Opposing Effects of Impurity Ion Sr2+ on the Heterogeneous Nucleation and Growth of Barite (BaSO4)

Yuan, Ke; Starchenko, Vitalii; Rampal, Nikhil; Yang, Fengchang; Yang, Xiaogang; Xiao, Xianghui; Lee, Wah; Stack, Andrew G.

doi:10.1021/acs.cgd.1c00715

Title: Opposing Effects of Impurity Ion Sr²⁺ on the Heterogeneous Nucleation and Growth of Barite (BaSO₄)

Journal Article · 07 September 2021 · Crystal Growth and Design

DOI: https://doi.org/10.1021/acs.cgd.1c00715 · OSTI ID:1822057

^[1];

^[1]; Rampal, Nikhil ^[2]; Yang, Fengchang ^[1]; Yang, Xiaogang ^[3]; Xiao, Xianghui ^[4]; Lee, Wah ^[4];

^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Columbia Univ., New York, NY (United States)
Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
Brookhaven National Lab. (BNL), Upton, NY (United States)

Nucleation of barite (BaSO₄) has broad implications in geological, environmental, and materials sciences. While impurity metals are common, our understanding of how they impact nucleation remains dim. In this work, we used classical optical microscopy compared to fast X-ray nanotomography (XnT) to investigate heterogeneous nucleation of barite on silica in situ with Sr²⁺ as an impurity ion. The observed barite nucleation rates were consistent with classical nucleation theory (CNT), where barite crystals displayed a nonuniform size distribution, exhibiting distinct morphologies and incubation periods in Sr-free solutions. While undetectable with optical microscopy, nanotomography revealed that addition of Sr2+ enhances nucleation rates driven by the pre-factor in CNT, likely because both adsorbed Ba²⁺ and Sr²⁺ act as precursor sites on which nucleation occurs. Sr²⁺ simultaneously inhibits growth, however, leading to a homogeneous distribution of smaller crystals. This finding will enable an improved predictive understanding of nucleation in natural and synthetic environments.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725; SC0012704

OSTI ID:: 1822057

Report Number(s):: BNL--222368-2021-JAAM

Journal Information:: Crystal Growth and Design, Journal Name: Crystal Growth and Design Journal Issue: 10 Vol. 12; ISSN 1528-7483

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (60)

A Bio-inspired approach to controlled crystallization at the nanoscale Aizenberg, Joanna Bell Labs Technical Journal, Vol. 10, Issue 3 https://doi.org/10.1002/bltj.20108	journal	September 2005
Polarization of water molecules at a charged interface: second harmonic studies of the silica/water interface Ong, Shaowei; Zhao, Xiaolin; Eisenthal, Kenneth B. Chemical Physics Letters, Vol. 191, Issue 3-4 https://doi.org/10.1016/0009-2614(92)85309-X	journal	April 1992
Interfacial tensions electrolyte crystal-aqueous solution, from nucleation data Nielsen, Arne E.; Söhnel, O. Journal of Crystal Growth, Vol. 11, Issue 3 https://doi.org/10.1016/0022-0248(71)90090-X	journal	December 1971
The composition of solid solutions crystallising from aqueous solutions: the influence of supersaturation and growth mechanisms Pina, Carlos M.; Enders, Michael; Putnis, Andrew Chemical Geology, Vol. 168, Issue 3-4 https://doi.org/10.1016/S0009-2541(00)00227-8	journal	August 2000
The kinetics of nucleation of solid solutions from aqueous solutions: a new model for calculating non-equilibrium distribution coefficients Pina, C. M.; Putnis, A. Geochimica et Cosmochimica Acta, Vol. 66, Issue 2 https://doi.org/10.1016/S0016-7037(01)00770-0	journal	January 2002
Evaluation of internally consistent parameters for the triple-layer model by the systematic analysis of oxide surface titration data Sahai, Nita; Sverjensky, Dimitri A. Geochimica et Cosmochimica Acta, Vol. 61, Issue 14 https://doi.org/10.1016/S0016-7037(97)00128-2	journal	July 1997
Geochemistry of barium in marine sediments: implications for its use as a paleoproxy McManus, James; Berelson, William M.; Klinkhammer, Gary P. Geochimica et Cosmochimica Acta, Vol. 62, Issue 21-22 https://doi.org/10.1016/S0016-7037(98)00248-8	journal	November 1998
Effect of impurities on the processes of crystal growth Sangwal, K. Journal of Crystal Growth, Vol. 128, Issue 1-4 https://doi.org/10.1016/S0022-0248(07)80129-1	journal	March 1993
Selection of pre-blended expanders for optimum lead/acid battery performance Boden, D. P. Journal of Power Sources, Vol. 73, Issue 1 https://doi.org/10.1016/S0378-7753(98)00026-3	journal	May 1998
Microbially mediated barite dissolution in anoxic brines Ouyang, Bingjie; Akob, Denise M.; Dunlap, Darren Applied Geochemistry, Vol. 76 https://doi.org/10.1016/j.apgeochem.2016.11.008	journal	January 2017
BoneJ: Free and extensible bone image analysis in ImageJ Doube, Michael; Kłosowski, Michał M.; Arganda-Carreras, Ignacio Bone, Vol. 47, Issue 6 https://doi.org/10.1016/j.bone.2010.08.023	journal	December 2010
Relationships between crystal morphology and composition in the (Ba,Sr)SO4–H2O solid solution–aqueous solution system Sánchez-Pastor, N.; Pina, C. M.; Fernández-Díaz, L. Chemical Geology, Vol. 225, Issue 3-4 https://doi.org/10.1016/j.chemgeo.2005.08.020	journal	January 2006
Retention of 226Ra by barite: The role of internal porosity Weber, Juliane; Barthel, Juri; Klinkenberg, Martina Chemical Geology, Vol. 466 https://doi.org/10.1016/j.chemgeo.2017.07.021	journal	September 2017
Barite formation in the ocean: Origin of amorphous and crystalline precipitates Martinez-Ruiz, F.; Paytan, A.; Gonzalez-Muñoz, M. T. Chemical Geology, Vol. 511 https://doi.org/10.1016/j.chemgeo.2018.09.011	journal	April 2019
Nanoscale effects of strontium on calcite growth: An in situ AFM study in the absence of vital effects Wasylenki, Laura E.; Dove, Patricia M.; Wilson, Darren S. Geochimica et Cosmochimica Acta, Vol. 69, Issue 12 https://doi.org/10.1016/j.gca.2004.12.019	journal	June 2005
Prediction of the speciation of alkaline earths adsorbed on mineral surfaces in salt solutions Sverjensky, Dimitri A. Geochimica et Cosmochimica Acta, Vol. 70, Issue 10 https://doi.org/10.1016/j.gca.2006.01.006	journal	May 2006
Radium uptake during barite recrystallization at 23±2°C as a function of solution composition: An experimental 133Ba and 226Ra tracer study Curti, E.; Fujiwara, K.; Iijima, K. Geochimica et Cosmochimica Acta, Vol. 74, Issue 12 https://doi.org/10.1016/j.gca.2010.03.018	journal	June 2010
Barite precipitation following celestite dissolution in a porous medium: A SEM/BSE and μ-XRD/XRF study Poonoosamy, J.; Curti, E.; Kosakowski, G. Geochimica et Cosmochimica Acta, Vol. 182 https://doi.org/10.1016/j.gca.2016.03.011	journal	June 2016
On the determination of the kinetic pre-factor in classical nucleation theory Schmelzer, Jürn W. P. Journal of Non-Crystalline Solids, Vol. 356, Issue 52-54 https://doi.org/10.1016/j.jnoncrysol.2010.02.026	journal	December 2010
Automated correlative segmentation of large Transmission X-ray Microscopy (TXM) tomograms using deep learning Shashank Kaira, C.; Yang, Xiaogang; De Andrade, Vincent Materials Characterization, Vol. 142 https://doi.org/10.1016/j.matchar.2018.05.053	journal	August 2018
In-situ liquid phase TEM observations of nucleation and growth processes De Yoreo, James J. Progress in Crystal Growth and Characterization of Materials, Vol. 62, Issue 2 https://doi.org/10.1016/j.pcrysgrow.2016.04.003	journal	June 2016
Growth of BaxSr1−xSO4 nano-steps on barite (001) face YuHang, Chen; Asenjo, Agustina; Sánchez-Pastor, Nuria Surface Science, Vol. 601, Issue 2 https://doi.org/10.1016/j.susc.2006.10.003	journal	January 2007
Inhibition of growth in solid solution–aqueous solution systems by non-incorporating impurities Pina, Carlos M. Surface Science, Vol. 605, Issue 5-6 https://doi.org/10.1016/j.susc.2010.12.014	journal	March 2011
Zinc Ions Modify Calcium Oxalate Growth by Distinct Transformation of Crystal Surface Termination Alamani, Bryan G.; Gale, Julian D.; Rimer, Jeffrey D. Crystal Growth & Design, Vol. 21, Issue 6 https://doi.org/10.1021/acs.cgd.1c00166	journal	May 2021
Barium Sulfate Crystallization from Synthetic Seawater Boon, Matthew; Jones, Franca Crystal Growth & Design, Vol. 16, Issue 8 https://doi.org/10.1021/acs.cgd.6b00729	journal	July 2016
Unraveling the Effects of Strontium Incorporation on Barite Growth—In Situ and Ex Situ Observations Using Multiscale Chemical Imaging Weber, Juliane; Bracco, Jacquelyn N.; Poplawsky, Jonathan D. Crystal Growth & Design, Vol. 18, Issue 9 https://doi.org/10.1021/acs.cgd.8b00839	journal	July 2018
Simultaneous Adsorption and Incorporation of Sr ²⁺ at the Barite (001)–Water Interface Bracco, Jacquelyn N.; Lee, Sang Soo; Stubbs, Joanne E. The Journal of Physical Chemistry C, Vol. 123, Issue 2 https://doi.org/10.1021/acs.jpcc.8b08848	journal	December 2018
Salinity-Induced Reduction of Interfacial Energies and Kinetic Factors during Calcium Carbonate Nucleation on Quartz Li, Qingyun; Jun, Young-Shin The Journal of Physical Chemistry C, Vol. 123, Issue 23 https://doi.org/10.1021/acs.jpcc.9b00378	journal	May 2019
Heterogeneous Nucleation and Growth of Barium Sulfate at Organic–Water Interfaces: Interplay between Surface Hydrophobicity and Ba ²⁺ Adsorption Dai, Chong; Stack, Andrew G.; Koishi, Ayumi Langmuir, Vol. 32, Issue 21 https://doi.org/10.1021/acs.langmuir.6b01036	journal	May 2016
Strontium Ions Function as Both an Accelerant and Structure-Directing Agent of Chabazite Crystallization Liang, Yu; Jacobson, Allan J.; Rimer, Jeffrey D. ACS Materials Letters, Vol. 3, Issue 2 https://doi.org/10.1021/acsmaterialslett.0c00460	journal	December 2020
Analysis of Nucleation Rate Measurements in Precipitation Processes Roelands, C. P. Mark; ter Horst, Joop H.; Kramer, Herman J. M. Crystal Growth & Design, Vol. 6, Issue 6 https://doi.org/10.1021/cg050678w	journal	May 2006
Calcite Growth Rates As a Function of Aqueous Calcium-to-Carbonate Ratio, Saturation Index, and Inhibitor Concentration: Insight into the Mechanism of Reaction and Poisoning by Strontium Bracco, Jacquelyn N.; Grantham, Meg C.; Stack, Andrew G. Crystal Growth & Design, Vol. 12, Issue 7 https://doi.org/10.1021/cg300350k	journal	June 2012
Self-Assembled Monolayers as Templates for Heme Crystallization Wang, Xuefeng; Ingall, Ellery; Lai, Barry Crystal Growth & Design, Vol. 10, Issue 2 https://doi.org/10.1021/cg901177c	journal	February 2010
In Situ Determination of Interfacial Energies between Heterogeneously Nucleated CaCO ₃ and Quartz Substrates: Thermodynamics of CO ₂ Mineral Trapping Fernandez-Martinez, Alejandro; Hu, Yandi; Lee, Byeongdu Environmental Science & Technology, Vol. 47, Issue 1 https://doi.org/10.1021/es3014826	journal	June 2012
Accurate Rates of the Complex Mechanisms for Growth and Dissolution of Minerals Using a Combination of Rare-Event Theories Stack, Andrew G.; Raiteri, Paolo; Gale, Julian D. Journal of the American Chemical Society, Vol. 134, Issue 1 https://doi.org/10.1021/ja204714k	journal	July 2011
Hydrated Cation Speciation at the Muscovite (001)−Water Interface Lee, Sang Soo; Fenter, Paul; Park, Changyong Langmuir, Vol. 26, Issue 22 https://doi.org/10.1021/la1032866	journal	November 2010
Formation of calcium sulfate through the aggregation of sub-3 nanometre primary species Stawski, Tomasz M.; van Driessche, Alexander E. S.; Ossorio, Mercedes Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms11177	journal	April 2016
Observing classical nucleation theory at work by monitoring phase transitions with molecular precision Sleutel, Mike; Lutsko, Jim; Van Driessche, Alexander E. S. Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms6598	journal	December 2014
Calcium carbonate nucleation driven by ion binding in a biomimetic matrix revealed by in situ electron microscopy Smeets, Paul J. M.; Cho, Kang Rae; Kempen, Ralph G. E. Nature Materials, Vol. 14, Issue 4 https://doi.org/10.1038/nmat4193	journal	January 2015
Fiji: an open-source platform for biological-image analysis Schindelin, Johannes; Arganda-Carreras, Ignacio; Frise, Erwin Nature Methods, Vol. 9, Issue 7 https://doi.org/10.1038/nmeth.2019	journal	June 2012
Barium bioaccumulation by bacterial biofilms and implications for Ba cycling and use of Ba proxies Martinez-Ruiz, Francisca; Jroundi, Fadwa; Paytan, Adina Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-04069-z	journal	April 2018
The dynamic nature of crystal growth in pores Godinho, Jose R. A.; Gerke, Kirill M.; Stack, Andrew G. Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/srep33086	journal	September 2016
Capturing an amorphous BaSO ₄ intermediate precursor to barite Ruiz-Agudo, Cristina; McDonogh, David; Avaro, Jonathan Thomas CrystEngComm, Vol. 22, Issue 8 https://doi.org/10.1039/C9CE01555H	journal	January 2020
Infrared investigation of barite and gypsum crystallization: Evidence for an amorphous to crystalline transition Jones, Franca CrystEngComm, Vol. 14, Issue 24 https://doi.org/10.1039/c2ce25918d	journal	January 2012
The thermodynamics of calcite nucleation at organic interfaces: Classical vs. non-classical pathways Hu, Q.; Nielsen, M. H.; Freeman, C. L. Faraday Discussions, Vol. 159 https://doi.org/10.1039/c2fd20124k	journal	January 2012
One-minute nano-tomography using hard X-ray full-field transmission microscope Ge, Mingyuan; Coburn, David Scott; Nazaretski, Evgeny Applied Physics Letters, Vol. 113, Issue 8 https://doi.org/10.1063/1.5048378	journal	August 2018
Reconciling disparate views of template-directed nucleation through measurement of calcite nucleation kinetics and binding energies Hamm, L. M.; Giuffre, A. J.; Han, N. Proceedings of the National Academy of Sciences, Vol. 111, Issue 4 https://doi.org/10.1073/pnas.1312369111	journal	January 2014
A classical view on nonclassical nucleation Smeets, Paul J. M.; Finney, Aaron R.; Habraken, Wouter J. E. M. Proceedings of the National Academy of Sciences, Vol. 114, Issue 38 https://doi.org/10.1073/pnas.1700342114	journal	September 2017
Organic–mineral interfacial chemistry drives heterogeneous nucleation of Sr-rich (Ba _x , Sr _{1− x} )SO ₄ from undersaturated solution Deng, Ning; Stack, Andrew G.; Weber, Juliane Proceedings of the National Academy of Sciences, Vol. 116, Issue 27 https://doi.org/10.1073/pnas.1821065116	journal	May 2019
Analysis of Adsorption Behavior of Cations onto Quartz Surface by Electrical Double-layer Model Kitamura, Akira; Fujiwara, Kenso; Yamamoto, Tadashi Journal of Nuclear Science and Technology, Vol. 36, Issue 12 https://doi.org/10.1080/18811248.1999.9726312	journal	December 1999
Metals Coprecipitation with Barite: Nano-XRF Observation of Enhanced Strontium Incorporation Hunter, Heather A.; Ling, Florence T.; Peters, Catherine A. Environmental Engineering Science, Vol. 37, Issue 4 https://doi.org/10.1089/ees.2019.0447	journal	April 2020
TomoPy: a framework for the analysis of synchrotron tomographic data Gürsoy, Dogˇa; De Carlo, Francesco; Xiao, Xianghui Journal of Synchrotron Radiation, Vol. 21, Issue 5 https://doi.org/10.1107/S1600577514013939	journal	August 2014
Scientific data exchange: a schema for HDF5-based storage of raw and analyzed data De Carlo, Francesco; Gürsoy, Dogˇa; Marone, Federica Journal of Synchrotron Radiation, Vol. 21, Issue 6 https://doi.org/10.1107/S160057751401604X	journal	October 2014
Integration of TomoPy and the ASTRA toolbox for advanced processing and reconstruction of tomographic synchrotron data Pelt, Daniël M.; Gürsoy, Dogˇa; Palenstijn, Willem Jan Journal of Synchrotron Radiation, Vol. 23, Issue 3 https://doi.org/10.1107/S1600577516005658	journal	April 2016
In situ TEM imaging of CaCO3 nucleation reveals coexistence of direct and indirect pathways Nielsen, M. H.; Aloni, S.; De Yoreo, J. J. Science, Vol. 345, Issue 6201 https://doi.org/10.1126/science.1254051	journal	September 2014
Crystallization by particle attachment in synthetic, biogenic, and geologic environments De Yoreo, J. J.; Gilbert, P. U. P. A.; Sommerdijk, N. A. J. M. Science, Vol. 349, Issue 6247 https://doi.org/10.1126/science.aaa6760	journal	July 2015
X-ray-driven reaction front dynamics at calcite-water interfaces Laanait, N.; Callagon, E. B. R.; Zhang, Z. Science, Vol. 349, Issue 6254 https://doi.org/10.1126/science.aab3272	journal	September 2015
A high-level 3D visualization API for Java and ImageJ Schmid, Benjamin; Schindelin, Johannes; Cardona, Albert BMC Bioinformatics, Vol. 11, Issue 1 https://doi.org/10.1186/1471-2105-11-274	journal	May 2010
3. Principles of Crystal Nucleation and Growth De Yoreo, James J.; Vekilov, Peter G. Biomineralization https://doi.org/10.1515/9781501509346-008	book	December 2003
Structure of the Solvated Strontium and Barium Ions in Aqueous, Dimethyl Sulfoxide and Pyridine Solution, and Crystal Structure of Strontium and Barium Hydroxide Octahydrate Persson, Ingmar; Sandström, Magnus; Yokoyama, Haruhiko Zeitschrift für Naturforschung A, Vol. 50, Issue 1 https://doi.org/10.1515/zna-1995-0105	journal	January 1995

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Title: Opposing Effects of Impurity Ion Sr2+ on the Heterogeneous Nucleation and Growth of Barite (BaSO4)

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Title: Opposing Effects of Impurity Ion Sr²⁺ on the Heterogeneous Nucleation and Growth of Barite (BaSO₄)