Correlating inter-particle forces and particle shape to shear-induced aggregation/fragmentation and rheology for dilute anisotropic particle suspensions: A complementary study via capillary rheometry and in-situ small and ultra-small angle X-ray scattering

Krzysko, Anthony J.; Nakouzi, Elias; Zhang, Xin; Graham, Trent R.; Rosso, Kevin M.; Schenter, Gregory K.; Ilavský, Ján; Kuzmenko, Ivan; Frith, Matthew G.; Ivory, Cornelius F.; Clark, Sue; Weston, Javen; Weigandt, Katie M.; Yoreo, James J. De; Chun, Jaehun; Anovitz, L. M.

doi:10.1016/j.jcis.2020.04.016

Cited by 25 publications

(16 citation statements)

References 60 publications

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“…Figure shows examples of the scattering data obtained in this experiment: data for pure water and those for the 4 m solutions of each of the five M 1+ nitrates. The patterns are qualitatively similar to each other and our previous results. ,, Beginning at high Q (smallest scales), each has a flat background beginning just below 10 –1 Å –1 due to hydrogen in the solution. This background is high enough that most of the data from the individual boehmite platelets are lost.…”

Section: Resultssupporting

confidence: 89%

“…To further characterize the aggregates, therefore, the scattering data have been fitted to an appropriate model. As we have shown previously, ,, this can be done using either a multilevel Guinier–Porod or unified fit. − In either case, the model describes scattering as originating from a series of structures (levels) of different sizes. Thus, the data are described as where eq represents the sum of scattering from each level.…”

Section: Resultsmentioning

confidence: 99%

“…A critical gap in the basic science needed to treat these wastes is a fundamental understanding of the effects of the tank solution components on the solid particulate structure. The extreme chemical environments impose limitations on the use of the Derjaguin–Landau–Verwey–Overbeek (DLVO) theory to describe the forces between particles, as previous work has shown that these depend on both the structures and geometry of the crystal surfaces − and the chemistry of the bulk and interfacial solutions. ,,− Direct experimental analysis of nanoparticle interactions under these extreme conditions is, therefore, needed to understand the complex correlations between chemistry and collective behaviors in the Hanford wastes and to inform effective treatment schemes.…”

Section: Introductionmentioning

confidence: 99%

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Frustrated Coulombic and Cation Size Effects on Nanoscale Boehmite Aggregation: A Tumbler Small- and Ultra-Small-Angle Neutron Scattering Study

et al. 2022

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To better understand the effects of solution chemistry on particle aggregation in the complex legacy tank wastes at the Hanford (WA) and Savannah River (SC) sites, we have performed a series of tumbler small- and ultra-small-angle neutron scattering experiments on 20 wt % solid slurries of nanoparticulate aluminum oxyhydroxide (boehmite) with M1+ nitrates of various concentrations and radii. The solutes consisted of H, Li, Na, K, and Rb nitrates at 10–5, 10–3, 10–1, 2, and 4 molal (m) concentrations, as well as in pure H2O. Synthetic boehmite nanoparticles were used with a size range from ∼20 to 30 nm. Tumbler cells were used to keep the solids from settling. Although particles initially form individual rhombohedral platelets, once placed in solution, they quickly form well-bonded stacks, primary aggregates, up to ∼1500 Å long, and a second level of aggregates whose concentration and structure vary as a function of cation type and concentration. Aggregation generally increases with increased solute concentration and with cation radius up to a concentration somewhat above 10–1 m, at which point the trend reverses. Primary aggregates become more rodlike and larger. The Kirkwood-like reversal probably reflects a change from Derjaguin–Landau–Verwey–Overbeek (DLVO)/Debye behavior controlled by surface chemistry to a frustrated Coulombic system controlled by the solution structure. These data suggest that an understanding of the effects of salt concentration and chemistry on nanoparticle aggregate structures provides useful physical insights into the microscopic origin of slurry rheology in the Hanford and Savannah River legacy wastes.

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Section: Resultssupporting

confidence: 89%

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Frustrated Coulombic and Cation Size Effects on Nanoscale Boehmite Aggregation: A Tumbler Small- and Ultra-Small-Angle Neutron Scattering Study

et al. 2022

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“…This leads to Mn c = 144πη s h 2 R 2 cl γc /(A H R ag ). Taking A H = 5.2kT and h 10 nm for boehmite particles 77,78 , we get Mn c = 0.06-1 in good agreement with a transition controlled by the Mason number 42 .…”

Section: Discussionsupporting

confidence: 62%

Shear-induced memory effects in boehmite gels

Sudreau,

Manneville,

Servel

et al. 2021

Preprint

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Colloidal gels are formed by the aggregation of Brownian particles into clusters that are, in turn, part of a space-spanning percolated network. In practice, the microstructure of colloidal gels, which dictates their mechanical properties, strongly depends on the particle concentration and on the nature of their interactions. Yet another critical control parameter is the shear history experienced by the sample, which controls the size and density of the cluster population, via particle aggregation, cluster breakup and restructuring. Here we investigate the impact of shear history on acid-induced gels of boehmite, an aluminum oxide. We show that following a primary gelation, these gels display a dual response depending on the shear rate γp used to rejuvenate their microstructure. We identify a critical shear rate γc , above which boehmite gels display a gel-like viscoelastic spectrum upon flow cessation, similar to that obtained following the primary gelation. However, upon flow cessation after shear rejuvenation below γc , boehmite gels display a glassy-like viscoelastic spectrum together with enhanced elastic properties. Moreover, the nonlinear rheological properties of boehmite gels also differ on both sides of γc : weak gels obtained after rejuvenation at γp > γc show a yield strain that is constant, independent of γp , whereas strong gels obtained with γp < γc display a yield strain that significantly increases with γp . Our results can be interpreted in light of previous literature on shear-induced cluster densification, which accounts for the reinforced elastic properties at γp < γc , while we rationalize the critical shear rate γc in terms of a dimensionless quantity, the Mason number, comparing the ratio of the strength of the shear flow to the interparticle bond force.

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“…Nanoporous materials often exhibit hierarchical structures, which are reflected in these data by the two Guinier “knees” indicated by the arrows on the SANS curves in Figure A. These knees result from separate distributions of scatterers (pores in this case) with similar sizes, and their locations correlate with the radii of gyration ( R g ) of the size limits of those distributions where R g ∼2π/ Q . , R g was used to represent the pore size because the pores of SPAC have irregular and tortuous shapes. The volume-weighted pore size distributions (Figure B) indicate the presence of two major populations of pores in all three samples (Figure A).…”

Section: Resultsmentioning

confidence: 99%

Degradation of Adsorbed Bisphenol A by Soluble Mn(III)

Sun

Shobnam

et al. 2021

Environ. Sci. Technol.

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Bisphenol A (BPA), a high production volume chemical and potential endocrine disruptor, is found to be associated with sediments and soils due to its hydrophobicity (log K OW of 3.42). We used superfine powdered activated carbon (SPAC) with a particle size of 1.38 ± 0.03 μm as a BPA sorbent and assessed degradation of BPA by oxidized manganese (Mn) species. SPAC strongly sorbed BPA, and desorption required organic solvents. No degradation of adsorbed BPA (278.7 ± 0.6 mg BPA g −1 SPAC) was observed with synthetic, solid α-MnO 2 with a particle size of 15.41 ± 1.35 μm; however, 89% mass reduction occurred following the addition of 0.5 mM soluble Mn(III). Small-angle neutron scattering data suggested that both adsorption and degradation of BPA occurred in SPAC pores. The findings demonstrate that Mn(III) mediates oxidative transformation of dissolved and adsorbed BPA, the latter observation challenging the paradigm that contaminant desorption and diffusion out of pore structures are required steps for degradation. Soluble Mn(III) is abundant near oxic-anoxic interfaces, and the observation that adsorbed BPA is susceptible to degradation has implications for predicting, and possibly managing, the fate and longevity of BPA in environmental systems.

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Correlating inter-particle forces and particle shape to shear-induced aggregation/fragmentation and rheology for dilute anisotropic particle suspensions: A complementary study via capillary rheometry and in-situ small and ultra-small angle X-ray scattering

Cited by 25 publications

References 60 publications

Frustrated Coulombic and Cation Size Effects on Nanoscale Boehmite Aggregation: A Tumbler Small- and Ultra-Small-Angle Neutron Scattering Study

Frustrated Coulombic and Cation Size Effects on Nanoscale Boehmite Aggregation: A Tumbler Small- and Ultra-Small-Angle Neutron Scattering Study

Shear-induced memory effects in boehmite gels

Degradation of Adsorbed Bisphenol A by Soluble Mn(III)

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