Two-Dimensional Mapping of Arsenic Concentration and Speciation with Diffusive Equilibrium in Thin-Film Gels
Andrea Castillejos Sepúlveda
Edouard Metzger
Sten Littmann
Heidi Taubner
Arjun Chennu
Lais Gatti
Dirk de Beer
Judith M. Klatt
Abstract
We present a new approach combining diffusive equilibrium in thin-film gels and spectrophotometric methods to determine the spatial distribution of arsenite, arsenate, and phosphate at submillimeter resolution. The method relies on the simultaneous deployment of three gel probes. Each retrieved gel is exposed to malachite green reagent gels differing in acidity and oxidant addition, leading to green coloration dependent on analyte speciation and concentration. Hyperspectral images of the gels enable mapping the three analytes in the 2.5–20 μM range. This method was applied in a contaminated brook in the Harz mountains, Germany, together with established mapping of dissolved iron. The use of two-dimensional (2D) gel probes was compared to traditional porewater extraction. The gels revealed banded porewater patterns on a mm-scale, which were undetectable using traditional methods. Small-scale correlation analyses of arsenic and iron microstructures in the gels suggested active iron-driven local redox cycling of arsenic. Overall, the results indicate continuous net release of arsenic from contaminant particles and deepen our understanding of arsenate transformation under anaerobic conditions. This study is the first fine-scale 2D characterization of arsenic speciation in porewater and represents a crucial step toward understanding the transfer and redox cycling of arsenic in contaminated sediment/soil ecosystems.
Castillejos Sepúlveda A., Metzger E., Littmann S., Taubner H., Chennu A., Gatti L., de Beer D. and Klatt J.M. (2023) Two-Dimensional Mapping of Arsenic Concentration and Speciation with Diffusive Equilibrium in Thin-Film Gels. Environmental Science & Technology 57(21): 8107-8117. 10.1021/acs.est.3c00887
@article{Castillejos Sepúlveda2023,
Title = {Two-Dimensional Mapping of Arsenic Concentration and Speciation with Diffusive Equilibrium in Thin-Film Gels},
Author = {Castillejos Sepúlveda, Andrea and Metzger, Edouard and Littmann, Sten and Taubner, Heidi and Chennu, Arjun and Gatti, Lais and de Beer, Dirk and Klatt, Judith M.},
Editor = {},
Journal = {Environmental Science & Technology},
Year = {2023},
Pages = {8107-8117},
Volume = {57},
Doi = {10.1021/acs.est.3c00887},
Abstract = {We present a new approach combining diffusive equilibrium in thin-film gels and spectrophotometric methods to determine the spatial distribution of arsenite, arsenate, and phosphate at submillimeter resolution. The method relies on the simultaneous deployment of three gel probes. Each retrieved gel is exposed to malachite green reagent gels differing in acidity and oxidant addition, leading to green coloration dependent on analyte speciation and concentration. Hyperspectral images of the gels enable mapping the three analytes in the 2.5–20 μM range. This method was applied in a contaminated brook in the Harz mountains, Germany, together with established mapping of dissolved iron. The use of two-dimensional (2D) gel probes was compared to traditional porewater extraction. The gels revealed banded porewater patterns on a mm-scale, which were undetectable using traditional methods. Small-scale correlation analyses of arsenic and iron microstructures in the gels suggested active iron-driven local redox cycling of arsenic. Overall, the results indicate continuous net release of arsenic from contaminant particles and deepen our understanding of arsenate transformation under anaerobic conditions. This study is the first fine-scale 2D characterization of arsenic speciation in porewater and represents a crucial step toward understanding the transfer and redox cycling of arsenic in contaminated sediment/soil ecosystems.},
}
TY - JOUR
AU - Castillejos Sepúlveda, Andrea
AU - Metzger, Edouard
AU - Littmann, Sten
AU - Taubner, Heidi
AU - Chennu, Arjun
AU - Gatti, Lais
AU - de Beer, Dirk
AU - Klatt, Judith M.
TI - Two-Dimensional Mapping of Arsenic Concentration and Speciation with Diffusive Equilibrium in Thin-Film Gels
T2 - Environmental Science & Technology
PY - 2023
SP - 8107-8117
VL - 57
DO - 10.1021/acs.est.3c00887
AB - We present a new approach combining diffusive equilibrium in thin-film gels and spectrophotometric methods to determine the spatial distribution of arsenite, arsenate, and phosphate at submillimeter resolution. The method relies on the simultaneous deployment of three gel probes. Each retrieved gel is exposed to malachite green reagent gels differing in acidity and oxidant addition, leading to green coloration dependent on analyte speciation and concentration. Hyperspectral images of the gels enable mapping the three analytes in the 2.5–20 μM range. This method was applied in a contaminated brook in the Harz mountains, Germany, together with established mapping of dissolved iron. The use of two-dimensional (2D) gel probes was compared to traditional porewater extraction. The gels revealed banded porewater patterns on a mm-scale, which were undetectable using traditional methods. Small-scale correlation analyses of arsenic and iron microstructures in the gels suggested active iron-driven local redox cycling of arsenic. Overall, the results indicate continuous net release of arsenic from contaminant particles and deepen our understanding of arsenate transformation under anaerobic conditions. This study is the first fine-scale 2D characterization of arsenic speciation in porewater and represents a crucial step toward understanding the transfer and redox cycling of arsenic in contaminated sediment/soil ecosystems.
ER -
