Department of Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), University of Science and Technology of China, Hefei 230026, China.
CAS Key Laboratory of Soft Matter Chemistry, University of Science and Technology of China, Hefei 230026, China.
ACS Appl Mater Interfaces. 2021 Sep 29;13(38):45269-45278. doi: 10.1021/acsami.1c12706. Epub 2021 Sep 14.
Rationally constructing single-atom enzymes (SAEs) with superior activity, robust stability, and good biocompatibility is crucial for tumor therapy but still remains a substantial challenge. In this work, we adopt biocompatible carbon dots as the carrier material to load Ru single atoms, achieving Ru SAEs with superior multiple enzyme-like activity and stability. Ru SAEs behave as oxidase, peroxidase, and glutathione oxidase mimics to synchronously catalyze the generation of reactive oxygen species (ROS) and the depletion of glutathione, thus amplifying the ROS damage and finally causing the death of cancer cells. Notably, Ru SAEs exhibit excellent peroxidase-like activity with a specific activity of 7.5 U/mg, which surpasses most of the reported SAEs and is 20 times higher than that of Ru/C. Theoretical results reveal that the electrons of the Ru 4d orbital in Ru SAEs are transferred to O atoms in HO and then efficiently activate HO to produce OH. Our work may provide some inspiration for the design of SAEs for cancer therapy.
理性构建具有优异活性、强稳定性和良好生物相容性的单原子酶（SAEs）对于肿瘤治疗至关重要，但仍然是一个巨大的挑战。在这项工作中，我们采用生物相容性的碳点作为载体材料来负载 Ru 单原子，从而实现了具有多种酶样活性和稳定性的 Ru SAE。Ru SAE 表现出氧化酶、过氧化物酶和谷胱甘肽氧化酶的模拟物活性，可同步催化活性氧（ROS）的产生和谷胱甘肽的消耗，从而放大 ROS 损伤，最终导致癌细胞死亡。值得注意的是，Ru SAE 表现出优异的过氧化物酶样活性，比活为 7.5 U/mg，超过了大多数报道的 SAE，比 Ru/C 高 20 倍。理论结果表明，Ru SAE 中 Ru 4d 轨道的电子转移到 HO 中的 O 原子上，然后有效地激活 HO 产生 OH。我们的工作可能为癌症治疗中单原子酶的设计提供一些启示。
