Activity

To date, the determination of sulfonamide metabolites in animal-derived food has universal disadvantages of low throughput and no integrated metabolites involved. this website In this study, a powerful and reliable strategy for high-throughput screening of sulfonamide metabolites in goat meat was proposed based on an aqueous two-phase separation procedure (ATPS) combined with ultrahigh-performance liquid chromatography quadrupole-Orbitrap high-resolution mass spectrometry (UHPLC-Q-Orbitrap). Noncovalent interactions including van der Waals force, hydrogen bonding, and hydrophobic effect were determined to be staple interactions between the sulfonamide metabolites and sheep serum albumin by fluorescence spectroscopy and molecular docking technology, and an 80% acetonitrile-water solution/(NH4)2SO4 was used as ATPS in order to release combined sulfonamide metabolites and minimize the influence of sheep serum albumin. Sulfonamide metabolites in the matrix were screened based on a mechanism of mass natural loss and core structure followed by identification combined with the pharmacokinetic. The developed strategy was validated according to EU standard 2002/657/EC with CCα ranging from 0.07 to 0.98 μg kg-1, accuracy recovery with 84-107%, and RSDs lower than 8.9%. Eighty seven goat meat samples were used for determination of 26 sulfonamides and 8 potential metabolites. On the basis of the established innovative process, this study has successfully implemented the comprehensive detection of sulfonamide metabolites, including N4-acetylated substitution, N4-hydroxylation, 4-nitroso, azo dimers, oxidized nitro, N4 monoglucose conjugation, β-d-glucuronide, and N-4-aminobenzenesulfonyl metabolites, which were shown to undergo oxidation, hydrogenation, sulfation, glucuronidation, glucosylation, and O-aminomethylation.ConspectusHeterogeneous catalysts are rather complex materials that come in many classes (e.g., metals, oxides, carbides) and shapes. At the same time, the interaction of the catalyst surface with even a relatively simple gas-phase environment such as syngas (CO and H2) may already produce a wide variety of reaction intermediates ranging from atoms to complex molecules. The starting point for creating predictive maps of, e.g., surface coverages or chemical activities of potential catalyst materials is the reliable prediction of adsorption enthalpies of all of these intermediates. For simple systems, direct density functional theory (DFT) calculations are currently the method of choice. However, a wider exploration of complex materials and reaction networks generally requires enthalpy predictions at lower computational cost.The use of machine learning (ML) and related techniques to make accurate and low-cost predictions of quantum-mechanical calculations has gained increasing attention lately. The employed applpies, there is also an emerging interest in our field to start using ML predictions to answer fundamental science questions about the functioning of heterogeneous catalysts or perhaps even to design better catalysts than we know today. This task is significantly simplified in works that make use of scaling-relation-based models (volcano curves), where the model outcome is determined by only one or two adsorption enthalpies and which consequently become the sole target for ML-based high-throughput screening or design. However, the availability of cheap ML energetics also allows going beyond scaling relations. On the basis of our own work in this direction, we will discuss the additional physical insight that can be achieved by integrating ML-based predictions with traditional catalysis modeling techniques from thermal and electrocatalysis, such as the computational hydrogen electrode and microkinetic modeling, as well as the challenges that lie ahead.A large diversity in the targeted hydration free energies (HFEs) during model parameterization of metal ions was reported in the literature with a difference by dozens of kcal/mol. Here, we developed a series of nonbonded dummy models of the Mg2+ ion targeting different HFE references in TIP3P water, followed by assessments of the designed models in the simulations of MgCl2 solution and biological systems. Together with the comparison of existing models, we conclude that the difference in the targeted HFEs has a limited influence on the model performance, while the usability of these models differs from case to case. The feasibility of reproducing more properties of Mg2+ such as diffusion constants and water exchange rates using a nonbonded dummy model is demonstrated. Underestimated activity derivative and osmotic coefficient of MgCl2 solutions in high concentration reveal a necessity for further optimization of ion-pair interactions. The developed dummy models are applicable to metal coordination with Asp, Glu, and His residues in metalloenzymes, and the performance in predicting monodentate or bidentate binding modes of Asp/Glu residues depends on the complexity of metal centers and the choice of protein force fields. When both the binding modes coexist, the nonbonded dummy models outperform point charge models, probably in need of considering polarization of metal-binding residues by, for instance, charge calibration in classical force fields. This work is valuable for the use and further development of magnesium ion models for simulations of metal-containing systems with good accuracy.Interfacial engineering plays a crucial role in regulating the quality and property of heterogeneous structures, especially for nanometer-scaled devices. However, traditional methods for interfacial modulation (IFM) generally treat all the interfaces uniformly, neglecting the inherent disparities of interfaces like their growth sequence. Herein, it is found that the growth-oriented characteristic of IFM strongly determines the main regions where the modulation takes effect. Specifically, in a semiconductor quantum well structure, the arsenic atoms modulated at the well-on-barrier (WoB) interface tend to diffuse into and thus affect the next-grown well layer. In contrast, the arsenic atoms introduced at the barrier-on-well (BoW) interface mainly take effect within the next-grown barrier layer. According to theoretical simulations and electron holography (EH) experiments, the depth of quantum wells and the height of potential barriers are extended by introducing arsenic atoms at WoB and BoW interfaces, respectively.