Biopolymer- and Natural Fiber-Based Biomimetic Tissues to Realize Smart Cosmeceuticals and Nutraceuticals Using an Innovative Approach

Abstract

More sustainable and smart cosmeceuticals and nutraceuticals are necessary due to the ecological transition. In this study, a pullulan-based water solution containing chitin nanofibril-nano-lignin (CN-LG) complexes that encapsulate fish collagen polypeptide, allantoin and nicotinamide was electrospun onto a nonwoven substrate made of bamboo fibers to obtain a smart nanostructured bilayer system for releasing active molecules onto the skin or other body tissues. Infrared spectroscopy was used to characterize the composition of the bilayer system before and after rapid washing of the sample with distilled water and liquids mimicking physiological fluids. The viability of keratinocytes was studied as well as the antioxidant activity, protective activity towards UV light, metalloproteinase release of aged fibroblasts and the inhibitor activity against collagen degradation. Immunomodulatory tests were performed to investigate the anti-inflammatory activity of the bilayer system as well as its indirect antimicrobial activity. The results indicate that the bilayer system can be used in the production of innovative sustainable cosmeceuticals. In general, the adopted strategy can be extended to several smart treatments for fast release that can be commercialized as solid products, thus avoiding the use of preservatives and water.

Keywords: allantoin; anti-inflammatory; antioxidant; bamboo; cosmeceutical; electrospinning; fish collagen polypeptide; niacinamide; pullulan.

Figure 1

(a) SEM micrograph related to CN-LG complexes; (b) picture of the bamboo nonwoven substrate modified on its surface by electrospinning of a pullulan tissue layer containing CN-LG complexes and active molecules; (c) scheme of the developed bilayer system.

Figure 1

(a) SEM micrograph related to CN-LG complexes; (b) picture of the bamboo nonwoven substrate modified on its surface by electrospinning of a pullulan tissue layer containing CN-LG complexes and active molecules; (c) scheme of the developed bilayer system.

Figure 2

SEM micrographs showing the morphology of the electrospun pullulan tissue: (a) Magnification 70×; (b) magnification 600×; (c) magnification 5000×; (d) magnification 20,000×.

Figure 3

Infrared spectra recorded by ATR accessory for the brown pullulan-based layer and the white bamboo nonwoven substrate.

Figure 4

Trial performed with saline solution: (a) Structure of the sample; (b) strip before the immersion; (c) strip after 10 s.

Figure 5

Infrared spectrum recorded onto the strip after immersion and drying in saline solution.

Figure 6

Effect of nanoparticles and bilayer tissue on the viability of human keratinocytes expressed as viability %, compared to the untreated control. Values having different symbols (anything, *, **, ***, etc…) belong to distinguishable samples. Significant vs. control (* p < 0.005).

Figure 7

Protective antioxidant effects on peroxidation of linoleic acid in the presence of nanoparticles and the final tissue. Values having different symbols (anything, *, **, ***, etc…) belong to distinguishable samples. Significant vs. control (* p < 0.005); Significant vs. CN-LG and Nanoparticles (** p < 0.005). Increased antioxidant activities of CN-LG and CN-LG containing active molecules with respect to the control were found. Interestingly, the final tissue displays the highest activity in terms of antioxidant properties, suggesting that pullulan acts as a synergistic component. When the final tissue is compared to the CN-LG nanoparticles, the difference is significant, with p < 0.005. Regarding the comparison between CN-LG nanoparticles and the control, the difference is significant, with p < 0.0001.

Figure 8

ATP levels in irradiated human keratinocyte cultures in the absence and the presence of pullulan tissue embedded with nanoparticles of CN-LG, encapsulating allantoin, nicotinamide and polypeptide from fish collagen. Results are reported as % of untreated control ATP content. Values having different symbols (anything, *, **, ***, etc…) belong to distinguishable samples. Significant vs. control (* p < 0.005); Significant vs. CN-LG and Nanoparticles (** p < 0.005).

Figure 9

MMPI release of aged fibroblast treated with CN-LG carrier, nanoparticles and the final functional tissue. Values having different symbols (anything, *, **, ***, etc…) belong to distinguishable samples. Significant vs. control (* p < 0.005).

Figure 10

Percentage of inhibitory activity vs. collagen degradation in fibroblast cultures incubated with collagenase enzyme after treatment with CN-LG carrier, nanoparticles or the final tissue. Significant vs. control (* p < 0.005).

Figure 11

Levels of expression of the proinflammatory cytokines IL-8, IL-6, IL-1 α and TNF-α; anti-inflammatory cytokine TGF-β; and antimicrobial peptide HBD-2.