DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Metals Coprecipitation with Barite: Nano-XRF Observation of Enhanced Strontium Incorporation

Abstract

Coprecipitation can be an effective treatment method for the removal of environmentally relevant metals from industrial wastewaters such as produced waters from the oil and gas industry. The precipitation of barite, BaSO4, through the addition of sulfate removes barium while coprecipitating strontium and other alkaline earth metals even when these are present at concentrations below their solubility limit. Among other analytical methods, X-ray fluorescence (XRF) nanospectroscopy at the Hard X-ray Nanoprobe (HXN) beamline at the National Synchrotron Light Source II (NSLS-II) was used to quantify Sr incorporation into barite. Thermodynamic modeling of (Ba,Sr)SO4 solid solutions was done using solid solution—aqueous solution (SS-AS) theory. The quantitative, high-resolution nano-XRF data show clearly that the Sr content in (Ba,Sr)SO4 solid solutions varies widely among particles and even within a single particle. We observed substantial Sr incorporation that is far larger than thermodynamic models predict, likely indicating the formation of metastable solid solutions. We also observed that increasing barite supersaturation of the aqueous phase led to increased Sr incorporation, as predicted by available kinetic models. These results suggest that coprecipitation offers significant potential for designing treatment systems for aqueous metals’ removal in desired metastable compositions. Solution conditions may be optimized to enhance the incorporationmore » of Sr by increasing sulfate addition such that the barite saturation index remains above *3 or by increasing the aqueous Sr to Ba ratio.« less

Authors:
 [1];  [1];  [1]
  1. Princeton Univ., NJ (United States). Dept. of Civil & Environmental Engineering
Publication Date:
Research Org.:
Univ. of Chicago, IL (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1800763
Grant/Contract Number:  
FG02-92ER14244; SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Environmental Engineering Science (Online)
Additional Journal Information:
Journal Name: Environmental Engineering Science (Online); Journal Volume: 37; Journal Issue: 4; Journal ID: ISSN 1557-9018
Publisher:
Mary Ann Liebert, Inc.
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING; 54 ENVIRONMENTAL SCIENCES; Engineering; Environmental Sciences & Ecology; barite; coprecipitation; industrial wastewater; metals; solid solution; strontium; trace elements

Citation Formats

Hunter, Heather A., Ling, Florence T., and Peters, Catherine A. Metals Coprecipitation with Barite: Nano-XRF Observation of Enhanced Strontium Incorporation. United States: N. p., 2020. Web. doi:10.1089/ees.2019.0447.
Hunter, Heather A., Ling, Florence T., & Peters, Catherine A. Metals Coprecipitation with Barite: Nano-XRF Observation of Enhanced Strontium Incorporation. United States. https://doi.org/10.1089/ees.2019.0447
Hunter, Heather A., Ling, Florence T., and Peters, Catherine A. Wed . "Metals Coprecipitation with Barite: Nano-XRF Observation of Enhanced Strontium Incorporation". United States. https://doi.org/10.1089/ees.2019.0447. https://www.osti.gov/servlets/purl/1800763.
@article{osti_1800763,
title = {Metals Coprecipitation with Barite: Nano-XRF Observation of Enhanced Strontium Incorporation},
author = {Hunter, Heather A. and Ling, Florence T. and Peters, Catherine A.},
abstractNote = {Coprecipitation can be an effective treatment method for the removal of environmentally relevant metals from industrial wastewaters such as produced waters from the oil and gas industry. The precipitation of barite, BaSO4, through the addition of sulfate removes barium while coprecipitating strontium and other alkaline earth metals even when these are present at concentrations below their solubility limit. Among other analytical methods, X-ray fluorescence (XRF) nanospectroscopy at the Hard X-ray Nanoprobe (HXN) beamline at the National Synchrotron Light Source II (NSLS-II) was used to quantify Sr incorporation into barite. Thermodynamic modeling of (Ba,Sr)SO4 solid solutions was done using solid solution—aqueous solution (SS-AS) theory. The quantitative, high-resolution nano-XRF data show clearly that the Sr content in (Ba,Sr)SO4 solid solutions varies widely among particles and even within a single particle. We observed substantial Sr incorporation that is far larger than thermodynamic models predict, likely indicating the formation of metastable solid solutions. We also observed that increasing barite supersaturation of the aqueous phase led to increased Sr incorporation, as predicted by available kinetic models. These results suggest that coprecipitation offers significant potential for designing treatment systems for aqueous metals’ removal in desired metastable compositions. Solution conditions may be optimized to enhance the incorporation of Sr by increasing sulfate addition such that the barite saturation index remains above *3 or by increasing the aqueous Sr to Ba ratio.},
doi = {10.1089/ees.2019.0447},
journal = {Environmental Engineering Science (Online)},
number = 4,
volume = 37,
place = {United States},
year = {Wed Apr 01 00:00:00 EDT 2020},
month = {Wed Apr 01 00:00:00 EDT 2020}
}

Works referenced in this record:

Radium uptake during barite recrystallization at 23±2°C as a function of solution composition: An experimental 133Ba and 226Ra tracer study
journal, June 2010


A model of oscillatory zoning in solid solutions grown from aqueous solutions: Applications to the (Ba,Sr)SO 4 system
journal, February 2002


Celestite (SrSO4(s)) solubility in water, seawater and NaCl solution
journal, January 1987


A Critical Review of the Risks to Water Resources from Unconventional Shale Gas Development and Hydraulic Fracturing in the United States
journal, March 2014

  • Vengosh, Avner; Jackson, Robert B.; Warner, Nathaniel
  • Environmental Science & Technology, Vol. 48, Issue 15
  • DOI: 10.1021/es405118y

Vibrational spectroscopy of functional group chemistry and arsenate coordination in ettringite
journal, November 1998

  • Myneni, Satish C. B.; Traina, Samuel J.; Waychunas, Glenn A.
  • Geochimica et Cosmochimica Acta, Vol. 62, Issue 21-22
  • DOI: 10.1016/S0016-7037(98)00221-X

Impact of Shale Gas Development on Regional Water Quality
journal, May 2013


Determination of interfacial tension from crystallization and dissolution data: a comparison with other methods
journal, February 1999


Crystallization behavior of solid solutions from aqueous solutions: An environmental perspective
journal, September 2016

  • Prieto, Manuel; Heberling, Frank; Rodríguez-Galán, Rosa M.
  • Progress in Crystal Growth and Characterization of Materials, Vol. 62, Issue 3
  • DOI: 10.1016/j.pcrysgrow.2016.05.001

Hydraulic “Fracking”: Are surface water impacts an ecological concern?: Hydraulic fracturing versus surface waters
journal, July 2014

  • Burton, G. Allen; Basu, Niladri; Ellis, Brian R.
  • Environmental Toxicology and Chemistry, Vol. 33, Issue 8
  • DOI: 10.1002/etc.2619

Removal of Radium from Synthetic Shale Gas Brines by Ion Exchange Resin
journal, October 2016

  • Bi, Yuqiang; Zhang, Hui; Ellis, Brian R.
  • Environmental Engineering Science, Vol. 33, Issue 10
  • DOI: 10.1089/ees.2016.0002

Hydraulic Fracturing Fluid Compositions Induce Differential Enrichment of Soil Bacterial Communities
journal, April 2019

  • Lozano, Tania M.; McCutchan, Aubrey Lynn; Krzmarzick, Mark James
  • Environmental Engineering Science, Vol. 36, Issue 4
  • DOI: 10.1089/ees.2018.0271

Chemical dissolution of oilfield strontium sulfate (SrSO4) scale by chelating agents
journal, July 2019


Impact of Aluminum and Iron (III) Ions on Removal of Fluoride Ion (F ) by Calcite
journal, November 2019

  • Toumari, Arman; Stenstrom, Michael K.; Suffet, I. H. (Mel)
  • Environmental Engineering Science, Vol. 36, Issue 11
  • DOI: 10.1089/ees.2019.0189

Geochemical evaluation of flowback brine from Marcellus gas wells in Pennsylvania, USA
journal, January 2013


Thermodynamic properties of the (Ba,Pb)SO4 solid solution under ambient conditions: Implications for the behavior of Pb and Ra in the environment
journal, March 2013

  • Fernández-González, Angeles; Carneiro, Joana; Katsikopoulos, Dionisis
  • Geochimica et Cosmochimica Acta, Vol. 105
  • DOI: 10.1016/j.gca.2012.11.042

How well suited are current thermodynamic models to predict or interpret the composition of (Ba,Sr)SO4 solid-solutions in geothermal scalings?
journal, June 2017


A new technique for removing strontium from seawater by coprecipitation with barite
journal, October 2018


Contrasting sources and mobility of trace metals in recent sediments of western Lake Erie
journal, October 2018


Life Cycle Water Consumption and Wastewater Generation Impacts of a Marcellus Shale Gas Well
journal, January 2014

  • Jiang, Mohan; Hendrickson, Chris T.; VanBriesen, Jeanne M.
  • Environmental Science & Technology, Vol. 48, Issue 3
  • DOI: 10.1021/es4047654

Radium removal in a large scale evaporitic system
journal, February 2013

  • Rosenberg, Yoav Oved; Metz, Volker; Ganor, Jiwchar
  • Geochimica et Cosmochimica Acta, Vol. 103
  • DOI: 10.1016/j.gca.2012.10.046

Nucleation, growth, and zoning phenomena in crystallizing (Ba,Sr)CO3, Ba(SO4,CrO4), (Ba,Sr)SO4, and (Cd,Ca)CO3 solid solutions from aqueous solutions
journal, August 1997


Nucleation and growth kinetics of RaxBa1−xSO4 solid solution in NaCl aqueous solutions
journal, January 2014


On-site treatment of flowback and produced water from shale gas hydraulic fracturing: A review and economic evaluation
journal, December 2018


Solid-Solution Solubilities and Thermodynamics: Sulfates, Carbonates and Halides
journal, January 2000


Coprecipitation in the barite isostructural family: 1. binary mixing properties
journal, August 2004


Reaction paths and equilibrium end-points in solid-solution aqueous-solution systems
journal, February 1990


Co-precipitation of Radium with Barium and Strontium Sulfate and Its Impact on the Fate of Radium during Treatment of Produced Water from Unconventional Gas Extraction
journal, March 2014

  • Zhang, Tieyuan; Gregory, Kelvin; Hammack, Richard W.
  • Environmental Science & Technology, Vol. 48, Issue 8
  • DOI: 10.1021/es405168b

Incorporation of Metals into Calcite in a Deep Anoxic Granite Aquifer
journal, January 2018

  • Drake, Henrik; Mathurin, Frédéric A.; Zack, Thomas
  • Environmental Science & Technology, Vol. 52, Issue 2
  • DOI: 10.1021/acs.est.7b05258

Nanospectroscopy Captures Nanoscale Compositional Zonation in Barite Solid Solutions
journal, August 2018


Thermodynamics of Solid Solution-Aqueous Solution Systems
journal, January 2009


Organic–mineral interfacial chemistry drives heterogeneous nucleation of Sr-rich (Ba x , Sr 1− x )SO 4 from undersaturated solution
journal, May 2019

  • Deng, Ning; Stack, Andrew G.; Weber, Juliane
  • Proceedings of the National Academy of Sciences, Vol. 116, Issue 27
  • DOI: 10.1073/pnas.1821065116

Unraveling the Effects of Strontium Incorporation on Barite Growth—In Situ and Ex Situ Observations Using Multiscale Chemical Imaging
journal, July 2018

  • Weber, Juliane; Bracco, Jacquelyn N.; Poplawsky, Jonathan D.
  • Crystal Growth & Design, Vol. 18, Issue 9
  • DOI: 10.1021/acs.cgd.8b00839

Element mobilization from Bakken shales as a function of water chemistry
journal, April 2016


An Apatite II permeable reactive barrier to remediate groundwater containing Zn, Pb and Cd
journal, August 2006


Scale formation in porous media and its impact on reservoir performance during water flooding
journal, March 2017

  • Hajirezaie, Sassan; Wu, Xingru; Peters, Catherine A.
  • Journal of Natural Gas Science and Engineering, Vol. 39
  • DOI: 10.1016/j.jngse.2017.01.019

Review of technologies for oil and gas produced water treatment
journal, October 2009

  • Fakhru’l-Razi, Ahmadun; Pendashteh, Alireza; Abdullah, Luqman Chuah
  • Journal of Hazardous Materials, Vol. 170, Issue 2-3
  • DOI: 10.1016/j.jhazmat.2009.05.044

Kinetics and Equilibrium of Barium and Strontium Sulfate Formation in Marcellus Shale Flowback Water
journal, May 2014


Impact of Water Chemistry on Element Mobilization from Eagle Ford Shale
journal, April 2015

  • Wang, Lin; Fortner, John D.; Giammar, Daniel E.
  • Environmental Engineering Science, Vol. 32, Issue 4
  • DOI: 10.1089/ees.2014.0342

Effective Removal of Selenite and Selenate Ions from Aqueous Solution by Barite
journal, July 2017

  • Tokunaga, Kohei; Takahashi, Yoshio
  • Environmental Science & Technology, Vol. 51, Issue 16
  • DOI: 10.1021/acs.est.7b01219

Barite–Celestine Geochemistry and Environments of Formation
journal, January 2000


A unified approach to model uptake kinetics of trace elements in complex aqueous – solid solution systems
journal, February 2014


Solubility of pyromorphite Pb5(PO4)3Cl–mimetite Pb5(AsO4)3Cl solid solution series
journal, April 2011

  • Flis, Justyna; Manecki, Maciej; Bajda, Tomasz
  • Geochimica et Cosmochimica Acta, Vol. 75, Issue 7
  • DOI: 10.1016/j.gca.2011.01.021

Removal of heavy metal ions from wastewaters: A review
journal, March 2011


Current perspective on produced water management challenges during hydraulic fracturing for oil and gas recovery
journal, January 2015

  • Gregory, Kelvin; Mohan, Arvind Murali
  • Environmental Chemistry, Vol. 12, Issue 3
  • DOI: 10.1071/EN15001

Simulation of the nucleation and growth of binary solid solutions in aqueous solutions
journal, January 2010


The Nucleation Kinetics of Barium Sulfate in NaCl Solutions up to 6 m and 90°C
journal, September 1995

  • He, Shiliang; Oddo, John E.; Tomson, Mason B.
  • Journal of Colloid and Interface Science, Vol. 174, Issue 2
  • DOI: 10.1006/jcis.1995.1397