College of Polymer Science and Engineering, Med-X Center for Materials, State Key Laboratory of Polymer Materials Engineering, Sichuan University, Chengdu 610065, China.
Department of Endocrinology, Hospital of Chengdu University of Traditional Chinese Medicine, Chengdu 610072, China.
ACS Nano. 2023 Feb 14;17(3):2943-2957. doi: 10.1021/acsnano.2c11448. Epub 2023 Jan 23.
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 broad-spectrum 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; turnover number, 2.00 s), 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. 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 bringing amorphous catalytic structures.
在糖尿病溃疡伤口中,高活性氧 (ROS) 水平、炎症反应和氧化应激效应的微环境导致干细胞的增殖和分化严重受到抑制,从而严重抑制了其有效的愈合。在这里,为了克服 ROS 催化中不平衡的多电子反应,我们开发了一种基于硒化钴的生物催化剂,具有非晶态 Ru@CoSe 纳米层,用于超快和广谱催化 ROS 消除。由于 Ru 原子的电子丰富和更多未占据轨道,配备非晶态 Ru@CoSe 纳米层的生物催化剂表现出出色的类过氧化物酶动力学(最大反应速度为 23.05 μM s;周转数为 2.00 s),超过了目前大多数报道的金属化合物。理论研究表明,Ru 原子充当“调节剂”来调节 Co 位点的电子状态并调节氧中间体的相互作用,从而改善活性位点的可逆氧化还原性质。因此,Ru@CoSe 可以有效地挽救间充质干细胞的增殖,并在氧化应激环境中维持其血管生成潜力。实验揭示了 Ru@CoSe 在炎症性糖尿病伤口中具有优越的 ROS 消除能力。本研究为催化 ROS 清除和炎症性伤口的超快愈合提供了有效的纳米医学,并为设计具有非晶态催化结构的生物催化金属化合物提供了一种策略。