Notes

A new near-infrared neon probe in line with the hemicyanine skeletal frame to the discovery involving hydrogen peroxide in vivo.
The biosynthetic gene cluster governing the production of antibacterial julichromes was identified from marine gastropod mollusk-associated Streptomyces sampsonii SCSIO 054. selleck chemicals llc Post-PKS assembly/tailoring enzymes JuiL, JuiM, JuiI, and JuiN represent key assembly enzymes. JuiL serves as a ketoreductase. JuiM is an acetyltransferase. JuiI carries out an intriguing biaryl coupling of two julichrome Q6 units (immediate JuiL, JuiM product) to afford julichrome Q6-6. JuiN carries out tailoring steps on julichrome Q6-6, transforming Q6-6 into Q3-3.Molecular dynamics simulations are performed to explore if isotopic chirality can induce unidirectional rotary motion in molecular motors operated through double-bond photoisomerizations. Using a high-quantum yield motor featuring a chemically asymmetric carbon atom as reference, it is found that isotopically chiral counterparts of this motor sustain such motion almost equally well. Overall, the study reveals a previously unexplored role for isotopic chirality in the design of rotary molecular motors.Total syntheses of (±)-walsucochin B and (±)-walsucochinoids M and N have been achieved from farnesyl bromide. The key steps of the synthetic sequence are the titanocene-mediated radical cyclization and base-induced cycloaromatization for the rapid construction of the 6/6/5/6-fused tetracyclic skeleton. Importantly, a Cu-mediated remote C-H hydroxylation reaction has been developed to site-selectively install the oxygen function at the C-7 position of the target molecules, thus solving the biggest challenge for the synthesis of the compounds.Improving the antifrosting ability of stainless steel is crucial. In previous reports, many efforts have been dedicated to enhancing the antifrosting performance of superhydrophobic surface by fabricating different surface morphology. However, no researchers have proposed what kind of surface morphology can effectively prevent the frost based on the theory of superhydrophobic surfaces. In this article, we build a simulation model to study the effects of different surface morphology on antifrosting based on the Cassie model. We find that the higher the proportion of air between the droplet and the substrate, the better the antifrosting performance of the superhydrophobic surface. Therefore, we propose one superhydrophobic surface (denoted as sample #R) fabricated by selective growth. It can contain more air between the droplet and the surface. link2 Further frosting experiments at a low temperature of -21 °C and a humidity of 75% show that 15% frost coverage on sample #R can be delayed to 63 h, as compared to less than 3 h for untreated stainless steel. In addition, the preparation method is generally applicable to other metals. Therefore, this work provides new insights into the rational design of a superhydrophobic surface with antifrosting in a harsh environment.Cs4PbBr6 is regarded as an outstanding luminescent material with good thermal stability and optical performance. However, the mechanism of green emission from Cs4PbBr6 has been controversial. Here we show that isolated CsPbBr3 nanoparticles embedded within a Cs4PbBr6 matrix give rise to a "normal" green luminescence while superfluorescence at longer wavelengths is suppressed. High-resolution transmission electron microscopy shows that the embedded CsPbBr3 nanoparticles are around 3.8 nm in diameter and are well-separated from each other, perhaps by a strain-driven mechanism. This mechanism may enable other efficient luminescent composites to be developed by embedding optically active nanoparticles epitaxially within inert host lattices.We report the highly regio- and enantioselective alkynylation of alkynyl 1,2-diketones under Lewis acid catalysis, leading to the formation of a series of biologically important 3(2H)-furanones with high to excellent ee values. Moreover, a slight change of the reaction conditions produces a range of highly functionalized α-hydroxy ketones with a high level of enantioselectivity. A variety of further transformations can be easily achieved, demonstrating the synthetic potential of this protocol.To enhance the advantage of a long-term stability and low-toxicity active packaging system, two biodegradable covalent immobilized antibacterial packaging films were developed and applied to fresh beef preservation in this study. A polylactic acid (PLA) film was prepared by the extrusion-casting method. The surface of the PLA film was modified with plasma treatment to generate carboxylic acid groups, and then antibacterial agent nisin or ε-poly lysine (ε-PL) was covalently attached to the modified film surface. Physical, chemical, and antimicrobial properties of films were then characterized. Scanning electron microscopy and water contact angle images confirmed that nisin or ε-PL was successfully grafted onto the film surface. The values of protein loading on the nisin-g-PLA film and ε-PL-g-PLA film were 5.34 ± 0.26 and 3.04 ± 0.25 μg of protein/cm2 on the surface. Microbial analysis indicated that the grafted films effectively inhibit the growth of bacteria. Finally, the effects of the nisin-g-PLA film or ε-PL-g-PLA film on physicochemical changes and microbiological counts of fresh beef during cold storage at 4 °C were investigated. The total viable count of the control sample exceeded 7 logarithms of the number of colony forming units per gram (log CFU/g) after 11 days of cold storage (7.01 ± 0.14 log CFU/g) versus 15 days for the ε-PL-g-PLA film (7.37 ± 0.06 log CFU/g) and the nisin-g-PLA film (6.83 ± 0.10 log CFU/g). The results showed that covalent immobilized antibacterial packaging films had positive impacts on the shelf life and quality of fresh beef. Therefore, a covalent immobilized antibacterial packaging system could be a novel preservative method for foods.Celastrol, a friedelane-type triterpenoid isolated from the genus Triperygium, possesses antitumor, anti-inflammatory, and immunosuppressive activities. A total of 42 celastrol derivatives (1a-1t, 2a-2l, and 3a-3j) were synthesized and evaluated for their immunosuppressive activities. Compounds 2a-2e showed immunosuppressive effects, with IC50 values ranging from 25 to 83 nM, and weak cytotoxicity (CC50 > 1 μM). Compound 2a, with a selectivity index value 31 times higher than that of celastrol, was selected as a lead compound. Further research showed that 2a exerted its immunosuppressive effects by inducing apoptosis and inhibiting cytokine secretion via Lck- and ZAP-70-mediated signaling pathways.Black sorghum [Sorghum bicolor (L.) Moench] is characterized by the black appearance of the pericarp and production of 3-deoxyanthocyanidins (3-DOA), which are valued for their cytotoxicity to cancer cells and as natural food colorants and antioxidant additives. The black pericarp phenotype is not fully penetrant in all environments, which implicates the light spectrum and/or photoperiod as the critical factor for trait expression. In this study, black- or red-pericarp genotypes were grown under regimes of visible light, visible light supplemented with UVA or supplemented with UVA plus UVB (or dark control). Pericarp 3-DOAs and pericarp pigmentation were maximized in the black genotype exposed to a light regime supplemented with UVB. Changes in gene expression during black pericarp development revealed that ultraviolet light activates genes related to plant defense, reactive oxygen species, and secondary metabolism, suggesting that 3-DOA accumulation is associated with activation of flavonoid biosynthesis and several overlapping defense and stress signaling pathways.Simulating chemical systems on quantum computers has been limited to a few electrons in a minimal basis. We demonstrate experimentally that the virtual quantum subspace expansion (Takeshita, T.; Phys. Rev. X 2020, 10, 011004, 10.1103/PhysRevX.10.011004) can achieve full basis accuracy for hydrogen and lithium dimers, comparable to simulations requiring 20 or more qubits. We developed an approach to minimize the impact of experimental noise on the stability of the generalized eigenvalue problem, a crucial component of the quantum algorithm. In addition, we were able to obtain an accurate potential energy curve for the nitrogen dimer in a quantum simulation on a classical computer.Indium selenide (InSe) has a high electron mobility and tunable direct band gap, enabling its potential applications to electronic and optoelectronic devices. Here, we report the fabrication of InSe photodetectors with high on/off ratios and ultrahigh photoresponsivity, using ferroelectric poly(vinylidene fluoride-trifluoroethylene) (P(VDF-TrFE)) copolymer films as the top-gate dielectric. Benefiting from the successful suppression of the dark current down to ∼10-14A in the InSe channel by tuning the three different polarization states in ferroelectric P(VDF-TrFE) and improved interface properties using h-BN as a substrate, the ferroelectric-gated InSe photodetectors show a high on/off ratio of over 108, a high photoresponsivity up to 14 250 AW-1, a high detectivity up to 1.63 × 1013 Jones, and a fast response time of 600 μs even at zero-gate voltage. link3 The present results highlight the role of ferroelectric P(VDF-TrFE) in tuning the carrier transport of InSe and may provide an avenue for the development of InSe-based photodetectors.Major light-harvesting complex (LHCII) trimers in plants induce the thermal dissipation of absorbed excitation energy against photooxidative damage under excess light conditions. LHCII trimers in green algae have been thought to be incapable of energy dissipation without additional quencher proteins, although LHCIIs in plants and green algae are homologous. In this study, we investigated the energy-dissipative capabilities of four distinct types of LHCII trimers isolated from the model green alga Chlamydomonas reinhardtii using spectroscopic analysis. Our results revealed that the LHCII trimers possessing LHCII type II (LHCBM5) and LHCII type IV (LHCBM1) had efficient energy-dissipative capabilities, whereas LHCII type I (LHCBM3/4/6/8/9) and type III (LHCBM2/7) did not. On the basis of the amino acid sequences of LHCBM5 and LHCBM1 compared with the other LHCBMs, we propose that positively charged extra N-terminal amino acid residues mediate the interactions between LHCII trimers to form energy-dissipative states.Deacetoxycephalosporin C synthase (DAOCS) is a nonheme iron(II) and 2-oxoglutarate (α-KG)-dependent oxygenase that catalyzes the oxidative ring expansion of penicillin N (penN) to deacetoxycephalosporin C (DAOC). Earlier reported crystal structures of DAOCS indicated that the substrate penicillin binds at the same site of succinate, leading to the proposal of the unusual "ping-pong" mechanism. However, more recent data provided evidence of the formation of ternary DAOCS·α-KG·penN complex, and thus DAOCS should follow the usual consensus mechanism of α-KG-dependent nonheme iron(II) oxygenases. Nevertheless, how DAOCS catalyzes the ring expansion is unknown. In this paper, on the basis of the crystal structure, we constructed two reactant models and performed a series of combined quantum mechanics/molecular mechanics (QM/MM) calculations to illuminate the catalysis of DAOCS. The binding mode of substrate was found to be crucial in determining which hydrogen atom in two methyl groups is first abstracted and whether the second H-abstraction to be abstracted in the final desaturation step locates in a suitable orientation.
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