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Atomic-Level Regulation of Cobalt Single-Atom Nanozymes: Engineering High-Efficiency Catalase Mimics
Authors:Dr Yuanjun Chen  Dr Bing Jiang  Prof Haigang Hao  Dr Haijing Li  Chenyue Qiu  Xiao Liang  Qingyun Qu  Zedong Zhang  Prof Rui Gao  Prof Demin Duan  Dr Shufang Ji  Prof Dingsheng Wang  Prof Minmin Liang
Institution:1. Department of Chemistry, Tsinghua University, Beijing, 100084 China

Department of Electrical and Computer Engineering, University of Toronto, Toronto, Ontario, M5S1A4 Canada

These authors contributed equally to this work.;2. Experimental Center of Advanced Materials, School of Materials Science & Engineering, Beijing Institute of Technology, Beijing, 100081 China

These authors contributed equally to this work.;3. College of Chemistry and Chemical Engineering, Inner Mongolia University, Hohhot, 010021 China

These authors contributed equally to this work.;4. Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100049 China;5. Department of Materials Science and Engineering, University of Toronto, Toronto, Ontario, M5S3E4 Canada;6. Department of Chemistry, Tsinghua University, Beijing, 100084 China;7. College of Chemistry and Chemical Engineering, Inner Mongolia University, Hohhot, 010021 China;8. CAS Engineering Laboratory for Nanozyme, Institute of Biophysics, Chinese Academic of Science, Beijing, 100101 China;9. Department of Chemistry, University of Toronto, Ontario, M5S3H6 Canada;10. Experimental Center of Advanced Materials, School of Materials Science & Engineering, Beijing Institute of Technology, Beijing, 100081 China

Abstract:Nanozymes aim to mimic the highly evolved active centers of natural enzymes. Despite progress in nanozyme engineering, their catalytic performance is much less favorable compared with natural enzymes. This study shows that precise control over the atomic configuration of the active centers of Co single-atom nanozymes (SAzymes) enables the rational regulation of their catalase-like performance guided by theorical calculations. The constructed Co-N3PS SAzyme exhibits an excellent catalase-like activity and kinetics, exceeding the representative controls of Co-based SAzymes with different atomic configurations. Moreover, we developed an ordered structure-oriented coordination design strategy for rationally engineering SAzymes and established a correlation between the structure and enzyme-like performance. This work demonstrates that precise control over the active centers of SAzymes is an efficient strategy to mimic the highly evolved active sites of natural enzymes.
Keywords:Atomic-Level Regulation  Catalase Mimics  Co Single-Atom  Nanozymes
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