Issue 25, 2021

Bound oxygen-atom transfer endows peroxidase-mimic M–N–C with high substrate selectivity

Abstract

Advances in nanoscience have stimulated the wide exploration of nanozymes as alternatives to enzymes. Nonetheless, nanozymes often catalyze multiple reactions and are not specialized to a specific substrate, restricting their broad application. Here, we report that the substrate selectivity of the peroxidase-mimic M–N–C can be significantly altered via forming bound intermediates with variable interactions with substrates according to the type of metal. Taking two essential reactions in chemical sensing as an example, Fe–N–C and Co–N–C showed opposite catalytic selectivity for the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) and 3-aminophthalhydrazide (luminol), respectively, by factors of up to 200-fold. It was revealed that specific transition metal-N coordination was the origin of the selective activation of H2O2 forming critically bound oxygen intermediates (M[double bond, length as m-dash]O) for oxygen-atom transfer and the consequent oxidization of substrates. Notably, owing to the embedded ligands in the rigid graphitic framework, surprisingly, the selectivity of M–N–C was even superior to that of commonly used horseradish peroxidase (HRP).

Graphical abstract: Bound oxygen-atom transfer endows peroxidase-mimic M–N–C with high substrate selectivity

Supplementary files

Article information

Article type
Edge Article
Submitted
17 apr 2021
Accepted
06 may 2021
First published
06 may 2021
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2021,12, 8865-8871

Bound oxygen-atom transfer endows peroxidase-mimic M–N–C with high substrate selectivity

X. Chen, L. Zhao, K. Wu, H. Yang, Q. Zhou, Y. Xu, Y. Zheng, Y. Shen, S. Liu and Y. Zhang, Chem. Sci., 2021, 12, 8865 DOI: 10.1039/D1SC02170B

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