Effects of Ionic Strength, Salt, and pH on Aggregation of Boehmite Nanocrystals: Tumbler Small-Angle Neutron and X-ray Scattering and Imaging Analysis

Anovitz, L. M.; Zhang, Xin; Soltis, Jennifer; Nakouzi, Elias; Krzysko, Anthony J.; Chun, Jaehun; Schenter, Greg K.; Graham, Trenton R.; Rosso, Kevin M.; De Yoreo, James J.; Stack, A. G.; Bleuel, Markus; Gagnon, Cedric; Mildner, D. F.  R.; Ilavsky, J.; Kuzmenko, I.

doi:10.1021/acs.langmuir.8b00865

Title: Effects of Ionic Strength, Salt, and pH on Aggregation of Boehmite Nanocrystals: Tumbler Small-Angle Neutron and X-ray Scattering and Imaging Analysis

Journal Article · 15 October 2018 · Langmuir

DOI: https://doi.org/10.1021/acs.langmuir.8b00865 · OSTI ID:1501864

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^[2]; Nakouzi, Elias ^[2];

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^[2]; Schenter, Greg K. ^[2];

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^[1]; Bleuel, Markus ^[4]; Gagnon, Cedric ^[4]; Mildner, D. F. R. ^[5]; Ilavsky, J. ^[6]; Kuzmenko, I. ^[6]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Washington State Univ., Pullman, WA (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States); Univ. of Maryland, College Park, MD (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)

The U.S. government currently spends significant resources annually managing the legacies of the Cold War, including 300 million liters of highly radioactive wastes stored in hundreds of tanks at the Hanford Site (WA) and the Savannah River Site (SC). The materials in these tanks consist of highly radioactive slurries and sludges at very high pH and salt concentrations. The solid particles primarily consist of aluminum hydroxides and oxyhydroxides (gibbsite and boehmite), although many other materials are present. These form complex aggregates that dramatically affect the rheology of the solutions and, therefore, efforts to recover and treat these wastes. In this paper we have used a combination of transmission and cryo-transmission electron microscopy, dynamic light scattering, and X-ray and neutron small- and ultra-small angle scattering to study the aggregation in controlled environments of synthetic nano-boehmite particles at pH 9 (approximately the point of zero charge) and 12, and sodium-nitrate and calcium-nitrate concentrations up to 1 molal. While the initial particles form individual rhombohedral platelets, once placed in solution they quickly form well-bonded stacks, primary aggregates, up to ~ 150 nm long. These are more prevalent at pH=12. Addition of calcium-nitrate or sodium-nitrate has a similar effect as lowering pH, but approximately one hundred times less calcium than sodium is needed to observe this effect. These aggregates have fractal dimension between 2.5 and 2.6 that are relatively unaffected by salt concentration for calcium-nitrate at high pH. Larger aggregates (> ~ 400 nm) are also formed, but their size distributions are discrete rather than continuous. The fractal dimensions of these aggregates are strongly pH dependent but only become dependent on solute at high salt concentrations.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Interfacial Dynamics in Radioactive Environments and Materials (IDREAM); Argonne National Laboratory (ANL), Argonne, IL (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:: AC02-06CH11357; AC05-00OR22725; AC05-76RL01830

OSTI ID:: 1501864

Alternate ID(s):: OSTI ID: 1494398; OSTI ID: 1772650

Report Number(s):: PNNL-SA-132707; 148331

Journal Information:: Langmuir, Vol. 34, Issue 51; ISSN 0743-7463

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 23 works

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Zn2+ and Sr2+ adsorption at the TiO2 (110)–electrolyte interface: Influence of ionic strength, coverage, and anions Zhang, Z.; Fenter, P.; Cheng, L. Journal of Colloid and Interface Science, Vol. 295, Issue 1 https://doi.org/10.1016/j.jcis.2005.08.018	journal	March 2006
Structure of rutile TiO2 (110) in water and 1molal Rb+ at pH 12: Inter-relationship among surface charge, interfacial hydration structure, and substrate structural displacements Zhang, Zhan; Fenter, Paul; Sturchio, Neil C. Surface Science, Vol. 601, Issue 4 https://doi.org/10.1016/j.susc.2006.12.007	journal	February 2007
Surface complexation of neodymium at the rutile-water interface: A potentiometric and modeling study in NaCl media to 250°C Ridley, Moira K.; Machesky, Michael L.; Wesolowski, David J. Geochimica et Cosmochimica Acta, Vol. 69, Issue 1 https://doi.org/10.1016/j.gca.2004.06.028	journal	January 2005
Effect of particle size distribution on slurry rheology: Nuclear waste simulant slurries Chun, Jaehun; Oh, Takkeun; Luna, Maria Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 384, Issue 1-3 https://doi.org/10.1016/j.colsurfa.2011.04.003	journal	July 2011