Publication
Title
Lability of nanoparticulate metal complexes at a macroscopic metal responsive (bio)interface : expression and asymptotic scaling laws
Author
Abstract
The lability of metal complexes expresses the extent of the dissociative contribution of the complex species to the flux of metal ions toward a macroscopic metal-responsive (bio)interface, for example, an electrodic sensor or an organism. While the case of molecular ligands is well-established, it is only recently that a definition was elaborated for the lability of metal complexes with nanoparticles (NPs) in aqueous dispersions. The definition includes the thickness of the nonequilibrium reaction layer operational at the (bio)interface and the extent of geometrical exclusion of NPs therefrom. In this work, an explicit expression is derived for the lability of nanoparticulate metal complexes (MNP) toward a macroscopic reactive (bio)interface. Interpretation accounts for the MNP chemodynamic properties that depend on the NP size, electrostatics, metal diffusion and dehydration rates, and density of metal binding sites for various NP types, for example, soft/coreshell and hard NPs having volume and surface site distribution, respectively. Computational examples under practical conditions illustrate how these factors jointly determine the remarkable nonmonotonous dependence of the MNP lability parameter on the NP size. The analysis is supported by the formulation of asymptotic scaling laws clarifying how local MNP dissociation dynamics affect the lability parameter for MNP complexes at the scale of the macroscopic (bio)interface.
Language
English
Source (journal)
The journal of physical chemistry: C : nanomaterials and interfaces. - Washington, D.C., 2007, currens
Publication
Washington, D.C. : 2018
ISSN
1932-7447 [print]
1932-7455 [online]
DOI
10.1021/ACS.JPCC.7B11982
Volume/pages
122 :11 (2018) , p. 6052-6065
ISI
000428356700024
Full text (Publisher's DOI)
Full text (open access)
UAntwerpen
Faculty/Department
Research group
Publication type
Subject
Affiliation
Publications with a UAntwerp address
External links
Web of Science
Record
Identifier
Creation 03.04.2018
Last edited 02.10.2024
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