Partner: Urszula Stachewicz, PhD, DSc

AGH University of Science and Technology (PL)

Supervision of doctoral theses
1.2022-10-24Krysiak Zuzanna  
(Akademia Górniczo-Hutnicza w Krakowie)
Designing and characterization of electrospun patches for atopic skin 

Recent publications
1.Zaszczyńska A., Gradys A. D., Kołbuk-Konieczny D., Zabielski K., Szewczyk P., Stachewicz U., Sajkiewicz P. Ł., Poly(L-lactide)/nano-hydroxyapatite piezoelectric scaffolds for tissue engineering, Micron, ISSN: 0968-4328, DOI: 10.1016/j.micron.2024.103743, Vol.188, pp.103743-1-15, 2025
Abstract:

The development of bone tissue engineering, a field with significant potential, requires a biomaterial with high bioactivity. The aim of this manuscript was to fabricate a nanofibrous poly(L-lactide) (PLLA) scaffold containing nano-hydroxyapatite (nHA) to investigate PLLA/nHA composites, particularly the effect of fiber arrangement and the addition of nHA on the piezoelectric phases and piezoelectricity of PLLA samples. In this study, we evaluated the effect of nHA particles on a PLLA-based electrospun scaffold with random and aligned fiber orientations. The addition of nHA increased the surface free energy of PLLA/nHA (42.9 mN/m) compared to PLLA (33.1 mN/m) in the case of aligned fibers. WAXS results indicated that at room temperature, all the fibers are in an amorphous state indicated by a lack of diffraction peaks and amorphous halo. DSC analysis showed that all samples located in the amorphous/disordered alpha' phase crystallize intensively at temperatures just above the Tg and recrystallize on further heating, achieving significantly higher crystallinity for pure PLLA than for doped nHA, 70 % vs 40 %, respectively. Additionally, PLLA/nHA fibers show a lower heat capacity for PLLA in the amorphous state, indicating that nHA reduces the molecular mobility of PLLA. Moreover, piezoelectric constant d33 was found to increase with the addition of nHA and for the aligned orientation of the fibers. In vitro tests confirmed that the addition of nHA and the aligned orientation of nanofibers increased osteoblast proliferation.

Keywords:

Scaffolds, Tissue engineering, Bone tissue engineering, Smart medicine, Biodegradable polymers, Regenerative medicine

Affiliations:
Zaszczyńska A.-IPPT PAN
Gradys A. D.-IPPT PAN
Kołbuk-Konieczny D.-IPPT PAN
Zabielski K.-IPPT PAN
Szewczyk P.-other affiliation
Stachewicz U.-AGH University of Science and Technology (PL)
Sajkiewicz P. Ł.-IPPT PAN
2.Zaszczyńska A., Gradys A.D., Ziemiecka A., Szewczyk P., Tymkiewicz R., Lewandowska-Szumieł M., Stachewicz U., Sajkiewicz P.Ł., Enhanced Electroactive Phases of Poly(vinylidene Fluoride) Fibers for Tissue Engineering Applications, International Journal of Molecular Sciences, ISSN: 1422-0067, DOI: 10.3390/ijms25094980, Vol.25, No.9, pp.4980-1-25, 2024
Abstract:

Nanofibrous materials generated through electrospinning have gained significant attention in tissue regeneration, particularly in the domain of bone reconstruction. There is high interest in designing a material resembling bone tissue, and many scientists are trying to create materials applicable to bone tissue engineering with piezoelectricity similar to bone. One of the prospective candidates is highly piezoelectric poly(vinylidene fluoride) (PVDF), which was used for fibrous scaffold formation by electrospinning. In this study, we focused on the effect of PVDF molecular weight (180,000 g/mol and 530,000 g/mol) and process parameters, such as the rotational speed of the collector, applied voltage, and solution flow rate on the properties of the final scaffold. Fourier Transform Infrared Spectroscopy allows for determining the effect of molecular weight and processing parameters on the content of the electroactive phases. It can be concluded that the higher molecular weight of the PVDF and higher collector rotational speed increase nanofibers’ diameter, electroactive phase content, and piezoelectric coefficient. Various electrospinning parameters showed changes in electroactive phase content with the maximum at the applied voltage of 22 kV and flow rate of 0.8 mL/h. Moreover, the cytocompatibility of the scaffolds was confirmed in the culture of human adipose-derived stromal cells with known potential for osteogenic differentiation. Based on the results obtained, it can be concluded that PVDF scaffolds may be taken into account as a tool in bone tissue engineering and are worth further investigation.

Keywords:

scaffolds,polymers,piezoelectricity,bone tissue engineering,nanofibers,regenerative medicine

Affiliations:
Zaszczyńska A.-IPPT PAN
Gradys A.D.-IPPT PAN
Ziemiecka A.-other affiliation
Szewczyk P.-other affiliation
Tymkiewicz R.-IPPT PAN
Lewandowska-Szumieł M.-other affiliation
Stachewicz U.-AGH University of Science and Technology (PL)
Sajkiewicz P.Ł.-IPPT PAN
3.Szewczyk P., Kopacz M., Krysiak Z., Stachewicz U., Oil-Infused Polymer Fiber Membranes as Porous Patches for Long-Term Skin Hydration and Moisturization, Macromolecular Materials and Engineering, ISSN: 1438-7492, DOI: 10.1002/mame.202300291, Vol.309, No.2, pp.2300291-1-8, 2024
Abstract:

Skin allergies and diseases, including atopic dermatitis (AD), affect millions worldwide. Current treatments for AD are often expensive, leading to a need for cost-effective solutions. Here, using fiber-based patches to maintain and increase skin hydration is explored, which helps treat eczema and AD. Nanofiber membranes are manufactured via electrospinning of eight different polymers: nylon 6 (PA6), polyimide (PI), poly(3-hydroxybuty-rate-co-3-hydroxyvalerate (PHBV), poly(l-lactide) (PLLA), polycaprolactone (PCL), and polystyrene (PS), and two molecular weights poly(vinyl butyral-co-vinyl alcohol-co-vinyl acetate) (PVB). Further, their morphology is examined through scanning electron microscopy (SEM), fibers, and pores diameter, wettability, and membrane thickness. Additionally, water vapor transmission rates (WVTR) are measured, and notably, skin hydration tests are conducted before and after using evening primrose oil-infused patches. The comparison and findings highlight the flexibility of electrospun patches, demonstrating their potential in maintaining skin hydration for 6 h and enhancing skin moisture, which are necessary in AD treatment. These insights, which focus on selecting the most effective performance patches, help improve skin moisture, leading to tailored treatments for AD, which can significantly impact the efforts to reduce healthcare costs and simplify skincare steps.

Affiliations:
Szewczyk P.-other affiliation
Kopacz M.-other affiliation
Krysiak Z.-IPPT PAN
Stachewicz U.-AGH University of Science and Technology (PL)
4.Krysiak Z., Stachewicz U., Electrospun fibers as carriers for topical drug delivery and release in skin bandages and patches for atopic dermatitis treatment, WIREs Nanomedicine and Nanobiotechnology, ISSN: 1939-0041, DOI: 10.1002/wnan.1829, Vol.15, No.1, pp.e1829-1-35, 2023
Abstract:

The skin is a complex layer system and the most important barrier between the environment and the organism. In this review, we describe some widespread skin problems, with a focus on eczema, which are affecting more and more people all over the world. Most of treatment methods for atopic dermatitis (AD) are focused on increasing skin moisture and protecting from bacterial infection and external irritation. Topical and transdermal treatments have specific requirements for drug delivery. Breathability, flexibility, good mechanical properties, biocompatibility, and efficacy are important for the patches used for skin. Up to today, electrospun fibers are mostly used for wound dressing. Their properties, however, meet the requirements for skin patches for the treatment of AD. Active agents can be incorporated into fibers by blending, coaxial or side-by-side electrospinning, and also by physical absorption post-processing. Drug release from the electrospun membranes is affected by drug and polymer properties and the technique used to combine them into the patch. We describe in detail the in vitro release mechanisms, parameters affecting the drug transport, and their kinetics, including theoretical approaches. In addition, we present the current research on skin patch design. This review summarizes the current extensive know-how on electrospun fibers as skin drug delivery systems, while underlining the advantages in their prospective use as patches for atopic dermatitis.

This article is categorized under:

Implantable Materials and Surgical Technologies > Nanomaterials and Implants
Implantable Materials and Surgical Technologies > Nanotechnology in Tissue Repair and Replacement
Therapeutic Approaches and Drug Discovery > Emerging Technologies

Keywords:

atopic dermatitis, drug delivery, electrospinning, electrospun fibers, release, skin patches

Affiliations:
Krysiak Z.-IPPT PAN
Stachewicz U.-AGH University of Science and Technology (PL)
5.Krysiak Z., Hamed A., Shweta A., Stachewicz U., Inkjet Printing of Electrodes on Electrospun Micro- and Nanofiber Hydrophobic Membranes for Flexible and Smart Textile Applications, Polymers, ISSN: 2073-4360, DOI: 10.3390/polym14225043, Vol.14, No.22, pp.5043-1-14, 2022
Abstract:

With the increasing demand for smart textile and sensor applications, the interest in printed electronics is rising. In this study, we explore the applicability of electrospun membranes, characterized by high porosity and hydrophobicity, as potential substrates for printed electronics. The two most common inks, silver and carbon, were used in inkjet printing to create a conductive paths on electrospun membranes. As substrates, we selected hydrophobic polymers, such as polyimide (PI), low- and high-molecular-weight poly (vinyl butyral-co-vinyl alcohol-co-vinyl acetate) (PVB) and polystyrene (PS). Electrospinning of PI and PVB resulted in nanofibers in the range of 300–500 nm and PVB and PS microfibers (1–5 μm). The printed patterns were investigated with a scanning electron microscope (SEM) and resistance measurements. To verify the biocompatibility of printed electrodes on the membranes, an indirect cytotoxicity test with cells (MG-63) was performed. In this research, we demonstrated good printability of silver and carbon inks on flexible PI, PVB and PS electrospun membranes, leading to electrodes with excellent conductivity. The cytotoxicity study indicated the possibility of using manufactured printed electronics for various sensors and also as topical wearable devices.

Keywords:

printed electronics, inkjet printing, electrospinning, fibers, hydrophobicity, cells, membrane

Affiliations:
Krysiak Z.-IPPT PAN
Hamed A.-other affiliation
Shweta A.-other affiliation
Stachewicz U.-AGH University of Science and Technology (PL)
6.Krysiak Z., Stachewicz U., Urea-Based Patches with Controlled Release for Potential Atopic Dermatitis Treatment, Pharmaceutics, ISSN: 1999-4923, DOI: 10.3390/pharmaceutics14071494, Vol.14, No.7, pp.1494-1-10, 2022
Abstract:

Skin diseases such as atopic dermatitis (AD) are widespread and affect people all over the world. Current treatments for dry and itchy skin are mostly focused on pharmaceutical solutions, while supportive therapies such as ointments bring immediate relief. Electrospun membranes are commonly used as a drug delivery system, as they have a high surface to volume area, resulting in high loading capacity. Within this study we present the manufacturing strategies of skin patches using polymer membranes with active substances for treating various skin problems. Here, we manufactured the skin patches using electrospun poly(vinyl butyral-co-vinyl alcohol-co-vinyl acetate) (PVB) fibers blended and electrosprayed with urea. The highest cumulative release of urea was obtained from the PVB patches manufactured via blend electrospinning with 5% of the urea incorporated in the fiber. The maximum concentration of released urea was acquired after 30 min, which was followed up by 6 h of constant release level. The simultaneous electrospinning and electrospraying limited the urea deposition and resulted in the lowest urea incorporation followed by the low release level. The urea-based patches, manufactured via blend electrospinning, exhibited a great potential as overnight treatment for various skin problems and their development can bring new trends to the textile-based therapies for AD.

Keywords:

PVB, electrospinning, electrospray, fibers, urea

Affiliations:
Krysiak Z.-other affiliation
Stachewicz U.-AGH University of Science and Technology (PL)
7.Kaniuk Ł., Ferraris S., Spriano S., Luxbacher T., Krysiak Z., Berniak K., Zaszczyńska A., Marzec M.M., Bernasik A., Sajkiewicz P., Stachewicz U., Time-dependent effects on physicochemical and surface properties of PHBV fibers and films in relation to their interactions with fibroblasts, APPLIED SURFACE SCIENCE, ISSN: 0169-4332, DOI: 10.1016/j.apsusc.2021.148983, Vol.545, pp.148983-1-13, 2021
Abstract:

Biodegradability or materials physicochemical stability are the key biomaterials selection parameters for various medical and tissue engineering applications. Poly(3-hydroxybutyrate-co-3-hydroxyvalerate) (PHBV) is a natural copolymer known from its biocompatibility with great support for cells growth and attachment on films and fibers. In our studies, the physicochemical properties of electrospun PHBV fibers and spin-coated films aged for 1, 4 and 8 weeks were analyzed using bulk (FTIR) and surface chemistry (XPS) methods and water contact angle. Further, we characterized the zeta potential changes after aging, by means of electrokinetic measurements, and cell responses to it, using NIH 3T3 murine fibroblasts. Colorimetric MTS cell viability test allowed the assessment of cell proliferation. Additionally, the morphology of fibroblasts and biointerfaces were studied by confocal laser and electron scanning microscopy (CLSM and SEM). These studies indicated that the activity, attachment and proliferation of fibroblasts is independent of aging of PHBV fibers and films. PHBV films show very stable zeta potential over 8 weeks of aging, opposite to PHBV fibers. Importantly, the flat film of PHBV increases cell proliferation, while the fibrous meshes are an excellent support for their stretching. The results of the study revealed clear advantages of PHBV films and fibrous meshes in cell-material interaction.

Keywords:

cell morphology, fibroblast, electrospun fibers, PHBV, Zeta potential

Affiliations:
Kaniuk Ł.-other affiliation
Ferraris S.-other affiliation
Spriano S.-other affiliation
Luxbacher T.-other affiliation
Krysiak Z.-other affiliation
Berniak K.-other affiliation
Zaszczyńska A.-IPPT PAN
Marzec M.M.-other affiliation
Bernasik A.-other affiliation
Sajkiewicz P.-IPPT PAN
Stachewicz U.-AGH University of Science and Technology (PL)
8.Szewczyk P.K., Gradys A., Kyun Kim S., Persano L., Marzec M., Kryshtal A., Busolo T., Toncelli A., Pisignano D., Bernasik A., Kar-Narayan S., Sajkiewicz P., Stachewicz U., Enhanced piezoelectricity of electrospun polyvinylidene fluoride fibers for energy harvesting, ACS Applied Materials and Interfaces, ISSN: 1944-8244, DOI: 10.1021/acsami.0c02578, Vol.12, No.11, pp.13575-13583, 2020
Abstract:

Piezoelectric polymers are promising energy materials for wearable and implantable applications for replacing bulky batteries in small and flexible electronics. Therefore, many research studies are focused on understanding the behavior of polymers at a molecular level and designing new polymer-based generators using polyvinylidene fluoride (PVDF). In this work, we investigated the influence of voltage polarity and ambient relative humidity in electrospinning of PVDF for energy-harvesting applications. A multitechnique approach combining microscopy and spectroscopy was used to study the content of the β-phase and piezoelectric properties of PVDF fibers. We shed new light on β-phase crystallization in electrospun PVDF and showed the enhanced piezoelectric response of the PVDF fiber-based generator produced with the negative voltage polarity at a relative humidity of 60%. Above all, we proved that not only crystallinity but also surface chemistry is crucial for improving piezoelectric performance in PVDF fibers. Controlling relative humidity and voltage polarity increased the d33 piezoelectric coefficient for PVDF fibers by more than three times and allowed us to generate a power density of 0.6 μW·cm^–2 from PVDF membranes. This study showed that the electrospinning technique can be used as a single-step process for obtaining a vast spectrum of PVDF fibers exhibiting different physicochemical properties with β-phase crystallinity reaching up to 74%. The humidity and voltage polarity are critical factors in respect of chemistry of the material on piezoelectricity of PVDF fibers, which establishes a novel route to engineer materials for energy-harvesting and sensing applications.

Keywords:

PVDF, polymer crystallinity, electrospinning, piezoelectricity, voltage polarity

Affiliations:
Szewczyk P.K.-other affiliation
Gradys A.-IPPT PAN
Kyun Kim S.-other affiliation
Persano L.-other affiliation
Marzec M.-other affiliation
Kryshtal A.-other affiliation
Busolo T.-other affiliation
Toncelli A.-other affiliation
Pisignano D.-other affiliation
Bernasik A.-other affiliation
Kar-Narayan S.-other affiliation
Sajkiewicz P.-IPPT PAN
Stachewicz U.-AGH University of Science and Technology (PL)
9.Ura D.P., Rosell-Llompart J., Zaszczyńska A., Vasilyev G., Gradys A., Szewczyk P.K., Knapczyk-Korczak J., Avrahami R., Šišková A.O., Arinstein A., Sajkiewicz P., Zussman E., Stachewicz U., The role of electrical polarity in electrospinning and on the mechanical and structural properties of as-spun fibers, Materials, ISSN: 1996-1944, DOI: 10.3390/ma13184169, Vol.13, No.18, pp.4169-1-18, 2020
Abstract:

Electric field strength and polarity in electrospinning processes and their effect on process dynamics and the physical properties of as-spun fibers is studied. Using a solution of the neutral polymer such as poly(methyl methacrylate) (PMMA) we explored the electrospun jet motion issued from a Taylor cone. We focused on the straight jet section up to the incipient stage of the bending instability and on the radius of the disk of the fibers deposited on the collecting electrode. A new correlation formula using dimensionless parameters was found, characterizing the effect of the electric field on the length of the straight jet, L˜E~E˜0.55. This correlation was found to be valid when the spinneret was either negatively or positively charged and the electrode grounded. The fiber deposition radius was found to be independent of the electric field strength and polarity. When the spinneret was negatively charged, L˜E was longer, the as-spun fibers were wider. The positively charged setup resulted in fibers with enhanced mechanical properties and higher crystallinity. This work demonstrates that often-overlooked electrical polarity and field strength parameters influence the dynamics of fiber electrospinning, which is crucial for designing polymer fiber properties and optimizing their collection.

Keywords:

fibers, electrical polarity, charges, electrospinning, PMMA, mechanical properties

Affiliations:
Ura D.P.-AGH University of Science and Technology (PL)
Rosell-Llompart J.-other affiliation
Zaszczyńska A.-IPPT PAN
Vasilyev G.-Technion-Israel Institute of Technology (IL)
Gradys A.-IPPT PAN
Szewczyk P.K.-other affiliation
Knapczyk-Korczak J.-other affiliation
Avrahami R.-other affiliation
Šišková A.O.-other affiliation
Arinstein A.-Technion-Israel Institute of Technology (IL)
Sajkiewicz P.-IPPT PAN
Zussman E.-Technion-Israel Institute of Technology (IL)
Stachewicz U.-AGH University of Science and Technology (PL)

Conference abstracts
1.Ura D.P., Gradys A., Zaszczyńska A., Sajkiewicz P., Stachewicz U., Controlling of mechanical properties of electrospun PMMA fibers via voltage polarity, 7th Dresden Nanoanalysis Symposium: Nano-scale characterization for cutting-edge materials research and sustainable materials development, 2019-08-30/08-30, Dresden (DE), pp.1-2, 2019
2.Ura D.P., Gradys A., Zaszczyńska A., Sajkiewicz P., Stachewicz U., Controlling of mechanical properties of electrospun PMMA fibers via voltage polarity, 8th International PhD Meeting, 2019-08-28/08-29, Dresden (DE), pp.1, 2019
3.Ura P.D., Zaszczyńska A., Gradys A., Sajkiewicz P., Stachewicz U., Mechanical properties of electrospun non-woven PMMA mats produced with positive and negative voltage polarities, AMT 2019, XXII Physical Metallurgy and Materials Science Conference: Advanced Materials and Technologies, 2019-06-09/06-12, Bukowina Tatrzańska (PL), pp.1, 2019
4.Ura D.P., Gradys A., Zaszczyńska A., Sajkiewicz P., Stachewicz U., Effect of voltage polarity on mechanical properties of electrospun PMMA fibers, Frontiers in Polymer Science, 2019-05-05/05-08, Budapest (HU), pp.1-2, 2019