In this work, we have successfully synthesized a bimetallic (Zinc and Cobalt) Zeolitic Imidazolate Framework (Zn50Co50-ZIF), a class in a wider microporous Metal-Organic Framework (MOF) family. The synthesized nanostructures maintain both water stability like ZIF-8 (solely Zn containing) and charge transfer electronic band in the visible optical spectrum as ZIF-67 (solely Co containing). Crystal structure from XRD, high resolution transmission electron microscopy (HRTEM) followed by elemental mapping (EDAX) confirm structural stability and omnipresence of the metal atoms (Zn and Co) across the nanomaterial with equal proportion. Existence of charge transfer state consistent with ZIF67 and intact ultrafast excited state dynamics of the imidazolate moiety in both ZIF-8 and ZIF-67, is evidenced from steady state and time resolved optical spectroscopy. The thermal and aqueous stabilities of Zn50Co50-ZIF are found to be better than ZIF-67 but comparable to ZIF-8 as evidenced by solubility, scanning electron microscopy (SEM) and XRD studies of the material in water. We have evaluated the photoinduced ROS generation by the mixed ZIF employing dichloro-dihydro-fluorescein diacetate (DCFH-DA) assay. We have also explored the potentiality of the synthesized material for the alternate remediation of methicillin resistant Staphylococcus aureus (MRSA) infection through the photoinduced reactive oxygen species (ROS) generation and methylene blue (MB) degradation kinetics.
Aim:To test the potential of orally administered citrate functionalized Mn3O4 nanoparticles (C-Mn3O4 NPs) as a therapeutic agent against hepatic fibrosis and associated chronic liver diseases.Materials & methods:C-Mn3O4 NPs were synthesized and the pH dependent antioxidant mechanism was characterized by in vitro studies. CCl4 intoxicated mice were orally treated with C-Mn3O4 NPs to test its in vivo antioxidant and antifibrotic ability.Results:We demonstrated ultrahigh efficacy of the C-Mn3O4 NPs in treatment of chronic liver diseases such as hepatic fibrosis and cirrhosis in mice compared with conventional medicine silymarin without any toxicological implications.Conclusion:These findings may pave the way for practical clinical use of the NPs as safe medication of chronic liver diseases associated with fibrosis and cirrhosis in human subjects.
Multidrug resistance (MDR) of bacteria is a major threat to public health globally and its unprecedented increase calls for immediate alternative medical strategies. Antimicrobial photodynamic therapy (aPDT) offers alternative modalities to combat the growing MDR typically by means of targeted cellular internalization of a photosensitizer (PS) capable of producing photoinduced reactive oxygen species (ROS). However, aPDT is severely limited by the self-aggregation behavior and hydrophobicity of PS molecules, which significantly curbs its viability for clinical application. The present study reports the use of modified nanoscale metal–organic frameworks (NMOFs) encapsulating a hydrophobic PS drug squaraine (SQ) to enhance aPDT efficacy against drug-resistant planktonic bacteria and its biofilm for the first time. Zeolitic imidazolate framework (ZIF-8) NMOF nanocrystals are attached postsynthetically with SQ (designated as ZIF8-SQ) and the resultant drug-doped NMOF is characterized by TEM, FESEM, PXRD, Raman spectroscopy, UV–vis spectroscopy, and steady-state and time-resolved fluorescence techniques. The microporous structures of ZIF-8 behave as molecular cages ceasing the self-aggregation of hydrophobic SQ. In addition, the formulated ZIF8-SQ produces cytotoxic ROS under red-light irradiation (650 nm) in a pH sensitive way primarily due to molecular level interaction and charge separation between ZIF-8 and SQ depicting a dual-stimuli-responsive nature. Most notably, ZIF8-SQ provides unparalleled aPDT action against methicillin-resistant Staphylococcus aureus (MRSA) and leads to complete loss of adherence of structurally robust bacterial biofilms. Finally, the nontoxic nature of the nanoconjugate toward human cells holds great promise for effective treatment of MRSA and other detrimental antibiotic-resistant microbes in clinical models.
Nanomaterials with antimicrobial properties triggered by external stimuli appear to be a promising and innovative substitute for the destruction of antibiotic-resistant superbugs as they can induce multiple disruptions in the cellular mechanism. This study demonstrates the use of squaraine (SQ) dye as the photosensitive material, activated in the near-infrared tissue-transparent therapeutic window. The dye has been covalently attached to the ZnO nanoparticle surface, forming ZnO-SQ nanohybrids. The formation of the nanohybrids is confirmed using Fourier transform infrared and other optical spectroscopic methods. The photoinduced interfacial electron transfer process (as confirmed using the time-resolved fluorescence technique) from the excited state of SQ to the conduction band of ZnO is responsible for the greater reactive oxygen species (ROS) generation ability of the nanohybrid. The production of photoactivated ROS (especially singlet oxygen species) by ZnO-SQ provides remarkable antimicrobial action against clinically significant Staphylococcus aureus. Detailed investigations suggest synergistic involvement of cell membrane disruption and nanoparticle internalization followed by photoinduced intracellular ROS generation, which result in an unprecedented 95% bacterial killing activity by the nanohybrid. Moreover, the efficacy of the nanohybrid for disruption of bacterial biofilms has been examined. The electron microscopic images suggest significant bacterial cell death following structural alteration and reduced adherence property of the biofilms. Nanodimension-driven greater internalization of ZnO-SQ followed by an improved dissolution of ZnO in an acidic environment of the biofilm as well as red-light-driven interfacial charge separation and ROS generation improves the efficacy of the material for biofilm destruction. An artificial medical implant mimicking titanium sheets coated with ZnO-SQ depicts light-triggered disruption in the adherence property of matured biofilms. The cytotoxicity and hemolysis assays show inherent biocompatibility of the photoactive nanohybrid. This study is notably promising for the treatment of life-threatening drug-resistant infections and eradication of biofilms formed within artificial implants.
Metal exchange process in metallo–curcumin leading to duality in action: enhancement of both aqueous stability and anti-oxidant property.
Near-infrared (NIR) light harvesting has enormous importance for different potential applications in the modern era of research. Some NIR cyanine dyes such as IR820 have achieved great success in energy harvesting and cancer therapy. However, their action is limited for low photostability, considerable thermal degradation, short circulation times, and nonspecific biodistribution. Our present study is an attempt to overcome such limitations by attaching a model cyanine dye IR820 with ZnO nanoparticles. We prepared an IR820-ZnO nanohybrid and characterized it using microscopic and optical spectroscopic tools. Thermogravimetric analysis depicted greater thermal stability of the IR820-ZnO nanohybrid compared to free dye. We explored the enhancement in the photostability of IR820 upon nanohybrid formation. We detected generation of photoinduced reactive oxygen species (ROS) such as superoxide, singlet oxygen, and so forth using appropriate molecular probes. The formation of IR820-ZnO nanohybrid reduced production of photoinduced singlet oxygen. However, it revealed an alternative trend in overall ROS formation (increases total ROS) under red light illumination. To correlate the enhanced photostability of IR820 on the ZnO surface, we explored excited-state dynamical processes at the interface in nanohybrids. We illustrated the photoinduced excited-state electron-transfer process from the lowest unoccupied molecular orbital of IR820 to the conduction band of ZnO. This photoelectron-transfer process enhances the production of ROS and decreases the formation of singlet oxygen that altogether leads to improvement in photostability and overall activity. A quencher of singlet oxygen sodium azide (NaN3) was used to further confirm the direct association of singlet oxygen generation with the photostability issue of IR820. Also, ZnO is able to deliver the dye selectively in acidic environment, which suggests its diseased site-specific targeted activity. Our results provide promising improvement for potential use of IR820 through formation of a nanohybrid that could be translated for other NIR cyanine dyes.
Drug sensitization with various inorganic nanoparticles (NPs) has proved to be a promising and an emergent concept in the field of nanomedicine. Rose bengal (RB), a notable photosensitizer, triggers the formation of reactive oxygen species under green-light irradiation, and consequently, it induces cytotoxicity and cell death. In the present study, the effect of photoinduced dynamics of RB upon complexation with semiconductor zinc oxide NPs is explored. To accomplish this, we successfully synthesized nanohybrids of RB with ZnO NPs with a particle size of 24 nm and optically characterized them. The uniform size and integrity of the particles were confirmed by high-resolution transmission electron microscopy. UV/Vis absorption and steady-state fluorescence studies reveal the formation of the nanohybrids. ultrafast picosecond-resolved fluorescence studies of RB-ZnO nanohybrids demonstrate an efficient electron transfer from the photoexcited drug to the semiconductor NPs. Picosecond-resolved Förster resonance energy transfer from ZnO NPs to RB unravel the proximity of the drug to the semiconductor at the molecular level. The photoinduced ROS formation was monitored using a dichlorofluorescin oxidation assay, which is a conventional oxidative stress indicator. It is observed that the ROS generation under green light illumination is greater at low concentrations of RB-ZnO nanohybrids compared with free RB. Substantial photodynamic activity of the nanohybrids in bacterial and fungal cell lines validated the in vitro toxicity results. Furthermore, the cytotoxic effect of the nanohybrids in HeLa cells, which was monitored by MTT assay, is also noteworthy.
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