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Unraveling the Role of Capillarity in Arsenic Mobility: Insights from a Sedimentary–Karstic Aquifer in Semiarid Soil

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Abstract

Arsenic (As) contamination in soil and groundwater poses significant environmental and human health concerns. While chemical mechanisms like solubility equilibria, oxidation–reduction, and ionic exchange reactions have been studied to understand As retention in soil, the influence of capillarity on As transport remains poorly understood, particularly in semiarid soils with broader capillary fringes. This research aims to shed light on the capillary contribution to As attenuation and mobilization in the groundwater, focusing on degraded soil in the northeast of San Luis Potosí, Mexico. Groundwater surveys revealed a remarkable depletion of As concentrations from 91.50 to 11.27 mg L−1, indicating potential As sorption by the underlying shallow aquifer. We examined soil samples collected from the topsoil to the saturated zone using advanced analytical techniques such as X-ray diffraction (XRD), X-ray fluorescence (XRF), scanning electron microscopy (SEM), and wet chemical analyses. Our findings unveiled the presence of three distinct zones in the soil column: (1) the A horizon with heavy metals, (2) dispersed calcium sulfate dihydrate crystals and stratified gypsum, and (3) a higher concentration of arsenic in the capillary fringe. Notably, the capillary fringe exhibited a significant accumulation of As, constituting 40% (169.22 mg kg−1) of the total arsenic proportion accumulated (359.27 mg kg−1). The arsenic behavior in the capillary fringe solid phase correlated with total iron behavior, but they were distributed among different mineral fractions. The labile fraction, rich in arsenic, contrasted with the more recalcitrant fractions, which exhibited higher iron content. Further, thermodynamic stability assessments using the geochemical code PHREEQC revealed the critical role of Ca5H2(AsO4)4:9H2O in controlling HAsO42− and the formation of HAsO4:2H2O and CaHAsO4:H2O. During experimentation, we observed arsenate dissolution, indicating the potential mobilization of As in aqueous species. This mobilization was found to vary depending on redox conditions and may become labile during flooding events or water table variations, especially when As concentrations are low compared to metal cations, as demonstrated in our experiments. Our research underscores the significance of developing accurate geochemical conceptual models that incorporate capillarity to predict As leaching and remobilization accurately. This study presents novel insights into the understanding of As transport mechanisms and suggests the necessity of considering capillarity in geochemical models. By comprehending the capillary contribution to As attenuation, we can develop effective strategies to mitigate As contamination in semiarid soils and safeguard groundwater quality, thereby addressing crucial environmental and public health concerns.

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Acknowledgements

This paper and the research behind it would not have been possible without the exceptional support of the National Laboratory for Research in Nanosciences and Nanotechnology (LINAN), the Petrophysics and Petrography laboratory, the Geophysics laboratory both of the Applied Geosciences Division, the Stable Isotope Laboratory of the Environmental Sciences Division all of IPICYT, to Mtr. Beatriz Adriana Rivera Escoto, to Mtr. Ana Iris Peña Maldonado, Mtra. María Mercedes Zavala Arriaga, and Mtra. Alejandra Colunga Álvarez. This research was supported by Consejo Nacional de Ciencia y Tecnología (CONACYT; Grants No. CB-2012–183025 and 7073) and the Royal Society (Grant No. NA 140182). NVM is thankful to British Council-COPOCYT for

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  1. División de Geociencias Aplicadas, Instituto Potosino de Investigación Científica y Tecnológica (IPICYT), Camino a la Presa San José No. 2055, Col. Lomas 4a Sec., 78216, San Luis Potosí, SLP, Mexico

    Andrea Gómez-Hernández, Nadia Martínez-Villegas & Jejanny Lucero Hernández-Martínez

  2. Instituto de Metalurgia, Universidad Autónoma de San Luis Potosí (UASLP), 78210, San Luis Potosí, SLP, Mexico

    Javier Aguilar Carrillo de Albornoz

  3. Departamento de Geología, Universidad de Sonora (UNISON), 83260, Hermosillo, SON, Mexico

    Diana Meza-Figueroa

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AG-H contributed to conceptualization, methodology, validation, formal analysis, investigation, data curation, writing—original draft, writing—review and editing, visualization, and supervision. JLH-M contributed to methodology, writing—review and editing, visualization, and supervision. JACdA contributed to writing—original draft and writing—review and editing. DMF contributed to writing—original draft and writing—review and editing. NM-V contributed to formal analysis, investigation, resources, writing—review and editing, supervision, project administration, and funding acquisition.

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Gómez-Hernández, A., Martínez-Villegas, N., Hernández-Martínez, J.L. et al. Unraveling the Role of Capillarity in Arsenic Mobility: Insights from a Sedimentary–Karstic Aquifer in Semiarid Soil. Aquat Geochem (2024). https://doi.org/10.1007/s10498-024-09422-x

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