Journal
ACS NANO
Volume 8, Issue 6, Pages 5725-5737Publisher
AMER CHEMICAL SOC
DOI: 10.1021/nn500512x
Keywords
discoidal capsules; layer-by-layer; multilayer hydrogels; pH-responsive shapes; cellular uptake
Categories
Funding
- NSF CAREER Award [1350370]
- Cancer Institute (NCI), National NIH [U54 CA143837]
- NCI, NIH [1U54CA151668-01]
- Division Of Materials Research
- Direct For Mathematical & Physical Scien [1350370] Funding Source: National Science Foundation
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We report On naturally inspired hydrogel capsules with pH-induced transitions from discoids to oblate ellipsoids and their interactions with cells. We integrate characteristics of erythrocytes such as discoidal shape, hollow structure, and elasticity with reversible pH-responsiveness of poly(methacrylic acid) (PMAA) to design a new type of drug delivery carrier to be potentially triggered by chemical stimuli in the tumor lesion. The capsules are fabricated from cross-linked PMAA multilayers using sacrificial discoid silicon templates. The degree of capsule shape transition is controlled by the pH-tuned volume change, which in turn is regulated by the capsule wall composition. The (PMAA)15 capsules undergo a dramatic 24-fold volume change, while a moderate 2.3-fold volume variation is observed for more rigid PMAA (poly(N-vinylpyrrolidone) (PMAA-PVPON)(5) capsules when solution pH is varied between 7.4 and 4. Despite that both types of capsules exhibit discoid-to-oblate ellipsoid transitions, a 3-fold greater swelling in radial dimensions is found for one-component systems due to a greater degree of the circular face bulging. We also show that (PMAA-PVPON)(5) discoidal capsules interact differently with J774A.1 macrophages, HMVEC endothelial cells, and 411 breast cancer cells. The discoidal capsules show 60% lower internalization as compared to spherical capsules. Finally, hydrogel capsules demonstrate a 2-fold decrease in size upon internalization. These capsules represent a unique example of elastic hydrogel discoids capable of pH-induced drastic and reversible variations in aspect ratios. Considering the RBC-mimicking shape, their dimensions, and their capability to undergo pH-triggered intracellular responses, the hydrogel capsules demonstrate considerable potential as novel carriers in shape-regulated transport and cellular uptake.
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