title: Chemodynamics of Soft Nanoparticulate Metal Complexes: From the Local Particle/Medium Interface to a Macroscopic Sensor Surface.
abstract: The lability of a complex species between a metal ion M and a binding site S, MS, is conventionally defined with respect to an ongoing process at a reactive interface, for example, the conversion or accumulation of the free metal ion M by a sensor. In the case of soft charged multisite nanoparticulate complexes, the chemodynamic features that are operative within the micro environment of the particle body generally differ substantially from those for dissolved similar single-site complexes in the same medium. Here we develop a conceptual framework for the chemodynamics and the ensuing lability of soft (3D) nanoparticulate metal complexes. The approach considers the dynamic features of MS at the intraparticulate level and their impact on the overall reactivity of free metal ions at the surface of a macroscopic sensing interface. Chemodynamics at the intraparticulate level is shown to involve a local reaction layer at the particle/medium interface, while at the macroscopic sensor level an operational reaction layer is invoked. Under a certain window of conditions, volume exclusion of the nanoparticle body near the medium/sensor interface is substantial and affects the properties of the reaction layer and the overall lability of the nanoparticulate MS complex toward the reactive surface.
authors.affiliation: Systemic Physiological and Ecotoxicological Research (SPHERE), Department of Biology, University of Antwerp , Groenenborgerlaan 171, 2020 Antwerp, Belgium.|Physical Chemistry and Soft Matter, Wageningen University & Research , Stippeneng 4, 6708 WE Wageningen, The Netherlands.
authors.forename: Raewyn M
authors.identifier: 0000-0001-9505-1465
authors.initials: RM
authors.lastname: Town
authors.affiliation: Université de Lorraine , Laboratoire Interdisciplinaire des Environnements Continentaux, UMR 7360 CNRS, 15 avenue du Charmois, 54500 Vandoeuvre-les-Nancy, France.|Physical Chemistry and Soft Matter, Wageningen University & Research , Stippeneng 4, 6708 WE Wageningen, The Netherlands.
authors.forename: José Paulo
authors.identifier: 0000-0001-7925-9733
authors.initials: JP
authors.lastname: Pinheiro
authors.affiliation: Physical Chemistry and Soft Matter, Wageningen University & Research , Stippeneng 4, 6708 WE Wageningen, The Netherlands.
authors.forename: Herman P
authors.initials: HP
authors.lastname: van Leeuwen