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 jun 2023
First published
21 jun 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

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements