Spatial engineering of single-atom Fe adjacent to Cu-assisted nanozymes for biomimetic O2 activation

Abstract The precise design of single-atom nanozymes (SAzymes) and understanding of their biocatalytic mechanisms hold great promise for developing ideal bio-enzyme substitutes. While considerable efforts have been directed towards mimicking partial bio-inspired structures, the integration of hetero...

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Main Authors: Ying Wang, Vinod K. Paidi, Weizhen Wang, Yong Wang, Guangri Jia, Tingyu Yan, Xiaoqiang Cui, Songhua Cai, Jingxiang Zhao, Kug-Seung Lee, Lawrence Yoon Suk Lee, Kwok-Yin Wong
Format: Article
Language:English
Published: Nature Portfolio 2024-03-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-024-46528-w
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author Ying Wang
Vinod K. Paidi
Weizhen Wang
Yong Wang
Guangri Jia
Tingyu Yan
Xiaoqiang Cui
Songhua Cai
Jingxiang Zhao
Kug-Seung Lee
Lawrence Yoon Suk Lee
Kwok-Yin Wong
author_facet Ying Wang
Vinod K. Paidi
Weizhen Wang
Yong Wang
Guangri Jia
Tingyu Yan
Xiaoqiang Cui
Songhua Cai
Jingxiang Zhao
Kug-Seung Lee
Lawrence Yoon Suk Lee
Kwok-Yin Wong
author_sort Ying Wang
collection DOAJ
description Abstract The precise design of single-atom nanozymes (SAzymes) and understanding of their biocatalytic mechanisms hold great promise for developing ideal bio-enzyme substitutes. While considerable efforts have been directed towards mimicking partial bio-inspired structures, the integration of heterogeneous SAzymes configurations and homogeneous enzyme-like mechanism remains an enormous challenge. Here, we show a spatial engineering strategy to fabricate dual-sites SAzymes with atomic Fe active center and adjacent Cu sites. Compared to planar Fe–Cu dual-atomic sites, vertically stacked Fe–Cu geometry in FePc@2D-Cu–N–C possesses highly optimized scaffolds, favorable substrate affinity, and fast electron transfer. These characteristics of FePc@2D-Cu–N–C SAzyme induces biomimetic O2 activation through homogenous enzymatic pathway, resembling functional and mechanistic similarity to natural cytochrome c oxidase. Furthermore, it presents an appealing alternative of cytochrome P450 3A4 for drug metabolism and drug–drug interaction. These findings are expected to deepen the fundamental understanding of atomic-level design in next-generation bio-inspired nanozymes.
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spelling doaj.art-12a30d95a3ea441eb0ad34ef80ae72092024-03-17T12:31:50ZengNature PortfolioNature Communications2041-17232024-03-0115111310.1038/s41467-024-46528-wSpatial engineering of single-atom Fe adjacent to Cu-assisted nanozymes for biomimetic O2 activationYing Wang0Vinod K. Paidi1Weizhen Wang2Yong Wang3Guangri Jia4Tingyu Yan5Xiaoqiang Cui6Songhua Cai7Jingxiang Zhao8Kug-Seung Lee9Lawrence Yoon Suk Lee10Kwok-Yin Wong11State Key Laboratory of Chemical Biology and Drug Discovery, Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung HomEuropean Synchrotron Radiation FacilityDepartment of Applied Physics, The Hong Kong Polytechnic University, Hung HomState Key Laboratory of Chemical Biology and Drug Discovery, Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung HomState Key Laboratory of Automotive Simulation and Control, Department of Materials Science, Key Laboratory of Automobile Materials of MOE, Jilin UniversityKey Laboratory of Photonic and Electronic Bandgap Materials of MOE, College of Chemistry and Chemical Engineering, Harbin Normal UniversityState Key Laboratory of Automotive Simulation and Control, Department of Materials Science, Key Laboratory of Automobile Materials of MOE, Jilin UniversityDepartment of Applied Physics, The Hong Kong Polytechnic University, Hung HomKey Laboratory of Photonic and Electronic Bandgap Materials of MOE, College of Chemistry and Chemical Engineering, Harbin Normal UniversityPohang Accelerator Laboratory (PAL), Pohang University of Science and Technology (POSTECH)State Key Laboratory of Chemical Biology and Drug Discovery, Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung HomState Key Laboratory of Chemical Biology and Drug Discovery, Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung HomAbstract The precise design of single-atom nanozymes (SAzymes) and understanding of their biocatalytic mechanisms hold great promise for developing ideal bio-enzyme substitutes. While considerable efforts have been directed towards mimicking partial bio-inspired structures, the integration of heterogeneous SAzymes configurations and homogeneous enzyme-like mechanism remains an enormous challenge. Here, we show a spatial engineering strategy to fabricate dual-sites SAzymes with atomic Fe active center and adjacent Cu sites. Compared to planar Fe–Cu dual-atomic sites, vertically stacked Fe–Cu geometry in FePc@2D-Cu–N–C possesses highly optimized scaffolds, favorable substrate affinity, and fast electron transfer. These characteristics of FePc@2D-Cu–N–C SAzyme induces biomimetic O2 activation through homogenous enzymatic pathway, resembling functional and mechanistic similarity to natural cytochrome c oxidase. Furthermore, it presents an appealing alternative of cytochrome P450 3A4 for drug metabolism and drug–drug interaction. These findings are expected to deepen the fundamental understanding of atomic-level design in next-generation bio-inspired nanozymes.https://doi.org/10.1038/s41467-024-46528-w
spellingShingle Ying Wang
Vinod K. Paidi
Weizhen Wang
Yong Wang
Guangri Jia
Tingyu Yan
Xiaoqiang Cui
Songhua Cai
Jingxiang Zhao
Kug-Seung Lee
Lawrence Yoon Suk Lee
Kwok-Yin Wong
Spatial engineering of single-atom Fe adjacent to Cu-assisted nanozymes for biomimetic O2 activation
Nature Communications
title Spatial engineering of single-atom Fe adjacent to Cu-assisted nanozymes for biomimetic O2 activation
title_full Spatial engineering of single-atom Fe adjacent to Cu-assisted nanozymes for biomimetic O2 activation
title_fullStr Spatial engineering of single-atom Fe adjacent to Cu-assisted nanozymes for biomimetic O2 activation
title_full_unstemmed Spatial engineering of single-atom Fe adjacent to Cu-assisted nanozymes for biomimetic O2 activation
title_short Spatial engineering of single-atom Fe adjacent to Cu-assisted nanozymes for biomimetic O2 activation
title_sort spatial engineering of single atom fe adjacent to cu assisted nanozymes for biomimetic o2 activation
url https://doi.org/10.1038/s41467-024-46528-w
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