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Title: Nanospectroscopy Captures Nanoscale Compositional Zonation in Barite Solid Solutions

Abstract

Scientists have long suspected that compositionally zoned particles can form under far-from equilibrium precipitation conditions, but their inferences have been based on bulk solid and solution measurements. We are the first to directly observe nanoscale trace element compositional zonation in <10 µm-sized particles using X-ray fluorescence nanospectroscopy at the Hard X-ray Nanoprobe (HXN) Beamline at National Synchrotron Light Source II (NSLS-II). Through high-resolution images, compositional zonation was observed in barite (BaSO 4) particles precipitated from aqueous solution, in which Sr 2+ cations as well as HAsO 4 2- anions were co-precipitated into (Ba,Sr)SO 4 or Ba(SO 4,HAsO 4) solid solutions. Under high salinity conditions (NaCl ≥ 1.0 M), bands contained ~3.5 to ~5 times more trace element compared to the center of the particle formed in early stages of particle growth. Quantitative analysis of Sr and As fractional substitution allowed us to determine that different crystallographic growth directions incorporated trace elements to different extents. These findings provide supporting evidence that barite solid solutions have great potential for trace element incorporation and that this has significant implications for environmental and engineered systems that remove hazardous substances from water.

Authors:
; ; ; ORCiD logo; ; ; ; ORCiD logo;
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF)
OSTI Identifier:
1466065
Alternate Identifier(s):
OSTI ID: 1476291
Report Number(s):
[BNL-209125-2018-JAAM]
[Journal ID: ISSN 2045-2322; 13041; PII: 31335]
Grant/Contract Number:  
[SC0012704; CBET-1438278; FG02-92ER14244]
Resource Type:
Published Article
Journal Name:
Scientific Reports
Additional Journal Information:
[Journal Name: Scientific Reports Journal Volume: 8 Journal Issue: 1]; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United Kingdom
Language:
English
Subject:
58 GEOSCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 42 ENGINEERING

Citation Formats

Ling, Florence T., Hunter, Heather A., Fitts, Jeffrey P., Peters, Catherine A., Acerbo, Alvin S., Huang, Xiaojing, Yan, Hanfei, Nazaretski, Evgeny, and Chu, Yong S. Nanospectroscopy Captures Nanoscale Compositional Zonation in Barite Solid Solutions. United Kingdom: N. p., 2018. Web. doi:10.1038/s41598-018-31335-3.
Ling, Florence T., Hunter, Heather A., Fitts, Jeffrey P., Peters, Catherine A., Acerbo, Alvin S., Huang, Xiaojing, Yan, Hanfei, Nazaretski, Evgeny, & Chu, Yong S. Nanospectroscopy Captures Nanoscale Compositional Zonation in Barite Solid Solutions. United Kingdom. doi:10.1038/s41598-018-31335-3.
Ling, Florence T., Hunter, Heather A., Fitts, Jeffrey P., Peters, Catherine A., Acerbo, Alvin S., Huang, Xiaojing, Yan, Hanfei, Nazaretski, Evgeny, and Chu, Yong S. Wed . "Nanospectroscopy Captures Nanoscale Compositional Zonation in Barite Solid Solutions". United Kingdom. doi:10.1038/s41598-018-31335-3.
@article{osti_1466065,
title = {Nanospectroscopy Captures Nanoscale Compositional Zonation in Barite Solid Solutions},
author = {Ling, Florence T. and Hunter, Heather A. and Fitts, Jeffrey P. and Peters, Catherine A. and Acerbo, Alvin S. and Huang, Xiaojing and Yan, Hanfei and Nazaretski, Evgeny and Chu, Yong S.},
abstractNote = {Scientists have long suspected that compositionally zoned particles can form under far-from equilibrium precipitation conditions, but their inferences have been based on bulk solid and solution measurements. We are the first to directly observe nanoscale trace element compositional zonation in <10 µm-sized particles using X-ray fluorescence nanospectroscopy at the Hard X-ray Nanoprobe (HXN) Beamline at National Synchrotron Light Source II (NSLS-II). Through high-resolution images, compositional zonation was observed in barite (BaSO4) particles precipitated from aqueous solution, in which Sr2+ cations as well as HAsO42- anions were co-precipitated into (Ba,Sr)SO4 or Ba(SO4,HAsO4) solid solutions. Under high salinity conditions (NaCl ≥ 1.0 M), bands contained ~3.5 to ~5 times more trace element compared to the center of the particle formed in early stages of particle growth. Quantitative analysis of Sr and As fractional substitution allowed us to determine that different crystallographic growth directions incorporated trace elements to different extents. These findings provide supporting evidence that barite solid solutions have great potential for trace element incorporation and that this has significant implications for environmental and engineered systems that remove hazardous substances from water.},
doi = {10.1038/s41598-018-31335-3},
journal = {Scientific Reports},
number = [1],
volume = [8],
place = {United Kingdom},
year = {2018},
month = {8}
}

Journal Article:
Free Publicly Available Full Text
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DOI: 10.1038/s41598-018-31335-3

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