Davidenko N, Bax DV, Hunter E
… +6 more, Hamaia SW, Malcor JD, Farndale RW, Sinha S, Best SM, Cameron RE
Biomacromolecules
· 2026 Jun · PMID 42185241
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Although matrix stiffness is an important determinant of cell behavior, experimentally isolating mechanical cues from the surface chemistry is challenging. Here, intact collagen (Col I) or a constant density of collagen-...Although matrix stiffness is an important determinant of cell behavior, experimentally isolating mechanical cues from the surface chemistry is challenging. Here, intact collagen (Col I) or a constant density of collagen-derived cell-adhesive triple-helical peptides (GFOGER or GLOGEN) was deposited on surfaces with physiologically relevant stiffnesses. Equivalent integrin ligation on each surface decoupled stiffness from collagen-receptor ligation. The cell response was highly cell type-specific. Human dermal fibroblast (HDF) adhesion was largely insensitive to matrix stiffness, while cytoskeletal organization was promoted on stiffer substrates, equivalently for GFOGER and GLOGEN. Human umbilical vein endothelial cells (HUVECs) and human dermal microvascular endothelial cells (HDMECs) adhered and formed PECAM-1-containing cell-cell junctions preferentially on lower-modulus substrates. For HUVECs, this was independent of the coating peptide; however, HDMECs possessed greater PECAM-1-containing cell junctions on GFOGER over GLOGEN. These results offer new insights into the effects of stiffness integrin ligation on the cellular response to materials.
Yu X, Li T, Hou X
… +4 more, Qin H, Shi Z, Xiong C, Yang Q
Biomacromolecules
· 2026 Jun · PMID 42179142
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Biobased thermal insulation textiles are attractive for passive body temperature regulation, whereas current fillers and coatings remain relatively thick, fossil-derived, and insufficiently biocompatible. Inspired by dow...Biobased thermal insulation textiles are attractive for passive body temperature regulation, whereas current fillers and coatings remain relatively thick, fossil-derived, and insufficiently biocompatible. Inspired by down feathers, a biobased cellulose/chitin coaxial cryogel fiber (CCF) was fabricated by wet spinning followed by freeze-drying. The CCF comprises a triple-barrier structure consisting of a microporous regenerated cellulose sheath, a trapped-air interfacial layer, and a nanoporous chitin core, which collectively suppress heat transfer. The regenerated cellulose sheath provides sufficient strength and flexibility for weaving into fabrics. With similar thickness and lower areal density, CCF fabrics exhibit a low thermal conductivity of 0.033 W m K and outperform fabrics made from single-component regenerated cellulose or chitin cryogel fibers. They also show better thermal insulation than the representative commercial textiles tested in this study under both high- and low-temperature conditions. This strategy provides a potentially scalable route to biobased thermal insulation textiles without supercritical drying.
Biomacromolecules
· 2026 Jun · PMID 42175893
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In this study, the crystalline structure of silk fibroin was regulated by controlling water molecule states under precise temperature and humidity. Low-field NMR revealed that strong bound water remained stable at 5-6%,...In this study, the crystalline structure of silk fibroin was regulated by controlling water molecule states under precise temperature and humidity. Low-field NMR revealed that strong bound water remained stable at 5-6%, while weak bound water varied significantly with environmental conditions. Thermal analysis showed that glass transition and crystallization temperatures decreased as weak bound water increased. X-ray diffraction indicated that weak bound water critically influences crystallization: at 4-60 °C, exceeding 4% weak bound water induced transformation to Silk I; below this threshold, the amorphous state remained. Above 70 °C, weak bound water dropped below 4%, leading to Silk II formation. Crystallization kinetics and molecular dynamics simulations confirmed that water molecules enhance chain segment mobility, accelerating structural transformation. This work provides a theoretical basis for regulating the processing, storage, and structural stability of protein-based biomaterials under nonphysiological conditions.
Biomacromolecules
· 2026 Jun · PMID 42174378
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Bacterial infections challenge global health due to rising resistance and antibacterial agent inactivation. Encapsulating antibacterial agents into polymeric delivery systems enhances their stability, prolongs circulatio...Bacterial infections challenge global health due to rising resistance and antibacterial agent inactivation. Encapsulating antibacterial agents into polymeric delivery systems enhances their stability, prolongs circulation, and reduces cytotoxicity. However, conventional polymeric carriers lack targeting and controlled release. In recent years, bacterial microenvironment-responsive polymers that react to pH, enzymes, or redox signals have enabled precise targeting and on-demand drug release. This review comprehensively summarizes recent advances in the application of bacterial microenvironment-responsive polymeric carriers for the delivery of antibacterial bioactive agents. Emphasis is placed on elucidating response mechanisms guided by bacterial microenvironmental characteristics, types of polymeric carriers, their applicable scenarios, and the delivery modalities. The review also highlights the advantages, challenges, and opportunities presented by various responsive platforms, offers insights into the material design principles and responsive schemes, and provides a theoretical foundation for the development of next-generation smart antibacterial agent delivery systems.
Jiang Y, Wen H, Xu J
… +5 more, Peng W, Zhou J, Mao H, Gu Z, He Y
Biomacromolecules
· 2026 Jun · PMID 42172545
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The management of chronic diabetic wounds, plagued by persistent oxidative stress, remains a major clinical challenge. We devised a CRISPR/Cas9-based gene therapy to fundamentally reprogram this pathological microenviron...The management of chronic diabetic wounds, plagued by persistent oxidative stress, remains a major clinical challenge. We devised a CRISPR/Cas9-based gene therapy to fundamentally reprogram this pathological microenvironment. A single system was engineered for the simultaneous knockdown of Keap1 and PHD2, key negative regulators of the Nrf2 and HIF-1α pathways, respectively. This payload was delivered by multifunctional peptide-modified lysine dendrimers (MsRNPs), which self-assembled into stable, positively charged nanoparticles that effectively complexed with DNA. The MsRNPs showed excellent biocompatibility and mediated efficient cellular uptake and gene editing in vitro, leading to reduced ROS levels. Consequently, a single topical application of the polyplexes in a diabetic mouse model robustly accelerated wound closure, enhanced collagen deposition, and promoted angiogenesis, driven by the synergistic activation of Nrf2 and HIF-1α. This study establishes a novel combinatorial gene-editing strategy and a versatile nanoplatform for treating oxidative stress-related pathologies.
Zhao J, Li P, Li N
… +7 more, Jin X, Zhang W, Yan Z, Xu Y, Duan B, Yuan J, Song Z
Biomacromolecules
· 2026 Jun · PMID 42167884
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The development of renal-targeting delivery systems has shown great potential to improve the therapeutic efficacy to treat kidney diseases. However, current nanocarriers often exhibit poor targeting efficiency or short r...The development of renal-targeting delivery systems has shown great potential to improve the therapeutic efficacy to treat kidney diseases. However, current nanocarriers often exhibit poor targeting efficiency or short renal retention, limiting their use in drug delivery. Herein, we report the simplified preparation of poly(-serine) (PSer) bearing hydroxyl side chains, which showed enhanced accumulation in kidney in the first several hours post intravenous injection. Starting from unprotected amino acids, the hydrophilic polypeptides were prepared in a two-step synthesis without tedious protection/deprotection procedures. With the improved uptake by renal tubular epithelial cells, PSer outperformed its threonine analogue, with the kidney-to-liver ratio of up to 7.7 (∼9% injected dose in kidney). Finally, the conjugates of PSer with dexamethasone exhibited enhanced therapeutic efficacy than free drug in an animal model of acute kidney injury. We believe this work improves our understanding to design nanomedicine with enhanced kidney accumulation, boosting its use to treat renal diseases.
Huang S, Shen C, Qian Y
… +3 more, Chen S, He J, Zhou C
Biomacromolecules
· 2026 Jun · PMID 42165818
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Microbes, including both Gram-positive and Gram-negative bacteria, contribute to tumor initiation, progression, and metastasis. This complex association requires agents for a concurrent broad-spectrum antibacterial and a...Microbes, including both Gram-positive and Gram-negative bacteria, contribute to tumor initiation, progression, and metastasis. This complex association requires agents for a concurrent broad-spectrum antibacterial and anticancer therapy. Herein, we report a novel dual-hyperbranched strategy that constructs host-defense peptide mimics with a hydrophobic aliphatic acid interlayer and an outer hydrophilic polylysine shell to address this challenge. This unique structure resulted in a shared membranolytic mechanism targeting membranes with excessive negative charges, achieving potent activity against various bacteria and cancer cells. More importantly, the dual-hyperbranched strategy reduces toxicity significantly, which was attributed to the restriction of the mobility of hydrophobic segments. experiments further confirmed these concurrent activities and safety to normal tissues. Collectively, this work provides a new strategy for the design of cationic HDP-mimetic polymers and highlights their potential for integrated antibacterial and anticancer therapy.
Biomacromolecules
· 2026 Jun · PMID 42165447
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ε-Poly-l-lysine (ε-PL) and epigallocatechin-3-gallate (EGCG) possess potent antibacterial properties; however, high aqueous solubility remains a major barrier to their use in stable surface coatings and solid-state syste...ε-Poly-l-lysine (ε-PL) and epigallocatechin-3-gallate (EGCG) possess potent antibacterial properties; however, high aqueous solubility remains a major barrier to their use in stable surface coatings and solid-state systems. To overcome this limitation, we report a green and facile synthesis of novel, insoluble EGCG:ε-PL polymer dots via conjugation at varying stoichiometric ratios. The polymer dots were insoluble in common solvents, displayed excellent solid-state fluorescence, and high biocompatibility (<5% hemolysis at 200 μg/mL). Structural characterizations (SEM, FTIR, XPS, and XRD) confirmed successful formation of the polymer dots. Among the synthesized polymer dots, EGCG:ε-PL (1:2) demonstrated potent broad-spectrum antibacterial activity against and at 10 μg/mL. Notably, they exhibited strong efficacy against clinically isolated multidrug-resistant pathogens, achieving 100% inhibition of at 10 μg/mL and >98% inhibition of methicillin-resistant (MRSA) at 25 μg/mL. Consequently, the polymer dots were successfully applied as antimicrobial coatings on cotton gauze. Mechanistic studies revealed ROS-mediated antibacterial action and membrane disruption, supported by DCFH-DA assays, live/dead staining, and SEM analysis. Furthermore, the dots displayed antioxidant activity, and their intrinsic fluorescence enabled effective bacterial cell labeling and HeLa cell imaging with minimal mammalian cytotoxicity. Overall, EGCG:ε-PL polymer dots represent a sustainable, multifunctional platform for antibacterial coatings and biomedical applications.
Liu J, Wu M, Yan X
… +6 more, Wang H, Chu G, Yang S, Song J, Zhang F, Guo J
Biomacromolecules
· 2026 Jun · PMID 42165112
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Structural color has emerged as a compelling alternative to conventional organic dyes and inorganic pigments, offering advantages including fade-resistant brilliance, eco-friendliness, and versatile functionality across...Structural color has emerged as a compelling alternative to conventional organic dyes and inorganic pigments, offering advantages including fade-resistant brilliance, eco-friendliness, and versatile functionality across numerous technological domains. In this study, we demonstrate the fabrication of cellulosic photonic pigments via shear-induced self-assembly of cholesteric liquid crystalline hydroxypropyl cellulose acrylate (HPCA) microspheres. The as-prepared photonic pigments exhibit vivid noniridescent structural colors with remarkable thermal stability across a broad temperature range of 25-70 °C. We comprehensively studied the internal structure of HPCA microspheres, elucidating the origin of their noniridescent optical properties and revealing the interactions between surfactants and the liquid crystalline HPCA phase during shearing. Moreover, a mask-assisted assembly process was employed to organize HPCA microspheres into region-specific color patterns of diverse shapes, which can act as photonic inks for information encryption and decoding. We envision that the synthesized cholesteric-organized photonic pigments can serve as a sustainable, high-performance alternative to conventional chemical dyes, exhibiting excellent market prospects in sensing, anticounterfeiting, and decorative applications.
Mahecha GL, Montiel A, Cárdenas-Toledo V
… +7 more, Soto-Bahamonde K, Urzua JI, Valenzuela ML, Aguilar-Bolados H, Douglas-Gallardo OA, Werlinger F, Martínez J
Biomacromolecules
· 2026 Jun · PMID 42154970
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This study presents an efficient method for producing biobased oligomers from waste cooking oils (WCOs), a renewable and sustainable feedstock. Epoxidized vegetable oils derived from olive (EOO), sunflower (ESO), and gra...This study presents an efficient method for producing biobased oligomers from waste cooking oils (WCOs), a renewable and sustainable feedstock. Epoxidized vegetable oils derived from olive (EOO), sunflower (ESO), and grape seed (EGSO) oils were copolymerized via ring-opening copolymerization (ROCOP) with cyclic anhydrides such as phthalic and maleic anhydride. The reaction was catalyzed using five ionic liquids as organocatalysts, combined with tetrabutylammonium iodide as a cocatalyst. Among them, 1-butyl-3-methylimidazolium () showed the highest activity, allowing quantitative conversion at 80 °C within 1 h. The resulting oligomers ( = 1021-1732 Da) were characterized by NMR, FT-IR, GPC, and TGA. A mechanistic study supported by NMR and DFT calculations revealed that ionic liquids promote epoxy ring opening through hydrogen-bond stabilization. Overall, the work highlights ionic liquids as effective catalysts for the rapid synthesis of biobased oligoesters via ROCOP.
Kuehl BW, Garg V, Hohmann A
… +10 more, Becker A, Forrester M, Roberts-Dobie J, Knepper J, McCaslin A, Goyal S, Dietrich H, Smith C, Herbst L, Cochran EW
Biomacromolecules
· 2026 Jun · PMID 42154635
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Poly(lactic acid) (PLA) is a leading biobased thermoplastic, but its brittleness limits broader use. Here, we report a one-pot Poly-100 route combining elastomer synthesis, formulation, and reactive extrusion without sol...Poly(lactic acid) (PLA) is a leading biobased thermoplastic, but its brittleness limits broader use. Here, we report a one-pot Poly-100 route combining elastomer synthesis, formulation, and reactive extrusion without solvent removal, purification, or waste generation. Hyperbranched soybean-oil-derived elastomers were synthesized by RAFT polymerization directly in epoxidized soybean oil, which serves as monomer precursor, nonvolatile reaction medium, and formulation component. Poly(acrylated epoxidized high-oleic soybean oil) (PAEHOSO) and poly(methacrylated epoxidized high-oleic soybean oil) (PMAEHOSO) were incorporated into PLA, where residual epoxide groups promote in situ grafting and improve interfacial adhesion. PMAEHOSO showed better compatibility, producing finer dispersions and shifting toughening from interfacial cavitation to matrix shear yielding. At 20 wt % loading, it increased elongation at break from 3% to 30% while delivering the highest tensile toughness. This work establishes a scalable pathway for toughened PLA and demonstrates how reaction media can align polymer performance with sustainability goals.
Li Y, Sun N, Guo Y
… +7 more, Weng X, Wang Y, Zhang M, Ma R, Wang S, Meng F, Yang W
Biomacromolecules
· 2026 Jun · PMID 42151113
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Although immunotherapy displays potent momentum in cancer treatment, its efficacy is limited due to tumor metabolic reprogramming. Aberrant tumor metabolism is pivotal in sustaining tumorigenesis and resulting in immunos...Although immunotherapy displays potent momentum in cancer treatment, its efficacy is limited due to tumor metabolic reprogramming. Aberrant tumor metabolism is pivotal in sustaining tumorigenesis and resulting in immunosuppression, achieved by the secretion of immunosuppressive metabolites as well as the metabolic competition between tumor cells and immune cells. Therefore, interfering with metabolism-immunity crosstalk via regulating tumor cell and immune cell metabolism is a promising strategy for potentiating antitumor immunity. Nanomaterials have been widely applied in cancer therapy as delivery vehicles due to their small size effect, good biocompatibility, high drug bioavailability, and facile synthesis for on-demand release. In this review, tumor metabolic patterns, including glucose metabolism, amino acid metabolism, lipid metabolism, and nucleotide metabolism, along with their characteristics, are first reviewed. The recent progress in nanomaterials-based immunometabolism inhibition of tumor cells, cancer-associated fibroblasts, and tumor-associated macrophages, and the metabolism reinforcement of dendritic cells and T lymphocytes, is then systematically summarized. The limitations, challenges, as well as future perspectives of nanomaterials-guided metabolism-immunity crosstalk are highlighted, underscoring the clinical translation needs of future studies.
De Oliveira S, Rojas T, Miklosic G
… +7 more, Hébert B, Veziers J, Coradin T, Guicheux J, Levisage C, D'Este M, Helary C
Biomacromolecules
· 2026 Jun · PMID 42148511
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Intervertebral disc degeneration is responsible for approximately 40% of low back pain cases and begins in the Nucleus Pulposus before compromising the integrity of the Annulus Fibrosus (AF), ultimately leading to disc h...Intervertebral disc degeneration is responsible for approximately 40% of low back pain cases and begins in the Nucleus Pulposus before compromising the integrity of the Annulus Fibrosus (AF), ultimately leading to disc herniation. Despite its clinical relevance, the pathophysiology remains poorly understood, due to inadequate animal models. In this study, a 3D-printed layered construct was developed to replicate key structural features of the native AF using type I collagen and tyramine-substituted hyaluronic acid (THA). A homogeneous bioink was obtained without polyionic complexation and used to fabricate anisotropic hydrogel layers via 3D printing. Photo-cross-linking of THA enhanced the mechanical properties of the construct. Human fibroblasts were seeded between hydrogel layers and remained viable, proliferated, and aligned along the anisotropic architecture of the construct. These results demonstrate that combining dense collagen with THA through 3D printing provides a promising biopolymer-based strategy for reproducing some essential physical characteristics of the human Annulus Fibrosus.
Chelfouh N, Foran G, Dollé M
… +1 more, Laventure A
Biomacromolecules
· 2026 Jun · PMID 42144701
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The gelation behavior of pectin from apple (AP) and poly(ethylene glycol) (PEG) systems in water offers a promising alternative to conventional high-solids and low-pH pectin gels, which often suffer from syneresis and st...The gelation behavior of pectin from apple (AP) and poly(ethylene glycol) (PEG) systems in water offers a promising alternative to conventional high-solids and low-pH pectin gels, which often suffer from syneresis and strict processing conditions. However, the structural complexity arising from polymer-polymer and polymer-solvent interactions in these systems remains poorly understood, necessitating a deeper characterization of their physicochemical behavior. This knowledge gap is particularly relevant given the sensitivity of gel formation to both composition and processing parameters. Herein, gelation in ternary AP/PEG/water systems is examined across a range of compositions (AP (4-10 wt %) and PEG (40-80 wt %)), using rheology and H NMR spectroscopy to probe the network formation, mechanical properties, and water dynamics. This work demonstrates that PEG acts as a water-activity modulator promoting junction zone formation, and provides a cross-scale mechanistic picture linking molecular water dynamics to macroscopic AP-PEG gel mechanics.
Yang X, Jiang M, Huang Z
… +3 more, Zhang Y, Zhao H, Liu H
Biomacromolecules
· 2026 Jun · PMID 42142081
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Publisher ↗
Wound closure by suture and staple demands surgical skills and carries risks of traumatic complications, whereas current tissue adhesives exhibit insufficient wet adhesion strength, unsatisfactory in vivo biodegradabilit...Wound closure by suture and staple demands surgical skills and carries risks of traumatic complications, whereas current tissue adhesives exhibit insufficient wet adhesion strength, unsatisfactory in vivo biodegradability, and durability. Inspired by the robust underwater adhesion of mussels, whose underwater adhesion derives from the synergy of hydrophobic and adhesive matrix, a tough bioadhesive (PLD) was developed by coassembly of lipoic acid (LA) and a dopamine-functionalized lipoic acid derivative (LAD). Mimicking the mussel's adhesion mechanism, PLD expelled interfacial water via hydrophobic chains, enabling catechol and carboxyl groups to form robust bonds with wet tissue. It exhibited water-strengthened underwater adhesion (approximately from 37.06 to 50.23 kPa after 180 min water immersion) due to water-activated aggregation of hydrophobic chains. Owing to the combined effect of hydrogen bonds, π-π interaction, and hydrophobic associations, PLD displayed durable wet adhesion because it had exceptional antiswelling properties with a remarkably low swelling ratio of 2.07% after 72 h in a physiological environment. In addition, it was bioresorbable, cytocompatible, and histocompatible. The PLD adhesive may offer a promising and multifunctional alternative to conventional sutures for wound closure.
Biomacromolecules
· 2026 Jun · PMID 42141505
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Publisher ↗
Oral insulin delivery represents a compelling alternative to conventional injections because of its enhanced patient compliance and administration convenience. However, this approach faces substantial challenges stemming...Oral insulin delivery represents a compelling alternative to conventional injections because of its enhanced patient compliance and administration convenience. However, this approach faces substantial challenges stemming from physiological barriers that include the gastrointestinal environment, mucus layer obstruction, and poor intestinal absorption. To overcome these limitations, we designed glycosylated proanthocyanidin (PC) nanoparticles using a sacrificial ZIF-8 template for insulin encapsulation. The resulting nanoparticles achieved high loading efficiency and combined two critical functions: gastric protection and enhanced intestinal absorption. Specifically, the nanoparticles preserved insulin stability under acidic gastric conditions and released their payload in response to physiological pH. Furthermore, surface glucose modifications significantly improved the cellular uptake through specific interactions with glucose transporters. When evaluated in a type 1 diabetic mouse model, this Ins@PC@PEG-Glu nanoparticle system showed markedly better therapeutic effects with 7.9% bioavailability, demonstrating its strong potential as an oral insulin delivery platform.
Totani M, Kawano T, Shigeoka M
… +1 more, Kadokawa JI
Biomacromolecules
· 2026 May · PMID 42136047
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Publisher ↗
In this study, a cardanol-bonded chitin was synthesized for the first time via acylation of chitin dissolved in an ionic liquid, 1-allyl-3-methylimidazolium bromide, with an activated cardanol, prepared from 3-pentadecyl...In this study, a cardanol-bonded chitin was synthesized for the first time via acylation of chitin dissolved in an ionic liquid, 1-allyl-3-methylimidazolium bromide, with an activated cardanol, prepared from 3-pentadecylphenoxy acetic acid and 1,1'-carbonyldiimidazole. Although the introduction of cardanol substituents induced no crystallization of the chitin chains and the appearance of a glass transition temperature (), the resulting derivative did not exhibit useful properties, such as thermoplasticity for melt-press processing, due to strong interaction among the cardanol substituents. Therefore, the remaining hydroxy groups were further acylated using several fatty acyl chlorides in a LiCl/DMAc solvent to afford a series of cardanol-bonded mixed chitin esters entirely composed of naturally occurring moieties. The chemical structures and degrees of substitution (DSs) of the products were characterized by IR and H NMR spectroscopies. The obtained cardanol-bonded mixed chitin esters exhibited thermoplastic behavior owing to the reduced interaction among the cardanol substituents, accompanied by the appearance of s, which enabled the film formation by melt-pressing at 150 °C at 15 MPa. The thermal properties of the derivatives, evaluated by differential scanning calorimetric analysis, were systematically discussed in accordance with structures and DSs of the substituents.
Biomacromolecules
· 2026 Jun · PMID 42132458
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Full text
Poly(3-hydroxybutyrate) (PHB) is a biodegradable polyester with a slow hydrolytic degradation rate linked to its high crystallinity. Here, PHB-lignin organogels were prepared using the bio-based solvent Cyrene to investi...Poly(3-hydroxybutyrate) (PHB) is a biodegradable polyester with a slow hydrolytic degradation rate linked to its high crystallinity. Here, PHB-lignin organogels were prepared using the bio-based solvent Cyrene to investigate how processing and lignin type, softwood (SKL) or hardwood (HKL) kraft lignin, affect structure and water stability. Freeze-dried organogels (up to 50 wt % lignin) were analyzed by FTIR spectroscopy, SEM, DSC, and XRD. Organogel formation reduced PHB crystallinity by about 10%, while lignin incorporation further decreased it by up to 84% (SKL) and 73% (HKL), lowering melting enthalpy and promoting cold crystallization. Although HKL caused slightly earlier crystallization suppression during cooling and smaller crystallites at low loadings, both lignin types produced similar crystallinity reductions and degradation behavior. Water exposure increased the mass loss compared with neat PHB, consistent with decreased crystallinity. Solvent extraction enabled partial lignin recovery and PHB recrystallization. Overall, a processing-based approach to tuning PHB crystallinity and degradation in lignin-containing biocomposites is demonstrated.
Rasmussen E, Mohammad SKA, Kelly K
… +8 more, Bounds AG, Hulugalla K, Jankoski P, Stacy E, Jarrett WL, Clemons T, Smith AE, Werfel TA
Biomacromolecules
· 2026 Jun · PMID 42130165
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Publisher ↗
New therapeutic regimens increasingly rely on coordinated, time-dependent delivery of multiple agents, placing new demands on biomaterials capable of precisely regulating release profiles. In this work, azlactone-functio...New therapeutic regimens increasingly rely on coordinated, time-dependent delivery of multiple agents, placing new demands on biomaterials capable of precisely regulating release profiles. In this work, azlactone-functional polymers were cross-linked with poly(ethylene glycol) (PEG) to create a tunable hydrogel platform in which cross-linking density and PEG-diol to PEG-diamine ratio (PEG-OH:PEG-NH) regulate network stability, hydrolytic degradation, and release kinetics. Herein, we evaluate how hydrogel composition influences network characteristics, degradation behavior, and the release of structurally diverse cargos, including small molecules, proteins, and nanoparticles. Across formulations, increasing PEG-OH:PEG-NH accelerated hydrolytic degradation, while decreasing cross-linking density expanded the initial mesh, together leading to differences in release kinetics. These programmable relationships enabled phased, multicargo release of small molecules and antibodies from the same hydrogel. Together, these findings highlight PEG-azlactone hydrogels as a promising platform for programmable, phased delivery of diverse therapeutic cargos.
Yao Y, Pan H, Liu S
… +8 more, Jiang N, Mao X, Hu Z, Yin A, Yan Z, Fan L, Zhang J, Zhang K
Biomacromolecules
· 2026 Jun · PMID 42127361
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Publisher ↗
Silk fibroin (SF) is an attractive matrix for flexible bioelectronics owing to its biocompatibility and chemical tunability, yet its limited mechanical robustness, lack of antibacterial function, and unstable electrical...Silk fibroin (SF) is an attractive matrix for flexible bioelectronics owing to its biocompatibility and chemical tunability, yet its limited mechanical robustness, lack of antibacterial function, and unstable electrical performance constrain its broader application. Here, we report a triple-network ionic hydrogel engineered from methacrylated SF (SFMA), acrylate-terminated silicone (SilMA), and the cationic monomer METAC. The SFMA/SilMA/METAC (SSM) hydrogel forms a uniform interpenetrating network that markedly strengthens mechanical properties, suppresses swelling and component leaching, and achieves >99% antibacterial efficacy against () and (), while preserving excellent cytocompatibility. As a resistive iontronic e-skin, the SSM hydrogel exhibits high pressure sensitivity (2.14 kPa), rapid response/recovery (6/12 ms), a low detection limit of 20 Pa, and long-term stability over 1500 cycles at 20 kPa with <2.3% signal decay. In addition, the hydrogel enables reversible pH sensing across pH 4.00-9.18 with a sensitivity of 21 pH, representing the first demonstration of dual-mode pressure and pH sensing in an SF-based ionic hydrogel. These combined features allow precise monitoring of human motion and underscore the potential of SSM hydrogels for intelligent wound care and implantable bioelectronic interfaces.