Quantification of morphine in exhaled breath condensate using a double network polymeric hybrid hydrogel functionalized with AuNPs.

BACKGROUND: Morphine serves as a foundation for creating other opioid derivatives, such as hydro/oxymorphine and heroin, which possess enhanced pain-relieving properties but are also prone to addiction and abuse. In cases of morphine overdose, it not only affects multiple immune functions but can also cause severe health complications. Given these concerns and the widespread use of morphine, it is crucial to develop efficient, uncomplicated, and precise methods for accurately detecting morphine in various biological and pharmaceutical samples. RESULTS: In this investigation, a novel gold nanoparticle (AuNPs)-based double network hydrogel (DNH) nanoprobe has been fabricated for sensitive quantification of morphine in exhaled breath condensate samples. For that, gelatin/agarose DNH was fabricated through a one-step heating-cooling method in the presence of AuNPs, providing not only chemical stability but also prevent the AuNPs aggregation during synthesis process. In this method, the absorbance intensity of the nanoprobe gradually decreased with increasing morphine concentration due to the interaction morphine with AuNPs surface plasmon. The aggregation of AuNPs by addition of morphine was verified by UV-Vis spectrophotometry. The sensor displayed high sensitivity with detection limit of 0.006 µg.mL-1 in the linear range from 0.01 to 1.0 µg.mL-1. A reliable performance was attained for the spectrophotometric method for determination of morphine in the real samples.

Efficient Pb(II) removal from contaminated soils by recyclable, robust lignosulfonate/polyacrylamide double-network hydrogels embedded with Fe2O3 via one-pot synthesis.

Soil heavy metal removal strategies are increasingly valued for effectively reducing contamination and preventing secondary pollution. In this work, a double network hydrogel (Fe2O3@LH), consisting of lignosulfonate (LS) and polyacrylamide with embedded Fe2O3 nanoparticles, was synthesized successfully via a one-pot method and subsequently applied to adsorb lead (Pb) from contaminated soil. Incorporating Fe2O3 into the hydrogel enhances the adsorption capacity of Fe2O3@LH for Pb(II). The Fe2O3@LH hydrogel demonstrates a maximum Pb(II) adsorption capacity of 143.11 mg g-1, with Pb(II) removal mechanisms involving electrostatic adsorption, cation exchange, precipitation reactions, and the formation of coordination complexes, achieving a 22.3 % maximum removal efficiency in soil cultivation experiments. Additionally, the application of Fe2O3@LH markedly reduces the concentrations of cadmium (Cd) and arsenic (As) in the soil, meanwhile enhances the levels of total nitrogen (TN), soil organic matter (SOM), and cation exchange capacity (CEC) by 23.1 %, 10.6 %, and 16.9 %, respectively. Following 90 days of continuous application in the soil, the recovery rate of Fe2O3@LH remains above 75 %. The toxicity assay using zebrafish larvae indicates that Fe2O3@LH demonstrates good biosafety. This study demonstrates the considerable potential of Fe2O3@LH hydrogel for practical application in reducing Pb(II) levels in contaminated soil.

Construction and characterization of sodium alginate/polyvinyl alcohol double-network hydrogel beads with surfactant-tailored adsorption capabilities for efficient tetracycline hydrochloride removal.

The extensive use of tetracycline (TC) for disease control and the residuals in wastewater has resulted in the spread and accumulation of antibiotic resistance genes, posing a severe threat to the human health and environmental safety. To solve this problem, a series of double-network hydrogel beads based on sodium alginate and polyvinyl alcohol were constructed with the introduction of various surfactants to modulate the morphology. The results showed that the introduction of surfactants can modulate the surface morphology and internal structure, which can also regulate the adsorption ability of the hydrogel beads. The SDS-B beads with SDS as surfactant exhibited highest adsorption efficiency for removal of TC with a maximum adsorption capacity up to 121.6 mg/g, which possessed a resistance to various cations and humic acid. The adsorption mechanism revealed that the superior adsorption performance of the hydrogel beads was primarily attributed to hydrogen bonding, electrostatic attraction, and π-π EDA interactions. Adsorption kinetics demonstrated that the pseudo-second-order model fitted the adsorption process well and adsorption isotherm showed the adsorption of TC occurred through both chemical and physical interactions. Moreover, the adsorption efficiency remained approximately 87.5 % after three adsorption-desorption cycles, which may have potential application and practical value in TC adsorption.

Thermal responsive sodium alginate/polyacrylamide/poly (N-isopropylacrylamide) ionic hydrogel composite via seeding calcium carbonate microparticles for the engineering of ultrasensitive wearable sensors.

The design of polyelectrolyte hydrogel with unique tensile and adhesive properties which can be applied across disciplines has gradually become a popular trend. However, the phenomenon of global warming and the emergence of extreme weather, it still faces some urgent problems that should be solved, such as the optimal utilization of polyelectrolyte hydrogel across a wide range of temperatures. Herein, a wide temperature sensitivity and conductivity hydrogel based on sodium alginate, acrylamide and N-isopropylacrylamide was constructed, which exhibited excellent adhesion and temperature conductivity. It is worth noting that after the inclusion of CaCO3 and NaCl in the hydrogel, the hydrogel showed excellent tensile properties (fracture strain >2000 %). Within a wide temperature range (-15-50 °C), it exhibits exceptional electrical conductivity (2.75 S ∗ m-1) and sensitivity (GF = 8.76 under high strain). This innovative intelligent polyelectrolyte hydrogel provides suitable strategy for flexible sensors, smart wearable devices and medical monitoring equipment.

Polyphenol-Mediated Adhesive and Anti-Inflammatory Double-Network Hydrogels for Repairing Postoperative Intervertebral Disc Defects.

Hydrogels have garnered tremendous attention for their applications in the repair of intervertebral disk (IVD) degeneration and postoperative IVD defects. However, it is still challenging to develop a hydrogel fulfilling the requirements for high mechanical properties, adhesive capability, biocompatibility, antibacterial properties, and anti-inflammatory performance. Herein, we report a multifunctional double-network (DN) hydrogel composed of physically cross-linked carboxymethyl chitosan (CMCS) and tannic acid (TA) networks as well as chemically cross-linked acrylamide (AM) networks, which integrates the properties of high strength, adhesion, biocompatibility, antimicrobial activity, and anti-inflammation for the repair of postoperative IVD defects. The treatment with CMCS/TA/PAM DN hydrogels can significantly decrease the levels of inflammatory cytokines and degeneration-related factors and upregulated collagen type II alpha 1. In addition, the hydrogels can effectively seal the annulus fibrosus defect, prevent nucleus pulposus degeneration, retain IVD height, and restore the biomechanical properties of the disc to some extent. This polyphenol-mediated DN hydrogel is promising for sealing IVD defects and preventing herniation after lumbar discectomy.

High-Performance Flexible Sensor with Sensitive Strain/Magnetic Dual-Mode Sensing Characteristics Based on Sodium Alginate and Carboxymethyl Cellulose.

Flexible sensors can measure various stimuli owing to their exceptional flexibility, stretchability, and electrical properties. However, the integration of multiple stimuli into a single sensor for measurement is challenging. To address this issue, the sensor developed in this study utilizes the natural biopolymers sodium alginate and carboxymethyl cellulose to construct a dual interpenetrating network, This results in a flexible porous sponge that exhibits a dual-modal response to strain and magnetic stimulation. The dual-mode flexible sensor achieved a maximum tensile strength of 429 kPa and elongation at break of 24.7%. It also exhibited rapid response times and reliable stability under both strain and magnetic stimuli. The porous foam sensor is intended for use as a wearable electronic device for monitoring joint movements of the body. It provides a swift and stable sensing response to mechanical stimuli arising from joint activities, such as stretching, compression, and bending. Furthermore, the sensor generates opposing response signals to strain and magnetic stimulation, enabling real-time decoupling of different stimuli. This study employed a simple and environmentally friendly manufacturing method for the dual-modal flexible sensor. Because of its remarkable performance, it has significant potential for application in smart wearable electronics and artificial electroskins.

Double Network Gel Electrolyte with High Ionic Conductivity and Mechanical Strength for Zinc-Ion Batteries.

Gel electrolytes hold promise for stabilizing zinc-ion batteries (ZIBs), but achieving both high ionic conductivity and strong mechanical properties remains challenging. This work presents a double network gel electrolyte based on poly(N-hydroxymethyl acrylamide) (PNMA) and sodium alginate (SA), overcoming this trade-off. The PNMA network provides mechanical strength and water retention, while the SA network facilitates rapid zinc-ion (Zn2+) diffusion through tailored solvation. This double network gel exhibits a tensile strength of up to 838 kPa, significantly higher than previous reports. The SA network provides ion channels for rapid transport of hydrated Zn2+, enhancing the ionic conductivity to a ground-breaking 33.1 mS cm-1. This value is even higher than the liquid electrolytes. The growth of Zn dendrites is also suppressed due to the mechanical constraint and rapid ion conduction. In symmetrical cells, the PNMA/SA gel demonstrates exceptional cycling stability (>2000 h). Characterizations show this is because of reduced free water amount, hindering cathode material dissolution. The full cells with sodium vanadate cathode manifest a high capacity (364.8 mA h g-1 at 0.5 A g-1) and excellent capacity retention (83% after 2500 cycles at 10 A g-1). This double network design offers a way to achieve high-performance and stable ZIBs.

A synergistic enhancement strategy for mechanical and conductive properties of hydrogels with dual ionically cross-linked κ-carrageenan/poly(sodium acrylate-co-acrylamide) network.

Applying conductive hydrogels in electronic skin, health monitoring, and wearable devices has aroused great research interest. Yet, it remains a significant challenge to prepare conductive hydrogels simultaneously with superior mechanical, self-recovery, and conductivity performance. Herein, a dual ionically cross-linked double network (DN) hydrogel is fabricated based on K+ and Fe3+ ion cross-linked κ-carrageenan (κ-CG) and Fe3+ ion cross-linked poly(sodium acrylate-co-acrylamide) P(AANa-co-AM). Benefiting from the abundance of hydrogen bonds and metal coordination bonds, the conductive hydrogel has excellent mechanical properties (fracture strain up to 1420 %, fracture stress up to 2.30 MPa, and toughness up to 20.63 MJ/m3) and good self-recovery performance (the recovery rate of the toughness can reach 85 % after waiting for 1 h). Meanwhile, due to the introduction of dual metal ions of K+ and Fe3+, the ionic conductivity of conductive hydrogel is up to 1.42 S/m. Furthermore, the hydrogel strain sensor has good sensitivity with a gauge factor (GF) of 2.41 (0-100 %). It can be a wearable sensor that monitors different human motions, such as sit-ups. This work offers a new synergistic strategy for designing a hydrogel strain sensor with high mechanical, self-recovery, and conductive properties.

Fabrication, digestion behavior and ß-carotene bioaccessibility of emulsion-filled double-network gel: Effect of corn fiber gum/soy protein isolate ratio and surfactant types.

Emulsion fortified with ß-carotene was added to corn fiber gum (CFG)/soy protein isolate (SPI) double network gel matrix to obtain emulsion-filled gels (EFG) via dual induction of laccase and glucono-δ-lactone. Protein digestion was accompanied by the release of ß-carotene from gel matrix during in vitro digestion. The surfactant types and corn fiber gum/soy protein isolate ratio affected the ß-carotene bioaccessibility via changing oil-water interfacial composition and emulsion particle size during in vitro digestion. As compared with Tween-20 EFGs, emulsion droplets released from SPI EFGs was more susceptible to flocculation, followed with coalescence due to proteolysis of interfacial SPI during gastric digestion. The resulting oil droplets with large particle size exhibited lower lipase adsorption, thus reducing the free fatty acid content and ß-carotene bioaccessibility. The confocal laser scanning microscope (CLSM) observation confirmed that protein hydrolysate from gel matrix were adsorbed onto the oil-water interface competing with Tween-20 during intestinal digestion. For EFGs with higher CFG content, steric hindrance of CFG molecules and less emulsion release could inhibit droplet flocculation, thus enhancing ß-carotene bioaccessibility.

Hydrogen bonds-pinned entanglement double network alginate hydrogel for electrical application.

In response to prevailing challenges encountered in electrical applications, including insufficient mechanical strength, subpar tensile properties, and limited adaptability to dynamic motion environments, we engineered a pioneering hydrogel adhesive. Simultaneously, we presented a novel interpretation of the application of ZnO in hydrogels. Our innovative approach entailed the intertwining of polyvinyl alcohol (PVA) and flexible sodium alginate (SA) double networks (DN) through cross-linking mechanisms, resulting in the formation of a hydrogen-bonding pinned DN hydrogel. This groundbreaking design substantially amplified the cohesive and adhesive properties of the hydrogel, while the incorporation of zinc oxide (ZnO) through modification served to enhance its electrical conductivity. Our hydrogel sensor demonstrated exceptional capabilities in monitoring human motion, adeptly meeting the demands of diverse motion scenarios. Furthermore, meticulous consideration had been given to the influence of perspiration on sensor performance, rendering our sensor exceptionally well-suited for real-world applications.

Macroporous PEG-Alginate Hybrid Double-Network Cryogels with Tunable Degradation Rates Prepared via Radical-Free Cross-Linking for Cartilage Tissue Engineering.

Trauma or repeated damage to joints can result in focal cartilage defects, significantly elevating the risk of osteoarthritis. Damaged cartilage has an inherently limited self-healing capacity and remains an urgent unmet clinical need. Consequently, there is growing interest in biodegradable hydrogels as potential scaffolds for the repair or reconstruction of cartilage defects. Here, we developed a biodegradable and macroporous hybrid double-network (DN) cryogel by combining two independently cross-linked networks of multiarm polyethylene glycol (PEG) acrylate and alginate.Hybrid DN cryogels are formed using highly biocompatible click reactions for the PEG network and ionic bonding for the alginate network. By judicious selection of various structurally similar cross-linkers to form the PEG network, we can generate hybrid DN cryogels with customizable degradation kinetics. The resulting PEG-alginate hybrid DN cryogels have an interconnected macroporous structure, high mechanical strength, and rapid swelling kinetics. The interconnected macropores in the cryogels support efficient mesenchymal stem cell infiltration at a high density. Finally, we demonstrate that PEG-alginate hybrid DN cryogels allow sustained release of chondrogenic growth factors and support chondrogenic differentiation of mouse mesenchymal stem cells. This study provides a novel method to generate macroporous hybrid DN cryogels with customizable degradation rates and a potential scaffold for cartilage tissue engineering.

Highly Selective Recovery of Gold by In Situ Magnetic Field-Assisted Fe/Co-MOF@PDA/NdFeB Double Network Gel.

There are enormous economic benefits to conveniently increasing the selective recovery capacity of gold. Fe/Co-MOF@PDA/NdFeB double-network organogel (Fe/Co-MOF@PDA NH) is synthesized by aggregation assembly strategy. The package of PDA provides a large number of nitrogen-containing functional groups that can serve as adsorption sites for gold ions, resulting in a 21.8% increase in the ability of the material to recover gold. Fe/Co-MOF@PDA NH possesses high gold recovery capacity (1478.87 mg g-1) and excellent gold selectivity (Kd = 5.71 mL g-1). With the assistance of an in situ magnetic field, the gold recovery capacity of Fe/Co-MOF@PDA NH is increased from 1217.93 to 1478.87 mg g-1, and the recovery rate increased by 24.7%. The above excellent performance is attributed to the efficient reduction of gold by FDC/FC+, Co2+/Co3+ double reducing couple, and the optimization of the reduction reaction by the magnetic field. After the samples are calcined, high-purity gold (95.6%, 22K gold) is recovered by magnetic separation. This study proposes a forward-looking in situ energy field-assisted strategy to enhance precious metal recovery, which has a guiding role in the development of low-carbon industries.

An Antibacterial, Highly Sensitive Strain Sensor Based on an Anionic Copolymer Interpenetrating with κ-Carrageenan.

Polysaccharide-based hydrogels are suitable for use in the field of flexible bioelectronics due to their benign mechanical properties and biocompatibility. However, the preparation of hydrogel sensors with high performance without affecting their physicochemical properties (e.g., flexibility, toughness, self-healing, and antibacterial activity) remains a challenge and needs to be solved. Herein, a metal ion cross-linking reinforced, double network hydrogel was formed from a 2-acrylamide-2-methylpropanesulfonic acid (AMPS) copolymer interpenetrating κ-carrageenan (CAR), followed by immersing the gel in a Cu2+ ion solution to obtain an antibacterial CAR/P(AM-co-AMPS)-Cu2+ conductive hydrogel. LiCl was added as the electrolyte. The presence of the LiCl electrolyte and sulfonated molecular chain units not only gives the hydrogel good electrical conductivity (conductivity up to 2.68 S/m) but also improves the sensitivity of the hydrogel as a stress-strain sensor, with a hydrogel sensitivity GF of up to 3.76 in the 20%-100% strain range and response time of up to 280 ms. The CAR double-helical structure and sol-gel properties and the interaction of multiple noncovalent bonds between polymers provide the hydrogel with excellent self-healing, with a self-healing efficiency of 68%. In addition, the electrostatic interaction of Cu2+ with Escherichia coli cells can inhibit their growth, exhibiting good antibacterial properties with an inhibition circle diameter of 20.5 mm. This work could provide an effective strategy for antibacterial multifunctional CAR-based bionic sensors.

Highly conductive and stable double network carrageenan organohydrogels for advanced strain sensing and signal recognition arrays.

Conductive hydrogels with excellent mechanical properties, a broad detection range, and stability in complex environments have remained a significant challenge for the development of flexible sensors. In this study, a straightforward freeze-thaw cycles strategy was developed to fabricate a polyvinyl alcohol (PVA)/carrageenan (CA)/calcium chloride (CaCl2)/MXene-based double network organohydrogel (PCCME) for highly flexible and responsive strain detection across a broad temperature spectrum. The PCCME organohydrogel features multiple interactive forces including hydrogen bonding, ionic interactions, and microphase crystallization, which contribute to the organohydrogel's exceptional mechanical and electrical performance. The PCCME organohydrogel exhibited excellent performance in a load-unload test repeated 100 times after being maintained at room temperature for 7 days, with a minimal mechanical decay of only 2.6%. Furthermore, the repaired PCCME organohydrogel retained its robust stability after storage at low temperatures followed by placement at room temperature. The organohydrogel sensor not only detects various movement amplitudes of the human body but also recognizes arrays of pressure signals and converts these into digital images, highlighting its significant potential for applications in rehabilitation monitoring, pressure sensing, and human-computer interaction.

Injectable Dual Fenton/Enzymatically Cross-Linked Double-Network Hydrogels Based on Acrylic/Phenolic Polymers with Highly Reinforced and Tunable Mechanical Properties.

Injectable hydrogels have been extensively used as promising therapeutic scaffolds for a wide range of biomedical applications, such as tissue regeneration and drug delivery. However, their low fracture toughness and brittleness often limit their scope of application. Double-network (DN) hydrogel, which is composed of independently cross-linked rigid and ductile polymer networks, has been proposed as an alternative technique to compensate for the weak mechanical properties of hydrogels. Nevertheless, some challenges still remain, such as the complicated and time-consuming process for DN formation, and the difficulty in controlling the mechanical properties of DN hydrogels. In this study, we introduce a simple, rapid, and controllable method to prepare in situ cross-linkable injectable DN hydrogels composed of acrylamide (AAm) and 4-arm-PPO-PEO-tyramine (TTA) via dual Fenton- and enzyme-mediated reactions. By varying the concentration of Fenton's reagent, the DN hydrogels were rapidly formed with controllable gelation rate. Importantly, the DN hydrogels showed a 13-fold increase in compressive strength and a 14-fold increase in tensile strength, compared to the single network hydrogels. The mechanical properties, elasticity, and plasticity of DN hydrogels could also be modulated by simply varying the preparation conditions, including the cross-linking density and reagent concentrations. At low cross-linker concentration (<0.05 wt %), the plastic DN hydrogel stretched to over 6,500%, whereas high cross-linker concentration (≥0.05 wt %) induced fully elastic hydrogels, without hysteresis. Besides, DN hydrogels were endowed with rapid self-recovery and highly enhanced adhesion, which can be further applied to wearable devices. Moreover, human dermal fibroblasts treated with DN hydrogels retained viability, demonstrating the biocompatibility of the cross-linking system. Therefore, we expect that the dual Fenton-/enzyme-mediated cross-linkable DN hydrogels offer great potential as advanced biomaterials applied for hard tissue regeneration and replacement.

Preparation, structural characterization, and functional properties of wheat gluten amyloid fibrils-chitosan double network hydrogel as delivery carriers for ferulic acid.

It has been demonstrated that ferulic acid (FA) can be effectively encapsulated using wheat gluten amyloid fibrils (AF) and chitosan (CS) in a double network hydrogel (DN) form, with cross-linking mediated by Genipin (GP). Within this system, the DN comprising gluten AF-FA and CS-FA exhibited optimal loading metrics at a formulation designated as DN8, achieving a load efficiency of 88.5 % and a load capacity of 0.78 %. Analysis through fluorescence quenching confirmed that DN8 harbored the highest quantity of FA. Fourier-transform infrared spectroscopy (FTIR) further verified a significant increase in ß-sheet content post-hydrogel formation, enhancing the binding capacity for FA. Rheological assessments indicated a transition from solution to gel, delineating the phase state of the DN. Comprehensive in vitro digestion studies revealed that DN8 provided superior sustained release properties, exhibited the highest total antioxidant capacity, and displayed potent inhibitory activities against angiotensin I converting enzyme (ACE) and acetylcholinesterase (Ach-E). Additionally, the DN significantly bolstered the stability of FA against photothermal degradation. Collectively, these findings lay foundational insights for the advancement of the wheat gluten AF-based delivery system for bioactive compounds and provided a theoretical basis for the development of functional foods.

A Rhodamine-Spiropyran Conjugate Empowering Tunable Mechanochromism in Polymers under Multiple Stimuli.

Mechanochromic functionality realized via the force-responsive mechanophores in polymers has great potential for damage sensing and information storage. Mechanophores with the ability to recognize multiple stimuli for tunable chromic characteristics are highly sought after for versatile sensing ability and color programmability. Nevertheless, the majority of mechanophores are based on single-component chromophores with limited sensitivity, or require additional fabrication technology for multi-modal chromism. Here, we report a novel multifunctional mechanophore capable of vividly detectable and tunable mechanochromism in polymers. This synergistic optical coupling relies on strategically fusing rhodamine and spiropyran (Rh-SP), and tethering polymer chains on both subunits. The mechanochromic behaviors of the Rh-SP-linked polymers under sonication and compression are thoroughly evaluated in response to changes in force and the light-controlled relaxation process. Non-sequential ring-opening of the two subunits under force is identified, endowing high-contrast mechanochromism. Light-induced differential ring-closing reactions of the two subunits, together with the acidichromism of the SP moiety, are employed to engineer elastomers with programmable and wide-spectrum colors. Our work presents an effective strategy for highly appreciable and regulable mechanochromic functionality, and also provides new insights into the rupture mechanisms of π-fused mechanophores, as well as how the stimuli history controls stress accumulation in polymers.

Mechanical and biological behavior of double network hydrogels reinforced with alginate versus gellan gum.

Alginate and gellan gum have both been used by researchers as reinforcing networks to create tough and biocompatible polyethylene glycol (PEG) based double network (DN) hydrogels; however, the relative advantages and disadvantages of each approach are not understood. This study directly compares the mechanical and biological properties of polyethylene glycol di-methacrylate (PEGDMA) hybrid DN hydrogels reinforced with either gellan gum or sodium alginate using PEGDMA concentrations from 10 to 20 wt% and reinforcing network concentrations of 1 and 2 wt%. The findings demonstrate that gellan gum reinforcement is more effective at increasing the strength, stiffness, and toughness of PEGDMA DN hydrogels. In contrast, alginate reinforcement yields DN hydrogels with greater stretchability compared to gellan gum reinforced PEGDMA. Furthermore, separate measurements of toughness via unnotched work of rupture testing and notched fracture toughness testing showed a strong correlation of these two properties for a single reinforcing network type, but not across the two types of reinforcing networks. This suggests that additional notched fracture toughness experiments are important for understanding the full mechanical response when comparing different tough DN hydrogel systems. Regarding the biological response, after conjugation of matrix protein to the surface of both materials robust cell attachment and spreading was supported with higher yes associated protein (YAP) nuclear expression observed in populations adhering to the stiffer gellan gum-PEGDMA material. This study provides valuable insights regarding how to design double network hydrogels for specific property requirements, e.g., for use in biomedical devices, as scaffolding for tissue engineering, or in soft robotic applications.

Digital light processing printed hydrogel scaffolds with adjustable modulus.

Hydrogels are extensively explored as biomaterials for tissue scaffolds, and their controlled fabrication has been the subject of wide investigation. However, the tedious mechanical property adjusting process through formula control hindered their application for diverse tissue scaffolds. To overcome this limitation, we proposed a two-step process to realize simple adjustment of mechanical modulus over a broad range, by combining digital light processing (DLP) and post-processing steps. UV-curable hydrogels (polyacrylamide-alginate) are 3D printed via DLP, with the ability to create complex 3D patterns. Subsequent post-processing with Fe3+ ions bath induces secondary crosslinking of hydrogel scaffolds, tuning the modulus as required through soaking in solutions with different Fe3+ concentrations. This innovative two-step process offers high-precision (10 µm) and broad modulus adjusting capability (15.8-345 kPa), covering a broad range of tissues in the human body. As a practical demonstration, hydrogel scaffolds with tissue-mimicking patterns were printed for cultivating cardiac tissue and vascular scaffolds, which can effectively support tissue growth and induce tissue morphologies.

Naturally derived double-network hydrogels with application as flexible adhesive sensors.

Hydrogels have been widely used in the biomedical field, including wearable sensors and biological adhesives. However, achieving a balance between various functionalities, such as wet adhesion, stable conductivity, and biocompatibility, in one customized hydrogel has been a challenging issue. In this study, we developed a multifunctional hydrogel comprising recombinant human collagen (RHC) and aldehyde-modified sodium alginate (Ald-alginate), which was primarily crosslinked through a Schiff-base reaction and metal chelation. Due to the combination of a dynamic covalent crosslinking network (imine linkage between RHC and Ald-alginate) and a dynamic ionic crosslinking network (ionic bonding between Ca2+ and Ald-alginate), the hydrogel exhibited excellent self-healing and injectable behaviors. Benefiting from the high Ca2+ content, the hydrogel also attained antifreezing and conductivity properties. In addition to its excellent conductivity and biocompatibility, the hydrogel exhibited strong wet tissue adhesion ability and could adhere rapidly and strongly to the surfaces of various objects or biological tissues, forming a good sealing environment. Moreover, the hydrogel could be directly adhered to a tissue surface as a flexible sensor to accurately detect physiological signals. The versatility of this multifunctional hydrogel will open new avenues for biomedical applications, such as bioadhesives and biosensing.