Issue 25, 2022

Biocatalytic cascades and intercommunicated biocatalytic cascades in microcapsule systems

Abstract

Biomolecule-loaded nucleic acid-functionalized carboxymethyl cellulose hydrogel-stabilized microcapsules (diameter ca. 2 μm) are introduced as cell-like containments. The microcapsules are loaded with two DNA tetrahedra, T1 and T2, functionalized with guanosine-rich G-quadruplex subunits, and/or with native enzymes (glucose oxidase, GOx, and/or β-galactosidase, β-gal). In the presence of K+-ions and hemin, the T1/T2 tetrahedra constituents, loaded in the microcapsules, assemble into a hemin/G-quadruplex bridged tetrahedra dimer DNAzyme catalyzing the oxidation of Amplex Red to Resorufin by generating H2O2. In the presence of co-loaded GOx or GOx/β-gal, the GOx//T1/T2 hemin/G-quadruplex cascade catalyzing the glucose-mediated oxidation of Amplex Red to Resorufin, and the three-biocatalysts cascade consisting of β-gal//GOx//hemin/G-quadruplex bridged T1/T2 catalyzing the lactose-driven oxidation of Amplex Red to Resorufin proceed in the microcapsules. Enhanced biocatalytic transformations in the microcapsules, as compared to the performance of the reactions in a homogeneous phase, are observed, due to the proximity of the biocatalysts in a confined volume. As the synthetic methodology to prepare the microcapsules yields boundaries functionalized with complementary nucleic acid tethers, the dynamic association of different microcapsules, loaded selectively with biomolecular catalysts, proceeds. The dynamic dimerization of GOx-loaded microcapsules and hemin/G-quadruplex bridged T1/T2 DNAzyme-loaded microcapsules yields effective intercommunicated microcapsules driving the GOx//hemin/G-quadruplex bridged T1/T2 DNAzyme cascade. In addition, the dynamic dimerization of GOx-loaded microcapsules with β-gal//hemin/G-quadruplex bridged T1/T2-loaded microcapsules enables the bi-directional intercommunicated operation of the lactose-stimulated three catalysts β-gal//GOx//hemin/G-quadruplex bridged T1/T2 DNAzyme cascade. The guided separation and formation of dynamic supramolecular dimer microcapsular containments, and the dictated switchable operation of intercommunicated biocatalytic cascades are demonstrated.

Graphical abstract: Biocatalytic cascades and intercommunicated biocatalytic cascades in microcapsule systems

Supplementary files

Article information

Article type
Edge Article
Submitted
17 mrt 2022
Accepted
29 apr 2022
First published
29 apr 2022
This article is Open Access

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

Chem. Sci., 2022,13, 7437-7448

Biocatalytic cascades and intercommunicated biocatalytic cascades in microcapsule systems

P. Zhang, A. Fischer, Y. Ouyang, J. Wang, Y. S. Sohn, O. Karmi, R. Nechushtai and I. Willner, Chem. Sci., 2022, 13, 7437 DOI: 10.1039/D2SC01542K

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. You can use material from this article in other publications without requesting further permissions from the RSC, provided that the correct acknowledgement is given.

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