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Title: Nanoscale heterogeneity of arsenic and selenium species in coal fly ash particles: analysis using enhanced spectroscopic imaging and speciation techniques

Journal Article · · Environmental Science: Nano
DOI:https://doi.org/10.1039/D2EN01056A· OSTI ID:1983983
ORCiD logo [1];  [2];  [1]; ORCiD logo [3];  [3];  [3]; ORCiD logo [4]; ORCiD logo [1]
  1. Department of Civil and Environmental Engineering, Duke University, Box 90287, Durham, North Carolina 27708, USA
  2. Department of Civil and Environmental Engineering, Princeton University, Princeton, New Jersey 08544, USA, Environmental Science Program, Department of Chemistry and Biochemistry, La Salle University, Philadelphia, PA 19141, USA
  3. National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, NY 11973, USA
  4. Department of Civil and Environmental Engineering, Princeton University, Princeton, New Jersey 08544, USA

Coal combustion byproducts are known to be enriched in arsenic (As) and selenium (Se). This enrichment is a concern during the handling, disposal, and reuse of the ash as both elements can be harmful to wildlife and humans if mobilized into water and soils. The leaching potential and bioaccessibility of As and Se in coal fly ash depends on the chemical forms of these elements and their association with the large variety of particles that comprise coal fly ash. The overall goal of this research was to determine nanoscale and microscale solid phase mineral associations and oxidation states of As and Se in fly ash. We utilized nanoscale 2D imaging (30–50 nm spot size) with the Hard X-ray Nanoprobe (HXN) in combination with microprobe X-ray capabilities (~5 μm resolution) to determine the As and Se elemental associations. Speciation of As and Se was also measured at the nano- to microscale with X-ray absorption spectroscopy. The enhanced resolution of HXN showed As and Se as either diffusely located around or comingled with Ca- and Fe-rich particles. The results also showed nanoparticles of Se attached to the surface of fly ash grains. Overall, a comparison of As and Se species across scales highlights the heterogeneity and complexity of chemical associations for these trace elements of concern in coal fly ash.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Duke Univ., Durham, NC (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER); National Institute of Environmental Health Sciences; National Institutes of Health (NIH); USDOE Office of Fossil Energy (FE), Clean Coal and Carbon Management
Grant/Contract Number:
FE0031748; AC02-76SF00515; SC0012704; 5U2CES030851; P30GM133894
OSTI ID:
1983983
Alternate ID(s):
OSTI ID: 1983769; OSTI ID: 1993718
Report Number(s):
BNL-224475-2023-JAAM; ESNNA4
Journal Information:
Environmental Science: Nano, Journal Name: Environmental Science: Nano Vol. 10 Journal Issue: 7; ISSN 2051-8153
Publisher:
Royal Society of Chemistry (RSC)Copyright Statement
Country of Publication:
United Kingdom
Language:
English

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