TY - JOUR

T1 - 3D printed and stimulus responsive drug delivery systems based on synthetic polyelectrolyte hydrogels manufactured via digital light processing

AU - Vaupel, Sonja

AU - Mau, Robert

AU - Kara, Selin

AU - Seitz, Hermann

AU - Kragl, Udo

AU - Meyer, Johanna

N1 - Funding Information: SV, RM, SH, UK, and JM thank the Bundesministerium für Bildung und Forschung (BMBF, Federal Ministry of Education and Research) within “Zwanzig20” (Response), grant number: 03ZZ0933L. SK and JM thank the Ministry for Science and Culture for Lower Saxony for the Holen & Halten starting grant (grant no 12.5-76251-17-9/20). We want to thank Sandra Diederich, Tom Kunde, Martina Weiß, Caroline Mueller, and Laura Schmitz, for their support in the daily laboratory routine and their help with the HPLC analytics. Furthermore, we thank Sven Barker for his help with the SEM images and David Knebel for his skillful assistance with the mechanical characterization. And most of all, we would like to thank the people who worked in systemically important jobs throughout all the lockdowns and got us through the last years of the pandemic.

PY - 2023

Y1 - 2023

N2 - Hydrogels are three-dimensional hydrophilic polymeric networks absorbing up to and even more than 90 wt% of water. These superabsorbent polymers retain their shape during the swelling process while enlarging their volume and mass. In addition to their swelling behavior, hydrogels can possess other interesting properties, such as biocompatibility, good rheological behavior, or even antimicrobial activity. This versatility qualifies hydrogels for many medical applications, especially drug delivery systems. As recently shown, polyelectrolyte-based hydrogels offer beneficial properties for long-term and stimulus-responsive applications. However, the fabrication of complex structures and shapes can be difficult to achieve with common polymerization methods. This obstacle can be overcome by the use of additive manufacturing. 3D printing technology is gaining more and more attention as a method of producing materials for biomedical applications and medical devices. Photopolymerizing 3D printing methods offer superior resolution and high control of the photopolymerization process, allowing the fabrication of complex and customizable designs while being less wasteful. In this work, novel synthetic hydrogels, consisting of [2-(acryloyloxy) ethyl]trimethylammonium chloride (AETMA) as an electrolyte monomer and poly(ethylene glycol)-diacrylate (PEGDA) as a crosslinker, 3D printed via Digital Light Processing (DLP) using a layer height of 100 μm, are reported. The hydrogels obtained showed a high swelling degree q ∞ m,t ∼ 12 (24 h in PBS; pH 7; 37 °C) and adjustable mechanical properties with high stretchability (ϵ max ∼ 300%). Additionally, we embedded the model drug acetylsalicylic acid (ASA) and investigated its stimulus-responsive drug release behaviour in different release media. The stimulus responsiveness of the hydrogels is mirrored in their release behavior and could be exploited in triggered as well as sequential release studies, demonstrating a clear ion exchange behavior. The received 3D-printed drug depots could also be printed in complex hollow geometry, exemplarily demonstrated via an individualized frontal neo-ostium implant prototype. Consequently, a drug-releasing, flexible, and swellable material was obtained, combining the best of both worlds: the properties of hydrogels and the ability to print complex shapes.

AB - Hydrogels are three-dimensional hydrophilic polymeric networks absorbing up to and even more than 90 wt% of water. These superabsorbent polymers retain their shape during the swelling process while enlarging their volume and mass. In addition to their swelling behavior, hydrogels can possess other interesting properties, such as biocompatibility, good rheological behavior, or even antimicrobial activity. This versatility qualifies hydrogels for many medical applications, especially drug delivery systems. As recently shown, polyelectrolyte-based hydrogels offer beneficial properties for long-term and stimulus-responsive applications. However, the fabrication of complex structures and shapes can be difficult to achieve with common polymerization methods. This obstacle can be overcome by the use of additive manufacturing. 3D printing technology is gaining more and more attention as a method of producing materials for biomedical applications and medical devices. Photopolymerizing 3D printing methods offer superior resolution and high control of the photopolymerization process, allowing the fabrication of complex and customizable designs while being less wasteful. In this work, novel synthetic hydrogels, consisting of [2-(acryloyloxy) ethyl]trimethylammonium chloride (AETMA) as an electrolyte monomer and poly(ethylene glycol)-diacrylate (PEGDA) as a crosslinker, 3D printed via Digital Light Processing (DLP) using a layer height of 100 μm, are reported. The hydrogels obtained showed a high swelling degree q ∞ m,t ∼ 12 (24 h in PBS; pH 7; 37 °C) and adjustable mechanical properties with high stretchability (ϵ max ∼ 300%). Additionally, we embedded the model drug acetylsalicylic acid (ASA) and investigated its stimulus-responsive drug release behaviour in different release media. The stimulus responsiveness of the hydrogels is mirrored in their release behavior and could be exploited in triggered as well as sequential release studies, demonstrating a clear ion exchange behavior. The received 3D-printed drug depots could also be printed in complex hollow geometry, exemplarily demonstrated via an individualized frontal neo-ostium implant prototype. Consequently, a drug-releasing, flexible, and swellable material was obtained, combining the best of both worlds: the properties of hydrogels and the ability to print complex shapes.

UR - http://www.scopus.com/inward/record.url?scp=85163636253&partnerID=8YFLogxK

U2 - 10.1039/d3tb00285c

DO - 10.1039/d3tb00285c

M3 - Article

VL - 11

SP - 6547

EP - 6559

JO - Journal of Materials Chemistry B

JF - Journal of Materials Chemistry B

SN - 2050-7518

IS - 28

ER -