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Catalyzed Bimolecular Reactions in Responsive Nanoreactors.

ABSTRACT: We describe a general theory for surface-catalyzed bimolecular reactions in responsive nanoreactors, catalytically active nanoparticles coated by a stimuli-responsive "gating" shell, whose permeability controls the activity of the process. We address two archetypal scenarios encountered in this system: the first, where two species diffusing from a bulk solution react at the catalyst's surface, and the second, where only one of the reactants diffuses from the bulk while the other is produced at the nanoparticle surface, e.g., by light conversion. We find that in both scenarios the total catalytic rate has the same mathematical structure, once diffusion rates are properly redefined. Moreover, the diffusional fluxes of the different reactants are strongly coupled, providing a behavior richer than that arising in unimolecular reactions. We also show that, in stark contrast to bulk reactions, the identification of a limiting reactant is not simply determined by the relative bulk concentrations but is controlled by the nanoreactor shell permeability. Finally, we describe an application of our theory by analyzing experimental data on the reaction between hexacyanoferrate(III) and borohydride ions in responsive hydrogel-based core-shell nanoreactors.

SUBMITTER: Roa R

PROVIDER: S-EPMC5617329 | biostudies-literature | 2017 Sep

REPOSITORIES: biostudies-literature

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Catalyzed Bimolecular Reactions in Responsive Nanoreactors.

Roa Rafael R Kim Won Kyu WK Kanduč Matej M Dzubiella Joachim J Angioletti-Uberti Stefano S

ACS catalysis 20170717 9

We describe a general theory for surface-catalyzed <i>bimolecular</i> reactions in responsive nanoreactors, catalytically active nanoparticles coated by a stimuli-responsive "gating" shell, whose permeability controls the activity of the process. We address two archetypal scenarios encountered in this system: the first, where two species diffusing from a bulk solution react at the catalyst's surface, and the second, where only one of the reactants diffuses from the bulk while the other is produc ...[more]

PMID: 28966839

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Project description:BackgroundPhotodynamic therapy (PDT), a typical reactive oxygen species (ROS)-dependent treatment with high controllability, has emerged as an alternative cancer therapy modality but its therapeutic efficacy is still unsatisfactory due to the limited light penetration and constant oxygen consumption. With the development of another ROS-dependent paradigm ferroptosis, several efforts have been made to conquer the poor efficacy by combining these two approaches; however the biocompatibility, tumor-targeting capacity and clinical translation prospect of current studies still exist great concerns. Herein, a novel hypoxia-responsive nanoreactor BCFe@SRF with sorafenib (SRF) loaded inside, constructed by covalently connecting chlorin e6 conjugated bovine serum albumin (BSA-Ce6) and ferritin through azobenzene (Azo) linker, were prepared to offer unmatched opportunities for high-efficient PDT and ferroptosis synergistic therapy.ResultsThe designed BCFe@SRF exhibited appropriate size distribution, stable dispersity, excellent ROS generation property, controllable drug release capacity, tumor accumulation ability, and outstanding biocompatibility. Importantly, the BCFe@SRF could be degraded under hypoxia environment to release BSA-Ce6 for laser-triggered PDT, ferritin for iron-catalyzed Fenton reaction and SRF for tumor antioxidative defense disruption. Meanwhile, besides PDT effects, it was found that BCFe@SRF mediated treatment upon laser irradiation in hypoxic environment not only could accelerate lipid peroxidation (LPO) generation but also could deplete intracellular glutathione (GSH) and decrease glutathione peroxidase (GPX4) expression, which was believed as three symbolic events during ferroptosis. All in all, the BCFe@SRF nanoreactor, employing multiple cascaded pathways to promote intracellular ROS accumulation, presented remarkably outstanding antitumor effects both in vitro and in vivo.ConclusionBCFe@SRF could serve as a promising candidate for synergistic PDT and ferroptosis therapy, which is applicable to boost oxidative damage within tumor site and will be informative to future design of ROS-dependent therapeutic nanoplatforms.

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Catalyzed Bimolecular Reactions in Responsive Nanoreactors.

Publications

Catalyzed Bimolecular Reactions in Responsive Nanoreactors.

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