Electron Lock Manipulates the Catalytic Selectivity of Nanozyme

Abstract

Nanomaterials with enzyme-mimicking functions, termed nanozymes, offer attractive opportunities for biocatalysis and biomedicine. However, manipulating nanozyme selectivity poses an insurmountable hurdle. Here, we propose the concept of an energy-governed electron lock that controls electron transfer between nanozyme and substrates to achieve selectivity manipulation of enzyme-like catalysis. An electron lock can be constructed and opened, via modulating the nanozyme's electron energy to match the energy barrier of enzymatic reactions. An iron-doped carbon dot (FeCD) nanozyme with easy-toregulate electron energy is selected as a proof of concept. Through regulating the conduction band which dominates electron energy, activatable oxidase and selective peroxidase (POD) with substrate affinity 123-fold higher than that of natural horseradish peroxidase (HRP) is achieved. Furthermore, while maintaining selectivity, FeCDs exhibit catalytic kinetics comparable to that of HRP upon transforming photons into electrons. Superior selectivity, efficient catalysis, and undetectable biotoxicity energize FeCDs as potent targeted drugs on antibiotic-resistant bacterial abscesses. An electron lock provides a robust strategy to manipulate selectivity toward advanced nanozymes.

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“…Nanozymes are a type of nanomaterial which possess a similar catalytic ability to natural enzymes; since Fe 3 O 4 NPs with peroxidase (POD)-mimicking activity was reported in 2007, a large amount of engineered nanomaterials based nanozymes have been fabricated with excellent enzyme-mimicking catalytic performance. − Recently, due to the horseradish peroxidase (HRP)-like catalytic signal amplification ability, POD-mimicking nanozymes have been combined with LFA for improved colorimetric detection sensitivity. − On the other hand, for nanozymes coupled with LFA, single-mode colorimetric readout may be affected by the experimental environmental interferences, system errors, and batch-to-batch variations; therefore, nanozymes based multimodal signal readout LFA should be developed to ensure that the multiple signals can complement and mutually confirm with each other to improve the accuracy. − In recent years, several nanozyme based multimodal biosensors obtained by using catalytic colorimetric signals combined with fluorescence, photothermal, chemiluminescent, and surface-enhanced Raman scattering (SERS) , have been reported. Among them, plasmonic nanozymes with LSPR (localized surface plasmon resonance) has been of concern due to both the SERS enhancement and enzyme-mimicking catalytic activity of nanozymes.…”

Approach of a small protein to the biomimetic bis-(μ-oxo) dicopper active-site installed in MOF-808 pores with restricted access perturbs substrate selectivity of oxidase nanozyme

“…While several reports highlight complex designs, efficiency, specificity, novel applications and mechanisms of nanozymes, 33–49 the lack of studies on side reactivities that can complicate their mode of action projects a huge gap in this field. We have also been working on the development and addressing challenges of nanozymes and catalysts with enzyme-like functions.…”