol m−2 s−1) of the Al–Si-material making up the loess sediments in the shallow aquifers in the Chaco-Pampean Plain as a function of pH and temperature is expressed as Rdiss=10−2.25·aH+0.20±0.01·e[Formula presented]+10−8.51·e[Formula presented] Simulations indicate that an initially high release of cations is due to rapid dissolution of fine particles and cation exchange between the exchangeable cations (Na, Ca, K and Mg) of the Al–Si-amorphous phase and those of the electrolyte solution. At steady state, dissolution of the coarse fraction was responsible for the cations release. The variation in the output As concentrations was simulated by considering two arsenic sources: (i) the arsenic from the As-rich fluorapatite and Fe-(hydr)oxides (e.g. ferrihydrite) that dissolve at acid pH and desorb As at basic pH, releasing arsenic into the solution, and (ii) Al–Si phases (e.g. volcanic glass), the dissolution of which releases the arsenic from the solid structure into the solution at any pH. At the start of the experiments, fluorapatite, ferrihydrite, glass an aluminosilicates contributed arsenic to the solution. At steady state, As was mainly released from the glass and the aluminosilicates, and the rate of As release from the loessial materials that constitute the Chaco-Pampean loess sediments was calculated using the aqueous As/Si ratios ((9.2 ± 8.8)·10−5 and (7.4 ± 2.2)·10−5 at acidic and basic pH, respectively). Thanks are due to Jordi Bellés (IDAEA-CSIC) and Maite Romero, Javier García-Veigas and David Artiaga (Scientific and Technical Services of Barcelona University) for their help in assisting in the laboratory, ICP-AES and SEM-EDX analyses, respectively. This study was partially funded by the PID75/2011 (Federal Water Resources Council (COHIFE)), PICT1805/2014 (National Agency of Science and Technological Promotion (ANPCYT)), 2017SGR 1733 (Catalan Government) projects and the CEX2018-000794-S Grant funded by MCIN/AEI/10.13039/501100011033 (Spanish Government). We also wish to thank the two anonymous reviewers for their constructive comments that have improved the quality of the paper. Peer reviewed 2022-05-03T05:40:20Z 2022-05-03T05:40:20Z 2022-05-01 artículo http://purl.org/coar/resource_type/c_6501 Applied Geochemistry 140: 105243 (2022) 08832927 http://hdl.handle.net/10261/268420 10.1016/j.apgeochem.2022.105243 http://dx.doi.org/10.13039/501100004837 2-s2.0-85127853490 https://api.elsevier.com/content/abstract/scopus_id/85127853490 en #PLACEHOLDER_PARENT_METADATA_VALUE# info:eu-repo/grantAgreement/MCIN/AEI/10.13039/501100011033 Applied Geochemistry Postprint https://doi.org/10.1016/j.apgeochem.2022.105243 Sí embargo_20240501 Elsevier