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Geometric Tuning of Single-Atom FeN4 Sites via Edge-Generation Enhances Multi-Enzymatic Properties

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Title
Geometric Tuning of Single-Atom FeN4 Sites via Edge-Generation Enhances Multi-Enzymatic Properties
Author(s)
Kang Kim; Jaewoo Lee; Ok Kyu Park; Jongseung Kim; Kim, Jiheon; Lee, Donghyun; Paidi, Vinod K. K.; Euiyeon Jung; Hyeon Seok Lee; Bowon Lee; Chan Woo Lee; Wonjae Ko; Kangjae Lee; Yoon Jung; Lee, Changha; Lee, Nohyun; Back, Seoin; Seung Hong Choi; Taeghwan Hyeon
Publication Date
2023-05
Journal
ADVANCED MATERIALS, v.35, no.19
Publisher
WILEY-V C H VERLAG GMBH
Abstract
Single-atom nanozymes (SAzymes) are considered promising alternatives to natural enzymes. The catalytic performance of SAzymes featuring homogeneous, well-defined active structures can be enhanced through elucidating structure-activity relationship and tailoring physicochemical properties. However, manipulating enzymatic properties through structural variation is an underdeveloped approach. Herein, the synthesis of edge-rich Fe single-atom nanozymes (FeNC-edge) via an H2O2-mediated edge generation is reported. By controlling the number of edge sites, the peroxidase (POD)- and oxidase (OXD)-like performance is significantly enhanced. The activity enhancement results from the presence of abundant edges, which provide new anchoring sites to mononuclear Fe. Experimental results combined with density functional theory (DFT) calculations reveal that FeN4 moieties in the edge sites display high electron density of Fe atoms and open N atoms. Finally, it is demonstrated that FeNC-edge nanozyme effectively inhibits tumor growth both in vitro and in vivo, suggesting that edge-tailoring is an efficient strategy for developing artificial enzymes as novel catalytic therapeutics.
URI
https://pr.ibs.re.kr/handle/8788114/13658
DOI
10.1002/adma.202207666
ISSN
0935-9648
Appears in Collections:
Center for Nanoparticle Research(나노입자 연구단) > 1. Journal Papers (저널논문)
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