Nanocrystal facet modulation to enhance transferrin binding and cellular delivery

Abstract

Binding of biomolecules to crystal surfaces is critical for effective biological applications of crystalline nanomaterials. Here, we present the modulation of exposed crystal facets as a feasible approach to enhance specific nanocrystal-biomolecule associations for improving cellular targeting and nanomaterial uptake. We demonstrate that facet-engineering significantly enhances transferrin binding to cadmium chalcogenide nanocrystals and their subsequent delivery into cancer cells, mediated by transferrin receptors, in a complex biological matrix.Competitive adsorption experiments coupled with theoretical calculations reveal that the (100) facet of cadmoselite and (002) facet of greenockite preferentially bind with transferrin via inner-sphere thiol complexation. Molecular dynamics simulation infers that facet-dependent transferrin binding is also induced by the differential affinity of crystal facets to water molecules in the first solvation shell, which affects access to exposed facets. Overall, this research underlines the promise of facet engineering to improve the efficacy of crystalline nanomaterials in biological applications.

Facet‐Dependent Surface Charge and Hydration of Semiconducting Nanoparticles at Variable pH

“…Anisotropy of shape and surface properties determine the functionality of faceted nanoparticles (NPs) in various contexts including crystal growth, [ 1 ] biosensing, [ 2 ] facet selective colloidal self‐assembly of complex materials, [ 3,4 ] enhanced selective cellular uptake, [ 5 ] and improved photo/electrocatalytic activity. [ 6,7 ] In all cases, the interplay between the intrinsic anisotropy of the NPs and their interaction with the (usually aqueous) ambient environment gives rise to the anisotropic interaction forces that control the performance of the NPs.…”

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“…The components of this corona can endow invading particles with properties that are distinct from the intrinsic properties of bare nanoparticles. This affects their environmental behavior, and their interactions with cells, including particle recognition, cellular internalization, stimulation of intracellular signaling pathways, and subsequent biological activities [10] , [22] , [23] .…”

Molecular Modeling of Protein Corona Formation and Its Interactions with Nanoparticles and Cell Membranes for Nanomedicine Applications

“…Sanchez-Guzman et al simulated oxyhemoglobin interacting with silica surfaces at pH 7 and pH 9 under different temperatures of 295 K, 322 K, 353 K, and 400 K, showing the dependence of the binding strength and structure on temperature and pH conditions [54]. Qi et al simulated TF that was bound to various cadmium selenide (CdSe) surfaces, such as (100) and (002) facets, and found that disulfide moieties of TF interact with the CdSe (100) surface rather than with the CdSe (002) surface, indicating the effect of different facets on the binding strength [55]. Hassanian et al showed that HSA binds to zinc oxide nanoparticles (ZnO NPs) mainly via electrostatic interactions between charged groups of HSA and ZnO NP, leading to the structural change of adsorbed HSA [56].…”