Notes

Proteins architectural with regard to natural product or service biosynthesis and synthetic the field of biology applications.
Here, we report on three new triphenylamine-based enamines synthesized by condensation of an appropriate primary amine with 2,2-diphenylacetaldehyde and characterized by experimental techniques and density functional theory (DFT) computations. Experimental results allow highlighting attractive properties including solid-state ionization potential in the range of 5.33-5.69 eV in solid-state and hole mobilities exceeding 10-3 cm2/V·s, which are higher than those in spiro-OMeTAD at the same electric fields. DFT-based analysis points to the presence of several conformers close in energy at room temperature. The newly synthesized hole-transporting materials (HTMs) were used in perovskite solar cells and exhibited performances comparable to that of spiro-OMeTAD. The device containing one newly synthesized hole-transporting enamine was characterized by a power conversion efficiency of 18.4%. Our analysis indicates that the perovskite-HTM interface dominates the properties of perovskite solar cells. PL measurements indicate smaller efficiency for perovskite-to-new HTM hole transfer as compared to spiro-OMeTAD. Nevertheless, the comparable power conversion efficiencies and simple synthesis of the new compounds make them attractive candidates for utilization in perovskite solar cells.A new hybrid non-ribosomal peptide-polyketide antibiotic (serratamid) for phytoprotection was isolated from the ethyl acetate layer of tryptic soy agar culture of the soil bacterium Serratia plymuthica C1 through bioassay-guided fractionation. Its chemical structure was elucidated using instrumental analyses, such as mass and nuclear magnetic resonance spectrometry. Serratamid showed antibacterial activity against 15 phytopathogenic bacteria, with minimum inhibitory concentration (MIC) values ranging from 0.244 to 31.25 μg/mL. In vitro, it displayed strong antibacterial activity against Ralstonia solanacearum and four Xanthomonas spp., with MIC values (0.244-0.488 μg/mL) superior to those of streptomycin sulfate, oxolinic acid, and oxytetracycline. Further, serratamid and the ethyl acetate layer of S. plymuthica C1 effectively reduced bacterial wilt caused by R. solanacearum on tomato seedlings and fire blight caused by Erwinia on apple fruits in a dose-dependent manner. These results suggest that serratamid is a promising candidate as a potent bactericide for controlling bacterial diseases.Desorption/ionization (DI) methods play an important role among the panel of mass spectrometric (MS) approaches for the rapid and sensitive quantification of drugs from the surface of solid samples. The possibility to implement these approaches for pharmacokinetic/pharmacodynamic investigations in early phase clinical trials depends on the ability to validate quantification assays according to regulatory guidelines (e.g., US Food and Drug Administration and European Medicines Agency) for bioanalytical method validation. However, these guidelines were designed for the validation of liquid chromatography-MS (LC-MS) methods and ligand binding assays. To apply the validation parameters to DI-MS methods (also referred here as on-surface MS) for drug quantification, it is important to consider the particularities of DI approaches compared to LC-MS methods. In this Perspective, we summarize the various applications of on-surface MS methods for drug quantification with their advantages over other MS methods, and provide our point of view regarding future proper method development and validation.During integration into materials, the inactivation of enzymes as a result of their interaction with nanometer size denaturing "hotspots" on surfaces represents a critical challenge. This challenge, which has received far less attention than improving the long-term stability of enzymes, may be overcome by limiting the exploration of surfaces by enzymes. One way this may be accomplished is through increasing the rate constant of the surface ligation reaction and thus the probability of immobilization with reactive surface sites (i.e., ligation efficiency). Here, the connection between ligation reaction efficiency and the retention of enzyme structure and activity was investigated by leveraging the extremely fast reaction of strained trans-cyclooctene (sTCOs) and tetrazines (Tet). Remarkably, upon immobilization via Tet-sTCO chemistry, carbonic anhydrase (CA) retained 77% of its solution-phase activity, while immobilization via less efficient reaction chemistries, such as thiol-maleimide and azide-dibenzocyclooctyne, led to activity retention of only 46% and 27%, respectively. Dynamic single-molecule fluorescence tracking methods further revealed that longer surface search distances prior to immobilization (>0.5 μm) dramatically increased the probability of CA unfolding. Notably, the CA distance to immobilization was significantly reduced through the use of Tet-sTCO chemistry, which correlated with the increased retention of structure and activity of immobilized CA compared to the use of slower ligation chemistries. These findings provide an unprecedented insight into the role of ligation reaction efficiency in mediating the exploration of denaturing hotspots on surfaces by enzymes, which, in turn, may have major ramifications in the creation of functional biohybrid materials.Sites isolation of active metals centers, systematically studied in homogeneous systems, has been an alternative to develop low metal consuming, highly active next generation catalysts in heterogeneous condition. Because of the high porosity and facile synthetic procedures, MOF-based catalysts are excellent candidates for heterogenization of well-defined homogeneous catalysts. Herein, we report the direct Pd coordination on the azobenzene linker within a MOF catalyst through a postsynthetic modification method for a Suzuki-Miyaura coupling reaction. The immobilized cyclopalladated complexes in MOFs were analyzed by a series of characterization techniques including XPS, PXRD, and deuterium NMR (2H NMR) spectroscopy. The heterogeneous nature of the catalyst as well as its stability were demonstrated though "hot filtration" and recycling experiments. Furthermore, we demonstrate that the MOF packed column promoted the reaction between phenyl boronic acid and bromobenzene under microflow conditions with a 85% yield continuously for 12 h. This work sheds light on the potential of site-isolated MOF catalysts in efficient, recyclable and continuous flow systems for industrial application.Interfaces govern thermal transport in a variety of nanostructured systems such as FinFETs, interconnects, and vias. Thermal boundary resistances, however, critically depend on the choice of materials, nanomanufacturing processes and conditions, and the planarity of interfaces. In this work, we study the interfacial thermal transport between a nonreactive metal (Pt) and a dielectric by engineering two differing bonding characters (i) the mechanical adhesion/van der Waals bonding offered by the physical vapor deposition (PVD) and (ii) the chemical bonding generated by plasma-enhanced atomic layer deposition (PEALD). We introduce 40-cycle (∼2 nm thick), nearly continuous PEALD Pt films between 98 nm PVD Pt and dielectric materials (8.0 nm TiO2/Si and 11.0 nm Al2O3/Si) treated with either O2 or O2 + H2 plasma to modulate their bonding strengths. By correlating the treatments through thermal transport measurements using time-domain thermoreflectance (TDTR), we find that the thermal boundary resistances are consistently reduced with the same increased treatment complexity that has been demonstrated in the literature to enhance mechanical adhesion. For samples on TiO2 (Al2O3), reductions in thermal resistance are at least 4% (10%) compared to those with no PEALD Pt at all, but could be as large as 34% (42%) given measurement uncertainties that could be improved with thinner nucleation layers. We suspect the O2 plasma generates stronger covalent bonds to the substrate, while the H2 plasma strips the PEALD Pt of contaminants such as carbon that gives rise to a less thermally resistive heat conduction pathway.Chemicals may cause adverse effects on human health through binding to peroxisome proliferator-activated receptor γ (PPARγ). Hence, binding affinity is useful for evaluating chemicals with potential endocrine-disrupting effects. Quantitative structure-activity relationship (QSAR) regression models with defined applicability domains (ADs) are important to enable efficient screening of chemicals with PPARγ binding activity. However, lack of large data sets hindered the development of QSAR models. In this study, based on PPARγ binding affinity data sets curated from various sources, 30 QSAR models were developed using molecular fingerprints, two-dimensional descriptors, and five machine learning algorithms. Structure-activity landscapes (SALs) of the training compounds were described by network-like similarity graphs (NSGs). Based on the NSGs, local discontinuity scores were calculated and found to be positively correlated with the cross-validation absolute prediction errors of the models using the different training sets, descriptors, and algorithms. Moreover, innovative ADs were defined based on pairwise similarities between compounds and were found to outperform some conventional ADs. Tanespimycin HSP (HSP90) inhibitor The curated data sets and developed regression models could be useful for evaluating PPARγ-involved adverse effects of chemicals. The SAL analysis and the innovative ADs could facilitate understanding of prediction results from QSAR models.With the rapid improvement of perovskite solar cells (PSCs), long-life operational stability has become a major requirement for their commercialization. In this work, we devised a pristine cesium-formamidinium-methylammonium (termed as CsFAMA) triple-cation-based perovskite precursor solution into the ionic liquid (IL)-assisted MAPbI3 nanoparticles (NPs) through a seeded growth approach in which the host IL-assisted MAPbI3 NPs remarkably promote high-quality perovskite films with large single-crystal domains, enhancing the device performance and stability. The power conversion efficiency (PCE) of the MAPbI3 NP-seeded growth of MAPbI3 NPs/CsFAMA-based PSCs is as high as 19.44%, which is superior to those of MAPbI3 NPs and pristine CsFAMA films as the photoactive layer (9.52 and 17.33%, respectively). The long-term light-soaking and moisture stability of IL-aided MAPbI3 NPs/CsFAMA-based devices (non-encapsulated) remain above 90 and 80%, respectively, of their initial output after 2 h of light illumination (1 sun) and 6000 h storage at ambient with a relative humidity range of 30-40%. The use of the IL-assisted MAPbI3 NP-seeded growth for PSCs is a significant step toward developing stable and reliable perovskite photovoltaic devices.The rational design of continuous covalent organic framework (COF)-based membranes is challenging for desalination applications, mainly due to the larger intrinsic pore size of COFs and defects in the crystalline film, which lead to a negligible NaCl rejection ratio. In this work, we first demonstrated a COF-based desalination membrane with in situ cross-linking of a COF-TpPa layer by trimesoyl chloride (TMC) to stitch the defects between COF crystals and cross-link the COF cavity with high-cross-linking degree networks to enhance NaCl rejection. With the addition of TMC monomers, both small spherical nodules and some elongated "leaf-like" features were observed on the membrane surface due to the appearance of nanovoids during cross-linking. The resulting COF-based desalination membrane had a water permeability of approximately 0.81 L m-2 h-1 bar-1 and offered substantial enhancement of the NaCl rejection ratio from being negligible to 93.3% at 5 bar. Mechanistic analysis indicated that the amidation reaction of the secondary amine in keto COF with TMC induced the formation of a highly porous network structure both in the cavity and on the exterior of COF, thereby successfully forming a continuous and nanovoid-containing selective layer for desalination.
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