2024年11月11日，Elsevier 旗下top期刊《Chemical Science》在线发表了云南师范大学化学与化工学院胡蓉教授与杨通副教授最新研究成果《Theory-guided design of S-doped Fe/Co dual-atom nanozymes for highly efficient oxidase mimics》。云南师范大学化学化工学院胡蓉教授、杨通副教授以及昆明理工大学Tang Jian教授为共同通讯作者。

https://pubs.rsc.org/en/content/articlelanding/2024/sc/d4sc03101f

Theory-guided design of S-doped Fe/Co dual-atom nanozymes for highly efficient oxidase mimics†

Huan Cheng,a   Yanyue Chen,a   Mingjia Liu,a   Hongling Tao,a   Lu Chen,a   Fupeng Wang,a   Long Huang,  a   Jian Tang,*c   Tong Yang  *a  and  Rong Hu  *ab  

 Author affiliations

*Corresponding authors

aCollege of Chemistry and Chemical Engineering, Yunnan Normal University, Kunming, Yunnan, P. R. ChinaE-mail: hudierong_168@163.com, yt09132149@163.com, yangtong@ynnu.edu.cn

bMolecular Science and Biomedicine Laboratory, State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Collaborative Innovation Center for Molecular Engineering for Theronastics, Hunan University, Changsha, China

cNational Engineering Research Center of Vacuum Metallurgy, Faculty of Metallurgy and Energy Engineering, Kunming University of Science and Technology, Kunming, Yunnan, ChinaE-mail: tangjian9090@163.com

Abstract

The advent of dual-atom nanozymes (DAzymes) featuring distinctive bimetallic active sites garnered significant attention, representing enhanced iterations of conventional single-atom nanozymes. The quest for an effective and universal strategy to modulate the catalytic activity of DAzymes posed a formidable challenge, yet few published reports addressed this. Herein, we designed and synthesized S-doped Fe/Co DAzymes (S-FeCo-NC) under theoretical guidance and revealed their excellent oxidase-like activity. Experimental and theoretical calculations indicated that the superior oxidase-like activity exhibited by S-FeCo-NC was attributed to the S-doping, which modulated the local electronic structure of the dual-atom active site. This modulation of the local electronic structure significantly optimizes oxygen adsorption energy, thereby accelerating the rate of enzyme-catalyzed reactions. As a proof-of-concept, this study integrated S-FeCo-NC with the cascade inhibition reaction of acetylcholinesterase (AChE) to devise a sensitive analytical platform for detecting organophosphorus pesticides. This study paved the way for elucidating the correlation between the local electronic structure of the active site and enzyme activity, offering novel methodologies and insights for the rational design of DAzymes.

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