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Vol. 11 (2019)

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

https://doi.org/10.1007/s40820-019-0324-7
Ying Wang
Key Laboratory of Automobile Materials of MOE, School of Materials Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun 130012, People’s Republic of China
Kun Qi
Key Laboratory of Automobile Materials of MOE, School of Materials Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun 130012, People’s Republic of China
Shansheng Yu
Key Laboratory of Automobile Materials of MOE, School of Materials Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun 130012, People’s Republic of China
Guangri Jia
Key Laboratory of Automobile Materials of MOE, School of Materials Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun 130012, People’s Republic of China
Zhiliang Cheng
Department of Bioengineering, University of Pennsylvania, 210 South 33rd Street, 240 Skirkanich Hall, Philadelphia, PA 19104, USA
Lirong Zheng
Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100190, People’s Republic of China
Qiong Wu
Key Laboratory of Automobile Materials of MOE, School of Materials Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun 130012, People’s Republic of China
Qiaoliang Bao
Department of Materials Science and Engineering, ARC Centre of Excellence in Future Low‑Energy Electronics Technologies (FLEET), Monash University, Clayton, VIC 3800, Australia
Qingqing Wang
School of Chemistry and Chemical Engineering, MOE Key Laboratory of Micro‑System and Micro‑Structure Manufacturing, Harbin Institute of Technology, Harbin 150001, People’s Republic of China
Jingxiang Zhao
Key Laboratory of Photonic and Electronic Bandgap Materials, Ministry of Education, College of Chemistry and Chemical Engineering, Harbin Normal University, Harbin 150025, People’s Republic of China
Xiaoqiang Cui
Key Laboratory of Automobile Materials of MOE, School of Materials Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun 130012, People’s Republic of China
Weitao Zheng
Key Laboratory of Automobile Materials of MOE, School of Materials Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun 130012, People’s Republic of China

Corresponding Author: Xiaoqiang Cui

xqcui@jlu.edu.cn

Nano-Micro Letters, Vol. 11 (2019), Article Number: 102

Abstract

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–MoS2 (SA Co–MoS2) is demonstrated to have excellent potential as a high-performance peroxidase mimic. Because of the well-defined structure of SA Co–MoS2, 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–MoS2 in the peroxidase-like reaction, SA Co favors electron transfer mechanisms, while MoS2 relies on Fenton-like reactions. The different catalytic pathways provide an intrinsic understanding of the remarkable performance of SA Co–MoS2. 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.


Highlights:


1 Single-atom Co–MoS2 (SA Co–MoS2) is prepared successfully to serve as a proof-of-concept nanozyme model, which exhibits peroxidase-like performance comparable to that of natural enzymes.
2 The different mechanisms between the single-atom metal center and the support are investigated experimentally and theoretically.

Keywords

Biocatalysis Nanozymes Peroxidase mimic Reaction mechanisms Single-atom catalysts
Wang, Ying, Kun Qi, Shansheng Yu, Guangri Jia, Zhiliang Cheng, Lirong Zheng, Qiong Wu, Qiaoliang Bao, Qingqing Wang, Jingxiang Zhao, Xiaoqiang Cui, and Weitao Zheng. 2019. “Revealing the Intrinsic Peroxidase-Like Catalytic Mechanism of Heterogeneous Single-Atom Co–MoS2”. Nano-Micro Letters 11 (November):102. https://doi.org/10.1007/s40820-019-0324-7.
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