Latest ArticlesIn this study, we proposed a novel method to investigate the advanced oxidation process of neonicotinoids (NNIs) from the perspective of concomitant chemiluminescence (CL) reaction. It was found that in the presence of cobalt ions with cyanoimino NNIs, acetamiprid (ACE) and thiacloprid (THI), could promote peroxymonosulfate and Ru(bpy)32+ to produce strong CL, but no CL occurred with nitro-involved NNIs as alternatives. Experimental dada from UV absorption spectra and chemiluminescence spectra suggested that new cyclic compounds might be formed during the reaction. Based on the results of free radical scavenging experiment and mass spectra, a new degradation and reaction mechanism of cyanoimino-containing NNIs was proposed. ACE or THI were first attacked by SO4•− to form benzyl radicals, which in turn reacted with the carbon atoms of cyano group through electrophilic addition reaction in the formation of intramolecular ring. Then a redox reaction between Ru(bpy)33+ and imino group immediately took place with CL emission (610 nm). The new mechanistic knowledge would be meaningful for other contaminants for their interactions with PMS.
Recent studies have proposed that the high-valent iron species (such as FeⅣO2+) rather than sulfate radical (SO4•−) and hydroxyl radical (•OH) are the main reactive oxidant species (ROS) in Fe(Ⅱ)/peroxydisulfate (PDS) system with the methyl phenyl sulfoxide (PMSO) as the FeⅣO2+ probe. However, many operational factors may interfere with the accuracy of this method, so the contribution of FeⅣO2+ calculated by this method is controversial. In this study, the possible effect of Fe(Ⅱ) concentration, pollutant type, reducing agent, or coexisted anions on FeⅣO2+ production and its corresponding contribution to the removal of target pollutants in the Fe(Ⅱ)/PDS system were investigated in detail, and the intrinsic mechanisms involved were also explored. This study shows that ROS generation is a complex process in the Fe(Ⅱ)/PDS system, and multiple combinatorial approaches are urgently required to deeply explore the contribution of ROS to the elimination of target contaminants.
High entropy oxides (HEOs) have attracted extensive attention of researchers due to their remarkable properties. The electrocatalytic activity of electrocatalysts is closely related to the reactivity of their surface atoms which usually shows a positive correlation. Excellenet stability of HEOs leads to their surface atoms with relative poor reactivity, limiting the applications for electrocatalysis. Therefore, it is significant to activate surface atoms of HEOs. Constructing amorphous structure, introducing oxygen defects and leaching are very effective strategies to improve the reactivity of surface atoms. Herein, to remove chemical inert, low-crystallinity (Fe, Co, Ni, Mn, Zn)3O4 (HEO-Origin) nanosheets with abundant oxygen vacancies was synthesized, showing an excellent catalytic activity with an overpotential of 265 mV at 10 mA/cm2, which outperforms as-synthesized HEO-500℃-air (335 mV). The excellent catalytic performance of HEO-Origin can be attributed to high activity surface atoms, the introduction of oxygen defects efficiently altered electron distribution on the surface of HEO-Origin. Apart from, HEO-Origin also exhibits an outstanding electrochemical stability for oxygen evolution reaction (OER).
Compared with noble metals, improving the sensitivity of semiconducting surface-enhanced Raman scattering (SERS) substrates is of great significance to their fundamental research and practical application of Raman spectroscopy. Herein, a simple chemical method is developed to synthesize a rhenium trioxide (ReO3) microtubes assembled with highly crystalline nanoparticles. The ReO3 microtubes show a strong and well-defined surface plasmon resonance (SPR) behavior in visible region, which is rare for non-noble metals. As a low-cost SERS substrate, the plasmonic ReO3 microtubes exhibit a Raman enhancement factor of 8.9 × 105 and a lowest detection limit of 1.0 × 10−9 mol/L for phenolic pollutants. Moreover, these ReO3 microtubule SERS substrates show excellent chemical stability and can resist the corrosion of strong acids and bases.
In this paper, we designed a three-dimensional cell co-cultured microfluidic chip, which generated interstitial flow and oxygen gradient to simulate the complex tumor microenvironment. It consisted of five parallel cell culture channels and one hypoxic channel. These channels were constructed for the culture of mouse liver tumor cells (Hepa1-6), mouse liver stellate cells (JS-1), the simulation of extracellular matrix, complex biochemical factors (hypoxia and interstitial flow), and the supply of cellular nutrients. The 3D-interstitial flow-hypoxia model was used to study the behavior of JS-1 cells under the effect of tumor microenvironment (TME). The results showed that by co-cultured with Hepa1-6 cells, hypoxia of Hepa1-6 cells, and adding TGF-β1 by interstitial flow, the migration of JS-1 cells could be promoted. Similarly, activated JS-1 cells could led to the epithelial-mesenchymal transformation in co-cultured Hepa1-6 cells, which secreted more TGF-β1.
Poly(ethylene glycol)-poly(lactic acid) block copolymer (PEG-PLA) is one of the most widely used biomedical polymers in clinical drug delivery owing to its biocompatibility and biodegradability. However, endowing PEG-PLA micelles with high drug loading, self-assembly stability and fast intracellular drug release is still challenging. Redox-responsive diblock copolymers (MPEG-SS-PMLA) of poly(ethylene glycol) and phenyl-functionalized poly(lactic acid) with disulfide bond as the linker are synthesized to prepare PLA-based micelles that demonstrate excellent colloidal stability and high Ru loading. Notably, MPEG-SS-PMLA achieved a remarkably high Ru loading efficiency of 84.3% due to the existence of strong π-π stacking between phenyl and Ru complex. MPEG-SS-PMLA exhibited good colloidal stability in physiological condition but quickly destabilized by reductive tumor microenvironment. Interestingly, about 74% of Ru complex was released under 10 mmol/L GSH concentration. Ru-loaded MEPG-SS-PMLA showed efficient delivery and release of Ru complex into MCF-7 cancer cells, achieving enhanced in vitro and in vivo antitumor activity of photodynamic therapy. This feasible functionalization method of MPEG-PLA has appeared to be a clinically viable platform for controlled delivery therapeutic agents and enhanced phototherapy.
During the past few years, the construction of BODIPY-based supramolecular fluorescent metallacages through coordination-driven self-assembly has gained increasing interest due to their unique photophysical properties and applications in catalysis, sensing, and bioimaging. In consideration of the rapid development of this field, it is time to summarize recent developments involving BODIPY-based metallacages. In this review, a comprehensive summary of the construction of BODIPY-based metallacages as well as their photophysical properties and applications will be presented.
Nitric oxide (NO) gas therapy has been regarded as a promising strategy for cancer treatment. However, its therapeutic efficiency is still unsatisfying due to the limitations of monotherapy. Previous preclinical and clinical studies have shown that combination therapy could significantly enhance therapeutic efficiency. Herein, a graphene oxide (GO)-L-arginine (L-Arg, a natural NO donor) hybrid nanogenerator is developed followed by surface functionalization of soybean lecithin (SL) for synergistic enhancement of cancer treatment through photothermal and gas therapy. The resultant GO-Arg-SL nanogenerator not only exhibited good biocompatibility and excellent endocytosis ability, but also exhibited excellent photothermal conversion capability and high sensitivity to release NO within tumor microenvironment via inducible NO synthase (iNOS) catalyzation. Moreover, the produced hyperthermia and intracellular NO could synergistically kill cancer cells both in vitro and in vivo. More importantly, this nanogenerator can efficiently eliminate tumor while inhibiting the tumor recurrence because of the immunogenic cell death (ICD) elicited by NIR laser-triggered hyperthermia and the immune response activation by massive NO generation. We envision that the GO-Arg-SL nanogenerator could provide a potential strategy for synergistic photothermal and gas therapy.
A novel thiazolothiazole-bridged imidazole derivative (1) was found to exhibit blue fluorescence in gaseous state or in methanol and yellow fluorescence in solid state. The N-alkylation of imidazole subunit(s) in 1 using n-propyl iodide generated unsymmetrically or symmetrically alkylated thiazolothiazole-bridged imidazolium salts with good water solubility and remarkably strong emission in solution. Furthermore, the replacement of iodide counter-anion by triflate or bis(trifluoromethane sulfonyl)imide achieved remarkably strong emission in solid state and in solution as well as good water solubility. The strong fluorescence of dicationic salts with triflate and NTf2– counter-anions in solid state can be ascribed to their twisted and rigid structures induced by interionic C−H···F hydrogen bonding.
Cell stress responses are associated with numerous diseases including diabetes, neurodegenerative diseases, and cancer. Several events occur under cell stress, in which, are protein expression and organelle-specific pH fluctuation. To understand the lysosomal pH variation under cell stress, a novel NIR ratiometric pH-responsive fluorescent probe (BLT) with lysosomes localization capability was developed. The quinoline ring of BLT combined with hydrogen ion which triggered the rearrangement of π electrons conjugated at low pH medium, meanwhile, the absorption and fluorescent spectra of BLT showed a red-shifts, which gived a ratiometric signal. Moreover, the probe BLT with a suitable pKa value has the potential to discern changes in lysosomal pH, either induced by heat stress or oxidative stress or acetaminophen-induced (APAP) injury stress. Importantly, this ratiometric fluorescent probe innovatively tracks pH changes in lysosome in APAP-induced liver injury in live cells, mice, and zebrafish. The probe BLT as a novel fluorescent probe possesses important value for exploring lysosomal-associated physiological varieties of drug-induced hepatotoxicity.
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