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We describe a photocatalytic system that reveals latent photooxidant behavior from one of the most reducing conventional photoredox catalysts, N-phenylphenothiazine (PTH). This aerobic photochemical reaction engages difficult to oxidize feedstocks, such as benzene, in C(sp2)-N coupling reactions through direct oxidation. Mechanistic studies are consistent with activation of PTH via photooxidation and with Lewis acid cocatalysts scavenging inhibitors inextricably formed in this process.An efficient technique using citric acid and glucose based natural deep eutectic solvent (G-C-NADES) was developed to obtain ultrahigh deamidated wheat gluten (UDWG) (deamidation degree (DD) > 90%). FTIR and 1H NMR indicated intensive hydrogen bonds (HBs) in G-C-NADES supermolecules. Daidzein datasheet Quantum chemical calculations and molecular dynamic simulations demonstrated that 10 wt % diluted G-C-NADES still had a myriad of HBs. Physicochemical results showed UDWG had DD up to 92.45% after G-C-NADES deamidation, that is, 22% higher than citric-acid-DWG with a weak degree of hydrolysis (1.75%). Conformational characterization demonstrated the obvious conversion from α-helix to β-sheet via FTIR, the least amount of disulfide bonds by Raman spectra, and more exposure of tryptophan residues by fluorescence measurement for UDWG. It is proven that enhanced accessible conformation of WG reached with HBs of G-C-NADESs could contribute to the improvement on nucleophilic attack of deamidation, declaring that G-C-NADES might be a potential solvent for obtaining an ultrahigh deamidation for WG to successfully guarantee the safety of wheat gluten based cereal food regarding to lowering its allergy.3-Deoxyglucosone (3-DG) is a Maillard reaction intermediate, which forms known beer aging compounds such as Strecker aldehydes. However, the role of 3-DG in beer aging stability has not been described yet. To investigate the influence of 3-DG toward beer aging stability, different concentrations of 3-DG were added to the freshly brewed beer at the beginning of storage. Analysis of well-known degradation products of 3-DG such as 3-deoxygalactosone (HPLC-UV), 5-hydroxymethylfurfural (HPLC-UV), Strecker aldehydes (GC-MS), and free glycated amino acids (HPLC-MS/MS) during beer aging revealed that a higher initial 3-DG concentration increases the formation of the products. In this study, the significant importance of 3-DG as a key precursor compound in beer aging has been shown, especially the increase of Strecker aldehydes.Within this work, a modified preparation of diethyl 4-azidobenzylphosphonate (L1) is presented and the family of 4- or 4'-azido-substituted aromatic phosphonate esters is increased by three new ligand platforms diisopropyl 4-azidobenzylphosphonate (L2), diisopropyl ((4'-azido-[1,1'-biphenyl]-4-yl)methyl)phosphonate (L3), and diisopropyl 4-azido-2,3,5,6-tetrafluorobenzylphosphonate (L4), which exhibit an anomalous splitting of the N3 stretching vibrations. Subsequent coordination to the in situ generated RPOSS (polyhedral oligomeric silsesquioxane)-cage-supported lanthanide precursors [(LnRPOSS)2(THF)m] (P1-P6) (Ln = La, Nd, Dy, Er; R = iBu, Ph; m = 0, 1) yields complexes of the general formula [LnRPOSS(L1-L4)n(S1)x(THF)m] (1-30) (n = 2, 3; x = 0, 1; m = 0-2) retaining the azide unit for future semiconductor surface immobilization. Because the latter compounds are mostly oils or viscous waxes, preliminary solution-state structure elucidations via DOSY-ECC-MW estimations have been carried out which are in accordance with 1H NMR integral ratios as well as solid-state structures, where available. Moreover, the optical properties of the Nd, Dy, and Er derivatives of complexes 1-30 are examined in the visible and NIR spectral regions, where applicable.The bottom-up assembly of periodically ordered structures provides a scalable way for producing metastructured materials with exotic optical and mechanical properties. However, direct self-assembly of small molecules into such metastructures beyond the nanoscale remains an unresolved issue. Here we demonstrate that metastructured assemblies of two-dimensional (2D) polymers, specifically 2D covalent organic frameworks (COFs), can be directly synthesized in solution. We applied 2D COF monomer polycondensation to prepare flower-shaped particles consisting of highly crystalline "petals" with sizes larger than 20 μm. The petal comprises periodically arranged COF nanoflake units with tunable lengths of 490-850 nm, thicknesses about 20 nm, interflake spacing around 14 nm, and Hermans orientation factors up to 0.998. Such a metastructure is mechanically robust and remains almost intact even after full pyrolysis at 900 °C. It also demonstrates unique birefringence and polarization-dependent resonances under visible-near-infrared light not observed in its constituents, 2D COF polycrystals, and with well-defined nanopores of 1.8 nm and the high surface area of 1576 m2/g. Such metastructured particles with nanopores are well-suited as novel particulate optical devices for collecting and storing information about their surroundings that can be easily read out by polarization imaging with high sensitivity, as demonstrated by their explosive detection and anticounterfeiting applications. Self-assembly of 2D polymers into metastructures may become an important method for developing functional materials with unprecedented properties and extensive applications.The aluminyl anion K[Al(NONDipp)] NONDipp = [O(SiMe2NDipp)2]2-; Dipp = 2,6-iPr2C6H3 engages in oxidative additions with the E-H (E = Si, P, N, or O) bonds of phenylsilane (PhSiH3), mesityl phosphane (MesPH2; Mes = 2,4,6-Me3C6H2), 2,6-di-iso-propylaniline (DippNH2), and 2,6-di-tert-butyl-4-methylphenol (ArOH). The resulting (hydrido)aluminate salts are formed regardless of the E-H bond polarity. All of the products were characterized by nuclear magnetic resonance and infrared spectroscopic techniques and single-crystal X-ray diffraction. This study highlights the versatility of aluminyl anions to activate hydridic, acidic, and (essentially) nonpolar E-H bonds.Inexpensive and efficient electrocatalysts are crucial for the development and practical application of energy conversion and storage technologies. Layered-double-hydroxide (LDH) materials have attracted much attention due to the special layered structure, but their electrocatalytic activity and stability are still limited. Herein, we propose to tune Co2+ occupancy and coordination in cobalt-based LDH nanosheets via Fe3+ doping for efficient and stable electrocatalysis for oxygen evolution reaction (OER). It is found that Fe doping regulates the occupancy and coordination of Co2+ in CoO4 tetrahedrons and CoO6 octahedrons of Co-LDHs. Through density functional theory calculation, we also clarified that Fe3+ not only modulated the Co2+ coordination but also functioned as an added catalytic active site. LDH nanosheets with a Co/Fe ratio of 51 show a low OER overpotential, much better than the commercial IrO2, owing to the modulation of Fe3+ doping on the crystal and electronic structures. After appropriate incorporation of Fe3+, the almost inactive octahedral coordinated Co2+ is significantly activated with a partial deletion of tetrahedral coordinated Co2+, which greatly boosts the overall electrocatalytic activity.
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