Geometric and defects engineering collaboration for enhanced cascade enzymatic nanoreactors

Highly evolved multi-enzyme cascade catalytic reactions in organisms facilitate rapid transfer of substrates and efficient conversion of intermediates in the catalytic unit, thus rationalizing their efficient biocatalysis. In this study, pore-ordered mesoporous single-atom (Fe) nitrogen-doped carbon...

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Bibliographic Details
Published in:Nano research 2024-04, Vol.17 (4), p.2451-2461
Main Authors: Yu, Zhichao, Zeng, Ruijin, Gong, Hexiang, Gao, Yuan, Chen, Shuyun, Wang, Yunsen, Tang, Dianping
Format: Article
Language:English
Subjects:
Atomic/Molecular Structure and Spectra
Biomedicine
Biotechnology
Carcinogenesis
Carcinogens
Cascade chemical reactions
Catalysis
Catalytic converters
Chemistry and Materials Science
Condensed Matter Physics
Defects
Density functional theory
Electron transfer
Enzymes
Intermediates
Materials Science
Nanotechnology
Nitrogen
Polarity
Pore size
Research Article
Sarcosine
Sarcosine oxidase
Substrates
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Summary:Highly evolved multi-enzyme cascade catalytic reactions in organisms facilitate rapid transfer of substrates and efficient conversion of intermediates in the catalytic unit, thus rationalizing their efficient biocatalysis. In this study, pore-ordered mesoporous single-atom (Fe) nitrogen-doped carbon nanoreactors (Mp-Fe-CN) were designed, in which a reasonable pore size was designed as a natural enzyme trap coupled to a simulated enzyme center. A polarity-mediated strategy was developed to obtain atomically dispersed nanoporous substrates, with the finding that polarity-guided engineering of the nitrogen-ligand environment and vacancy cluster defects clearly affects nanoporous activity, accompanied by appreciable mesoporous pore size elevation. The active center and distal N atom coordination of Fe-N 4 affect the catalytic process of the nanozyme exposed by density functional theory (DFT), determining the contribution of hybridized orbitals to electron transfer and the decisive step. A cascade nanoreactor-based domain-limited sarcosine oxidase developed for non-invasive monitoring of sarcosine levels in urine for evaluation of potential prostate carcinogenesis as a proof of concept. Based on the design of surface mesoporous channels of nanocatalytic units, a bridge was built for the interaction between nanozymes and natural enzymes to achieve cascade nanocatalysis of natural enzymatic products.
ISSN:1998-0124
1998-0000
DOI:10.1007/s12274-023-6119-7