Synthesis of Silk Fibroin Micro‐ and Submicron Spheres Using a Co‐Flow Capillary Device

Mitropoulos, Alexander N.; Perotto, Giovanni; Kim, Sunghwan; Marelli, Benedetto; Kaplan, David L.; Omenetto, Fiorenzo G.

doi:10.1002/adma.201304244

Cited by 71 publications

(56 citation statements)

References 42 publications

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“…A detailed understanding of the phase transition process that results in fiber formation is not only of great academic interest, but also provides key information for any successful attempt to mimic the exceptional material properties observed in natural silk134567. Many components of fibrillar silk can be chemically re-solubilized; in particular reconstituted silk fibroin (RSF)56, obtained by dissolving spun cocoons, has been used in a wide range of applications 5689101112131415. The widespread use of reconstituted silk feedstocks is largely enabled by the relative ease in which this material can be prepared and stored16.…”

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confidence: 99%

Silk micrococoons for protein stabilisation and molecular encapsulation

et al. 2017

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Naturally spun silks generate fibres with unique properties, including strength, elasticity and biocompatibility. Here we describe a microfluidics-based strategy to spin liquid native silk, obtained directly from the silk gland of Bombyx mori silkworms, into micron-scale capsules with controllable geometry and variable levels of intermolecular β-sheet content in their protein shells. We demonstrate that such micrococoons can store internally the otherwise highly unstable liquid native silk for several months and without apparent effect on its functionality. We further demonstrate that these native silk micrococoons enable the effective encapsulation, storage and release of other aggregation-prone proteins, such as functional antibodies. These results show that native silk micrococoons are capable of preserving the full activity of sensitive cargo proteins that can aggregate and lose function under conditions of bulk storage, and thus represent an attractive class of materials for the storage and release of active biomolecules.

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Silk micrococoons for protein stabilisation and molecular encapsulation

et al. 2017

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“…The technique involved an all aqueous processing at room temperature, unlike various other techniques of sphere fabrication which expose the drug or SF to heat, pH extremes or freezing and drying [24]. These conditions not only influence the surface of spheres but may also affect the drug release kinetics [23,24,38]. For the sphere fabrication, calculated amounts of SF, DoX and NDs in aqueous solutions were mixed together and flowed through the inner discrete phase channel at a flow rate of 40 µL/h of a co-flow capillary device.…”

Section: Synthesis Of Spheresmentioning

confidence: 99%

“…The fabrication of NDSX spheres was performed through the already developed co-flow technique [38]. The technique involved an all aqueous processing at room temperature, unlike various other techniques of sphere fabrication which expose the drug or SF to heat, pH extremes or freezing and drying [24].…”

Section: Synthesis Of Spheresmentioning

confidence: 99%

“…The factor was used to convert the diameters of individual particles to nm. A number of particles (25)(26)(27)(28)(29)(30)(31)(32)(33)(34)(35)(36)(37)(38)(39)(40) were selected for each sample and the size distribution was determined.…”

Section: Particle Size Measurementmentioning

confidence: 99%

“…The working solution was injected through the inner needle of a co-flow device [38] at a flow rate of 40 μL/h and spheres were collected in polyvinyl alcohol (PVA). PVA was the continuous phase, flowing through the outer needle at 4 mL/h, separating the working solution from the bulk forming consistent diameter spheres.…”

Section: Sphere Fabricationmentioning

confidence: 99%

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Doxorubicin loaded nanodiamond-silk spheres for fluorescence tracking and controlled drug release

Khalid

Mitropoulos

Marelli

et al. 2015

Biomed. Opt. Express

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Nanoparticle (NP) based technologies have proved to be considerably beneficial for advances in biomedicine especially in the areas of disease detection, drug delivery and bioimaging. Over the last few decades, NPs have garnered interest for their exemplary impacts on the detection, treatment, and prevention of cancer. The full potential of these technologies are yet to be employed for clinical use. The ongoing research and development in this field demands single multifunctional composite materials that can be employed simultaneously for drug delivery and biomedical imaging. In this manuscript, a unique combination of silk fibroin (SF) and nanodiamonds (NDs) in the form of nanospheres are fabricated and investigated. The spheres were loaded with the anthracyline Doxorubicin (DoX) and the drug release kinetics for these ND-SF-DoX (NDSX) spheres were studied. NDs provided the fluorescence modality for imaging while the degradable SF spheres stabilized and released the drug in a controlled manner. The emission and structural properties of the spheres were characterized during drug release. The degradability of SF and the subsequent release of DoX from the spheres were monitored through fluorescence of NDs inside the spheres. This research demonstrates the enormous potential of the ND-SF nanocomposite platforms for diagnostic and therapeutic purposes, which are both important for pharmaceutical research and clinical settings. "Nanodiamond-mediated drug delivery and imaging: challenges and opportunities," Expert Opin. Drug Deliv. 12(5), 735-749 (2015).

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Microporous Drug‐Eluting Large Silk Particles Through Cryo‐Granulation

Rodionov¹,

Abdullah²,

Kaplan³

2019

Adv Eng Mater

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A facile method for the preparation of large, microporous, drug-loaded particles is presented. High shear bollus injections of silk with cross-linker and drug colloids into super-cooled hexane were utilized to trigger phase separation of silk droplets, followed by immediate freezing at-60 o C. A subsequent-20 o C freeze-thaw of the frozen droplets resulted in self-assembly (crystallization) of the silk. The silk particles developed an internal interconnected microporous morphology with 0.1-10 µm in diameter pores. The silk particles ranged in diameter from 100 to 1,300 µm, with particle mean diameter and polydispersity controlled by the starting concentration of the cross-linking agent and silk, the rheology of the reaction mixture, and the injection pressure (80-300kPa). Cryogranulation provided a one-step process to produce microporous meso-scale silk particles with encapsulated drugs, such as doxorubicin chloride (DoxR), tobramycin sulfate (TS), kanamycin sulfate (KS) or gentamicin sulfate (GS). Almost 100% drug encapsulation efficiency was achieved in the process, and subsequent release profiles depended on the starting concentration of both the drug, silk, and pH of the elution medium. Kirby-Bauer tests and bioluminescent imaging confirmed the retention of anti-bacterial potency of the antibiotics pre-encapsulated in the cryo-particles, and macroparticles cytocompatibility towards human fibroblast and kidney cells.

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Synthesis of Silk Fibroin Micro‐ and Submicron Spheres Using a Co‐Flow Capillary Device

Abstract: A custom-made co-flow capillary device is used to synthesize monodisperse silk fibroin micro- and submicron-spheres with diameters tunable over a wide range of sizes. A model drug release is examined and control of degradation kinetics is obtained by changing sphere diameter.

Cited by 71 publications

References 42 publications

Silk micrococoons for protein stabilisation and molecular encapsulation

Silk micrococoons for protein stabilisation and molecular encapsulation

Doxorubicin loaded nanodiamond-silk spheres for fluorescence tracking and controlled drug release

Microporous Drug‐Eluting Large Silk Particles Through Cryo‐Granulation

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