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

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

doi:10.1107/s1600577519012785

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

Journal Article · 22 October 2019 · Journal of Synchrotron Radiation (Online)

DOI: https://doi.org/10.1107/s1600577519012785 · OSTI ID:1668639

Sharma, Aakriti ^[1]; Muyskens, Amanda ^[2]; Guinness, Joseph ^[3]; Polizzotto, Matthew L. ^[4]; Fuentes, Montserrat ^[5]; Tappero, Ryan V. ^[6]; Chen-Wiegart, Yu-chen K. ^[7]; Thieme, Juergen ^[6]; Williams, Garth J. ^[6]; Acerbo, Alvin S. ^[8]; Hesterberg, Dean ^[1]

North Carolina State Univ., Raleigh, NC (United States)
North Carolina State Univ., Raleigh, NC (United States); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
North Carolina State Univ., Raleigh, NC (United States); Cornell Univ., Ithaca, NY (United States)
North Carolina State Univ., Raleigh, NC (United States); Univ. of Oregon, Eugene, OR (United States)
North Carolina State Univ., Raleigh, NC (United States); Univ. of Iowa, Iowa City, IA (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II); Stony Brook Univ., NY (United States)
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)

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.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: SC0012704

OSTI ID:: 1668639

Report Number(s):: BNL--219858-2020-JAAM

Journal Information:: Journal of Synchrotron Radiation (Online), Journal Name: Journal of Synchrotron Radiation (Online) Journal Issue: 6 Vol. 26; ISSN 1600-5775

Publisher:: International Union of CrystallographyCopyright Statement

Country of Publication:: United States

Language:: English

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58 GEOSCIENCES
arsenic
multi-component complexity
partial correlation
reactive microsites
spatial regression

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

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