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

• Published in: Nano research 2022-02, Vol.15 (2), p.959-964
• Main Authors: Jiao, Lei, Ye, Wei, Kang, Yikun, Zhang, Yu, Xu, Weiqing, Wu, Yu, Gu, Wenling, Song, Weiyu, Xiong, Yujie, Zhu, Chengzhou
• Format: Article
• Language: English
• Subjects: Ascorbic acid; Atomic/Molecular Structure and Spectra; Biomedicine; Biomimetics; Biosensors; Biotechnology; Catalysis; Catalysts; Chemistry and Materials Science; Colorimetry; Condensed Matter Physics; Cytochrome-c oxidase; Cytochromes; Dispersion; Drinking water; Enzymes; Iron; L-Ascorbate peroxidase; Materials Science; Metal-organic frameworks; Mimicry; NADH; NADH oxidase; NADH peroxidase; Nanomaterials; Nanotechnology; Nicotinamide adenine dinucleotide; Nitrogen; Oxidase; Peroxidase; Research Article; Single atom catalysts
• ISSN: 1998-0124; 1998-0000
• DOI: 10.1007/s12274-021-3581-y

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, Fe 2 NC 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 Fe 2 NC 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 S 2− in tap water is established based on the inhibition of enzyme-like activity of Fe 2 NC nanozymes.