Notes

Multi-omics profiling: just how in the direction of precision treatments throughout metabolism conditions.
The substantial increase in multidrug-resistant (MDR) pathogenic bacteria is a major threat to global health. Recently, the Centers for Disease Control and Prevention reported possibilities of greater deaths due to bacterial infections than cancer. Nanomaterials, especially small-sized (size ≤10 nm) silver nanoparticles (AgNPs), can be employed to combat these deadly bacterial diseases. However, high reactivity, instability, susceptibility to fast oxidation, and cytotoxicity remain crucial shortcomings for their uptake and clinical application. In this review, we discuss various AgNPs-based approaches to eradicate bacterial infections and provide comprehensive mechanistic insights and recent advances in antibacterial activity, antibiofilm activity, and cytotoxicity (both in vitro and in vivo) of AgNPs. The mechanistic of antimicrobial activity involves four steps (i) adhesion of AgNPs to cell wall/membrane and its disruption; (ii) intracellular penetration and damage; (iii) oxidative stress; and (iv) modulation of signal transduction pathways. Numerous factors affecting the bactericidal activity of AgNPs such as shape, size, crystallinity, pH, and surface coating/charge have also been described in detail. The review also sheds light on antimicrobial photodynamic therapy and the role of AgNPs versus Ag+ ions release in bactericidal activities. In addition, different methods of synthesis of AgNPs have been discussed in brief.Phosphorus (P) is present in activated sludge from wastewater treatment plants in the form of metal salt precipitates, extracellular polymeric substances, or bound into the biomass, for example, as intracellular polyphosphate (poly-P). Several methods for a reliable quantification of the different P-fractions have recently been developed, and this study combines them to obtain a comprehensive P mass-balance of activated sludge from four enhanced biological phosphate removal (EBPR) plants. Chemical characterization by ICP-OES and sequential P fractionation showed that chemically bound P constituted 38-69% of total P, most likely in the form of Fe, Mg, or Al minerals. Raman microspectroscopy, solution state 31P NMR, and 31P MAS NMR spectroscopy applied before and after anaerobic P-release experiments, were used to quantify poly-P, which constituted 22-54% of total P and was found in approximately 25% of all bacterial cells. Raman microspectroscopy in combination with fluorescence in situ hybridization was used to quantify poly-P in known polyphosphate-accumulating organisms (PAO) (Tetrasphaera, Candidatus Accumulibacter, and Dechloromonas) and other microorganisms known to possess high level of poly-P, such as the filamentous Ca. Sanguinarine solubility dmso Microthrix. Interestingly, only 1-13% of total P was stored by unidentified PAO, highlighting that most PAOs in the full-scale EBPR plants investigated are known.Reactive oxygen species (ROS) are an important component for maintaining normal physiological activities in organisms, and abnormal changes in their level are often accompanied by many diseases. As the two most representative components of ROS, HClO and H2O2 play vital roles in many physiological and pathological processes and are interdependent and mutually transformable. Although there is a lot of work that has specifically detected HClO or H2O2, there are few reports on the simultaneous differential detection of HClO and H2O2. Here, we report a ratio-based fluorescent probe capable of simultaneously distinguishing HClO and H2O2 based on making the best use of the untapped potential of coumarin derivatives. This probe was triumphantly put into use in the discriminative identification of HClO and H2O2 in aqueous media with high sensitivity and selectivity, and the probe was appropriate in a wide pH range. Furthermore, the imaging experiment for HClO and H2O2 in cells and zebrafish was eventually proven to be feasible. Importantly, this probe was qualified for monitoring the variation of HClO and H2O2 levels in organisms with alcoholic liver injury.The characteristics, sources, and atmospheric oxidation processes of marine aerosol proteinaceous matter (APM), including total proteins and free amino acids (FAAs), were investigated using a set of 1 year total suspended particulate (TSP) samples collected in the coastal area of Okinawa Island in the western North Pacific rim. The concentrations of APM at this site (total proteins 0.16 ± 0.10 μg m-3 and total FAAs 9.7 ± 5.6 ng m-3, annual average) are comparable to those of marine APM. The major FAA species of APM are also similar to previously reported marine APM with glycine as the dominant species (31%). Based on the different seasonal trends and weak correlations of total proteins and FAAs, we found that they were contributed by different sources, especially with the influence of long-range transport from the Asian continent of northern China and Mongolia and the oceanic area of the Bohai Sea, Yellow Sea, and East China Sea. The photochemical oxidation processes of high-molecular-weight proteins releasing FAAs (especially glycine) were also considered as an important factor influencing the characteristics of APM at this site. In addition, we propose a degradation process based on the correlation with ozone and ultraviolet radiation, emphasizing their roles in the degradation of proteins. Our findings help to deepen the understanding of atmospheric photochemical reaction processes of organic aerosols.The development of direct and controlled oxidation of C(sp3)-H bonds is of great importance. Herein, an iodine-catalyzed controlled oxidation of (aryl)(heteroaryl)methanes to (aryl)(heteroaryl)methanols is disclosed under metal-free reaction conditions. A catalytic system comprised of iodine/silyl chloride with HI as an additive in the presence of dimethyl sulfoxide selectively oxidizes the C(sp3)-H bonds without being overoxidized to corresponding ketones. Therapeutically important aryl heteroaryl methanol derivatives were obtained in good yields. The preliminary mechanistic investigation proves that the primary source of oxygen is DMSO.Two belt-like expanded carbaporphyrins (NB1 and NB2) were prepared via a one-pot procedure that involves a [6 + 3] condensation between a pyrene-bearing tetrapyrrole precursor (2) and pentafluorobenzaldehyde, followed by oxidation. Single crystal X-ray diffraction analyses revealed that NB1 and NB2 both contain six dipyrromethene moieties and three bridging pyrene units. In the structure of NB1, there are two vertically orientated pyrene units and one transverse orientated pyrene unit; however, in NB2 all three pyrene units are vertically orientated. The structural differences between NB1 and NB2 are reflected in their respective physical properties as revealed by proton NMR, UV-vis, and fluorescence spectroscopies. In contrast to all-carbon nanobelts, NB1 and NB2 contain multiple pyrrolic nitrogen donors that could serve as potential metal coordination sites. As a test of this possibility, NB2 was used to prepare an unprecedented Zn complex containing 7 Zn2+ metal centers connected by a network of bridging atoms, as confirmed by a single crystal X-ray diffraction analysis. To the best of our knowledge, this is the first example of a belt-like molecular system that can coordinate multiple metal ions both along the backbone and within its central cavity.Potassium poly(heptazine imide) (KPHI) has recently garnered attention as a crystalline carbon nitride framework with considerable photoelectrochemical activity. Here, we report a Ca2+-complexed analogue of PHI calcium poly(heptazine imide) (CaPHI). Despite similar polymer backbone, CaPHI and KPHI exhibit markedly different crystal structures. Spectroscopic, crystallographic, and physisorptive characterization reveal that Ca2+ acts as a structure-directing agent to transform melon-based carbon nitride to crystalline CaPHI with ordered pore channels, extended visible light absorption, and altered band structure as compared to KPHI. Upon acid washing, protons replace Ca2+ atoms in CaPHI to yield H+/CaPHI and enhance porosity without disrupting crystal structure. Further, these proton-exchanged PHI frameworks exhibit large adsorption affinity for CO2 and exceptional performance for selective carbon capture from dilute streams. Compared to a state-of-the-art metal organic framework, UTSA-16, H+/CaPHI exhibits more than twice the selectivity (∼300 vs ∼120) and working capacity (∼1.2 mmol g-1 vs ∼0.5 mmol g-1) for a feed of 4% CO2 (1 bar, 30 °C).The selective 4e-/4H+ reduction of dioxygen to water is an important reaction that takes place at the cathode of fuel cells. Monomeric aromatic tetrapyrroles (such as porphyrins, phthalocyanines, and corroles) coordinated to Co(II) or Co(III) have been considered as oxygen reduction catalysts due to their low cost and relative ease of synthesis. However, these systems have been repeatedly shown to be selective for O2 reduction by the less desired 2e-/2H+ pathway to yield hydrogen peroxide. Herein, we report the initial synthesis and study of a Co(II) tetrapyrrole complex based on a nonaromatic isocorrole scaffold that is competent for 4e-/4H+ oxygen reduction reaction (ORR). This Co(II) 10,10-dimethyl isocorrole (Co[10-DMIC]) is obtained in just four simple steps and has excellent yield from a known dipyrromethane synthon. Evaluation of the steady state spectroscopic and redox properties of Co[10-DMIC] against those of Co porphyrin (cobalt 5,10,15,20-tetrakis(pentafluorophenyl)porphyrin, [Co(TPFPP)]) and corrrate pendant proton-transfer groups or ditopic molecular clefts or that impose cofacially oriented O2 binding sites. Accordingly, Co[10-DMIC] represents the first simple, unadorned, monomeric metalloisocorrole complex that can be easily prepared and shows a privileged performance for the 4e-/4H+ peractivation of O2 to water as compared to other simple cobalt containing tetrapyrroles.Silicon (Si) is a promising high-capacity material for lithium-ion batteries; however, its limited reversibility hinders commercial adoption. Approaches such as particle and crystallite size reduction, introduction of conductive carbon, and use of different electrolyte solvents have been explored to overcome these electrochemical limitations. Herein, operando isothermal microcalorimetry (IMC) is used to probe the influence of silicon particle size, electrode composition, and electrolyte additives fluoroethylene carbonate and vinylene carbonate on the heat flow during silicon lithiation. The IMC data are complemented by X-ray photoelectron and Raman spectroscopies to elucidate differences in solid electrolyte interphase (SEI) composition. Nanosized (∼50 nm, n-Si) and micrometer-sized (∼4 μm, μ-Si) silicon electrodes are formulated with and without amorphous carbon and electrochemically lithiated in ethylene carbonate (EC), fluoroethylene carbonate (FEC), or vinylene carbonate (VC) based electrolytes. Notably, n-Si electrodes generate 53-61% more normalized heat relative to their μ-Si counterparts, consistent with increased surface area and electrode/electrolyte reactivity. Introduction of amorphous carbon significantly alters the heat flow profile where multiple exothermic peaks and increased normalized heat dissipation are observed for all electrolyte types. Notably, the VC-containing electrolyte demonstrates the greatest normalized heat dissipation of the electrode compositions tested showing as much as a 50% increase compared to the EC or FEC counterparts. The results are relevant to the understanding of silicon negative electrode function in the presence of electrolyte additives and provide insight relative to silicon containing cell reactivity and safety.
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