Heterogeneous Lead Phosphate Nucleation at Organic–Water Interfaces: Implications for Lead Immobilization

Dai, Chong; Zhao, Juntao; Giammar, Daniel E.; Pasteris, Jill D.; Zuo, Xiaobing; Hu, Yandi

doi:10.1021/acsearthspacechem.8b00040

Title: Heterogeneous Lead Phosphate Nucleation at Organic–Water Interfaces: Implications for Lead Immobilization

Abstract

Phosphate is added to Pb-contaminated soils to induce lead immobilization through lead phosphate precipitation. Organic coatings on soils, which may affect heterogeneous lead phosphate nucleation, can impact the effectiveness of lead immobilization. SiO₂ surfaces were coated with silanol self-assembled thin films terminated with -COOH and -OH functional groups to act as model organic coatings on soil particles. Using grazing incidence small-angle X-ray scattering (GISAXS), heterogeneous lead phosphate nucleation on coatings was measured from mixed Pb(NO₃)₂ and Na₂HPO₄/NaH₂PO₄ solutions at pH 7 with varied ionic strengths (IS = 0.58, 4, and 11 mM). Raman spectroscopy identified the homogeneous precipitates in solution as hydroxylpyromorphite (Pb₅(PO₄)₃OH). The smallest lead phosphate nuclei (4.5 ± 0.5 nm) were observed on -COOH coatings, which resulted from the highest level of lead and phosphate ion adsorption on -COOH coatings. The IS of the solution also affected the sizes of the heterogeneous precipitates on -COOH coating, with smaller nuclei (1.3 ± 0.4 nm) forming under higher IS (4 and 11 mM). Finally, this study provided new findings that can improve our understanding of lead immobilization in contaminated soil environments.

Authors:

Dai, Chong ^[1]; Zhao, Juntao ^[1];

^[2]; Pasteris, Jill D. ^[3]; Zuo, Xiaobing ^[4];

^[1]

Univ. of Houston, TX (United States). Dept. of Civil & Environmental Engineering
Washington Univ., St. Louis, MO (United States). Dept. of Energy, Environmental and Chemical Engineering
Washington Univ., St. Louis, MO (United States). Dept. of Earth and Planetary Sciences
Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division

Publication Date:: 2018-07-06

Research Org.:: Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Houston, TX (United States); Washington Univ., St. Louis, MO (United States)

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

OSTI Identifier:: 1484682

Grant/Contract Number:: AC02-06CH11357; 1604042; 1603717

Resource Type:: Accepted Manuscript

Journal Name:: ACS Earth and Space Chemistry

Additional Journal Information:: Journal Volume: 2; Journal Issue: 9; Journal ID: ISSN 2472-3452

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; critical nuclei sizes; heterogeneous nucleation; hydroxylpyromorphite; ion adsorption; local supersaturation near substrates; organic coatings; recrystallization

Citation Formats


                    Dai, Chong, Zhao, Juntao, Giammar, Daniel E., Pasteris, Jill D., Zuo, Xiaobing, and Hu, Yandi. Heterogeneous Lead Phosphate Nucleation at Organic–Water Interfaces: Implications for Lead Immobilization.  United States: N. p., 2018. 
Web.  doi:10.1021/acsearthspacechem.8b00040.

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                    Dai, Chong, Zhao, Juntao, Giammar, Daniel E., Pasteris, Jill D., Zuo, Xiaobing, & Hu, Yandi. Heterogeneous Lead Phosphate Nucleation at Organic–Water Interfaces: Implications for Lead Immobilization.  United States.  https://doi.org/10.1021/acsearthspacechem.8b00040

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                    Dai, Chong, Zhao, Juntao, Giammar, Daniel E., Pasteris, Jill D., Zuo, Xiaobing, and Hu, Yandi. Fri .  
"Heterogeneous Lead Phosphate Nucleation at Organic–Water Interfaces: Implications for Lead Immobilization".  United States.  https://doi.org/10.1021/acsearthspacechem.8b00040.  https://www.osti.gov/servlets/purl/1484682.

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@article{osti_1484682,

  title        = {Heterogeneous Lead Phosphate Nucleation at Organic–Water Interfaces: Implications for Lead Immobilization},

  author       = {Dai, Chong and Zhao, Juntao and Giammar, Daniel E. and Pasteris, Jill D. and Zuo, Xiaobing and Hu, Yandi},

  abstractNote = {Phosphate is added to Pb-contaminated soils to induce lead immobilization through lead phosphate precipitation. Organic coatings on soils, which may affect heterogeneous lead phosphate nucleation, can impact the effectiveness of lead immobilization. SiO2 surfaces were coated with silanol self-assembled thin films terminated with -COOH and -OH functional groups to act as model organic coatings on soil particles. Using grazing incidence small-angle X-ray scattering (GISAXS), heterogeneous lead phosphate nucleation on coatings was measured from mixed Pb(NO3)2 and Na2HPO4/NaH2PO4 solutions at pH 7 with varied ionic strengths (IS = 0.58, 4, and 11 mM). Raman spectroscopy identified the homogeneous precipitates in solution as hydroxylpyromorphite (Pb5(PO4)3OH). The smallest lead phosphate nuclei (4.5 ± 0.5 nm) were observed on -COOH coatings, which resulted from the highest level of lead and phosphate ion adsorption on -COOH coatings. The IS of the solution also affected the sizes of the heterogeneous precipitates on -COOH coating, with smaller nuclei (1.3 ± 0.4 nm) forming under higher IS (4 and 11 mM). Finally, this study provided new findings that can improve our understanding of lead immobilization in contaminated soil environments.},

  doi          = {10.1021/acsearthspacechem.8b00040},

  journal      = {ACS Earth and Space Chemistry},

  number       = 9,

  volume       = 2,

  place        = {United States},

  year         = {2018},

  month        = {7}

}

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Works referencing / citing this record:

Organic–mineral interfacial chemistry drives heterogeneous nucleation of Sr-rich (Ba _x , Sr _{1− x} )SO ₄ from undersaturated solution
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Title: Heterogeneous Lead Phosphate Nucleation at Organic–Water Interfaces: Implications for Lead Immobilization

Abstract

Citation Formats

Control Technologies for Remediation of Contaminated Soil and Waste Deposits at Superf und Lead Battery Recycling Sites journal, July 1992

Lead Contamination of Sycamore and Soil from Lead Mining and Smelting Operations in Eastern Missouri journal, January 1980

Sustainable exposure prevention through innovative detection and remediation technologies from the NIEHS Superfund Research Program journal, March 2017

Influence of natural organic matter on the corrosion of leaded brass in potable water journal, January 2000

Investigation of the Reduction of Lead Dioxide by Natural Organic Matter journal, August 2007

Adsorption of Natural Organic Matter onto the Products of Water-Pipe Corrosion journal, June 2015

Chlorothalonil in a Quartz Sand Soil: Speciation and Kinetics journal, January 2000

Interfacial Free Energy of Nucleation for Iron Oxyhydroxide on Mixed Self-Assembled Monolayers † journal, January 1996

X-Ray Interactions: Photoabsorption, Scattering, Transmission, and Reflection at E = 50-30,000 eV, Z = 1-92 journal, July 1993

Irena : tool suite for modeling and analysis of small-angle scattering journal, February 2009

Regeneration of mesoporous silica aerogel for hydrocarbon adsorption and recovery journal, September 2017

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The effect of cadmium on the transformation of ferrihydrite into crystalline products at pH 8 journal, October 1996

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Control Technologies for Remediation of Contaminated Soil and Waste Deposits at Superf und Lead Battery Recycling Sites
journal, July 1992

Lead Contamination of Sycamore and Soil from Lead Mining and Smelting Operations in Eastern Missouri
journal, January 1980

Sustainable exposure prevention through innovative detection and remediation technologies from the NIEHS Superfund Research Program
journal, March 2017

Influence of natural organic matter on the corrosion of leaded brass in potable water
journal, January 2000

Investigation of the Reduction of Lead Dioxide by Natural Organic Matter
journal, August 2007

Adsorption of Natural Organic Matter onto the Products of Water-Pipe Corrosion
journal, June 2015

Chlorothalonil in a Quartz Sand Soil: Speciation and Kinetics
journal, January 2000

Interfacial Free Energy of Nucleation for Iron Oxyhydroxide on Mixed Self-Assembled Monolayers ^†
journal, January 1996

X-Ray Interactions: Photoabsorption, Scattering, Transmission, and Reflection at E = 50-30,000 eV, Z = 1-92
journal, July 1993

Irena : tool suite for modeling and analysis of small-angle scattering
journal, February 2009

Regeneration of mesoporous silica aerogel for hydrocarbon adsorption and recovery
journal, September 2017

Effects of Cu(II) on the Adsorption Behaviors of Cr(III) and Cr(VI) onto Kaolin
journal, January 2016

Removal of Methylene Blue from Aqueous Solution Using Agricultural Residue Walnut Shell: Equilibrium, Kinetic, and Thermodynamic Studies
journal, January 2017

Investigating calcite growth rates using a quartz crystal microbalance with dissipation (QCM-D)
journal, February 2018

Simultaneous dissolution of hydroxylapatite and precipitation of hydroxypyromorphite: direct evidence of homogeneous nucleation
journal, May 1998

Nucleation and growth of calcium phosphate on amine-, carboxyl- and hydroxyl-silane self-assembled monolayers
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The role of prenucleation clusters in surface-induced calcium phosphate crystallization
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The effect of cadmium on the transformation of ferrihydrite into crystalline products at pH 8
journal, October 1996

Effect of Cd(II) on the Ripening of Ferrihydrite in Alkaline Media
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