Self-Assembled Multifunctional Nanoreactors for Dephosphorylation Reactions

• Published in: ACS applied nano materials 2021-01, Vol.4 (1), p.644-651
• Main Authors: Demos, Willian, Bittencourt, Catiunaiara R, Nardino, Luigi, Nome, Faruk, Gerola, Adriana P
• Format: Article
• Language: English
• ISSN: 2574-0970; 2574-0970
• DOI: 10.1021/acsanm.0c02943

Nature is a source of inspiration for the self-assembly of functional molecular nanoarchitectures based on intermolecular bonds. This work investigates the self-assembly of molecules (i) polyacrylic acid (PAA, COO– group), (ii) cetyltrimethylammonium (CTA+), and (iii) alkylimidazole (ImR, imidazole group) as building blocks with different properties and functionalities. For the dephosphorylation reaction of diethyl 2,4-dinitrophenyl phosphate (DEDNPP) in aqueous medium, the building blocks PAA, ImR, and CTA+ did not show relevant catalytic activity. An increase in the rate constant was observed from the critical aggregation concentration (CAC) between the polymer and surfactant. This result was related to the formation of hydrophobic pockets of the nanostructured supramolecular complexes. For the PAA/CTAB/ImR system, the formation of hydrophobic microenvironments made it possible to partition the DEDNPP to regions close to the catalytic site. The increase in the rate constant was up to 1.5 × 107-fold higher than that obtained with spontaneous hydrolysis. Thus, the extensive catalytic activity of the self-assembled multicomponent nanoreactor demonstrated potential because of its ease of obtainment and its variety of characteristics. Therefore, the combination of different functional macromolecules is a strategy for the development of inexpensive, efficient, and selective nanocatalysts with characteristics similar to enzymes, the best-known catalysts.