2015
DOI: 10.1016/j.jcis.2015.01.094
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Acid-base dissociation mechanisms and energetics at the silica–water interface: An activationless process

Abstract: The protonation or deprotonation of isolated silanols in the presence of H3O(+) or OH(-), respectively, was shown to be a highly rapid, exothermic reaction with no significant activation energy. This process occurred via a concerted motion of the protons through 'water wires'. Geometry optimisations of large water clusters at the silica surface demonstrated proton transfer to the surface occurring via the rarely discussed 'proton holes' mechanism. This indicates that surface protonation is possible even when t… Show more

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Cited by 102 publications
(70 citation statements)
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References 78 publications
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“…174,175 The theoretical detection time for an individual proton is non-trivial to calculate due to the complexity introduced by acid-base equilibria and Grotthuss transport, which cannot be described by simple Brownian motion. 176 In summary, for BioFET design the limitations imposed by the mass transport, binding kinetics and geometry choices should be considered when designing for optimal response. 52,147,169,177 Non-specific response.…”
Section: Critical Review Analystmentioning
confidence: 99%
“…174,175 The theoretical detection time for an individual proton is non-trivial to calculate due to the complexity introduced by acid-base equilibria and Grotthuss transport, which cannot be described by simple Brownian motion. 176 In summary, for BioFET design the limitations imposed by the mass transport, binding kinetics and geometry choices should be considered when designing for optimal response. 52,147,169,177 Non-specific response.…”
Section: Critical Review Analystmentioning
confidence: 99%
“…The Nandoni Dam is also surrounded by activities that involve discharges from a sewer network, irrigation canals, drainage network and pumped groundwater which find their way to the lake via several tributaries. These activities result to the pH fluctuations depending on their hydronium and hydroxide ion dissociation potentials in water [28,29].…”
Section: Physico-chemical Analysismentioning
confidence: 99%
“…These results can be explained by consideration of interactions between protonated peptides and residual silanol groups of the stationary phase. At the mobile phase pH (between 3 and 3.5), residual silanols of the stationary phase are partially ionized, and the ionized silanols exist as anions . A triply charged peptide has a stronger interaction with the negatively charged silanols than a doubly charged peptide, based on the number of positive charges involved alone.…”
Section: Resultsmentioning
confidence: 99%
“…At the mobile phase pH (between 3 and 3.5), residual silanols of the stationary phase are partially ionized, and the ionized silanols exist as anions. 32 A triply charged peptide has a stronger interaction with the negatively charged silanols than a doubly charged peptide, based on the number of positive charges involved alone. If the synergistic effect is taken into consideration, 18,33 the interaction between a triply charged peptide and the silanols is significantly stronger than that between a doubly charged peptide and the silanols.…”
Section: Assessing In Vitro Degradation Of Peptides In Equine Plasmamentioning
confidence: 99%