Li Zhe, Liu Fangning, Chen Chuanxia, Jiang Yuanyuan, Ni Pengjuan, Song Ningning, Hu Yang, Xi Shibo, Liang Minmin, Lu Yizhong
School of Materials Science and Engineering, University of Jinan, Jinan 250022, China.
Experimental Center of Advanced Materials, School of Materials Science & Engineering, Beijing Institute of Technology, Beijing, 100081, China.
Nano Lett. 2023 Feb 22;23(4):1505-1513. doi: 10.1021/acs.nanolett.2c04944. Epub 2023 Feb 3.
Single-atom catalysts with well-defined atomic structures and precisely regulated coordination environments have been recognized as potential substitutes for natural metalloenzymes. Inspired by the metal coordination structure of natural enzymes, we show here that the oxidase-like activity of single-atom Co catalysts greatly depends on their local N coordination around the Co catalytic sites. We synthesized a series of Co single-atom catalysts with different nitrogen coordination numbers (Co-N(C), = 2, 3, and 4) and demonstrated that the oxidase-like activity of single-atom Co catalysts could be effectively tailored by fine-tuning the N coordination. Among the studied single-atom Co catalysts, the Co-N(C) with three-coordinate N atoms shows the optimum oxygen adsorption structure and robust reactive oxygen species (ROS) generation, thus presenting the preferable oxidase-like catalytic activity. This work facilitates the future development of rational nanozyme designs for targeting reactions at the atomic level.
具有明确原子结构和精确调控配位环境的单原子催化剂已被认为是天然金属酶的潜在替代品。受天然酶金属配位结构的启发，我们在此表明单原子钴催化剂的类氧化酶活性很大程度上取决于其钴催化位点周围的局部氮配位。我们合成了一系列具有不同氮配位数（Co-N(C)， = 2、3和4）的钴单原子催化剂，并证明通过微调氮配位可以有效调节单原子钴催化剂的类氧化酶活性。在所研究的单原子钴催化剂中，具有三配位氮原子的Co-N(C)表现出最佳的氧吸附结构和强大的活性氧（ROS）生成能力，从而呈现出更优的类氧化酶催化活性。这项工作有助于未来在原子水平上针对反应的合理纳米酶设计的发展。
