Multi-scale approach for modeling stability, aggregation, and network formation of nanoparticles suspended in aqueous solutions

Cardellini, Annalisa; Alberghini, Matteo; Rajan, Ananth Govind; Misra, Rahul Prasanna; Blankschtein, Daniel; Asinari, Pietro

doi:10.1039/c8nr08782b

Cited by 36 publications

(26 citation statements)

References 75 publications

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“…Note that a configuration with the SDS head oriented toward the NP is also tested, and the results are reported in the Supporting Information. The alumina bare NP (BNP), Figure 2a, has a diameter of about 4 nm, and it is built following the same protocol employed by Cardellini et al 34 Beyond the BNP, we also investigate coated NPs (CNPs) with 60, 40, and 10 wrapping molecules as shown in Figure 2c. Thus, a total of four study cases are studied.…”

Section: Methodsmentioning

confidence: 99%

Exploring the Free Energy Landscape To Predict the Surfactant Adsorption Isotherm at the Nanoparticle–Water Interface

2019

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The long-lasting stability of nanoparticle (NP) suspensions in aqueous solution is one of the main challenges in colloidal science. The addition of surfactants is generally adopted to increase the free energy barrier between NPs and hence to ensure a more stable condition avoiding the NP sedimentation. However, a tailored prediction of surfactant concentration enabling a good dispersion of NPs is still an ambitious objective. Here, we demonstrate the efficiency of coupling steered molecular dynamics (SMD) with the Langmuir theory of adsorption in the low surfactant concentration regime, to predict the adsorption isotherm of sodium-dodecyl-sulfate (SDS) on bare α-alumina NPs suspended in aqueous solution. The resulting adsorption free energy landscapes (FELs) are also investigated by tuning the percentage of SDS molecules coating the target bare NP. Our findings shed light on the competing role of enthalpic and entropic interaction contributions. On one hand, the adsorption is highly promoted by the tail–NP and tail–tail nonbonded interaction adhesion; on the other hand, our results unveil the entropic nature of water and surfactant steric effects occurring at the NP surface and preventing the adsorption. Finally, a thorough analysis on the steering works emphasizes the role of the NP curvature in the FEL of adsorption. In particular, we show that, moving from a solid infinite flat surface to a nanoscale particle, a deviation from a Markovian dynamics of adsorption occurs in close proximity to a curved solid–liquid interface. Here, both the NP curvature effect and nanoscale morphology promote a modification of the thermodynamics state of adsorption with a consequent splitting of the free energy profiles and the identification of specific sites of adsorption. The modeling framework suggested in this Article provides physical insights in the surfactant adsorption onto spherical NPs and suggests some guidelines to rationally design stable NP suspensions in aqueous solutions.

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Section: Methodsmentioning

confidence: 99%

Exploring the Free Energy Landscape To Predict the Surfactant Adsorption Isotherm at the Nanoparticle–Water Interface

2019

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“…In order to describe these complex interactions, the Derjaguin-Landau-Verwey-Overbeek (DLVO) theory is commonly applied (Romanello and Fidalgo de Cortalezzi, 2013;Cai et al, 2018), although it is restrictive to the balance between electrostatic and van der Waals forces. Several extensions of the DLVO theory have also been proposed to model inter-NP interactions in suspensions, for example, considering surface roughness, hydration forces, and steric effects (Wu et al, 1999;Walsh et al, 2012;Cardellini et al, 2019;Praetorius et al, 2020).…”

Section: Np Fate and Behavior In Sea Watermentioning

confidence: 99%

Behavior and Bio-Interactions of Anthropogenic Particles in Marine Environment for a More Realistic Ecological Risk Assessment

Corsi

Bergami

Grassi

2020

Front. Environ. Sci.

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Owing to production, usage, and disposal of nano-enabled products as well as fragmentation of bulk materials, anthropogenic nanoscale particles (NPs) can enter the natural environment and through different compartments (air, soil, and water) end up into the sea. With the continuous increase in production and associated emissions and discharges, they can reach concentrations able to exceed toxicity thresholds for living species inhabiting marine coastal areas. Behavior and fate of NPs in marine waters are driven by transformation processes occurring as a function of NP intrinsic and extrinsic properties in the receiving seawaters. All those aspects have been overlooked in ecological risk assessment. This review critically reports ecotoxicity studies in which size distribution, surface charges and bio−nano interactions have been considered for a more realistic risk assessment of NPs in marine environment. Two emerging and relevant NPs, the metal-based titanium dioxide (TiO 2), and polystyrene (PS), a proxy for nanoplastics, are reviewed, and their impact on marine biota (from planktonic species to invertebrates and fish) is discussed as a function of particle size and surface charges (negative vs. positive), which affect their behavior and interaction with the biological material. Uptake of NPs is related to their nanoscale size; however, in vivo studies clearly demonstrated that transformation (agglomerates/aggregates) occurring in both artificial and natural seawater drive to different exposure routes and biological responses at cellular and organism level. Adsorption of single particles or agglomerates onto the body surface or their internalization in feces can impair motility and affect sinking or floating behavior with consequences on populations and ecological function. Particle complex dynamics in natural seawater is almost unknown, although it determines the effective exposure scenarios. Based on the latest predicted environmental concentrations for TiO 2 and PS NPs in the marine environment, current knowledge gaps and future research challenges encompass the comprehensive study of bio−nano interactions. As such, the analysis of NP biomolecular coronas can enable a better assessment of particle uptake and related cellular pathways leading to toxic effects. Moreover, the formation of an environmentally derived corona (i.e., eco-corona) in seawater accounts for NP physical-chemical alterations, rebounding on interaction with living organisms and toxicity.

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“…The paragraphs above consider individual mechanisms by which LDHIs affect hydrates. To assemble the whole picture, one could implement stochastic models, e.g., kinetic Monte Carlo (kMC), which has been recently implemented to quantify nanoparticle formation [51] and fluid transport across pore networks [52]. Describing stochastically the formation of hydrate plugs requires, e.g., free energy barriers concerning nucleation, growth, dissociation and agglomeration of hydrates at different conditions.…”

Section: Recent Simulationsmentioning

confidence: 99%

Molecular properties of interfaces relevant for clathrate hydrate agglomeration

Striolo

Phan

Walsh

2019

Current Opinion in Chemical Engineering

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Clathrate hydrates of natural gases show promise for energy in regions traditionally poor of fossil fuels, suggest the possibility of mitigating the atmospheric impact of hydrocarbon consumption via CO2 sequestration, could advance high-tech applications to address global challenges, including the water-energy nexus, and can lead to significant economic loss and potential safety hazards when they form in oil and gas pipelines. This focused review is motivated by several recent contributions, which demonstrate how atomistic and coarsegrained simulations have become a useful tool. The examples provided suggest the time is right to take advantage of the enhanced understanding provided by simulations, to couple them with experiments that could help design new chemicals for managing hydrate formation in pipelines, for designing chemical processes and additives to advance high-tech applications such as water desalination and natural gas storage, and perhaps also for the production of methane from geological hydrate deposits with simultaneous carbon dioxide sequestration.

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Multi-scale approach for modeling stability, aggregation, and network formation of nanoparticles suspended in aqueous solutions

Abstract: Multi-scale computational framework to investigate interactions between bare and surfactant-coated nanoparticles in aqueous solutions beyond classical DLVO and aggregation theories.

Cited by 36 publications

References 75 publications

Exploring the Free Energy Landscape To Predict the Surfactant Adsorption Isotherm at the Nanoparticle–Water Interface

Exploring the Free Energy Landscape To Predict the Surfactant Adsorption Isotherm at the Nanoparticle–Water Interface

Behavior and Bio-Interactions of Anthropogenic Particles in Marine Environment for a More Realistic Ecological Risk Assessment

Molecular properties of interfaces relevant for clathrate hydrate agglomeration

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