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      Photosensitized reactive chlorine species-mediated therapeutic destruction of drug-resistant bacteria using plasmonic core–shell Ag@AgCl nanocubes as an external nanomedicine

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          Abstract

          Due to the rapid growth of drug-resistant bacterial infections, there is an urgent need to develop innovative antimicrobial strategies to conquer the bacterial antibiotic resistance problems.

          Abstract

          Due to the rapid growth of drug-resistant bacterial infections, there is an urgent need to develop innovative antimicrobial strategies to conquer the bacterial antibiotic resistance problems. Although a few nanomaterial-based antimicrobial strategies have been developed, the sensitized formation of cytotoxic reactive chlorine species (RCS), including chlorine gas and chlorine free radicals, by photo-activatable plasmonic nanoparticles for evading drug-resistant bacterial infections has not yet been reported. To address this challenge, herein, we report the synthesis of an unprecedented plasmonic core–shell Ag@AgCl nanocrystal through an in situ oxidation route for the photo-induced generation of highly cytotoxic RCS. We present the detailed in vitro and in vivo investigations of visible light activated Ag@AgCl nanostructure-mediated evasion of drug-resistant bacteria. In particular, the in vivo results demonstrate the complete reepithelialization of the methicillin-resistant Staphylococcus aureus (MRSA) infected wounds on skin upon phototherapeutic treatment mediated Ag@AgCl NCs. To the best of our knowledge, this is the first unique example of using Ag@AgCl NCs as an external nanomedicine for photo-induced generation of RCS to mediate effective killing of both Gram-positive and Gram-negative drug resistance bacteria and healing of the subcutaneous abscesses in an in vivo mouse model.

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          Most cited references45

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          Antibiotic resistance-the need for global solutions.

          The causes of antibiotic resistance are complex and include human behaviour at many levels of society; the consequences affect everybody in the world. Similarities with climate change are evident. Many efforts have been made to describe the many different facets of antibiotic resistance and the interventions needed to meet the challenge. However, coordinated action is largely absent, especially at the political level, both nationally and internationally. Antibiotics paved the way for unprecedented medical and societal developments, and are today indispensible in all health systems. Achievements in modern medicine, such as major surgery, organ transplantation, treatment of preterm babies, and cancer chemotherapy, which we today take for granted, would not be possible without access to effective treatment for bacterial infections. Within just a few years, we might be faced with dire setbacks, medically, socially, and economically, unless real and unprecedented global coordinated actions are immediately taken. Here, we describe the global situation of antibiotic resistance, its major causes and consequences, and identify key areas in which action is urgently needed. Copyright © 2013 Elsevier Ltd. All rights reserved.
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            Negligible particle-specific antibacterial activity of silver nanoparticles.

            For nearly a decade, researchers have debated the mechanisms by which AgNPs exert toxicity to bacteria and other organisms. The most elusive question has been whether the AgNPs exert direct "particle-specific" effects beyond the known antimicrobial activity of released silver ions (Ag(+)). Here, we infer that Ag(+) is the definitive molecular toxicant. We rule out direct particle-specific biological effects by showing the lack of toxicity of AgNPs when synthesized and tested under strictly anaerobic conditions that preclude Ag(0) oxidation and Ag(+) release. Furthermore, we demonstrate that the toxicity of various AgNPs (PEG- or PVP- coated, of three different sizes each) accurately follows the dose-response pattern of E. coli exposed to Ag(+) (added as AgNO(3)). Surprisingly, E. coli survival was stimulated by relatively low (sublethal) concentration of all tested AgNPs and AgNO(3) (at 3-8 μg/L Ag(+), or 12-31% of the minimum lethal concentration (MLC)), suggesting a hormetic response that would be counterproductive to antimicrobial applications. Overall, this work suggests that AgNP morphological properties known to affect antimicrobial activity are indirect effectors that primarily influence Ag(+) release. Accordingly, antibacterial activity could be controlled (and environmental impacts could be mitigated) by modulating Ag(+) release, possibly through manipulation of oxygen availability, particle size, shape, and/or type of coating.
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              Mechanism of photogenerated reactive oxygen species and correlation with the antibacterial properties of engineered metal-oxide nanoparticles.

              Oxidative stress induced by reactive oxygen species (ROS) is one of the most important antibacterial mechanisms of engineered nanoparticles (NPs). To elucidate the ROS generation mechanisms, we investigated the ROS production kinetics of seven selected metal-oxide NPs and their bulk counterparts under UV irradiation (365 nm). The results show that different metal oxides had distinct photogenerated ROS kinetics. Particularly, TiO(2) nanoparticles and ZnO nanoparticles generated three types of ROS (superoxide radical, hydroxyl radical, and singlet oxygen), whereas other metal oxides generated only one or two types or did not generate any type of ROS. Moreover, NPs yielded more ROS than their bulk counterparts likely due to larger surface areas of NPs providing more absorption sites for UV irradiation. The ROS generation mechanism was elucidated by comparing the electronic structures (i.e., band edge energy levels) of the metal oxides with the redox potentials of various ROS generation, which correctly interpreted the ROS generation of most metal oxides. To develop a quantitative relationship between oxidative stress and antibacterial activity of NPs, we examined the viability of E. coli cells in aqueous suspensions of NPs under UV irradiation, and a linear correlation was found between the average concentration of total ROS and the bacterial survival rates (R(2) = 0.84). Although some NPs (i.e., ZnO and CuO nanoparticles) released toxic ions that partially contributed to their antibacterial activity, this correlation quantitatively linked ROS production capability of NPs to their antibacterial activity as well as shed light on the applications of metal-oxide NPs as potential antibacterial agents.
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                Author and article information

                Contributors
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                Journal
                NANOHL
                Nanoscale
                Nanoscale
                Royal Society of Chemistry (RSC)
                2040-3364
                2040-3372
                June 25 2020
                2020
                : 12
                : 24
                : 12970-12984
                Affiliations
                [1 ]Department of Chemistry
                [2 ]National Tsing Hua University
                [3 ]Hsinchu 30013
                [4 ]Republic of China
                [5 ]Department of Biosciences and Bioengineering
                [6 ]Indian Institute of Technology Jodhpur
                [7 ]Jodhpur
                [8 ]India
                [9 ]Department of Biomedical Engineering and Environmental Sciences
                Article
                10.1039/D0NR01300E
                32525500
                d0ca6ffd-861d-4fdc-a1a5-a094c5575aa9
                © 2020

                http://rsc.li/journals-terms-of-use

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