ElectrostaticBarriers to Nanoparticle Accessibilityof a Porous Matrix
Figshare documentation (Figshare (United Kingdom))(2020)
摘要
Translocation
from one cavity to another through a narrow constriction
(i.e., a “hole”) represents the fundamental elementary
process underlying hindered mass transport of nanoparticles and macromolecules
within many natural and synthetic porous materials, including intracellular
environments. This process is complex and may be influenced by long-range
(e.g., electrostatic) particle–wall interactions, transient
adsorption/desorption, surface diffusion, and hydrodynamic effects.
Here, we used a three-dimensional (3D) tracking method to explicitly
visualize the process of nanoparticle diffusion within periodic porous
nanostructures, where electrostatic interactions were mediated via
ionic strength. The effects of electrostatic interactions on nanoparticle
transport were surprisingly large. For example, an increase in the
Debye length of only a few nanometers (in a material with a hole diameter
of ∼100 nm) increased the mean cavity escape time 3-fold. A
combination of computational and experimental analyses indicated that
this hindered cavity escape was due to an electrostatic energy barrier
in the region of the hole, which was quantitatively explained using
DLVO theory. These findings explicitly demonstrate that the cavity
escape process was barrier-limited and dominated by electrostatic
effects.
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关键词
nanoparticle accessibilityof
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