首页|Geometric and defects engineering collaboration for enhanced cascade enzymatic nanoreactors

Geometric and defects engineering collaboration for enhanced cascade enzymatic nanoreactors

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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-N4 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.

nanozymesingle-atom catalystbioreactorcascade catalysisnon-lnvasive sensing

Zhichao Yu、Ruijin Zeng、Hexiang Gong、Yuan Gao、Shuyun Chen、Yunsen Wang、Dianping Tang

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Key Laboratory for Analytical Science of Food Safety and Biology(MOE & Fujian Province),Department of Chemistry,Fuzhou University,Fuzhou 350108,China

National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of China

222740222187402221675029

2024

10.1007/s12274-023-6119-7

纳米研究(英文版)

纳米研究(英文版)

CSTPCD
ISSN：
年,卷(期)：2024.17(4)
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