Injectable silk fibroin hydrogel encapsulating pH-Responsive ZnS nanoparticles for synergistic redox modulation and diabetic wound healing

Dec 27, 2025Biomaterials advances

Injectable silk protein gel with pH-sensitive zinc sulfide nanoparticles for improving diabetic wound healing through combined redox balance

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Regenerative Health on OpenScience ↗PubMed ↗DOI ↗

Abstract

The injectable SF/ZnS hydrogel significantly accelerated wound closure in a diabetic mouse model.

The hydrogel is composed of methacrylated silk fibroin and pH-sensitive zinc sulfide nanoparticles.
Zinc sulfide nanoparticles provide controlled release of therapeutic hydrogen sulfide and zinc under varying pH conditions.
In vitro studies indicate that the nanoparticles effectively scavenge reactive oxygen species and support cell function.
The SF/ZnS hydrogel promotes macrophage polarization towards a reparative M2 phenotype.
In addition to enhancing wound healing, the hydrogel mitigates chronic inflammation and improves collagen remodeling.

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Chronic diabetic wounds remain a major clinical challenge due to excessive reactive oxygen species (ROS), persistent inflammation, and impaired cellular function. Current wound dressings offer limited capacity to simultaneously regulate redox imbalance and support tissue regeneration, highlighting the necessity for adaptive, intelligent, and multifunctional platforms for regenerative therapy. Herein, we developed an injectable hydrogel system composed of methacrylated silk fibroin (SilMA) and aqueous-phase, pH-sensitive zinc sulfide nanoparticles (ZnS NPs). Spherical ZnS NPs were synthesized via a green aqueous-phase hydrothermal method, offering stable colloidal properties and controlled release of therapeutic H₂S and Znunder different pH conditions. Upon UV crosslinking, SilMA formed a porous, shear-thinning hydrogel (SF hydrogel) that facilitates in situ application and localized drug delivery. ZnS NPs were loaded into SF hydrogels and the resulting SF/ZnS hydrogel exhibited suitable mechanical strength, swelling and biodegradability for wound healing application. In vitro studies demonstrated the ZnS NPs' potent ROS-scavenging capacity and cytocompatibility, while the SF/ZnS hydrogel effectively restored fibroblasts and endothelial cells' function under oxidative stress and promoted macrophage polarization toward a reparative M2 phenotype. In a streptozotocin-induced diabetic mouse model, SF/ZnS hydrogel significantly accelerated wound closure, enhanced re-epithelialisation and collagen remodelling, and promoted neovascularization, while mitigating chronic inflammation. The SF/ZnS hydrogel developed in this study presents a promising therapeutic platform for chronic diabetic wounds, integrating redox regulation, immunomodulation, and regenerative enhancement within a single injectable system. 2+

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Injectable silk fibroin hydrogel encapsulating pH-Responsive ZnS nanoparticles for synergistic redox modulation and diabetic wound healing

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