Biocatalysis is an established chemical synthesis technology that has by no means been restricted to research laboratories. The use of enzymes for organic synthesis has evolved greatly from early development to proof‐of‐concept – from small batch production to industrial scale. Different enzyme immobilization strategies contributed to this success story. Recently, the use of hydrogel materials for the immobilization of enzymes has been attracting great interest. Within this review, we pay special attention to recent developments in this key emerging field of research. Firstly, we will briefly introduce the concepts of both biocatalysis and hydrogel worlds. Then, we list recent interesting publications that link both concepts. Finally, we provide an outlook and comment on future perspectives of further exploration of enzyme immobilization strategies in hydrogels.

Polymers are commonly used in medical device manufacturing, e.g. for drug delivery systems, bone substitutes and stent coatings. Especially hydrogels exhibit very promising properties in this field. Hence, the development of new hydrogel systems for customized application is of great interest, especially regarding the swelling behavior and mechanical properties as well as the biocompatibility. The aim of this work was the preparation and investigation of various polyelectrolyte and poly-ionic liquid based hydrogels accessible by radical polymerization. The obtained polymers were covalently crosslinked with N,Nʼ-methylenebisacrylamide (MBAA) or different lengths of poly(ethyleneglycol)diacrylate (PEGDA). The effect of different crosslinker-to-monomer ratios has been examined. In addition to the compression curves and the maximum degree of swelling, the biocompatibility with L929 mouse fibroblasts of these materials was determined in direct cell seeding experiments and the outcome for the different hydrogels was compared.

In this work ion functionalized hydrogels as potent drug delivery systems are presented. The ion functionalization of the hydrogel enables the retention of ionic drug molecules and thus a reduction of burst release effects. Timolol maleate in combination with polymerized anionic 3‐sulfopropylmethacrylate potassium and ibuprofen combined with cationic poly‐[2‐(methacryloyloxy)ethyl] trimethylammonium chloride are investigated in respect to their drug release profile. The results are showing an ion exchange depending release behavior instead of a diffusion‐controlled drug release as it is known from common drug delivery systems. Furthermore, the suitability of such hydrogels for standard methods for sterilization is investigated.

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.

Hydrogels have become an increasingly interesting topic in numerous fields of application. In addition to their use as immobilization matrixes in (bio)catalysis, they are widely used in the medical sector, e.g., in drug delivery systems, contact lenses, biosensors, electrodes, and tissue engineering. Cartilage tissue engineering hydrogels from natural origins, such as collagen, hyaluronic acid, and gelatin, are widely known for their good biocompatibility. However, they often lack stability, reproducibility, and mechanical strength. Synthetic hydrogels, on the other hand, can have the advantage of tunable swelling and mechanical properties, as well as good reproducibility and lower costs. In this study, we investigated the swelling and mechanical properties of synthetic polyelectrolyte hydrogels. The resulting characteristics such as swelling degree, stiffness, stress, as well as stress-relaxation and cyclic loading behavior, were compared to a commercially available biomaterial, the ChondroFiller^® liquid, which is already used to treat articular cartilage lesions. Worth mentioning are the observed good reproducibility and high mechanical strength of the synthetic hydrogels. We managed to synthesize hydrogels with a wide range of compressive moduli from 2.5 ± 0.1 to 1708.7 ± 67.7 kPa, which addresses the span of human articular cartilage.