Atomically dispersed N-coordinated Fe-Fe dual-sites with enhanced enzyme-like activities

作者：Jiao, Lei; Ye, Wei; Kang, Yikun; Zhang, Yu; Xu, Weiqing; Wu, Yu; Gu, Wenling; Song, Weiyu^*; Xiong, Yujie^*; Zhu, Chengzhou^*

来源：Nano Research, 2022, 15(2): 959-964.

DOI：10.1007/s12274-021-3581-y

• nanozymes
• atomically dispersed dual-metal sites
• oxidase-like activities
• single-atom catalysis
• sensors

Replacement of enzymes with nanomaterials such as atomically dispersed metal catalysts is one of the most crucial steps in addressing the challenges in biocatalysis. Despite the breakthroughs of single-atom catalysts in enzyme-mimicking, a fundamental investigation on the development of an instructional strategy is still required for mimicking biatomic/multiatomic active sites in natural enzymes and constructing synergistically enhanced metal atom active sites. Herein, Fe2NC catalysts with atomically dispersed Fe-Fe dual-sites supported by the metal-organic frameworks-derived nitrogen-doped carbon are employed as biomimetic catalysts to perform proof-of-concept investigation. The effect of Fe atom number toward typical oxidase (cytochrome C oxidase, NADH oxidase, and ascorbic acid oxidase) and peroxidase (NADH peroxidase and ascorbic acid peroxidase) activities is systematically evaluated by experimental and theoretical investigations. A peroxo-like O-2 adsorption in Fe2NC nanozymes could accelerate the O-O activation and thus achieve the enhanced enzyme-like activities. This work achieves the vivid simulation of the enzyme active sites and provides the theoretical basis for the design of high-performance nanozymes. As a concept application, a colorimetric biosensor for the detection of S2- in tap water is established based on the inhibition of enzyme-like activity of Fe2NC nanozymes.

• 单位
  杭州师范大学