Catalytically potent and selective clusterzymes for modulation of neuroinflammation through single-atom substitutions

Haile Liu, Yonghui Li, Si Sun, Qi Xin, Shuhu Liu, Xiaoyu Mu, Xun Yuan, Ke Chen, Hao Wang, Kalman Varga, Wenbo Mi, Jiang Yang and Xiao-Dong Zhang ()
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Haile Liu: Tianjin University
Yonghui Li: Tianjin University
Si Sun: Tianjin University
Qi Xin: Tianjin University
Shuhu Liu: Chinese Academy of Sciences (CAS)
Xiaoyu Mu: Tianjin University
Xun Yuan: Qingdao University of Science and Technology
Ke Chen: Tianjin University
Hao Wang: Tianjin University
Kalman Varga: Vanderbilt University
Wenbo Mi: Tianjin University
Jiang Yang: Sun Yat-sen University
Xiao-Dong Zhang: Tianjin University

Nature Communications, 2021, vol. 12, issue 1, 1-14

Abstract: 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.

Date: 2021
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DOI: 10.1038/s41467-020-20275-0

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