writer：Ding Meng, Meng Tian, Song Lingjie, Sun Jian, Wang Lei*, Yin Jinghua, Luan Shifang*.
keywords：artificial enzyme, metal-organic frameworks
source：期刊
specific source：Chemistry of Materials
Issue time：2024年

Abstract:

Oxidase-like artificial enzymes (AEs) are rapidly developing for their attractive reactive oxygen species (ROS)-generating capacity in biological applications. However, efficient strategies to improve AE catalytic performance by modulating the electron transfer (ET) process remain limited. Herein, a new electron transfer pathway in the de novo designed MOFs-based oxidase mimics (ZCA-X) is reported. The electron structure of the active center is regulated to form a unique Au-N-Cu domain for boosting ROS against drug-resistant bacteria. Unlike classical cascade catalytic systems depending on hydrogen peroxide or photocatalysts with complex regulation of band structure, the oxidase-like ZCA-20 catalyzes oxygen reduction via a direct four-ET process without simulation or specific substrate. The Au-N-Cu active domain formed by charge transfer between Au NCs and CuN4 single site exhibits high catalytic efficiency (kcat = 3.61 s-1), generating ROS as intermediate products. ZCA-20 AE is employed in catalytic eradication against drug-resistant bacteria in ROS-mediated structural damage, showing remarkable therapeutic effects both in vitro and in vivo. This strategy to modulate the ET process by coupling different active sites might inspire the development of new AEs with high selectivity and enzymatic activity.