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Title: Multi-element effects on arsenate accumulation in a geochemical matrix determined using µ-XRF, µ-XANES and spatial statistics

Abstract

Soils regulate the environmental impacts of trace elements, but direct measurements of reaction mechanisms in these complex, multi-component systems can be challenging. The objective of this work was to develop approaches for assessing effects of co-localized geochemical matrix elements on the accumulation and chemical speciation of arsenate applied to a soil matrix. Synchrotron X-ray fluorescence microprobe (µ-XRF) images collected across 100 µm × 100 µm and 10 µm × 10 µm regions of a naturally weathered soil sand-grain coating before and after treatment with As(V) solution showed strong positive partial correlations (r' = 0.77 and 0.64, respectively) between accumulated As and soil Fe, with weaker partial correlations (r' > 0.1) between As and Ca, and As and Zn in the larger image. Spatial and non-spatial regression models revealed a dominant contribution of Fe and minor contributions of Ca and Ti in predicting accumulated As, depending on the size of the sample area analyzed. Time-of-flight secondary ion mass spectrometry analysis of an area of the sand grain showed a significant correlation (r = 0.51) between Fe and Al, so effects of Fe versus Al (hydr)oxides on accumulated As could not be separated. Fitting results from 25 As K-edge microscale X-ray absorptionmore » near-edge structure (µ-XANES) spectra collected across a separate 10 µm × 10 µm region showed ~60% variation in proportions of Fe(III) and Al(III)-bound As(V) standards, and fits to µ-XANES spectra collected across the 100 µm × 100 µm region were more variable. We find that, consistent with insights from studies on model systems, the results obtained here indicate a dominance of Fe and possibly Al (hydr)oxides in controlling As(V) accumulation within microsites of the soil matrix analyzed, but the analyses inferred minor augmentation from co-localized Ti, Ca and possibly Zn.« less

Authors:
 [1];  [2];  [3];  [4];  [5];  [6];  [7];  [6];  [6];  [8];  [1]
  1. North Carolina State Univ., Raleigh, NC (United States)
  2. North Carolina State Univ., Raleigh, NC (United States); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  3. North Carolina State Univ., Raleigh, NC (United States); Cornell Univ., Ithaca, NY (United States)
  4. North Carolina State Univ., Raleigh, NC (United States); Univ. of Oregon, Eugene, OR (United States)
  5. North Carolina State Univ., Raleigh, NC (United States); Univ. of Iowa, Iowa City, IA (United States)
  6. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  7. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II); Stony Brook Univ., NY (United States)
  8. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II); Univ. of Chicago, IL (United States). Center for Advanced Radiation Sources (CARS)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1668639
Report Number(s):
BNL-219858-2020-JAAM
Journal ID: ISSN 1600-5775
Grant/Contract Number:  
SC0012704; EAR-1349374; ECCS-1542015
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Synchrotron Radiation (Online)
Additional Journal Information:
Journal Name: Journal of Synchrotron Radiation (Online); Journal Volume: 26; Journal Issue: 6; Journal ID: ISSN 1600-5775
Publisher:
International Union of Crystallography
Country of Publication:
United States
Language:
English
Subject:
58 GEOSCIENCES; reactive microsites; multi-component complexity; arsenic; partial correlation; spatial regression

Citation Formats

Sharma, Aakriti, Muyskens, Amanda, Guinness, Joseph, Polizzotto, Matthew L., Fuentes, Montserrat, Tappero, Ryan V., Chen-Wiegart, Yu-chen K., Thieme, Juergen, Williams, Garth J., Acerbo, Alvin S., and Hesterberg, Dean. Multi-element effects on arsenate accumulation in a geochemical matrix determined using µ-XRF, µ-XANES and spatial statistics. United States: N. p., 2019. Web. doi:10.1107/s1600577519012785.
Sharma, Aakriti, Muyskens, Amanda, Guinness, Joseph, Polizzotto, Matthew L., Fuentes, Montserrat, Tappero, Ryan V., Chen-Wiegart, Yu-chen K., Thieme, Juergen, Williams, Garth J., Acerbo, Alvin S., & Hesterberg, Dean. Multi-element effects on arsenate accumulation in a geochemical matrix determined using µ-XRF, µ-XANES and spatial statistics. United States. https://doi.org/10.1107/s1600577519012785
Sharma, Aakriti, Muyskens, Amanda, Guinness, Joseph, Polizzotto, Matthew L., Fuentes, Montserrat, Tappero, Ryan V., Chen-Wiegart, Yu-chen K., Thieme, Juergen, Williams, Garth J., Acerbo, Alvin S., and Hesterberg, Dean. Tue . "Multi-element effects on arsenate accumulation in a geochemical matrix determined using µ-XRF, µ-XANES and spatial statistics". United States. https://doi.org/10.1107/s1600577519012785. https://www.osti.gov/servlets/purl/1668639.
@article{osti_1668639,
title = {Multi-element effects on arsenate accumulation in a geochemical matrix determined using µ-XRF, µ-XANES and spatial statistics},
author = {Sharma, Aakriti and Muyskens, Amanda and Guinness, Joseph and Polizzotto, Matthew L. and Fuentes, Montserrat and Tappero, Ryan V. and Chen-Wiegart, Yu-chen K. and Thieme, Juergen and Williams, Garth J. and Acerbo, Alvin S. and Hesterberg, Dean},
abstractNote = {Soils regulate the environmental impacts of trace elements, but direct measurements of reaction mechanisms in these complex, multi-component systems can be challenging. The objective of this work was to develop approaches for assessing effects of co-localized geochemical matrix elements on the accumulation and chemical speciation of arsenate applied to a soil matrix. Synchrotron X-ray fluorescence microprobe (µ-XRF) images collected across 100 µm × 100 µm and 10 µm × 10 µm regions of a naturally weathered soil sand-grain coating before and after treatment with As(V) solution showed strong positive partial correlations (r' = 0.77 and 0.64, respectively) between accumulated As and soil Fe, with weaker partial correlations (r' > 0.1) between As and Ca, and As and Zn in the larger image. Spatial and non-spatial regression models revealed a dominant contribution of Fe and minor contributions of Ca and Ti in predicting accumulated As, depending on the size of the sample area analyzed. Time-of-flight secondary ion mass spectrometry analysis of an area of the sand grain showed a significant correlation (r = 0.51) between Fe and Al, so effects of Fe versus Al (hydr)oxides on accumulated As could not be separated. Fitting results from 25 As K-edge microscale X-ray absorption near-edge structure (µ-XANES) spectra collected across a separate 10 µm × 10 µm region showed ~60% variation in proportions of Fe(III) and Al(III)-bound As(V) standards, and fits to µ-XANES spectra collected across the 100 µm × 100 µm region were more variable. We find that, consistent with insights from studies on model systems, the results obtained here indicate a dominance of Fe and possibly Al (hydr)oxides in controlling As(V) accumulation within microsites of the soil matrix analyzed, but the analyses inferred minor augmentation from co-localized Ti, Ca and possibly Zn.},
doi = {10.1107/s1600577519012785},
journal = {Journal of Synchrotron Radiation (Online)},
number = 6,
volume = 26,
place = {United States},
year = {2019},
month = {10}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Figures / Tables:

Figure 1 Figure 1: Micro-XRF images of As [before and after a 0.1 m$M$ As(V) treatment] and soil matrix elements (before treatment) collected on the SRX beamline, along with TOF-SIMS images of Fe and Al collected on the As(V) treated sand grain. These images represent ROI-100, which had visible Fe-oxide coatings (Fig.more » S1). In $μ$-XRF images, scale bars show that brighter colors in the image represent greater natural log-transformed fluorescence signals for a given element in imaged soil volumes (microsites), and the linear scale bar in TOF-SIMS images indicates greater ion counts. The red square in the As image after treatment delineates ROI-10a, a 10 $μ$m x 10 $μ$m sub-region of ROI-100.« less

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