Notes

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In-sewer stability of human excreted biomarkers is a critical factor of wastewater-based epidemiology in back-estimating illicit drug and pharmaceutical use in the community. Biomarker stability has been investigated in sewers with the presence of biofilms, but the understanding in sewer sediments is still lacking. This study for the first time employed a laboratory sediment reactor to measure 18 illicit drug and pharmaceutical biomarkers under gravity sewer environments with the presence of sediments. Biomarkers exhibited various stability patterns due to transformation processes occurring in the bulk wastewater and sediments. The attenuation of a biomarker by sediments is driven by complex processes involving biodegradation, diffusion, and sorption, which is directly proportional to the ratio of sediment surface area against wastewater volume. The sediment-driven transformation coefficients of biomarkers are higher than the accordingly biofilm-mediated rates because of stronger microbial activities in sediments. Additionally, the stability of most biomarkers was insensitive to the natural pH variation in sewers, except for a few compounds (e.g., methadone, ketamine, and paracetamol) susceptible to pH changes. In general, this study delineates the stability data of various biomarkers in gravity sewers with sediments, which are novel and long-missing information for wastewater-based epidemiology and improve the reliability of back-estimation in complex sewer networks.Blue phosphorescent tetradentate pyridyl-carbolinyl Pt(II) complexes, Pt(ppzOclpy-Me), Pt(ppzOclpy-iPr), and Pt(ppzOclpy-mesi), were purposefully synthesized and investigated with their photophysical and luminescent properties. The complexes, incorporating with carbolinyl moieties, have twisted planar structure. X-ray crystallography revealed that the intraligand N···H-C hydrogen bond reversely turned the twisty pyridyl moiety back into the chelating plane. Computational analyses confirmed that the metal-to-ligand charge-transfer transition character appears in the singlet manifolds. However, the ligand-centered transitions rule in their triplet states, which accounts for the phosphorescent emission. The Pt(II) complexes emit blue light with peak wavelengths (λmax) of 461-481 nm and moderate photoluminescent quantum yields (Φ = 34-46% in dichloromethane and Φ = 44-52% in films). The electroluminescent devices were fabricated by solution processes, giving blue emissions peaking at around 470 nm.Photodynamic therapy (PDT) using two-photon near-infrared light excitation is a very effective way to avoid the use of short-wavelength ultraviolet or visible light which cannot efficiently penetrate into the biological tissues and is harmful to the healthy cells. Herein, a series of cyclometalated Ir(III) complexes with a structurally simple diimine ligand were designed and the synthetic route and preparation procedure were optimized, so that the complexes could be obtained in apparently higher yield, productivity, and efficiency in comparison to the traditional methods. Their ground state and excited singlet and triplet state properties were studied by spectroscopy and quantum chemistry theoretical calculations to investigate the effect of substituent groups on the photophysical properties of the complexes. The Ir(III) complexes, especially Ir1 and Ir3, showed very low dark toxicities and high phototoxicities under both one-photon and two-photon excitation, indicating their great potential as PDT agents. They were also found to be highly sensitive two-photon mitochondria dyes.b-Series gangliosides are abundant in central nervous tissues and are involved in important nerve processes. However, their functions are complicated because of their properties of forming dynamic domains in cell plasma membranes (PMs), called lipid rafts. In this study, we aim to develop fluorescently labeled b-series gangliosides that are useful for single-molecule imaging. The chemical synthesis of fluorescent GD3 and GQ1b was achieved using sialylation and ganglioside synthetic methods previously developed by our group. Furthermore, biophysical evaluations demonstrated that synthesized fluorescent GD3 and GQ1b behaved as raft molecules on cell PMs, suggesting their applicability to the study of raft-associated interactions.ChaP is a non-heme iron-dependent dioxygenase belonging to the vicinal oxygen chelate (VOC) enzyme superfamily that catalyzes the final α-pyrone ring formation in the biosynthesis of chartreusin. In contrast to other common dioxygenases, for example, 2,3-catechol dioxygenase which uses the dioxygen molecule as the oxidant, ChaP requires the flavin-activated oxygen (O22-) as the equivalent. Previous experiments showed that the ChaP-catalyzed ring rearrangement contains two successive C-C bond cleavages and one lactonization; however, the detailed reaction mechanism is unknown. In this work, on the basis of the recently obtained crystal structure of ChaP, the computational model was constructed and the catalytic mechanism of ChaP was explored by performing quantum mechanical/molecular mechanical (QM/MM) calculations. Our calculation results reveal that ChaP uses the proximal oxygen in iron-coordinated HOO- to attack the carbonyl carbon of the substrate, whereas the previous proposal that Asp49 acts as a base to deprotonate the iron-coordinated HOO- to generate O22- is unlikely. In the first stage reaction, owing to the coordination of the substrate with iron, the substrate is activated by accepting an electron from iron and the resulting oxy-radical intermediate formed by O-O cleavage can easily trigger the ring rearrangement. In the final decarboxylation, the phenolic anion of the substrate cooperatively accepts the proton of iron-coordinated HOO- to facilitate the attack of the distal oxygen, and the proton-coupled electron transfer (PCET) from the substrate to the FeIV═O plays a key role for the decarboxylation. These findings may provide useful information for understanding the ChaP-catalyzed oxidative rearrangement and other flavin-dependent non-heme dioxygenases.One 14-metal Yb(III) nanoring [Yb14(HL)2L20(DMF)8(H2O)8] (1) with a size of about 1.1 × 2.5 × 2.7 nm was synthesized from a tridentate ligand. LY3522348 Under the excitation of ligand absorption bands, 1 exhibits the NIR luminescence of Yb(III) and displays high luminescence sensitivity and selectivity to Co(II), Cu(II), and 2,4,6-trinitrophenol (PA) at the parts per million level. The KSV values of 1 to Co(II), Cu(II), and PA are 6.0 × 104 M-1, 3.8 × 104 M-1, and 6.9 × 104 M-1, respectively. 1 exhibits high luminescent sensitivity to PA even in the presence of other explosives.
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