Revealing the Intrinsic Peroxidase-Like Catalytic Mechanism of Heterogeneous Single-Atom Co–MoS2

• Published in: Nano-micro letters Vol. 11; no. 1; pp. 1 - 13
• Main Authors: Wang, Ying, Qi, Kun, Yu, Shansheng, Jia, Guangri, Cheng, Zhiliang, Zheng, Lirong, Wu, Qiong, Bao, Qiaoliang, Wang, Qingqing, Zhao, Jingxiang, Cui, Xiaoqiang, Zheng, Weitao
• Format: Journal Article
• Language: English
• Published: Singapore Springer Singapore 01.12.2019; Springer Nature B.V; SpringerOpen
• Subjects: Biocatalysis; Electron transfer; Engineering; Molybdenum disulfide; Nanomaterials; Nanoscale Science and Technology; Nanotechnology; Nanotechnology and Microengineering; Nanozymes; Peroxidase; Peroxidase mimic; Reaction mechanisms; Single-atom catalysts; Substrates; Single-atom catalysts; Biocatalysis; Nanozymes; Reaction mechanisms; Peroxidase mimic
• ISSN: 2311-6706; 2150-5551; 2150-5551
• DOI: 10.1007/s40820-019-0324-7

Highlights Single-atom Co–MoS 2 (SA Co–MoS 2 ) is prepared successfully to serve as a proof-of-concept nanozyme model, which exhibits peroxidase-like performance comparable to that of natural enzymes. The different mechanisms between the single-atom metal center and the support are investigated experimentally and theoretically. The single-atom nanozyme is a new concept and has tremendous prospects to become a next-generation nanozyme. However, few studies have been carried out to elucidate the intrinsic mechanisms for both the single atoms and the supports in single-atom nanozymes. Herein, the heterogeneous single-atom Co–MoS 2 (SA Co–MoS 2 ) is demonstrated to have excellent potential as a high-performance peroxidase mimic. Because of the well-defined structure of SA Co–MoS 2 , its peroxidase-like mechanism is extensively interpreted through experimental and theoretical studies. Due to the different adsorption energies of substrates on different parts of SA Co–MoS 2 in the peroxidase-like reaction, SA Co favors electron transfer mechanisms, while MoS 2 relies on Fenton-like reactions. The different catalytic pathways provide an intrinsic understanding of the remarkable performance of SA Co–MoS 2 . The present study not only develops a new kind of single-atom catalyst (SAC) as an elegant platform for understanding the enzyme-like activities of heterogeneous nanomaterials but also facilitates the novel application of SACs in biocatalysis.