Amorphizing Metal Selenides-Based ROS Biocatalysts at Surface Nanolayer toward Ultrafast Inflammatory Diabetic Wound Healing

Abstract

The microenvironments with high reactive-oxygen-species (ROS) levels, inflammatory responses, and oxidative-stress effects in diabetic ulcer wounds, leading to poor proliferation and differentiation of stem cells, severely inhibit their efficient healing. Here, to overcome the unbalanced multielectron reactions in ROS catalysis, we develop a cobalt selenide-based biocatalyst with an amorphous Ru@CoSe nanolayer for ultrafast and broadspectrum catalytic ROS-elimination. Owing to the enriched electrons and more unoccupied orbitals of Ru atoms, the amorphous Ru@CoSe nanolayer-equipped biocatalyst displays excellent catalase-like kinetics (maximal reaction velocity, 23.05 μM s −1 ; turnover number, 2.00 s −1 ), which exceeds most of the currently reported metal compounds. The theoretical studies show that Ru atoms act as "regulators" to tune the electronic state of the Co sites and modulate the interaction of oxygen intermediates, thus improving the reversible redox properties of active sites. Consequently, the Ru@CoSe can efficiently rescue the proliferation of mesenchymal stem cells and maintain their angiogenic potential in the oxidative stress environment. In vivo experiments reveal the superior ROS-elimination ability of Ru@CoSe on the inflammatory diabetic wound. This study offers an effective nanomedicine for catalytic ROS-scavenging and ultrafast healing of inflammatory wounds and also provides a strategy to design biocatalytic metal compounds via bringing amorphous catalytic structures.

Cascade and Ultrafast Artificial Antioxidases Alleviate Inflammation and Bone Resorption in Periodontitis

“…In the past decade, abundant antioxidative defense strategies based on natural enzymes, artificial enzymes, and antioxidants have been developed to maintain the intracellular redox balance. − In the natural antioxidase systems, superoxide dismutase (SOD) and catalase (CAT) can efficiently eliminate ROS by cascade reactions between SOD (transform ·O 2 – into H 2 O 2 ) and CAT (transform H 2 O 2 into H 2 O and O 2 ) . However, when utilized for clinical treatments, natural enzymes are restricted to abundant intrinsic shortcomings, such as difficult storage, high cost, low stability, and potential immunogenicity .…”

Recent progress in nanozymes for the treatment of diabetic wounds

“…5(A)). 99 The Ru atom acts as a regulator, adjusting the electronic state of the Co Fig. 5 (A) Schematic of the mechanism of Ru@CoSe in diabetic wound healing.…”

“…(D) Ru@CoSe removal of H 2 O 2 . 99 Copyright 2023, American Chemical Society. (E) Preparation of PDMoT hydrogels and dual enzyme activity of MoS 2 @TA/Fe NSs.…”

Determination of the Maximum Velocity of a Peroxidase-like Nanozyme

“…12,13 Among them, peroxidase-like (POD-like) nanozymes, which can catalyze the oxidation of reducing substrates by hydrogen peroxide (H 2 O 2 ), have been studied most by far. 14,15 Demand for kinetic assays of them has been increasing to accurately compare activities, 16,17 deepen insights into catalytic mechanisms, 18,19 and develop highly active POD-like nanozymes with improved application performances. 20,21 The kinetics of catalytic reactions is about variations of their initial velocities (V 0 ) versus reaction conditions like temperature, pH, and substrate concentration.…”

“…Nanozymes, functional nanomaterials with enzyme-like activities, have grabbed much attention for their catalytic activities combined with unique nanoscale properties. − They have been widely used in the fields of bioanalysis, , medical diagnosis, , therapeutics, − and environmental protection. , Among them, peroxidase-like (POD-like) nanozymes, which can catalyze the oxidation of reducing substrates by hydrogen peroxide (H 2 O 2 ), have been studied most by far. , Demand for kinetic assays of them has been increasing to accurately compare activities, , deepen insights into catalytic mechanisms, , and develop highly active POD-like nanozymes with improved application performances. , …”