Abstract

Emerging artificial enzymes with reprogrammed and augmented catalytic activity and substrate selectivity have long been pursued with sustained efforts. The majority of current candidates have rather poor catalytic activity compared with natural molecules. To tackle this limitation, we design artificial enzymes based on a structurally well-defined Au25 cluster, namely clusterzymes, which are endowed with intrinsic high catalytic activity and selectivity driven by single-atom substitutions with modulated bond lengths. Au24Cu1 and Au24Cd1 clusterzymes exhibit 137 and 160 times higher antioxidant capacities than natural trolox, respectively. Meanwhile, the clusterzymes demonstrate preferential enzyme-mimicking catalytic activities, with Au25, Au24Cu1 and Au24Cd1 displaying compelling selectivity in glutathione peroxidase-like (GPx-like), catalase-like (CAT-like) and superoxide dismutase-like (SOD-like) activities, respectively. Au24Cu1 decreases peroxide in injured brain via catalytic reactions, while Au24Cd1 preferentially uses superoxide and nitrogenous signal molecules as substrates, and significantly decreases inflammation factors, indicative of an important role in mitigating neuroinflammation.

Artificial enzymes with reprogrammed and augmented catalytic activity and substrate selectivity have emerged to tackle limitations of noble metals or transition metal oxides. Here, the authors report Au25 clusterzymes which are endowed with high catalytic activity and selectivity in a range of enzyme-mimicking reactions.

Details

Title
Catalytically potent and selective clusterzymes for modulation of neuroinflammation through single-atom substitutions
Author
Liu, Haile 1 ; Li, Yonghui 1 ; Sun, Si 1 ; Qi, Xin 1 ; Liu Shuhu 2   VIAFID ORCID Logo  ; Mu Xiaoyu 1 ; Yuan Xun 3   VIAFID ORCID Logo  ; Chen, Ke 1 ; Wang, Hao 1 ; Varga Kalman 4 ; Mi Wenbo 1   VIAFID ORCID Logo  ; Jiang, Yang 5 ; Xiao-Dong, Zhang 6 

 Tianjin University, Department of Physics and Tianjin Key Laboratory of Low Dimensional Materials Physics and Preparing Technology, School of Sciences, Tianjin, China (GRID:grid.33763.32) (ISNI:0000 0004 1761 2484) 
 Chinese Academy of Sciences (CAS), Beijing Synchrotron Radiation Facility (BSRF), Institute of High Energy Physics (IHEP), Beijing, China (GRID:grid.9227.e) (ISNI:0000000119573309) 
 Qingdao University of Science and Technology, School of Materials Science and Engineering, Qingdao, China (GRID:grid.412610.0) (ISNI:0000 0001 2229 7077) 
 Vanderbilt University, Department of Physics and Astronomy, Nashville, USA (GRID:grid.152326.1) (ISNI:0000 0001 2264 7217) 
 Sun Yat-sen University, School of Medicine, Guangzhou, China (GRID:grid.12981.33) (ISNI:0000 0001 2360 039X) 
 Tianjin University, Department of Physics and Tianjin Key Laboratory of Low Dimensional Materials Physics and Preparing Technology, School of Sciences, Tianjin, China (GRID:grid.33763.32) (ISNI:0000 0004 1761 2484); Tianjin University, Tianjin Key Laboratory of Brain Science and Neural Engineering, Academy of Medical Engineering and Translational Medicine, Tianjin, China (GRID:grid.33763.32) (ISNI:0000 0004 1761 2484) 
Publication year
2021
Publication date
2021
Publisher
Nature Publishing Group
e-ISSN
20411723
Source type
Scholarly Journal
Language of publication
English
ProQuest document ID
2476049438
Copyright
© The Author(s) 2021. This work is published under http://creativecommons.org/licenses/by/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License.