Tianjin Key Laboratory of Low Dimensional Materials Physics and Preparing Technology, Institute of Advanced Materials Physics, School of Sciences, Tianjin University, Tianjin 300350, China.
Tianjin Key Laboratory of Brain Science and Neural Engineering, Academy of Medical Engineering and Translational Medicine, Tianjin University, Tianjin 300072, China.
Nano Lett. 2021 Mar 24;21(6):2562-2571. doi: 10.1021/acs.nanolett.0c05148. Epub 2021 Mar 15.
Natural enzymes are efficient and versatile biocatalysts but suffer in their environmental tolerance and catalytic stability. As artificial enzymes, nanozymes can improve the catalytic stability, but it is still a challenge to achieve high catalytic activity. Here, we employed atomic engineering to build the artificial enzyme named AuAg clusterzyme that hosts an ultrahigh catalytic activity as well as strong physiological stability via atom manipulation. The designed AuAg clusterzyme activates the Ag-S active site via lattice expansion in the oligomer atom layer, showing an antioxidant property 72 times higher than that of natural antioxidant Trolox. Enzyme-mimicked studies find that AuAg clusterzyme exhibits high catalase-like (CAT-like) and glutathione peroxidase-like (GPx-like) activity with a maximum reaction rate of 68.9 and 17.8 μM/min, respectively. Meanwhile, the unique catalytic landscape exhibits distinctive reactions against inflammation by inhibiting the cytokines at an early stage in the brain. Atomic engineering of clusterzymes provides a powerful and attractive platform with satisfactory atomic dispersion for tailoring biocatalysts freely at the atomic level.
天然酶是高效且多功能的生物催化剂,但在环境耐受性和催化稳定性方面存在不足。作为人工酶,纳米酶可以提高催化稳定性,但要实现高催化活性仍然是一个挑战。在这里,我们采用原子工程构建了一种名为 AuAg 团簇酶的人工酶,通过原子操纵,它具有超高的催化活性和强大的生理稳定性。设计的 AuAg 团簇酶通过在低聚物原子层中晶格扩展来激活 Ag-S 活性位点,表现出比天然抗氧化剂 Trolox 高 72 倍的抗氧化性能。酶模拟研究发现,AuAg 团簇酶具有高过氧化氢酶样(CAT 样)和谷胱甘肽过氧化物酶样(GPx 样)活性,最大反应速率分别为 68.9 和 17.8 μM/min。同时,独特的催化景观通过在大脑早期抑制细胞因子来表现出对炎症的明显反应。团簇酶的原子工程提供了一个强大而有吸引力的平台,具有令人满意的原子分散性,可以在原子水平上自由定制生物催化剂。