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The delivery of hydrophilic drugs from hydrophobic polymers is a long-standing challenge in the biomaterials field due to the limited solubility of the therapeutic agent within the polymer matrix. In this work, we develop a drug delivery mechanism that enables the impregnation and subsequent elution of hydrophilic drugs from a hydrophobic polymer material. This was achieved by synthesizing core cross-linked star polymer amphiphiles with hydrophilic cores and hydrophobic coronas. While significant work has been done to create nanocarriers for hydrophilic drugs, this work is distinct from previous work in that it designs amphiphilic and core cross-linked particles for controlled release from hydrophobic matrices. Ultraviolet-mediated atom transfer radical polymerization was used to synthesize the poly(ethylene glycol) (PEG)-based hydrophilic cores of the star polymers, and hydrophobic coronas of poly(caprolactone) (PCL) were then built onto the stars using ring-opening polymerization. We illustrated the cytocompatibility of PCL loaded with these star polymers through human endothelial cell adhesion and proliferation for up to 7 days, with star loadings of up to 40 wt %. We demonstrated successful loading of the hydrophilic drug heparin into the star polymer core, achieving a loading efficiency and content of 50 and 5%, respectively. Finally, the heparin-loaded star polymers were incorporated into a PCL matrix and sustained release of heparin was illustrated for over 40 days. These results support the use of core cross-linked star polymer amphiphiles for the delivery of hydrophilic drugs from hydrophobic polymer matrices. These materials were developed for application as drug-eluting and biodegradable coronary artery stents, but this flexible drug delivery platform could have impact in a broad range of medical applications.

Author(s): Sauret, Alban; Somszor, Katarzyna; Villermaux, Emmanuel; Dressaire, Emilie | Abstract: During the transport of colloidal suspensions in microchannels, the deposition of particles can lead to the formation of clogs, typically at constrictions. Once a clog is formed in a microchannel, advected particles form an aggregate upstream from the site of the blockage. This aggregate grows over time, which leads to a dramatic reduction of the flow rate. In this paper, we present a model that predicts the growth of the aggregate formed upon clogging of a microchannel. We develop an analytical description that captures the time evolution of the volume of the aggregate, as confirmed by experiments performed using a pressure-driven suspension flow in a microfluidic device. We show that the growth of the aggregate increases the hydraulic resistance in the channel and leads to a drop in the flow rate of the suspensions. We then derive a model for the growth of aggregates in multiple parallel microchannels where the clogging events are described using a stochastic approach. The aggregate growths in the different channels are coupled. Our work illustrates the critical influence of clogging events on the evolution of the flow rate in microchannels. The coupled dynamics of the aggregates described here for parallel channels is key to bridge clogging at the pore scale with macroscopic observations of the flow rate evolution at the filter scale.

International audience; Various materials are made of long thin fibers that are randomly oriented to form a complex network in which drops of wetting liquid tend to accumulate at the nodes. The capillary force exerted by the liquid can bend flexible fibers, which in turn influences the morphology adopted by the liquid. In this paper, we investigate through a model situation the role of the fiber flexibility on the shape of a small volume of liquid on a pair of crossed flexible fibers. We characterize the liquid morphologies as we vary the volume of liquid, the angle between the fibers, and the length of the fibers. The drop morphologies previously reported for rigid crossed fibers, i.e., a drop, a column and a mixed morphology, are also observed on flexible crossed fibers with modified domains of existence. In addition, at small tilt angles between the fibers, a new behavior is observed: the fibers bend and collapse. Depending on the volume of liquid, a thin column with or without a drop is reported on the collapsed fibers. Our study suggests that the fiber flexibility adds a rich variety of behaviors that may be important for some applications.