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In situ surface-enhanced Raman scattering (SERS) spectroscopy is used to identify the key reaction intermediates during the plasma-based removal of NO and SO2 under dry and wet conditions on Ag nanoparticles. Density functional theory (DFT) calculations are used to confirm the experimental observations by calculating the vibrational modes of the surface-bound intermediate species. Here, we provide spectroscopic evidence that the wet plasma increases the SO2 and the NOx removal through the formation of highly reactive OH radicals, driving the reactions to H2SO4 and HNO3, respectively. We observed the formation of SO3 and SO4 species in the SO2 wet-plasma-driven remediation, while in the dry plasma, we only identified SO3 adsorbed on the Ag surface. gp91ds-tat nmr During the removal of NO in the dry and wet plasma, both NO2 and NO3 species were observed on the Ag surface; however, the concentration of NO3 species was enhanced under wet-plasma conditions. By closing the loop between the experimental and DFT-calculated spectra, we identified not only the adsorbed species associated with each peak in the SERS spectra but also their orientation and adsorption site, providing a detailed atomistic picture of the chemical reaction pathway and surface interaction chemistry.The efficiency of PbS quantum dot (QD) solar cells has significantly increased in recent years, strengthening their potential for industrial applications. The vast majority of state-of-the-art devices utilize 1,2-ethanedithiol (EDT)-coated PbS QD hole extraction layers, which lead to high initial performance, but result in poor device stability. While excellent performance has also been demonstrated with organic extraction layers, these devices include a molybdenum trioxide (MoO3) layer, which is also known to decrease device stability. Herein, we demonstrate that organic layers based on a poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] (PTAA) polymer doped with C60F48 can serve as hole extraction layers for efficient EDT-free and MoO3-free QD solar cells. Such layers are shown to offer high conductivity for facile hole transport to the anode, while effectively blocking electrons due to their low electron affinity. We show that our approach is versatile and is applicable also to AgBiS2 QD solar cells.Beer antioxidants originate mainly from malts, classified as colored, caramel, and roasted, according to the malting process. This study aimed to characterize, in terms of phenolic antioxidants, three types of Pale Ale craft beers brewed using increasing percentage of dark malt (0, 5, and 15% Caraamber malt, called PA100, PA95, PA85, respectively) and to evaluate the impact of dealcoholization by osmotic distillation (OD) on the same antioxidants. All the alcoholic (PA, 6.2-6.8 vol %) and low alcoholic (LA-PA, 1 vol %) beers were analyzed by HPLC-ESI-MS/MS, total phenolic content (TPC), and antioxidant activity (AA) similar phenolic profiles were evidenced and 43 compounds identified or tentatively identified. Some differences were found among PA100, PA95, and PA85 PA85 was richer in free phenolic compounds (10.55 mg/L) and had a higher TPC (463.7 GAE mg/L) and AA (852.1 TE mg/L). LA-PA beers showed the same phenolic profile and similar TPC and AA compared to PA beers; however, there were some differences regarding LA-PA85 (5.91 mg/L). Dealcoholization by OD seemed to weakly affect the phenolic fraction. ESI-MS/MS infusion experiments evidenced oligosaccharides, small organic acids, and amino acids, whose presence was confirmed and quantitated by NMR besides ethanol and other alcohols, weak to strong loss of low-molecular-weight metabolites was evidenced in LA-PA beers.Two heterocycle-fused cytochalasan homodimers, bisaspochalasins D (1) and E (2), were isolated from an endophytic Aspergillus flavipes. Their chemical structures were elucidated using a combination of HRESIMS, NMR, theoretical calculations, and crystallographic techniques. Bisaspochalasin D (1) is dimerized by the first reported naturally occurring triple heterobridged 3,8-dioxa-6-azabicyclo[3.2.1]octane framework, while bisaspochalasin E (2) employs a pyrrole ring as the linking moiety. Possible dimerization mechanisms of bisaspochalasins D and E were proposed. The bioassay screening revealed that bisaspochalasin D showed cytotoxic activities against five cancer cell lines (HL-60, SMMC-7721, A-549, MCF-7, and SW-480) with IC50 values ranging from 4.45 to 22.99 μM. Additionally, bisaspochalasin D exhibited neurotrophic activities in a PC12 cell-based assay. At a concentration of 10 μM, bisaspochalasin D can promote neurite growth by inducing a differentiation rate of 12.52% for PC12 cells.Plasmodione (PD) is a potent antimalarial redox-active 3-benzyl-menadione acting at low nanomolar range concentrations on different malaria parasite stages. The specific bioactivation of PD was proposed to occur via a cascade of redox reactions starting from one-electron reduction and then benzylic oxidation, leading to the generation of several key metabolites including corresponding benzylic alcohol (PD-bzol, for PD benzhydrol) and 3-benzoylmenadione (PDO, for PD oxide). In this study, we showed that the benzylic oxidation of PD is closely related to the formation of a benzylic semiquinone radical, which can be produced under two conditions UV photoirradiation or catalysis by Plasmodium falciparum apicoplast ferredoxin-NADP+ reductase (PfFNR) redox cycling in the presence of oxygen and the parent PD. Electrochemical properties of both PD metabolites were investigated in DMSO and in water. The single-electron reduction potential values of PD, PD-bzol, PDO, and a series of 3-benzoylmenadiones were determined according to ascorbate oxidation kinetics. These compounds possess enhanced reactivity toward PfFNR as compared with model quinones. Optimal conditions were set up to obtain the best conversion of the starting PD to the corresponding metabolites. UV irradiation of PD in isopropanol under positive oxygen pressure led to an isolated yield of 31% PDO through the transient semiquinone species formed in a cascade of reactions. In the presence of PfFNR, PDO and PD-bzol could be observed during long lasting redox cycling of PD continuously fueled by NADPH regenerated by an enzymatic system. Finally, we observed and quantified the effect of PD on the production of oxidative stress in the apicoplast of transgenic 3D7[Api-roGFP2-hGrx1] P. falciparum parasites by using the described genetically encoded glutathione redox sensor hGrx1-roGFP2 methodology. The observed fast reactive oxygen species (ROS) pulse released in the apicoplast is proposed to be mediated by PD redox cycling catalyzed by PfFNR.The bioessential nature of cobalt and the rich photochemistry of its coordination complexes can be exploited to develop potential next-generation photochemotherapeutics. A series of six novel mixed-ligand cobalt(III) complexes of the formulation [Co(B)2(L)]ClO4 (1-6), where B is an N,N-donor phenanthroline base, namely, 1,10-phenanthroline (phen in 1 and 4), dipyrido[3,2-d2',3'-f]quinoxaline (dpq in 2 and 5), and dipyrido[3,2-a2',3'-c]phenazine (dppz in 3 and 6), and L is an O,O-donor dianionic ligand derived from catechol (1,2-dihydroxybenzene, cat2-, in 1-3) or esculetin (6,7-dihydoxycoumarin, esc2-, in 4-6), have been prepared and characterized, and their light-triggered cytotoxicity has been studied in cancer cells. The single-crystal X-ray diffraction structures of complexes 1 (as PF6- salt, 1a) and 2 show distorted octahedral geometries around the cobalt(III) center formed by the set of N4O2 donor atoms. The low-spin and 11 electrolytic complexes 1-6 display a d-d transition around 700 nm. Complexes 4-6ercoiled DNA to its nicked circular form when irradiated with visible light via a photoredox type 1 pathway involving hydroxyl radicals (HO•). Thus, complex 6 showing remarkable visible-light-triggered cytotoxicity but negligible toxicity in the dark is a good candidate for cancer photochemotherapy applications.Proteogenomic approaches have enabled the generat̲ion of novel information levels when compared to single omics studies although burdened by extensive experimental efforts. Here, we improved a data-independent acquisition mass spectrometry proteogenomic workflow to reveal distinct molecular features related to mammographic appearances in breast cancer. Our results reveal splicing processes detectable at the protein level and highlight quantitation and pathway complementarity between RNA and protein data. Furthermore, we confirm previously detected enrichments of molecular pathways associated with estrogen receptor-dependent activity and provide novel evidence of epithelial-to-mesenchymal activity in mammography-detected spiculated tumors. Several transcript-protein pairs displayed radically different abundances depending on the overall clinical properties of the tumor. These results demonstrate that there are differentially regulated protein networks in clinically relevant tumor subgroups, which in turn alter both cancer biology and the abundance of biomarker candidates and drug targets.As a new psychoactive substance, abuse of fentanyl (FTN) is currently spreading around the world, resulting in an urgent need of on-site and rapid analytical methods for detection of FTN. Here, we present a synergistic recognition strategy for rapid, cost-effective, selective, sensitive, and visual colorimetric detection of FTN by taking advantage of Rose Bengal (RB) as the specific probe. This assay is based on the halogen- and hydrogen-bonding interactions between them, generating a charge transfer and accompanying a red shift in the RB absorption band as well as color change from red to purple. The utility of the present visual colorimetric assay is demonstrated in aqueous solution, diluted urine, and domestic sewage samples. A detection limit of 0.7 mg·L-1 in aqueous solution is achieved, and the naked-eye detection of FTN is also realized in different real matrices within 6 min. Moreover, this method is insusceptible to interference from various substances (other opioids, cutting agents of street drugs, FTN precursors, amino acids, and small-molecular amines). Additionally, we successfully fabricate a smartphone-based portable device to determine FTN, which is appropriate for field tests. The present work not only provides the first visual assay for FTN but also reveals the molecular structure-property relationship, which will guide the design and development of various probes for recognizing FTN.The expansion of a hexanucleotide repeat GGGGCC (G4C2) in the C9orf72 gene is the most common cause of amyotrophic lateral sclerosis (ALS) and frontotemporal dementia (FTD). The G4C2 expansion leads to repeat-associated non-AUG (RAN) translation and the production of toxic dipeptide repeat (DPR) proteins, but the mechanisms of RAN translation remain enigmatic. Here, we report that the RNA helicase DHX36 is a robust positive regulator of C9orf72 RAN translation. DHX36 has a high affinity for the G4C2 repeat RNA, preferentially binds to the repeat RNA's G-quadruplex conformation, and efficiently unwinds the G4C2 G-quadruplex structures. Native DHX36 interacts with the G4C2 repeat RNA and is essential for effective RAN translation in the cell. In induced pluripotent stem cells and differentiated motor neurons derived from C9orf72-linked ALS patients, reducing DHX36 significantly decreased the levels of endogenous DPR proteins. DHX36 is also aberrantly upregulated in tissues of C9orf72-linked ALS patients. These results indicate that DHX36 facilitates C9orf72 RAN translation by resolving repeat RNA G-quadruplex structures and may be a potential target for therapeutic intervention.
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