LUMO-Mediated Se and HOMO-Mediated Te Nanozymes for Selective Redox Biocatalysis
Kaijin Liu, Jiaxue Niu, Ling Liu, Fangzhen Tian, Hongmei Nie, Xiaoyu Liu, Ke Chen, Ruoli Zhao, Si Sun, Menglu Jiao, Maoye Tian, Xinyu Sun, Lanfei Niu, Xinyi Sun, Hao Wang, Wei Long, Liefeng Feng, Xiaoyu Mu, Xiaodong Zhang
Abstract
Selenium (Se) and tellurium (Te) nanomaterials with novel chain-like structures have attracted widespread interest owing to their intriguing properties. Unfortunately, the still-unclear catalytic mechanisms have severely limited the development of biocatalytic performance. In this work, we developed chitosan-coated Se nanozymes with a 23-fold higher antioxidative activity than Trolox and bovine serum albumin coated Te nanozymes with stronger prooxidative biocatalytic effects. Based on density functional theory calculations, we first propose that the Se nanozyme with Se/Se 2– active centers favored reactive oxygen species (ROS) clearance via a LUMO-mediated mechanism, while the Te nanozyme with Te/Te 4+ active centers promoted ROS production through a HOMO-mediated mechanism. Furthermore, biological experiments confirmed that the survival rate of γ-irritated mice treated with the Se nanozyme was maintained at 100% for 30 days by inhibiting oxidation. However, the Te nanozyme had the opposite biological effect via promoting radiation oxidation. The present work provides a new strategy for improving the catalytic activities of Se and Te nanozymes.