Robust and Responsive Silk Ionomer Microcapsules

Ye, Chunhong; Shchepelina, Olga; Calabrese, Rossella; Drachuk, Irina; Kaplan, David L.; Tsukruk, Vladimir V.

doi:10.1021/bm201246f

Cited by 60 publications

(106 citation statements)

References 68 publications

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“…shell, which reveals a gradual densification of the shells and porosity reduction. 10,22 The observation is consist with the morphology change as demonstrated by AFM and TEM measurements (Figure 4, 5a, b 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 transport thus indicating that Coulombic interactions play minor role in the particle transport in these open pore morphologies in contrast to traditional polymer microcapsules. Figure 7a).…”

Section: Resultsmentioning

confidence: 99%

“…21 Furthermore, currently explored microcapsules which are mostly composed of synthetic polymers or biopolymers usually possess dense shells with a mesh size of few nanometers for ionic-bonded shells and usually below 10 nm for hydrogen-bonded shells. 10,22,23,24,25,26,27,28 These uniform shells are only permeable to small molecules or mid-sized macromolecules (well below 10 6 Daltons) even in a highly swollen state. 29,30 Thus, across-shell transport and encapsulation of large objects such as nano-and microparticles is forbidden with current material choices.…”

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confidence: 99%

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Cellulose Nanocrystal Microcapsules as Tunable Cages for Nano- and Microparticles

Malak

et al. 2015

ACS Nano

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We demonstrate the fabrication of highly open spherical cages with large through pores using high aspect ratio cellulose nanocrystals with "haystack" shell morphology. In contrast to traditional ultrathin shell polymer microcapsules with random porous morphology and pore sizes below 10 nm with limited molecular permeability of individual macromolecules, the resilient cage-like microcapsules show a remarkable open network morphology that facilitates across-shell transport of large solid particles with a diameter from 30 to 100 nm. Moreover, the transport properties of solid nanoparticles through these shells can be pH-triggered without disassembly of these shells. Such behavior allows for the controlled loading and unloading of solid nanoparticles with much larger dimensions than molecular objects reported for conventional polymeric microcapsules.

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Section: Resultsmentioning

confidence: 99%

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confidence: 99%

Cellulose Nanocrystal Microcapsules as Tunable Cages for Nano- and Microparticles

Malak

et al. 2015

ACS Nano

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“…In order to obtain charged hydrogels, we could not use simple mixing to form the hydrogels, as they are based on electrostatic interactions between opposite charged ionomers [22–23]. In previous work we demonstrated the ultrasonication technique as a useful way to obtain silk-based hydrogels [21].…”

Section: Resultsmentioning

confidence: 99%

“…Furthermore, using layer by layer techniques, these silk ionomers can be used for the formation of pH-sensitive shell microcapsules for the encapsulation and delivery of macromolecules or cells [23]. …”

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confidence: 99%

Silk ionomers for encapsulation and differentiation of human MSCs

Calabrese

Kaplan

2012

Biomaterials

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The response of human bone marrow derived human mesenchymal stem cells (hMSCs) encapsulated in silk ionomer hydrogels was studied. Silk aqueous solutions with silk-poly-L-lysine or silk-poly-L-glutamate were formed into hydrogels via ultrasonication in situ with different net charges. hMSCs were encapsulated within the hydrogels and the impact of matrix charge was assessed over weeks in osteogenic, adipogenic and maintenance growth media. These modified silk charged polymers supported cell viability and proliferative potential, and the hMSCs were able to differentiate toward osteogenic or adipogenic lineages in the corresponding differentiation media. The silk/silk-poly-L-lysine hydrogels exhibited a positive effect on selective osteogenesis of hMSCs, inducing differentiation toward an osteogenic lineage even in the absence of osteogenic supplements, while also inhibiting adipogenesis. In contrast, silk/silk fibroin-poly-L-glutamate hydrogels supported both osteogenic and adipogenic differentiation of hMSCs when cultured under induction conditions. The results demonstrate the potential utility of silk-based ionomers in gel formats for hMSCs encapsulation and for directing hMSCs long term functional differentiation toward specific lineages.

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“…Thickness of (silk/PVCL) films increased with increase in PVCL molecular weight and decrease in deposition pH. 26 The partial knowledge about silk-based multilayers is largely because of the complexity of intermolecular binding. These systems show a significant rise in thickness with increase in PVCL molecular weight at pH<5 but become independent on polymer chain length at pH≥5.…”

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confidence: 99%

Tuning assembly and enzymatic degradation of silk/poly(N-vinylcaprolactam) multilayers via molecular weight and hydrophobicity

et al. 2015

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We report on enzymatically degradable nanothin coatings obtained by layer-by-layer (LbL) assembly of silk fibroin with poly(N-vinylcaprolactam) (PVCL) via hydrogen bonding and hydrophobic interactions. We found that both silk β-sheet content, controlled through dipping and spin-assisted LbL, and PVCL molecular weight regulate film thickness, microstructure, pH-stability, and biodegradability with a nanoscale precision. Thickness of (silk/PVCL) films increased with increase in PVCL molecular weight and decrease in deposition pH. The impact of assembly pH on film growth was more dramatic for dipped films. These systems show a significant rise in thickness with increase in PVCL molecular weight at pH < 5 but become independent on polymer chain length at pH ≥ 5. We also found that spin-assisted films exhibited a greater stability at elevated pH and against enzymatic degradation as compared to their dipped counterparts. For both film types, the pH and enzymatic stability was improved with increasing PVCL length and β-sheet content, indicating enhanced hydrophobic and hydrogen-bonded interactions between PVCL and silk. Finally, we fabricated spherical and cubical (silk/PVCL) LbL capsules of regulated permeability and enzymatic degradation. Our approach gives a unique opportunity to tune thickness, morphology, structure, and biodegradability rate of silk films and capsules by varying silk secondary structure and PVCL length. Accounting for all-aqueous fabrication and the biocompatibility of both polymers these biodegradable materials provide novel platforms for delivery systems and medical devices.

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Robust and Responsive Silk Ionomer Microcapsules

Cited by 60 publications

References 68 publications

Cellulose Nanocrystal Microcapsules as Tunable Cages for Nano- and Microparticles

Cellulose Nanocrystal Microcapsules as Tunable Cages for Nano- and Microparticles

Silk ionomers for encapsulation and differentiation of human MSCs

Tuning assembly and enzymatic degradation of silk/poly(N-vinylcaprolactam) multilayers via molecular weight and hydrophobicity

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