Probing the molecular-level control of aluminosilicate dissolution: A sensitive solid-state NMR proxy for reactive surface area

Washton, Nancy M.; Brantley, Susan L.; Mueller, Karl T.

doi:10.1016/j.gca.2008.09.018

Cited by 29 publications

(36 citation statements)

References 62 publications

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“…An analogous protocol has also been developed using 3,3,3-(trifluoropropyl)dimethylchlorosilane to assay the concentration of free hydroxyl groups on silica surfaces. [82] Compared with XPS peak-fitting methods, CD offers a far more quantitative method to assay those functional groups for which selective derivatising reactions exist.…”

Section: Elemental (Bulk) Compositionmentioning

confidence: 99%

Assessing the colloidal properties of engineered nanoparticles in water: case studies from fullerene C60 nanoparticles and carbon nanotubes

Chen¹,

Smith²,

Ball³

et al. 2010

Environ. Chem.

136

114

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Environmental context. The fate and bioavailability of engineered nanoparticles in natural aquatic systems are strongly influenced by their ability to remain dispersed in water. Consequently, understanding the colloidal properties of engineered nanoparticles through rigorous characterisation of physicochemical properties and measurements of particle stability will allow for a more accurate prediction of their environmental, health, and safety effects in aquatic systems.This review highlights some important techniques suitable for the assessment of the colloidal properties of engineered nanoparticles and discusses some recent findings obtained by using these techniques on two popular carbon-based nanoparticles, fullerene C 60 and multi-walled carbon nanotubes.Abstract. The colloidal properties of engineered nanoparticles directly affect their use in a wide variety of applications and also control their environmental fate and mobility. The colloidal stability of engineered nanoparticles depends on their physicochemical properties within the given aqueous medium and is ultimately reflected in the particles' aggregation and deposition behaviour. This review presents some of the key experimental methods that are currently used to probe colloidal properties and quantify engineered nanoparticle stability in water. Case studies from fullerene C 60 nanoparticles and multi-walled carbon nanotubes illustrate how the characterisation and measurement methods are used to understand and predict nanoparticle fate in aquatic systems. Consideration of the comparisons between these two classes of carbonbased nanoparticles provides useful insights into some major current knowledge gaps while also revealing clues about needed future developments. Key issues to be resolved relate to the nature of near-range surface forces and the origins of surface charge, particularly for the reportedly unmodified or 'pure' carbon-based nanoparticles.

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Section: Elemental (Bulk) Compositionmentioning

confidence: 99%

Assessing the colloidal properties of engineered nanoparticles in water: case studies from fullerene C60 nanoparticles and carbon nanotubes

Chen¹,

Smith²,

Ball³

et al. 2010

Environ. Chem.

136

114

View full text Add to dashboard Cite

show abstract

“…Washton et al (2008) measured the number of reactive sites on aluminosilicate glass surfaces with 19 F NMR spectroscopy using a fluorine-containing TFS [(3,3,3-trifluoropropyl)dimethylchorosilane] probe molecule. The TFS-reactive T-OH species on the glass surface are known to be non-H-bonded Q 3 groups, and may represent loci that are accessible to and affected by proton-mediated dissolution.…”

Section: Experimental Validationmentioning

confidence: 99%

“…The calculated surface site density will be compared to that determined by NMR studies for different glass compositions. Hydroxylated glass surface models will be used to calculate activation energy barriers for different potential network-breaking reactions and to evaluate if the calculated highly-reactive sites are consistent with those proposed through NMR studies (e.g., Washton et al, 2008). …”

mentioning

confidence: 99%

Progress toward bridging from atomistic to continuum modeling to predict nuclear waste glass dissolution.

Zapol

Bourg

Criscenti³

et al. 2011

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This report summarizes research performed for the Nuclear Energy Advanced Modeling and Simulation (NEAMS) Subcontinuum and Upscaling Task. The work conducted focused on developing a roadmap to include molecular scale, mechanistic information in continuum-scale models of nuclear waste glass dissolution. This information is derived from molecular-scale modeling efforts that are validated through comparison with experimental data. In addition to developing a master plan to incorporate a subcontinuum mechanistic understanding of glass dissolution into continuum models, methods were developed to generate constitutive dissolution rate expressions from quantum calculations, force field models were selected to generate multicomponent glass structures and gel layers, classical molecular modeling was used to study diffusion through nanopores analogous to those in the interfacial gel layer, and a micro-continuum model (KµC) was developed to study coupled diffusion and reaction at the glass-gel-solution interface. We would also like to acknowledge discussions with the International Corrosion Working Group members including Stéphane Gin,

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“…These more energetic and reactive sites could be disproportionately important in reaction kinetics and difficult to identify experimentally. Of course, continued collaboration with analytical chemists will be the key in identifying and quantifying the reactive surface area of materials in the environment [113].…”

Section: Summary and Futurementioning

confidence: 99%

Computational Spectroscopy in Environmental Chemistry

Kubicki

Mueller

2010

Computational Spectroscopy

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Probing the molecular-level control of aluminosilicate dissolution: A sensitive solid-state NMR proxy for reactive surface area

Cited by 29 publications

References 62 publications

Assessing the colloidal properties of engineered nanoparticles in water: case studies from fullerene C60 nanoparticles and carbon nanotubes

Assessing the colloidal properties of engineered nanoparticles in water: case studies from fullerene C60 nanoparticles and carbon nanotubes

Progress toward bridging from atomistic to continuum modeling to predict nuclear waste glass dissolution.

Computational Spectroscopy in Environmental Chemistry

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