Solid-phase arsenic speciation in aquifer sediments: A micro-X-ray absorption spectroscopy approach for quantifying trace-level speciation
Abstract
Arsenic (As) is a geogenic contaminant affecting groundwater in geologically diverse systems globally. Arsenic release from aquifer sediments to groundwater is favored when biogeochemical conditions, especially oxidation-reduction (redox) potential, in aquifers fluctuate. The specific objective of this research is to identify the solid-phase sources and geochemical mechanisms of release of As in aquifers of the Des Moines Lobe glacial advance. The overarching concept is that conditions present at the aquifer-aquitard interfaces promote a suite of geochemical reactions leading to mineral alteration and release of As to groundwater. A microprobe X-ray absorption spectroscopy (μXAS) approach is developed and applied to rotosonic drill core samples to identify the solid-phase speciation of As in aquifer, aquitard, and aquifer-aquitard interface sediments. This approach addresses the low solid-phase As concentrations, as well as the fine-scale physical and chemical heterogeneity of the sediments. The spectroscopy data are analyzed using novel cosine-distance and correlation-distance hierarchical clustering for Fe 1s and As 1s μXAS datasets. The solid-phase Fe and As speciation is then interpreted using sediment and well-water chemical data to propose solid-phase As reservoirs and release mechanisms. The results confirm that in two of the three locations studied, the glacial sediment forming the aquitard is the sourcemore »
- Authors:
-
- Univ. of Minnesota, Saint Paul, MN (United States); National Univ. of Ireland, Galway (Ireland)
- Minnesota Water Science Center, Mounds View, MN (United States)
- Minnesota Geological Survey, Saint Paul, MN (United States)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
- Univ. of Arizona, Tucson, AZ (United States); Univ. of Minnesota, Saint Paul, MN (United States)
- Univ. of Minnesota, Saint Paul, MN (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1379920
- Alternate Identifier(s):
- OSTI ID: 1550072
- Grant/Contract Number:
- AC02-05CH11231; AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Geochimica et Cosmochimica Acta
- Additional Journal Information:
- Journal Volume: 211; Journal Issue: C; Journal ID: ISSN 0016-7037
- Publisher:
- The Geochemical Society; The Meteoritical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 54 ENVIRONMENTAL SCIENCES
Citation Formats
Nicholas, Sarah L., Erickson, Melinda L., Woodruff, Laurel G., Knaeble, Alan R., Marcus, Matthew A., Lynch, Joshua K., and Toner, Brandy M. Solid-phase arsenic speciation in aquifer sediments: A micro-X-ray absorption spectroscopy approach for quantifying trace-level speciation. United States: N. p., 2017.
Web. doi:10.1016/j.gca.2017.05.018.
Nicholas, Sarah L., Erickson, Melinda L., Woodruff, Laurel G., Knaeble, Alan R., Marcus, Matthew A., Lynch, Joshua K., & Toner, Brandy M. Solid-phase arsenic speciation in aquifer sediments: A micro-X-ray absorption spectroscopy approach for quantifying trace-level speciation. United States. https://doi.org/10.1016/j.gca.2017.05.018
Nicholas, Sarah L., Erickson, Melinda L., Woodruff, Laurel G., Knaeble, Alan R., Marcus, Matthew A., Lynch, Joshua K., and Toner, Brandy M. Fri .
"Solid-phase arsenic speciation in aquifer sediments: A micro-X-ray absorption spectroscopy approach for quantifying trace-level speciation". United States. https://doi.org/10.1016/j.gca.2017.05.018. https://www.osti.gov/servlets/purl/1379920.
@article{osti_1379920,
title = {Solid-phase arsenic speciation in aquifer sediments: A micro-X-ray absorption spectroscopy approach for quantifying trace-level speciation},
author = {Nicholas, Sarah L. and Erickson, Melinda L. and Woodruff, Laurel G. and Knaeble, Alan R. and Marcus, Matthew A. and Lynch, Joshua K. and Toner, Brandy M.},
abstractNote = {Arsenic (As) is a geogenic contaminant affecting groundwater in geologically diverse systems globally. Arsenic release from aquifer sediments to groundwater is favored when biogeochemical conditions, especially oxidation-reduction (redox) potential, in aquifers fluctuate. The specific objective of this research is to identify the solid-phase sources and geochemical mechanisms of release of As in aquifers of the Des Moines Lobe glacial advance. The overarching concept is that conditions present at the aquifer-aquitard interfaces promote a suite of geochemical reactions leading to mineral alteration and release of As to groundwater. A microprobe X-ray absorption spectroscopy (μXAS) approach is developed and applied to rotosonic drill core samples to identify the solid-phase speciation of As in aquifer, aquitard, and aquifer-aquitard interface sediments. This approach addresses the low solid-phase As concentrations, as well as the fine-scale physical and chemical heterogeneity of the sediments. The spectroscopy data are analyzed using novel cosine-distance and correlation-distance hierarchical clustering for Fe 1s and As 1s μXAS datasets. The solid-phase Fe and As speciation is then interpreted using sediment and well-water chemical data to propose solid-phase As reservoirs and release mechanisms. The results confirm that in two of the three locations studied, the glacial sediment forming the aquitard is the source of As to the aquifer sediments. The results are consistent with three different As release mechanisms: (1) desorption from Fe (oxyhydr)oxides, (2) reductive dissolution of Fe (oxyhydr)oxides, and (3) oxidative dissolution of Fe sulfides. The findings confirm that glacial sediments at the interface between aquifer and aquitard are geochemically active zones for As. The diversity of As release mechanisms is consistent with the geographic heterogeneity seen in the distribution of elevated-As wells.},
doi = {10.1016/j.gca.2017.05.018},
journal = {Geochimica et Cosmochimica Acta},
number = C,
volume = 211,
place = {United States},
year = {Fri May 19 00:00:00 EDT 2017},
month = {Fri May 19 00:00:00 EDT 2017}
}
Web of Science
Works referenced in this record:
In situ characterization of Mn(II) oxidation by spores of the marine Bacillus sp. strain SG-1
journal, August 2000
- Bargar, J. R.; Tebo, B. M.; Villinski, J. E.
- Geochimica et Cosmochimica Acta, Vol. 64, Issue 16
Biogeochemical Redox Processes and their Impact on Contaminant Dynamics
journal, January 2010
- Borch, Thomas; Kretzschmar, Ruben; Kappler, Andreas
- Environmental Science & Technology, Vol. 44, Issue 1
Standard molar enthalpies of formation of realgar (α-AsS) and orpiment (As2S3) by high-temperature direct-synthesis calorimetry
journal, June 1988
- Bryndzia, L. Taras; Kleppa, O. J.
- The Journal of Chemical Thermodynamics, Vol. 20, Issue 6
Arsenopyrite oxidation – A review
journal, December 2009
- Corkhill, C. L.; Vaughan, D. J.
- Applied Geochemistry, Vol. 24, Issue 12
Environmental arsenopyrite stability and dissolution: theory, experiment, and field observations
journal, August 2003
- Craw, D.; Falconer, D.; Youngson, J. H.
- Chemical Geology, Vol. 199, Issue 1-2
How does gene expression clustering work?
journal, December 2005
- D'haeseleer, Patrik
- Nature Biotechnology, Vol. 23, Issue 12
The solubility of amorphous As2S3 from 25 to 90°C
journal, June 1992
- Eary, L. E.
- Geochimica et Cosmochimica Acta, Vol. 56, Issue 6
Cluster analysis and display of genome-wide expression patterns
journal, December 1998
- Eisen, M. B.; Spellman, P. T.; Brown, P. O.
- Proceedings of the National Academy of Sciences, Vol. 95, Issue 25
Well characteristics influencing arsenic concentrations in ground water
journal, October 2005
- Erickson, Melinda L.; Barnes, Randal J.
- Water Research, Vol. 39, Issue 16
Inferring Correlation Networks from Genomic Survey Data
journal, September 2012
- Friedman, Jonathan; Alm, Eric J.
- PLoS Computational Biology, Vol. 8, Issue 9
Effects of Water Use on Arsenic Release to Well Water in a Confined Aquifer
journal, July 2004
- Gotkowitz, Madeline B.; Schreiber, Madeline E.; Simo, J. A.
- Ground Water, Vol. 42, Issue 4
Dominance of sulfur-fueled iron oxide reduction in low-sulfate freshwater sediments
journal, April 2015
- Hansel, Colleen M.; Lentini, Chris J.; Tang, Yuanzhi
- The ISME Journal, Vol. 9, Issue 11
Evaluating mobilization and transport of arsenic in sediments and groundwaters of Aquia aquifer, Maryland, USA
journal, July 2008
- Haque, Shama; Ji, Junfeng; Johannesson, Karen H.
- Journal of Contaminant Hydrology, Vol. 99, Issue 1-4
Matplotlib: A 2D Graphics Environment
journal, January 2007
- Hunter, John D.
- Computing in Science & Engineering, Vol. 9, Issue 3
Terrestrial ice streams—a view from the lobe
journal, April 2006
- Jennings, Carrie E.
- Geomorphology, Vol. 75, Issue 1-2
Integrated biogeochemical and hydrologic processes driving arsenic release from shallow sediments to groundwaters of the Mekong delta
journal, November 2008
- Kocar, Benjamin D.; Polizzotto, Matthew L.; Benner, Shawn G.
- Applied Geochemistry, Vol. 23, Issue 11
The speciation of marine particulate iron adjacent to active and passive continental margins
journal, March 2012
- Lam, Phoebe J.; Ohnemus, Daniel C.; Marcus, Matthew A.
- Geochimica et Cosmochimica Acta, Vol. 80
Beamline 10.3.2 at ALS: a hard X-ray microprobe for environmental and materials sciences
journal, April 2004
- Marcus, Matthew A.; MacDowell, Alastair A.; Celestre, Richard
- Journal of Synchrotron Radiation, Vol. 11, Issue 3
Classification of Fe-bearing species from K -edge XANES data using two-parameter correlation plots
journal, August 2008
- Marcus, Matthew A.; Westphal, Andrew J.; Fakra, Sirine C.
- Journal of Synchrotron Radiation, Vol. 15, Issue 5
X-ray photon-in/photon-out methods for chemical imaging
journal, June 2010
- Marcus, Matthew A.
- TrAC Trends in Analytical Chemistry, Vol. 29, Issue 6
Microscale Imaging and Identification of Fe Speciation and Distribution during Fluid–Mineral Reactions under Highly Reducing Conditions
journal, May 2011
- Mayhew, L. E.; Webb, S. M.; Templeton, A. S.
- Environmental Science & Technology, Vol. 45, Issue 10
Aquifer/aquitard interfaces: mixing zones that enhance biogeochemical reactions
journal, February 2001
- McMahon, P.
- Hydrogeology Journal, Vol. 9, Issue 1
Oxidation of arsenopyrite by air and air-saturated, distilled water, and implications for mechanism of oxidation
journal, May 1995
- Nesbitt, H. W.; Muir, I. J.; Prarr, A. R.
- Geochimica et Cosmochimica Acta, Vol. 59, Issue 9
Oxidation states and speciation of secondary products on pyrite and arsenopyrite reacted with mine waste waters and air
journal, March 1998
- Nesbitt, H. W.; Muir, I. J.
- Mineralogy and Petrology, Vol. 62, Issue 1-2
The influence of sulfur and iron on dissolved arsenic concentrations in the shallow subsurface under changing redox conditions
journal, September 2004
- O'Day, P. A.; Vlassopoulos, D.; Root, R.
- Proceedings of the National Academy of Sciences, Vol. 101, Issue 38
Python for Scientific Computing
journal, January 2007
- Oliphant, Travis E.
- Computing in Science & Engineering, Vol. 9, Issue 3
Laurentide glacial landscapes: The role of ice streams
journal, January 1998
- Patterson, Carrie J.
- Geology, Vol. 26, Issue 7
Localizing the Chemical Forms of Sulfur in Vivo Using X-ray Fluorescence Spectroscopic Imaging: Application to Onion ( Allium cepa ) Tissues
journal, July 2009
- Pickering, Ingrid J.; Sneeden, Eileen Yu; Prince, Roger C.
- Biochemistry, Vol. 48, Issue 29
Linking organic matter deposition and iron mineral transformations to groundwater arsenic levels in the Mekong delta, Cambodia
journal, November 2008
- Quicksall, Andrew N.; Bostick, Benjamin C.; Sampson, M. L.
- Applied Geochemistry, Vol. 23, Issue 11
Arsenopyrite: a spectroscopic investigation of altered surfaces
journal, April 1989
- Richardson, S.; Vaughan, D. J.
- Mineralogical Magazine, Vol. 53, Issue 370
Changes in Iron, Sulfur, and Arsenic Speciation Associated with Bacterial Sulfate Reduction in Ferrihydrite-Rich Systems
journal, October 2009
- Saalfield, Samantha L.; Bostick, Benjamin C.
- Environmental Science & Technology, Vol. 43, Issue 23
Trace element source terms for mineral dissolution
journal, October 2013
- Schreiber, Madeline E.; Rimstidt, J. Donald
- Applied Geochemistry, Vol. 37
Stratigraphic and geochemical controls on naturally occurring arsenic in groundwater, eastern Wisconsin, USA
journal, May 2000
- Schreiber, M. E.; Simo, J. A.; Freiberg, P. G.
- Hydrogeology Journal, Vol. 8, Issue 2
Detection of Significant Groups in Hierarchical Clustering by Resampling
journal, August 2016
- Sebastiani, Paola; Perls, Thomas T.
- Frontiers in Genetics, Vol. 7
A review of the source, behaviour and distribution of arsenic in natural waters
journal, May 2002
- Smedley, P. L.; Kinniburgh, D. G.
- Applied Geochemistry, Vol. 17, Issue 5
Petrology of glacial sand: implications for the origin and mechanical durability of lithic fragments
journal, April 1981
- Slatt, Roger M.; Eyles, Nicholas
- Sedimentology, Vol. 28, Issue 2
Peat formation concentrates arsenic within sediment deposits of the Mekong Delta
journal, January 2015
- Stuckey, Jason W.; Schaefer, Michael V.; Kocar, Benjamin D.
- Geochimica et Cosmochimica Acta, Vol. 149
Measuring the Form of Iron in Hydrothermal Plume Particles
journal, March 2012
- Toner, Brandy; Marcus, Matthew; Edwards, Katrina
- Oceanography, Vol. 25, Issue 1
Scaling up: fulfilling the promise of X-ray microprobe for biogeochemical research
journal, January 2014
- Toner, Brandy M.; Nicholas, Sarah L.; Wasik, Jill K. Coleman
- Environmental Chemistry, Vol. 11, Issue 1
Deciphering the Complex Chemistry of Deep-Ocean Particles Using Complementary Synchrotron X-ray Microscope and Microprobe Instruments
journal, December 2015
- Toner, Brandy M.; German, Christopher R.; Dick, Gregory J.
- Accounts of Chemical Research, Vol. 49, Issue 1
Reductive Processes Controlling Arsenic Retention: Revealing the Relative Importance of Iron and Arsenic Reduction
journal, November 2008
- Tufano, Katharine J.; Reyes, Carolina; Saltikov, Chad W.
- Environmental Science & Technology, Vol. 42, Issue 22
Arsenic in Ground Water of the United States: Occurrence and Geochemistry
journal, July 2000
- Welch, Alan H.; Westjohn, D. B.; Helsel, Dennis R.
- Ground Water, Vol. 38, Issue 4
Arsenic release from chlorine-promoted alteration of a sulfide cement horizon: Evidence from batch studies on the St. Peter Sandstone, Wisconsin, USA
journal, November 2012
- West, Nicole; Schreiber, Madeline; Gotkowitz, Madeline
- Applied Geochemistry, Vol. 27, Issue 11
Rates of Arsenopyrite Oxidation by Oxygen and Fe(III) at pH 1.8−12.6 and 15−45 °C
journal, September 2007
- Yu, Yunmei; Zhu, Yongxuan; Gao, Zhenmin
- Environmental Science & Technology, Vol. 41, Issue 18
Microscale Characterization of Sulfur Speciation in Lake Sediments
journal, February 2013
- Zeng, Teng; Arnold, William A.; Toner, Brandy M.
- Environmental Science & Technology, Vol. 47, Issue 3
Works referencing / citing this record:
Predicting geogenic Arsenic in Drinking Water Wells in Glacial Aquifers, North‐Central USA: Accounting for Depth‐Dependent Features
journal, December 2018
- Erickson, M. L.; Elliott, S. M.; Christenson, C. A.
- Water Resources Research, Vol. 54, Issue 12
How or When Samples Are Collected Affects Measured Arsenic Concentration in New Drinking Water Wells
journal, March 2018
- Erickson, Melinda L.; Malenda, Helen F.; Berquist, Emily C.
- Groundwater, Vol. 56, Issue 6
How or When Samples Are Collected Affects Measured Arsenic Concentration in New Drinking Water Wells
journal, March 2018
- Erickson, Melinda L.; Malenda, Helen F.; Berquist, Emily C.
- Groundwater, Vol. 56, Issue 6