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Research Article

Geometric and defects engineering collaboration for enhanced cascade enzymatic nanoreactors

Zhichao Yu§, Ruijin Zeng§, Hexiang Gong, Yuan Gao, Shuyun Chen, Yunsen Wang, Dianping Tang( )
Key Laboratory for Analytical Science of Food Safety and Biology (MOE & Fujian Province), Department of Chemistry, Fuzhou University, Fuzhou 350108, China

§ Zhichao Yu and Ruijin Zeng contributed equally to this work.

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Graphical Abstract

An efficient natural enzyme-nanozyme co-catalytic nanoreactor was developed for non-invasive prostate cancer surveillance by structural optimization and defect state design with single-atom Fe as the catalytic center.

Abstract

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.

Keywords

nanozymesingle-atom catalystbioreactorcascade catalysisnon-Invasive sensing

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Nano Research
Volume 17 Issue 4,
April 2024
Pages 2451-2461
DOI: 10.1007/s12274-023-6119-7
Cite this article:
Yu Z, Zeng R, Gong H, et al. Geometric and defects engineering collaboration for enhanced cascade enzymatic nanoreactors. Nano Research, 2024, 17(4): 2451-2461. https://doi.org/10.1007/s12274-023-6119-7
Topics:
Enzyme immobilizationMesoporous materials Nanocatalysts

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Received: 14 July 2023
Revised: 08 August 2023
Accepted: 21 August 2023
Published: 30 September 2023
© Tsinghua University Press 2023
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