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Abstract Bioelectronics holds great potential as therapeutics, but introducing conductive structures within the body poses great challenges. While implanted rigid and substrate‐bound electrodes often result in inflammation and scarring in vivo, they outperform the in situ‐formed, more biocompatible electrodes by providing superior control over electrode geometry. For example, one of the most researched methodologies, the formation of conductive polymers through enzymatic catalysis in vivo, is governed by diffusion control due to the slow kinetics, with curing times that span several hours to days. Herein, the discovery of the formation of biocompatible conductive structures through photopolymerization in vivo, enabling spatial control of electrode patterns is reported. The process involves photopolymerizing novel photoactive monomers, 3Es (EDOT‐trimers) alone and in a mixture to cure the poly(3, 4‐ethylenedioxythiophene)butoxy‐1‐sulfonate (PEDOT‐S) derivative A5, resulting in conductive structures defined by photolithography masks. These reactions are adapted to in vivo conditions using green and red lights, with short curing times of 5–30 min. In contrast to the basic electrode structures formed through other in situ methods, the formation of specific and layered patterns is shown. This opens up the creation of more complex 3D layers‐on‐layer circuits in vivo.

Abstract The purpose of this work is to explore the properties of the lignin-derived amine-free photoinitiating systems (PISs) during the curing process. Four novel hydrogen donors (HD1, HD2, HD3, and HD4) derived from lignin α-O-4 structural were designed and synthesized by simple methods, and their low C–H bond dissociation energies on methylene were determined by molecular orbitals theory. Four experimental groups using CQ (camphorquinone)/HD PIs formulated with Bis-GMA/TEGDMA (70 w%/30 w%) were compared to CQ/EDB (ethyl 4-dimethylamino benzoate) system. The photopolymerization profiles and double bond conversion rate was tracked by FTIR experiments; the color bleaching ability of the samples and color aging test assay were performed using color indexes measurements; The cytotoxicity of the samples was also compared to EDB related systems. All of the experimental groups with new HDs were compared to the control group with EDB by statistical analysis. Compared to CQ/EDB system, new lignin-derived hydrogen donors combined with CQ showed comparable or even better performances in polymerization initiation to form resin samples, under a blue dental LED in air. Excellent color bleaching property was observed with the new HDs. Aging tests and cytotoxicity examination of the resin were performed, indicating the new lignin compounds to be efficient hydrogen donors for amine-free CQ-based photo-initiating system. Novel lignin α-O-4 derived hydrogen donors are promising for further usage in light-curing materials.

The additive manufacturing route is a notably promising alternative option to obtain complex shaped parts, precise prototypes, and direct-usage system components for lots of independent sectors like medicine, dentistry, automotive, aviation, and construction. Compared to the conventional strategies, this methodology provides cleaner, healthier, and faster manufacturing opportunities for engineers and manufacturers. In this paper, actual applications of photopolymerization-oriented 3D printing in the field of dentistry are evaluated in light of the literature efforts, sectoral feedback, and additional original interpretations. Concordantly, the process backgrounds and printing materials were analyzed meticulously together with the evaluations of the physical and mechanical features of the dental components. When real implementations like models, surgical guides, aligners, temporary teeth, and implants are considered, it is seen that there is still a lot of room to be enlightened on this topic for a healthier future. In this context, this article aims to draw a broad perspective on the new interdisciplinary efforts and to emphasize the great potential of layer-by-layer production in the field of dentistry.

Abstract Inspired by natural wrinkled surfaces, artificial surfaces with biomimetic wrinkled structures have been widely used to improve optical properties, wettability, and antibacterial properties. However, the preparation of wrinkled structures has the disadvantages of long-time consumption and complex processes. Herein, we prepared a self-wrinkling polyurethane-acrylate (PUA) wood coating via biomimetic self-wrinkling patterns by using a light-emitting diode (LED)/excimer/mercury lamp curing system, which was capable of self-matting, anti-fingerprint and skin-tactile performance. By adjusting the irradiation intensity in the curing system, the wavelength (λ) and amplitude (A) of wrinkles on the coating surface were controlled to enhance the coating performance. After curing by the LED, excimer, and mercury lamps at energy intensities of 500, 30, and 300 mW/cm2 respectively, the self-wrinkling coating showed excellent surface performance. The self-wrinkling coating represented low gloss of 4.1 GU at 85°, high hardness of 4H. Interestingly, the coating surface had a high hydrophobicity (104.5°) and low surface energy (29–30 mN/m) and low coefficient (COF) of friction (0.1–0.2), which were consistent with those of the human skin surface. Besides, the wrinkled structure also improved the thermal stability of the coating samples. This study provided a promising technique for the mass production of self-wrinkling coatings that could be used in wood-based panels, furniture, and leather.

Abstract Polymerization in the solid state is generally infeasible due to restrictions on mobility. However, in this work, the solid‐state photopolymerization of crystalline dicyclopentadiene is demonstrated via photoinitiated ring‐opening metathesis polymerization. The source of mobility in the solid state is attributed to the plastic crystal nature of dicyclopentadiene, which yields local short‐range mobility due to orientational degrees of freedom. Polymerization in the solid state enables photopatterning, volumetric additive manufacturing of free‐standing structures, and fabrication with embedded components. Solid‐state photopolymerization of dicyclopentadiene offers a new paradigm for advanced and freeform fabrication of high‐performance thermosets.

Additive manufacturing techniques have gone beyond their reputation for rapid prototype production and are increasingly adopted for the manufacture of functional components comprising high-end materials and intricate lattice structures. Silicon nitride, renowned for its exceptional mechanical properties and thermal stability, has emerged as a promising candidate for lightweight structural applications. Nonetheless, its high refractive index and density have limited the fabrication of highly complex structures using extrusion and photopolymerization based techniques. In this work, a highly reactive silicon nitride-based ink with high solid loading is developed for the fabrication of ultra-lightweight, truss-based structures. By employing a robot UV-assisted direct ink writing process, it is possible to control the printing head orientation, thus overcoming the limited curing depth of silicon nitride-based inks. The failure behavior of the sintered lattice beam structures under 4-point bending loading has been modeled by applying a linear elastic fracture mechanics (LEFM) based approach to the results of finite element (FE) simulations.

This study evaluated the potential of gelatin methacryloyl (GelMA) for single-cell screening compared to polyethylene glycol diacrylate (PEGDA). GelMA photopolymerized at 1000–2000 mJ/cm2 produced consistent patterns and supported HeLa cell viability. GelMA (5%w/v) facilitated better cell collection within 2 days due to its shape retention. GelMA demonstrated biocompatibility with HeLa cells exhibiting exponential proliferation and biodegradation over 5 days. The average cell displacement over 2 days was 16 µm. Two targeted cell recovery strategies using trypsin were developed: one for adherent cells encapsulated at 800 mJ/cm2, and another for floating cells encapsulated at 800 mJ/cm2, enabling the selective removal of unwanted cells. These findings suggest GelMA as a promising biomaterial for single-cell screening applications, offering advantages over PEGDA in cell encapsulation and targeted recovery.

Microlenses or arrays are key elements in many applications. However, their construction methods involve multiple fabrication processes, thereby increasing the complexity and cost of fabrication. In this study, we demonstrate an optically anisotropic, electrically tunable liquid crystal (LC) microlens array using a simple, one-step fabrication method. The microlens array is formed via photopolymerization-induced phase separation inside a polymer/LC composite. It possesses both polarization-dependent and electrically tunable focusing and imaging properties. Without applying voltage, the microlens array has a natural focal length of 8 mm, which is a result of its inherent gradient refractive index profile. Upon applying voltage above the threshold, the LC molecules reorient along the electric field direction and the focal length of the microlens array gradually increases. Based on its superior properties, the microlens array is further used for integral imaging applications, demonstrating electrically tunable central depth plane. Such LC microlens arrays could find numerous potential applications owing to their advantageous features of being flat, ultra-thin, and tunable, including 3D displays, optical interconnects, and more.

Abstract To facilitate the ongoing transition toward a circular economy, renewable 3D print materials that are both sustainable and competitive must be accessible. However, the growing demand for bio‐based thermosetting resins, which are used as ink for vat photopolymerization, gives rise to environmental concerns in terms of plastic waste management. Therefore, photocurable materials that are renewable and recyclable at the same time are needed. In this work, a mechanically robust and reprocessable 3D printed photopolymer is developed from renewable feedstock. Reaction of malic acid with glycidyl methacrylate introduces both methacrylate moieties that can undergo photopolymerization in the 3D printer, and β‐hydroxyester linkages that can act as dynamic crosslinks via bond exchange reactions. By combining modified malic acid with reactive diluents, a photoinitiator, and phosphate catalyst, three distinct resins are formulated, resulting in bio‐based contents ranging from 43% to 49%. The formulations demonstrate good layer fusion and accurate print quality, while the 3D printed specimens are robust and thermally stable. Notably, the printed object with shortest relaxation time displayed Arrhenius flow behavior with an activation energy of 36.0 kJ mol−1, and its mechanical performance is maintained after being recycled three times. This contributes to the end‐of‐life perspective of photocurable resins in additive manufacturing.

In this work, we developed and analyzed a biphasic calcium phosphate (BCP) bioceramic for bone regeneration using stereolithography (SLA). The SLA method is a promising additive manufacturing (AM) technique capable of creating BCp parts with high accuracy and efficiency. However, the ceramic suspension used in SLA exhibits significantly higher viscosity and is not environmentally friendly. Therefore, adequate preparation of a suspension with low viscosity and high solid loading is essential. In this paper, we optimized the effects of surfactant doses and solid loading on the BCp slurry, and initially examined the process parameters of photocuring, debinding, and sintering. The utilization of 9 wt % Disperbyk (BYK) with a 40 vol % loading of BCp bioceramics exhibited a reasonably low viscosity of 8.9 mPa·s at a shear level of 46.5 s−1. Functional and structural analyses confirmed that BCp was retained after photocuring and subsequent treatment, which were incorporated into the BYK dispersion. The 3D printed objects with different sintered temperatures, specifically at 1100 °C, 1200 °C, and 1300 °C, were further optimized. Additionally, the surface roughness, porosity, and mechanical properties of BCp green parts were systematically investigated. Most importantly, in vitro analysis of cell attachment, differentiation, and red alizarin analysis could support the application of bone regeneration.

Approaches aiming to recover proteins without denaturation represent attractive strategies. To accomplish this, a membrane lysis agent based on poly(styrene-alt-maleic acid) or PSMA was synthesized by photopolymerization using Irgacure® 2959 and carbon tetrabromide (CBr4) as a radical initiator and a reversible chain transfer agent, respectively. Structural elucidation of our in-house synthesized PSMA, so-called photo-PSMA, was performed by using NMR spectroscopy. The use of this photo-PSMA in soybean enzyme extraction was also demonstrated for the first time in this study. Without a severe cell rupture, energy input or any organic solvent, recovery of lipolytic enzymes directly into nanometric-sized particles was accomplished in one-step process. Due to the improved structural regularity along the photo-PSMA backbone, the most effective protective reservoir for enzyme immobilization was generated through the PSMA aggregation. Formation of such reservoir enabled soybean enzymes to be shielded from the surroundings and resolved in their full functioning state. This was convinced by the increased specific lipolytic activity to 1,950 mU/mg, significantly higher than those of sodium dodecyl sulfate (SDS) and the two commercially-available PSMA sources (1000P and 2000P). Our photo-PSMA had thus demonstrated its great potential for cell lyse application, especially for soybean hydrolase extraction.

The process of additive manufacturing (AM), commonly known as 3D printing, is a method of constructing a component by progressively adding material in layers using digital 3D design information. As part of 'Industry 4.0,' many industrial technologies are rapidly increasing to thrive in the twenty-first century. This study goes over seven different types of additive manufacturing in great detail. These technologies make it possible to make complex, high-value parts quickly and in small quantities without using as much energy or material or making as many tools as subtractive manufacturing does. Besides, AM also possesses some particular challenges, like post-processing, material unavailability, software issues, etc. The application of AM is expanding rapidly from micro to macro-scale sectors. 3D printing technology will change industrial operations in the following years. Eventually, the elected technology will be closely related to the proposed function.

DOI: 10.26456/pcascnn/2023.15.1029 Abstract: In this paper we investigate the changes in the surface topology of inorganic polymer-derived films resulted from photostimulated polymerization. With the use of the atomic-force microscopy, the surface structure changes of mixed molybdenum-vanadium oxide thin films (V2O5:MoO3 = 3:2) resulted from the UV light-induced polymerization was investigated. The analysis of atomic-force images evidenced that the solid-state polymerization in the mixed oxide films obtained by condensation of corresponding oxoacids occurs through 3D mechanism. As the result of exposure, MoO3/V2O5 films lose the intrinsic anisotropy which is due to the directional agglomeration of belt-like mixed oxide oligomers. The photopolymerization processes in the mixed oxide film yield agglomerates of nuclei built from the faceted nanometer-sized pseudocrystallites. The exposure is also accompanied with solid-state recrystallization of initially amorphous oxide resulting in the rougher relief of the exposed film. The selective acidic etching uncovers the latent structure of the film, this etching being accompanied with pseudocrystallite dispergation that results in the smoothing of the microrelief of the oxide film surface. These structural features of photosensitive mixed oxide MoO3/V2O5 films facilitate their application as the inorganic photoresists.

The design of biosourced and/or bioinspired photoinitiators is an active research field as it offers a unique opportunity to develop photoinitiating systems exhibiting better biocompatibility as well as reduced toxicity. In this field, flavonoids can be found in numerous fruits and vegetables so these structures can be of interest for developing, in the future, polymerization processes, offering a reduced environmental impact but also better biocompatibility of the polymers. In this review, the different flavonoids reported to date as photoinitiators of polymerization are presented. Over the years, different modifications of the flavonoid scaffold have been examined including the grafting of well-known chromophores, the preparation of Type II photoinitiators or the introduction of photocleavable groups enabling the generation of Type I photoinitiators. Different families of flavonoids have also been investigated, enabling to design of high-performance photoinitiating systems.

This study investigates the synthesis, characterization, and antimicrobial properties of hydrogels synthesized through the UV-pulsed laser photopolymerization of a polymer–photoinitiator–chlorpromazine mixture. Chlorpromazine was used for its known enhanced antimicrobial properties when exposed to UV laser radiation. The hydrogel was formed from a mixture containing 0.05% Irgacure 2959, 10% gelatin methacryloyl, and various concentrations of chlorpromazine (1, 2, and 4 mg/mL). Laser-induced fluorescence spectroscopy was employed to monitor the photoinduced changes of chlorpromazine and Irgacure 2959 during hydrogel formation, providing insight into the photodegradation dynamics. FTIR spectroscopy confirmed the incorporation of irradiated chlorpromazine within the hydrogel matrix, while the release profiles of chlorpromazine showed sustained release only in hydrogels containing 1 mg/mL of CPZ. The hydrogel showed significant antimicrobial activity against MRSA bacteria when compared to that of penicillin. These findings highlight the potential of CPZ loaded during the photopolymerization process into hydrogels as effective antimicrobial agents with sustained release properties, making them suitable for combating resistant bacterial strains.

As the metal additive manufacturing (AM) field evolves with an increasing demand for highly complex and customizable products, there is a critical need to close the gap in productivity between metal AM and traditional manufacturing (TM) processes such as continuous casting, machining, etc., designed for mass production. This paper presents the development of the scalable and expeditious additive manufacturing (SEAM) process, which hybridizes binder jet printing and stereolithography principles, and capitalizes on their advantages to improve productivity. The proposed SEAM process was applied to stainless steel 420 (SS420) and the processing conditions (green part printing, debinding, and sintering) were optimized. Finally, an SS420 turbine fabricated using these conditions successfully reached a relative density of 99.7%. The SEAM process is not only suitable for a high-volume production environment but is also capable of fabricating components with excellent accuracy and resolution. Once fully developed, the process is well-suited to bridge the productivity gap between metal AM and TM processes, making it an attractive candidate for further development and future commercialization as a feasible solution to high-volume production AM.

Photopolymerization is becoming increasingly popular in industry due to its copious advantages. The vital factor in the entire pre-polymerization formulation is the presence of photoinitiators. Depending on the application, photoinitiators have different features. Hence, scientists are particularly interested in developing new photoinitiators that can expand the scope of applications and be used to create products with the features demanded by current trends. This brief review summarizes the photoinitiators used in dental materials and hydrogels and those obtained from natural and synthetic sources.

One of the most challenging issues in DLP 3D printing is separation. Thus, the capability to employ a variety of polymer membranes can considerably aid in the development of the DLP technology. The primary purpose of this study is to thoroughly explore the characteristics influencing separation force and time on the FEP industrial membrane and the proposed PP membrane. Therefore, the impact of image cross section geometry and separation speed on separation force and separation time is investigated. As a consequence, changing the percentage of surface porosity has a negligible effect on the amount of separation force. According to the findings, reducing the cross-sectional area by 1.36% reduced the separation force by 6.5 times. Moreover, the outcomes are consistent with the mathematical model given. the separation force rose by 230% in the FEP membrane with an increase of 96 times of the speed, whereas the separation time decreased by 18.8 times. For the proposed PP membrane, as the speed increases, the separation force rate increases by 175% and the separation time falls by 29.6 times. The aforementioned findings show that the PP film may be used as a practical and affordable solution with quick separation that can reduce printing time when producing three-dimensional lattice pieces at varying speeds.

We present an enhanced methodology for the synthesis of graphene, from photo-polymerized self-assembled monolayers (SAMs) of 1,1ʹ-biphenyl-4-thiol on both electropolished and oxidized copper substrates. The SAMs were subjected to a two-step process involving light-induced polymerization followed by annealing in a vacuum furnace to yield the two-dimensional solid. Comprehensive characterization using contact angle measurements, X-ray photoelectron spectroscopy, and Raman spectroscopy, as well as scanning electron and transmission electron microscopy, provided conclusive evidence of growth of single-layer graphene. Notably, our findings revealed superior quality graphene on oxidized copper substrates compared to their electropolished counterparts, highlighting the impact of substrate choice on the quality of the resultant material.

Abstract The first aim of this study is to develop a photo‐ATRP process using methyl methacrylate (MMA) by employing a novel perylenediimide derivative (PDI) as photoinitiator. The analysis of the MMA photopolymerization process kinetics is performed in solution and in bulk, demonstrating control over the reaction progress even if the polymerizations display a slow initiation step. The photo‐ATRP process for MMA in suspension is also developed and the obtained PMMA particles are further used to reinitiate the ATRP polymerization of thermoresponsive polymers (different molecular weights poly(ethylene glycol) methyl ether methacrylate and poly(N‐isopropylacrylamide)) (PNIPAM) in solution and surface‐initiated processes. The synthesized polymers by surface‐initiated process display a bimodal molecular weight distribution with a clear modification of the signal areas ratio depending on the grafted monomer and on the reaction conditions. The grafting process can take place on the surface of the polymer particles (Mn2), or it can also involve polymer chains located further at the interior of the polymer particles (Mn1). The lower critical solution temperature (LCST) transition is demonstrated for the PNIPAM functionalized polymer particles.

UV-activated catalytic hydrosilation is a low-temperature crosslinking process that has attracted attention for its high efficiency and lower energy demand relative to thermal curing. In this study, formulations comprising industrially relevant model silanes and Pt photocatalysts trimethyl(methylcyclopentadienyl)platinum(IV) and trimethyl(pentamethylcyclopentadienyl)platinum(IV) (MeCpPtMe3 and Cp*PtMe3, respectively) were prepared with and without a photosensitizer (PS) and assessed for catalytic performance by a novel strategy. Photopolymerizations were initiated using different wavelengths from LEDs and monitored in real-time using an Attenuated Total Reflectance-Fourier Transform Infrared (ATR-FTIR) “well” strategy to track the degree of cure in ultra-thin films by consumption of hydride via the disappearance of the Si-H bending absorption band at 915 cm−1. Irradiation of formulations with 365 nm excitation showed higher conversions relative to 400 nm light and improvements to calculated initial reaction rates by incorporation of a PS suggested increased sensitization to 365 nm irradiation. To the best of our knowledge, this is the first study to report catalytic performance, electronic absorption spectroscopic data, and the crystal structure of Cp*PtMe3.

Three-dimensional (3D) printing or Additive Manufacturing (AM) technology is an innovative tool with great potential and diverse applications in various fields. As 3D printing has been burgeoning in recent times, a tremendous transformation can be envisaged in medical care, especially the manufacturing procedures leading to personalized medicine. Stereolithography (SLA), a vat-photopolymerization technique, that uses a laser beam, is known for its ability to fabricate complex 3D structures ranging from micron-size needles to life-size organs, because of its high resolution, precision, accuracy, and speed. This review presents a glimpse of varied 3D printing techniques, mainly expounding SLA in terms of the materials used, the orientation of printing, and the working mechanisms. The previous works that focused on developing pharmaceutical dosage forms, drug-eluting devices, and tissue scaffolds are presented in this paper, followed by the challenges associated with SLA from an industrial and regulatory perspective. Due to its excellent advantages, this technology could transform the conventional “one dose fits all” concept to bring digitalized patient-centric medication into reality.

Large and deterministic 3D structures with nanoscale features and porosities are valuable for various applications but are challenging to print due to the proximity effects that lead to the merging of adjacently printed features. Here, this challenge has been overcome by minimising the proximity effects in projection two-photon lithography (P-TPL), which is a high-throughput photopolymerization-based 3D printing technique. Through empirical studies and physics-based computational models, it is demonstrated that the proximity effects arise from distinct optical and chemical sources. Processing conditions that individually minimise these sources have been identified. These insights have been leveraged to generate an interspersing P-TPL technique capable of rapidly printing 3D structures with features smaller than 300 nm, pores finer than 700 nm, and at rates greater than 0.5 mm2/s per layer. As interspersing P-TPL is up to 50 times faster than conventional point-scanning TPL, it can enable the scalable printing of nanoporous 3D structures.

Ionic liquids (ILs) are materials with fascinating preorganized and programmable solvent structures and distinctive physicochemical features. ILs have recently been used to create polymeric materials with customized sizes, dimensionalities, morphologies, and functions that are challenging to obtain when using common organic solvents. ILs are individual macromolecules that contain cationic and anionic sites either adjacent to or inside the polymer backbones. The device manufacturing technology using 3D printing can realize the on-demand manufacturing of devices and the design of devices from small to large. Arbitrary devices can also be manufactured by adding various functional substances to ink raw materials—one of the most widely used technologies in additives, energy storage, photoactive, biomedical, sensitive innovative materials, emerging areas, etc. This study provides a literature analysis of recent work on three-dimensional (3D) printing technology over the past few years, emphasizing the distinctive properties of ILs in new 3D printing applications. Finally, we briefly summarize several growth prospects that might result in new developments in this fascinating research area.

Abstract Photoinduced reversible deactivation radical polymerization (photo‐RDRP) or photoinduced controlled/living radical polymerization has emerged as a versatile and powerful technique for preparing functional and advanced polymer materials under mild conditions by harnessing light energy. While UV and visible light (λ = 400–700 nm) are extensively employed in photo‐RDRP, the utilization of near‐infrared (NIR) wavelengths (λ = 700–2500 nm) beyond the visible region remains relatively unexplored. NIR light possesses unique properties, including enhanced light penetration, reduced light scattering, and low biomolecule absorption, thereby providing opportunities for applying photo‐RDRP in the fields of manufacturing and medicine. This comprehensive review categorizes all known NIR light‐induced RDRP (NIR‐RDRP) systems into four mechanism‐based types: mediation by upconversion nanoparticles, mediation by photocatalysts, photothermal conversion, and two‐photon absorption. The distinct photoinitiation pathways associated with each mechanism are discussed. Furthermore, this review highlights the diverse applications of NIR‐RDRP reported to date, including 3D printing, polymer brush fabrication, drug delivery, nanoparticle synthesis, and hydrogel formation. By presenting these applications, the review underscores the exceptional capabilities of NIR‐RDRP and offers guidance for developing high‐performance and versatile photopolymerization systems. Exploiting the unique properties of NIR light unlocks new opportunities for synthesizing functional and advanced polymer materials.

The recent development of light-based 3D printing technologies has marked a turning point in additive manufacturing. Through photopolymerization, liquid resins can be solidified into complex objects. Usually, the polymerization is triggered by exciting a photoinitiator with ultraviolet (UV) or blue light. In two-photon printing (TPP), the excitation is done through the non-linear absorption of two photons; it enables printing 100-nm voxels but requires expensive femtosecond lasers which strongly limit their broad dissemination. Upconversion nanoparticles (UCNPs) have recently been proposed as an alternative to TPP for photopolymerization but using continuous-wave lasers. UCNPs convert near-infrared (NIR) into visible/UV light to initiate the polymerization locally as in TPP. Here we provide a study of this multi-photon mechanism and demonstrate how the non-linearity impacts the printing process. In particular, we report on the possibility of fine-tuning the size of the printed voxel by adjusting the NIR excitation intensity. Using gelatin-based hydrogel, we are able to vary the transverse voxel size from 1.3 to 2.8 μm and the axial size from 7.7 to 59 μm by adjusting the NIR power without changing the degree of polymerization. This work opens up new opportunities to construct 3D structures with micrometer feature size by direct laser writing with continuous wave inexpensive light sources.

Abstract Photoinitiating systems (PISs) are key components in photocurable formulations (inks) for three-dimensional (3D) printing. Natural PISs are promising and more environmentally friendly alternatives to conventional photoinitiators. These systems offer enhanced features such as less toxicity and therefore, higher biocompatibility. Furthermore, they can be found in a large “color palette” variety (absorbing in the different regions of the UV-visible spectrum) enabling new possibilities in the field of 3D printing. In this review, we outline the current efforts to implement natural and naturally derived PISs in light-based 3D printing. First, recently applied natural PISs and their performance for light-based 3D printing are discussed. In a second part, an overview of naturally derived PISs including the most common synthetic strategies are provided. Last, current challenges as well as future perspectives of the field are discussed. Introduction Natural Photoinitiating Systems Naturally Derived Photoinitiating Systems Conclusions and Outlook

Abstract 3D printing is an attractive method to accurately construct artificial organs or alternative materials with complicated structures and functional performance. Naturally derived hydrogels have emerged as promising materials for the preparation of biomimetic 3D organization or scaffolds by 3D printing due to their good biocompatibility, high water content, and fascinating 3D network. However, the poor printing properties and weak structural stability of naturally derived hydrogels limit their applications. In this study, photopolymerizable hydrogels are designed based on maleic chitosan (MCS) and thiolated sodium hyaluronate (SHHA). The Michael addition between MCS and SHHA improves the viscosity of the mixed solution. Moreover, it benefits the 3D printing process, followed by photopolymerization (acrylate‐thiol step‐chain polymerization and acrylate–acrylate chain polymerization) to form a stable covalent network rapidly. The rheological property, swelling behaviors, microstructure, and in vitro degradation are tuned by adjusting the molar ratio of the thiol group and acrylate group. In addition, MCS/SHHA hydrogel scaffolds with good accuracy and enhanced structural stability are prepared using extrusion‐based 3D printing and photopolymerization technology. The hydrogels display excellent cytocompatibility and can support adherence of L929 cells, which can be used as prospective materials for tissue engineering applications.

Polysilazane-based coatings exhibit excellent mechanical properties and chemical resistance, but thermal curing limits their range of applications. Therefore, the aim of the study was to evaluate the more resource-efficient curing of polyorganosilazane-based coatings on a stainless-steel substrate by photo-induced thiol-ene “click” reaction at room temperature compared to the conventional thermally induced polymerization using a radical initiator. As expected crosslinking at higher temperatures led to the formation of a pronounced Si-O-Si network. However, crosslinking via UV radiation at room temperature suppressed the incorporation of oxygen remarkably also after a subsequent additional treatment at 135 °C in air. Both the chemical stability of the layers cured by means of UV radiation and the mechanical properties are comparable to those of the thermally crosslinked coatings. Therefore, curing using UV radiation at low temperatures is a suitable alternative method for producing protective coatings on substrates with limited thermal stability.

Vat photopolymerization is a technique that uses photocurable resin having photoinitiator (PI) to initiate polymerization reaction when exposed to UV light. This process forms long chains polymers by combination of small chains monomers and oligomers. Vat photopolymerization depends on various parameters. This work focusses on the optimization of viscosity and composition of acrylate resin-Cu powder mixture for vat photopolymerization of metallic samples. Anycubic acrylate-based photopolymer resin and fine copper powder is used. Five configurations (50%Cu-50%resin, 55%Cu-45%resin, 60%Cu-40%resin, 65%Cu-35%resin & 70%Cu-30%resin) are formed to determine the highest possible density in each sample. These samples are then sintered in order to optimize the sintering parameters like debinding and sintering temperatures, oxygen and carbon contents. Then, the sample with maximum Cu density is used to optimize the viscosity of mixture using ethylene glycol as diluent. It is observed that ethylene glycol is useable as it effectively reduces the viscosity of resin without altering the chemical nature and curing time of photocurable resin. By equating the viscosity of optimized Cu-resin mixture with pure resin, difference in curing times is calculated for finite thickness of layer. This shows that 28% increase in curing time is observed when Cu-resin mixture is used as compared to pure resin. Sintering profile used is good in terms of debinding and sintering temperatures however hydrogen curing environment is essential to reduce carbon and oxygen contents in final samples.

Upconversion nanoparticle (UCNP)-driven polymerization attracts great attention due to the ability of near-infrared light to penetrate deeper into biological media and synthetic materials than ultraviolet or visible light. Despite significant progress, the limitation of near-infrared light-triggered polymerization is associated with a key element of the photocurable composition, a UCNP/photoinitiator complex or a nanoinitiator. To determine the impact of resonance energy transfer from UCNPs to photoinitiator (PI) and its effect on polymerization, we developed two different photocurable compositions consisting of the polyethylene glycol diacrylate (PEG-DA), ultraviolet- and blue-emitting NaYF4: Yb3+, Tm3+ UCNPs with hydrophobic surface combined with water-soluble or insoluble PI. We found that transfer energy in these nanoinitiators proceeds differently: in UCNP/water-soluble PI (lithium phenyl-2,4,6-trimethylbenzoylphosphinate or LAP), it occurs through the photon-mediated transfer while in UCNP/water-insoluble PI (2-benzyl-2-(dimethylamino)-4′-morpholinobutyrophenone or Irgacure 369), it takes place via the non-radiative resonant energy transfer. The impact of these processes in homolytic decomposition of initiator is extremely important in terms of the precisely controlled fabrication of polymer structures. PEG-DA facilitates the affinity between hydrophilic and hydrophobic components of the photocurable composition, which provides UCNP-driven cross-linking of biopolymers such as methacrylated hyaluronic acid and gelatin. 3D structures were prototyped to demonstrate the one-step rapid procedure of nanoinitiator preparation and emphasize the control of the energy transfer in UCNP/PI complexes for further development of UCNP-driven polymerization.

Electrically conductive composite materials are widely used for several applications, particularly flexible strain sensors for wearable electronic devices to detect human motions or apply to soft robotic technologies. Among the carbon nanotube (CNT) composites for strain sensors, the CNT composites with polypyrrole (PPy) have been scarcely found for electromechanical property improvement via digital light processing (DLP) 3D printing. Thus, this research presents a 3D printing fabrication of flexible polyurethane/CNT/PPy (FPU/CNT/PPy) composites for high complexity and model specifications, particularly strain sensing. The FPU/CNT/PPy composites were prepared as photopolymer resin with various proportions of the three components. The composites successfully achieved a gauge factor of 91.9 at 20 percent strain with high durability in 100 stretching-releasing cycles. More than 85% of printing accuracy was also found under the DLP 3D printing method. The small deformation of the composites could be detected during the stretching-releasing process during time-dependent testing. Examples of simple human activity and complex spring motion could be successfully detected due to the high responsibility and reproducibility of the finger motion. The composites mentioned in this study could reach the field of strain sensing and can further be applied to other fields such as healthcare and soft robotics.

Ceramic 3D printing based on stereolithography has attracted wide attention because it can fabricate complex ceramic components with high dimensional accuracy, good surface finish, uniform microstructure, and excellent mechanical properties. It is one of the important technical means to achieve high-performance parts by additive manufacturing. The core of the technology is to prepare ceramic slurries with high solid loading and good printability, and its composition has a vital influence on the curing effect and printing process. In this review, two main additive manufacturing methods, stereolithography (SL) and digital light processing (DLP), commonly used in ceramic 3D printing were introduced, and advantages and disadvantages of the two methods were compared. Based on the research work in the field of ceramic slurries in recent years, the effects of monomer/oligomer and diluent, dispersant, physical properties of ceramic particles and solid loading on viscosity, shear thinning/thickening behavior, viscoelasticity, yield stress were discussed. Finally, the main development trends and challenges of ceramic slurries via stereolithography were put forward in, and a general guiding principle for the construction of ceramic slurries with high solid loading was provided.

Single-network hydrogels can have an internal porous structure and biocompatibility, but have lower mechanical properties. Combining these properties with another biocompatible and mechanically strong network can help in mimicking the extracellular matrix of native tissues to make them suitable for tissue scaffolds with desired performance. In the current objective, we combine the properties of poly (ethylene glycol) dimethacrylate (PEGDMA) macromer and polysaccharides as the two components in double networks (DN) for synergistic effects of both components resulting in the interpenetrating polymeric network for making it functional for replacement of injured tissues. The hydrogels were characterized by physical properties like swelling ratio, mechanical properties like tensile and compressive modulus, and rheological behavior. The chemical composition was studied using Fourier transform infrared spectroscopy (FTIR), and the thermal behavior using differential scanning calorimetry (DSC) experiments. Biodegradability and mechanical strength both are gained using double networks (DN), thus making it resemble more like living tissues. DN hydrogels were tested for cell compatibility for possible application in tissue engineering. Furthermore, these properties may allow their application as tissue-engineered scaffolds.

Two-photon lithography (TPL) is a laser-based additive manufacturing technique that enables the printing of arbitrarily complex cm-scale polymeric 3D structures with sub-micron features. Although various approaches have been investigated to enable the printing of fine features in TPL, it is still challenging to achieve rapid sub-100 nm 3D printing. A key limitation is that the physical phenomena that govern the theoretical and practical limits of the minimum feature size are not well known. Here, we investigate these limits in the projection TPL (P-PTL) process, which is a high-throughput variant of TPL, wherein entire 2D layers are printed at once. We quantify the effects of the projected feature size, optical power, exposure time, and photoinitiator concentration on the printed feature size through finite element modeling of photopolymerization. Simulations are performed rapidly over a vast parameter set exceeding 10,000 combinations through a dynamic programming scheme, which is implemented on high-performance computing resources. We demonstrate that there is no physics-based limit to the minimum feature sizes achievable with a precise and well-calibrated P-TPL system, despite the discrete nature of illumination. However, the practically achievable minimum feature size is limited by the increased sensitivity of the degree of polymer conversion to the processing parameters in the sub-100 nm regime. The insights generated here can serve as a roadmap towards fast, precise, and predictable sub-100 nm 3D printing.

Vanillin acrylate-based thermo-responsive shape memory photopolymers with high thermal stability, tunable mechanical properties, and antimicrobial activity have been developed. Photocurable resins containing one of the three commercial vanillin derivatives, vanillin diacrylate, vanillin dimethacrylate, and vanillin hydroxypropane dimethacrylate, and 1,3-benzenedithiol were tested. The results of dual curing systems with different ratios of thiol and acrylate (1:1 and 0.5:1) were compared. The reduction of thiol content increased the rate of photocuring, improved the mechanical performance of polymers (Young’s modulus was increased from 1.4–3.5 to 3952.3–11339.4 MPa), and their heat resistance (the 10% weight loss increased from 277–327 to 294–341 °C). All polymers were able to return to their primary shape after deformation and maintain their temporary shape at a temperature lower than their glass transition temperature (–3–46 °C). Furthermore, allpolymer films exhibited significant antibacterial activity against Escherichia coli and Staphylococcus aureus (cell reduction reached 99.8–100% after 24 h) and antifungal activity against Aspergillus flavus and Aspergillus niger (cell reduction reached 72.3–100% after 24 h).

In this work, two new water-soluble photoinitiators based on the α-alkoxy-arylketone scaffold have been synthesized and investigated for their ability to initiate photopolymerization for the preparation of hydrogels. The efficiency of these new Type I photoinitiators was compared to that of benchmark ones (2-hydroxy-4′-(2-hydroxyethoxy)-2-methylpropiophenone—Irgacure 2959 and 2-hydroxy-2-methyl propiophenone—Irgacure 1173). In combination with additive (carbene-borane), a good initiating ability was found under air. Mechanical properties of the prepared hydrogels were investigated by tensile tests and dynamic mechanical analysis (DMA). Markedly, hydrogels could be prepared with the newly proposed initiating systems in mild conditions (i.e., under air, using low light intensity @405 or 395 nm and without specialized glassware) and exhibited similar properties to those prepared by harsher approaches (thermal treatment or UV light).

Providing a 3D environment that mimics the native extracellular matrix is becoming increasingly important for various applications such as cell function studies, regenerative medicine, and drug discovery. Among the most critical parameters to consider are the scaffold’s complicated micro-scale geometry and material properties. Therefore, stereolithography based on photopolymerization is an emerging technique because of its ability to selectively form volumetric structures from liquid resin through localized polymerization reactions. However, one of the most important parameters of the scaffold is biocompatibility, which depends not only on the material but also on the exposure conditions and post-processing, which is currently underestimated. To investigate this systematically, microporous scaffolds with pore sizes of 0.05 mm3 corresponding to a porosity of 16,4% were fabricated using the stereolithography printer Asiga PICO2 39 UV from the widely used resins FormLabs Clear and Flexible. The use of various polymers is usually limited for cells because, after wet chemical development, the non-negligible amount of remaining monomers intertwined in the photopolymerized structures is significantly toxic to cells. Therefore, the aim of this research was to find the best method to remove monomers from the 3D scaffold by additional UV exposure. For this purpose, a Soxhlet extractor was used for the first time, and the monomers were immersed in different alcohols. A Raman microspectroscopy was also used to investigate whether different post-processing methods affect DC (cross-linking) to find out if this specifically affects the biocompatibility of the scaffolds. Finally, mesenchymal stem cells from rat dental pulp were examined to confirm the increased biocompatibility of the scaffolds and their ability to support cell differentiation into bone tissue cells.

A number of photoinitiators are available in chemical industry, but less of them in biomedicine or clinical therapy due to the limitation of their cytotoxicity and biocompatibility. Thus, it is urgently necessary to find non-toxic or low-toxic photoinitiators to meet clinical demands. Aceanthrenequinone (AATQ) is a novel photosensitizer with high-photoinitiating ability, but no reports contribute, to date, to its cytotoxicity and biocompatibility. Here, primary cells and various cell lines were exposed to different concentrations of AATQ with or without irradiation. AATQ had the similar photoinitiating conversion efficiency to the extensively used bis(2,4,6-trimethylbenzoyl)-phenylphosphine oxide (BAPO) and higher one than 9,10-phenanthrenequinone (PANQ) with the similar extent of polymerization in depth within a certain range, but displayed much lower cytotoxicity than BAPO under non-irradiation or irradiation. The biocompatibility of BisGMA/TEGDMA polymer prepared by AATQ was superior to that of PANQ, but inferior to that of camphorquinone (CQ) although the far lower dose of AATQ is enough to initiate polymerization of monomer than that of CQ. Hence, AATQ offers a valuable alternative in applications of industrial or biomedical areas.

Abstract Multimaterial surfaces with hierarchical features have many potential applications in self‐cleaning, droplet manipulation, microfluidics, and biomedicine, owing to their wide range of functionalities induced by structural and material contrasts. Here, a fast and sustainable manufacturing method, acoustic assembly photopolymerization (AAP), is presented for productions of such surfaces. In the novel AAP process, an external acoustic field is used to assemble microparticles to microsized patterns, while the photocuring is combined with the acoustic assembly to produce multilevel hierarchical features, such as cones and wrinkles ranging from nanometer to micrometer. The mechanism underlying the proposed multimaterial surface structuring technique is discussed, and the relationship between process parameters and surface structures is modeled. Effects of surface material composition patterns and surface topology on the hydrodynamic properties are studied. To demonstrate potential applications, three microreactors are designed and automated droplet manipulations are demonstrated. The application of the proposed surface manufacturing approach is further extended to fog harvesting. The AAP technology and the fabricated multimaterial hierarchically‐structured surfaces demonstrated in this study can be employed in many other advanced applications in microfluidics, tissue engineering, and also potentially many other fields such as mechanical systems and battery systems.

Molecularly Imprinted Polymers (MIP) have demonstrated considerable potential when combined with electrochemical sensors, exhibiting high sensitivity, selectivity and reproducibility levels. The aim of this work is to detect Zivudine (ZDV) in serum samples by means of an interface imprinting technique-based electrochemical sensor. Thus, ZDV was used as a template for the creation of an MIP-based electrochemical sensor, and differential pulse voltammetry (DPV) was used as the determination technique for the molecule. Electrochemical impedance spectroscopy (EIS) and cyclic voltammetry (CV) techniques were also used to characterize the electrochemical sensor capabilities, which showed a good linearity between 1.0 × 10−10 M and 1.0 × 10−9 M. ZDV was detected with a detection limit of 1.63 × 10−11 M, while the recovery analysis of spiked serum samples demonstrated that the sensor was highly selective.

Over a short period of time, electronic assemblies have been dramatically developed with smaller size and lighter weight and 3D printing plays a crucial role in their future production. However, it is difficult to develop epoxy resins and other thermoset resins for this process because of the polymer's liquid state during processing. This work uses a UV curing technique for making flexible epoxy/multi-walled carbon nanotubes (MWCNTs) composites that are suitable for future 3D printing applications. The synthesized carbazole-coated TiO2 nanoparticles, used as a photosensitizer, were characterized by their photoabsorbance, morphology, and surface property before use. The results indicated that the TiO2 nanoparticles coated with 75 wt% carbazole were appropriate for UV-cured flexible epoxy/MWCNT composites because of its fast cure kinetics after irradiation by a UV light source. The epoxy/MWCNT composites displayed low tensile properties because of the agglomeration of MWCNTs inside the epoxy matrix. In addition, the epoxy/MWCNT composites showed slightly lower thermal expansion with high electrical properties with a large amount of MWCNTs in the epoxy composites.

We demonstrate a new approach for decreasing the feature size in multiphoton absorption polymerization (MAP). Acrylic photoresists containing the photoinitiator KL68 (bis-[4-(diphenylamino) stryl]-1-(2-ethylhexyloxy), 4-(methoxy)benzene) exhibit a proportional velocity (PROVE) dependence, yielding smaller feature sizes at lower fabrication speeds. The feature size in this photoresist decreases substantially with a temperature increase of less than 10°C when all other fabrication parameters are kept constant, suggesting that the PROVE behavior results from local heating. Although higher temperatures have previously been associated with decreased feature sizes in MAP, the effect observed here is considerably stronger than in previous work, and is shown to be a property of the photoinitiator. This discovery opens the door to exploiting thermal gradients to improve resolution in MAP lithography.

Objective: Two-photon polymerization (TPP) utilizes an optical nonlinear absorption process to initiate the polymerization of photopolymerizable materials. To date, it is the only technique capable of fabricating complex 3D microstructures with finely adjusted geometry on the cell and sub-cell scales. TPP shows a very promising potential in biomedical applications related to high-resolution features, including drug delivery, tissue engineering, microfluidic devices, and so forth. Therefore, it is of high significance to grasp the global scientific achievements in this field. An analysis of publications concerning the applications of TPP in the biomedical field was performed, and the knowledge domain, research hotspots, frontiers, and research directions in this topic were identified according to the research results.Methods: The publications concerning TPP applications in biomedical field were retrieved from WoSCC between 2003 and 2022, Bibliometrics and visual analysis employing CiteSpace software and R-language package Bibliometrix were performed in this study.Results: A total of 415 publications regarding the TPP applications in the biomedical field were retrieved from WoSCC, including 377 articles, and 38 review articles. The studies pertaining to the biomedical applications of TPP began back in 2003 and showed an upward trend constantly. Especially in the recent 5 years, studies of TPP in biomedical field have increased rapidly, with the number of publications from 2017 to 2021 accounting for 52.29% of the total. In terms of output, China was the leading country and Chinese Acad Sci, Tech Inst Phys and Chem was the leading institution. The United States showed the closest cooperation with other countries. ACS applied materials and interfaces was the most prolific journal (n = 13), followed by Biofabrication (n = 11) and Optics express (n = 10). The journals having the top cited papers were Biomaterials, Advanced materials, and Applied physic letters. The most productive author was Aleksandr Ovsianikov (27 articles). Meanwhile, researchers who had close cooperation with other researchers were also prolific authors. “cell behavior”, " (tissue engineering) scaffolds”, “biomaterials,” and “hydrogel” were the main co-occurrence keywords and “additional manufacturing”, “3D printing,” and “microstructures” were the recent burst keywords. The Keyword clusters, “stem cells,” and “mucosal delivery”, appeared recently. A paper reporting unprecedented high-resolution bull models fabricated by TPP was the most locally cited reference (cited 60 times). “Magnetic actuation” and “additive manufacturing” were recently co-cited reference clusters and an article concerning ultracompact compound lens systems manufactured by TPP was the latest burst reference.Conclusion: The applications of TPP in biomedical field is an interdisciplinary research topic and the development of this field requires the active collaboration of researchers and experts from all relevant disciplines. Bringing up a better utilization of TPP as an additive manufacturing technology to better serve the biomedical development has always been the research focus in this field. Research on stem cells behaviors and mucosal delivery based on microstructures fabricated using TPP were becoming new hotspots. And it can be predicted that using TPP as a sourcing technique to fabricate biomedical-related structures and devices is a new research direction. In addition, the research of functional polymers, such as magnetic-driven polymers, was the frontier topic of TPP biomedical applications.

The needs for high-resolution, well-defined and complex 3D microstructures in diverse fields call for the rapid development of novel 3D microfabrication techniques. Among those, two-photon polymerization (TPP) attracted extensive attention owing to its unique and useful characteristics. As an approach to implementing additive manufacturing, TPP has truly 3D writing ability to fabricate artificially designed constructs with arbitrary geometry. The spatial resolution of the manufactured structures via TPP can exceed the diffraction limit. The 3D structures fabricated by TPP could properly mimic the microenvironment of natural extracellular matrix, providing powerful tools for the study of cell behavior. TPP can meet the requirements of manufacturing technique for 3D scaffolds (engineering cell culture matrices) used in cytobiology, tissue engineering and regenerative medicine. In this review, we demonstrated the development in 3D microfabrication techniques and we presented an overview of the applications of TPP as an advanced manufacturing technique in complex 3D biomedical scaffolds fabrication. Given this multidisciplinary field, we discussed the perspectives of physics, materials science, chemistry, biomedicine and mechanical engineering. Additionally, we dived into the principles of tow-photon absorption (TPA) and TPP, requirements of 3D biomedical scaffolders, developed-to-date materials and chemical approaches used by TPP and manufacturing strategies based on mechanical engineering. In the end, we draw out the limitations of TPP on 3D manufacturing for now along with some prospects of its future outlook towards the fabrication of 3D biomedical scaffolds.

Here we show the effect of the ionic liquid nature, its content and monomer/crosslinker ratio on the copolymerization of N-vinylpyrrolidone (NVP) with triethylene glycol dimethacrylate (TEGDMA) induced by UV or heat irradiation. For the first time, kinetics curves of photopolymerization NVP with TEGDMA in the presence of ionic liquids are obtained. The ionic liquids EmimBF4, BmimBF4, OmimBF4 and EmimTFSI with different cation and anion structures and lengths of the alkyl radical were varied in photopolymer compositions. To understand the influence of ionic liquids on the polymerization kinetics, photo-DSC, dynamic DSC, and FTIR were performed. Parameters obtained from photo-DSC curves allowed to develop the methodology for the stereolithography of ionogels. The presented data constitutes the complete dataset useful for 3D-printing of ionogels with high accuracy, which is reported in the main article.

UV-curable particle-free ceramic compositions for stereolithography-based 3D printing technologies present a promising alternative to the commonly used particle-based compositions. So far, such compositions were mainly based on solutions of pre-ceramic polymers which limit their applications to silicon-containing materials. However, the application of particle-free inks for the fabrication of other ceramic materials, in particular dense polycrystalline ones, is very little explored. We present a new and general fabrication approach based on all-solution compositions, by combining sol–gel chemistry and photopolymerization, for obtaining dense 3D ceramic structures by DLP printing. The process is demonstrated here for the fabrication of barium titanate (BaTiO3). By using chelating solvent and monomer, a stable UV-curable solution is obtained. An aging period of 8–14 days was crucial for obtaining dense ceramic objects without any secondary phases. The heat treatment was found to affect the microstructure, density and hardness of the resulting ceramics. The presented process enables obtaining objects free of carbon materials, having a density as high as 98% of the theoretical value, and a hardness of 4.3 GPa.

Electrochemical capacitors operating in an aqueous electrolyte solution have become ever-more popular in recent years, mainly because they are cheap and ecofriendly. Additionally, aqueous electrolytes have a higher ionic conductivity than organic electrolytes and ionic liquids. These materials can exist in the form of a liquid or a solid (hydrogel). The latter form is a very promising alternative to liquid electrolytes because it is solid, which prevents electrolyte leakage. In our work, hydrogel polymer electrolytes (HPEs) were obtained via photopolymerization of a mixture of acrylic oligomer Exothane 108 with methacrylic acid (MAA) in ethanol, which was later replaced by electrolytes (1 M Na2SO4). Through the conducted research, the effects of the monomers ratio and the organic solvent concentration (ethanol) on the mechanical properties (tensile test), electrolyte sorption, and ionic conductivity were examined. Finally, hydrogel polymer electrolytes with high ionic conductivity (σ = 26.5 mS∙cm−1) and sufficient mechanical stability (σmax = 0.25 MPa, εmax = 20%) were tested using an AC/AC electrochemical double layer capacitor (EDLC). The electrochemical properties of the devices were investigated via cyclic voltammetry, galvanostatic charge/discharge, and impedance spectroscopy. The obtained results show the application potential of the obtained HPE in EDLC.