Bridging the Catalytic Turnover Gap Between Single-Atom Iron Nanozymes and Natural Enzymes by Engineering the First and Second Shell Coordination

© 2024 Wiley‐VCH GmbH.

Bibliographische Detailangaben
Veröffentlicht in:Advanced materials (Deerfield Beach, Fla.). - 1998. - 36(2024), 13 vom: 10. März, Seite e2306602
1. Verfasser: Choi, Daeeun (VerfasserIn)
Weitere Verfasser: Jung, Hyeonjung, Im, Jihye, Yi, Seung Yeop, Kim, Seongbeen, Lee, Donghyun, Park, Seonhye, Lee, Changha, Kim, Jaeyun, Han, Jeong Woo, Lee, Jinwoo
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2024
Zugriff auf das übergeordnete Werk:Advanced materials (Deerfield Beach, Fla.)
Schlagworte:Journal Article bioinspired design local coordination environment peroxidase‐like activity single‐atom nanozymes tumor catalytic therapy Iron E1UOL152H7 Carbon 7440-44-0
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520 |a Single-atom nanozymes (SAzymes) constitute a promising category of enzyme-mimicking materials with outstanding catalytic performance. The performance of SAzymes improves through modification of the coordination environments around the metal center. However, the catalytic turnover rates of SAzymes, which are key measures of the effectiveness of active site modifications, remain lower than those of natural enzymes, especially in peroxidase-reactions. Here, the first and second shell coordination tuning strategy that yields SAzymes with structures and activities analogous to those of natural enzymes is reported. The optimized SAzyme exhibits a turnover rate of 52.7 s-1 and a catalytic efficiency of 6.97 × 105 M-1 s-1. A computational study reveals that axial S-ligands induce an alternative reaction mechanism, and SO2- functional groups provide hydrogen bonds to reduce the activation energy. In addition, SAzyme shows superior anti-tumor ability in vitro and in vivo. These results demonstrate the validity of coordination engineering strategies and the carcinostatic potential of SAzymes 
650 4 |a Journal Article 
650 4 |a bioinspired design 
650 4 |a local coordination environment 
650 4 |a peroxidase‐like activity 
650 4 |a single‐atom nanozymes 
650 4 |a tumor catalytic therapy 
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700 1 |a Jung, Hyeonjung  |e verfasserin  |4 aut 
700 1 |a Im, Jihye  |e verfasserin  |4 aut 
700 1 |a Yi, Seung Yeop  |e verfasserin  |4 aut 
700 1 |a Kim, Seongbeen  |e verfasserin  |4 aut 
700 1 |a Lee, Donghyun  |e verfasserin  |4 aut 
700 1 |a Park, Seonhye  |e verfasserin  |4 aut 
700 1 |a Lee, Changha  |e verfasserin  |4 aut 
700 1 |a Kim, Jaeyun  |e verfasserin  |4 aut 
700 1 |a Han, Jeong Woo  |e verfasserin  |4 aut 
700 1 |a Lee, Jinwoo  |e verfasserin  |4 aut 
773 0 8 |i Enthalten in  |t Advanced materials (Deerfield Beach, Fla.)  |d 1998  |g 36(2024), 13 vom: 10. März, Seite e2306602  |w (DE-627)NLM098206397  |x 1521-4095  |7 nnns 
773 1 8 |g volume:36  |g year:2024  |g number:13  |g day:10  |g month:03  |g pages:e2306602 
856 4 0 |u http://dx.doi.org/10.1002/adma.202306602  |3 Volltext 
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