Issue 30, 2023

A nucleotide–copper(ii) complex possessing a monooxygenase-like catalytic function

Abstract

The de novo design of artificial biocatalysts with enzyme-like active sites and catalytic functions has long been an attractive yet challenging goal. In this study, we present a nucleotide-Cu2+ complex, synthesized through a one-pot approach, capable of catalyzing ortho-hydroxylation reactions resembling those of minimalist monooxygenases. Both experimental and theoretical findings demonstrate that the catalyst, in which Cu2+ coordinates with both the nucleobase and phosphate moieties, forms a ternary-complex intermediate with H2O2 and tyramine substrates through multiple weak interactions. The subsequent electron transfer and hydrogen (or proton) transfer steps lead to the ortho-hydroxylation of tyramine, where the single copper center exhibits a similar function to natural dicopper sites. Moreover, Cu2+ bound to nucleotides or oligonucleotides exhibits thermophilic catalytic properties within the temperature range of 25 °C to 75 °C, while native enzymes are fully deactivated above 35 °C. This study may provide insights for the future design of oxidase-mimetic catalysts and serve as a guide for the design of primitive metallocentre-dependent enzymes.

Graphical abstract: A nucleotide–copper(ii) complex possessing a monooxygenase-like catalytic function

Supplementary files

Article information

Article type
Paper
Submitted
09 apr 2023
Accepted
20 iyn 2023
First published
21 iyn 2023

J. Mater. Chem. B, 2023,11, 7117-7125

A nucleotide–copper(II) complex possessing a monooxygenase-like catalytic function

H. Wu, S. Xu, P. Du, Y. Liu, H. Li, H. Yang, T. Wang and Z. Wang, J. Mater. Chem. B, 2023, 11, 7117 DOI: 10.1039/D3TB00780D

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