Hexagonal boron nitride (h-BN) and nanotubes (BNNT) were recently reported as highly selective catalysts for the oxidative dehydrogenation (ODH) of alkanes to olefins in gas phase. Previous studies revealed a substantial increase surface oxygen content after exposure ODH conditions (heating ca. 500 °C under flow alkane oxygen); however, complexity these materials has thus far precluded an in-depth understanding oxygenated species. In this contribution, we combine advanced NMR spectroscopy...

We report on the oxidative dehydrogenation (ODH) activity of silica-supported boron oxide prepared via incipient wetness impregnation. Characterization pristine and spent catalysts with infrared, Raman, solid-state NMR spectroscopy reveals presence both isolated aggregated oxidized sites. The results these investigations, in combination our earlier work bulk boron-containing ODH (e.g., h-BN, metal borides, elemental boron), give direct evidence that species formed situ surface materials are...

Abstract Boron‐containing materials have recently been identified as highly selective catalysts for the oxidative dehydrogenation (ODH) of alkanes to olefins. It has previously demonstrated by several spectroscopic characterization techniques that surface these boron‐containing ODH oxidize and hydrolyze under reaction conditions, forming an amorphous B 2 (OH) x O (3− /2) ( x= 0–6) layer. Yet, precise nature active site(s) remains elusive. In this Communication, we provide a detailed zeolite...

Rational design of materials for energy storage systems relies on our ability to probe these at various length scales. Solid-state NMR spectroscopy is a powerful approach gaining chemical and structural insights the atomic/molecular level, but its low detection sensitivity often limits applicability. This limitation can be overcome by transferring high polarization electron spins sample interest in process called dynamic nuclear (DNP). Here, we employ first time metal ion-based DNP pristine...

A bottom-up investigation strategy for eumelanin's structure–property relationship by a multidisciplinary approach, using 3D electron diffraction, solid-state NMR, density functional theory and electronic spectroscopy.

Determining the structure of sitagliptin is crucial for ensuring its effectiveness and safety as a DPP-4 inhibitor used to treat type 2 diabetes. Accurate determination vital both drug development maintaining quality control in manufacturing. This study integrates advanced techniques solid-state nuclear magnetic resonance (NMR) spectroscopy, three-dimensional (3D) electron diffraction, density functional theory (DFT) calculations investigate structural intricacies sitagliptin. Solid-state...

Abstract Clean energy carriers obtained from renewable, earth‐abundant materials and by using the virtually unlimited supply of sunlight have potential to serve as future sustainable power sources. A quest for new oxygen evolution catalytic water oxidation carbon dioxide reduction, which aim build up solar‐to‐fuel conversion devices that use raw material, has been developing during last two decades. Most research in field science chemistry focused on development inorganic molecular complexes...

In dynamic nuclear polarization magnetic resonance (DNP-NMR) experiments, the large Boltzmann of unpaired electrons is transferred to surrounding nuclei, leading a significant increase in sensitivity NMR signal. order obtain gains bulk inorganic samples, paramagnetic metal ions are introduced as minor dopants acting polarizing agents. While this approach has been shown be very efficient crystalline oxides, significantly lower enhancements have reported when applying oxide glasses....

The largest light-harvesting antenna in nature, the chlorosome, is a heterogeneous helical BChl self-assembly that has evolved green bacteria to harvest light for performing photosynthesis low-light environments. Guided by NMR chemical shifts and distance constraints Chlorobaculum tepidum wild-type chlorosomes, two contrasting packing modes syn-anti parallel stacks of c form polar 2D arrays, with dipole moments adding up, are explored. Layered assemblies were optimized using local orbital...

Mixed bandgap and tunability in semiconductors is critical expanding their use. Composition alterations through single-crystal epitaxial growth the formation of multilayer tandem structures are often employed to achieve mixed bandgaps, albeit with limited tunability. Herein, self-assembled one-dimensional coordination polymers provide facile synthons templates for graphitic C-doped mesoporous oxides, gC-β-Ga2O3 or gC-In2O3 via controlled oxidative ligand ablation. These materials have...

Coordination polymers are ideal synthons for high aspect ratio nanomaterials. Using conjugate acid-base pairs, liquid metals etched and chelated <italic>in situ</italic>. Solubility-driven polymerization, precipitation, self-assembly gives tunable structures.

An interdisciplinary approach to derive the structure of a disordered supramolecular system.

Abstract Boron‐containing materials have recently been identified as highly selective catalysts for the oxidative dehydrogenation (ODH) of alkanes to olefins. It has previously demonstrated by several spectroscopic characterization techniques that surface these boron‐containing ODH oxidize and hydrolyze under reaction conditions, forming an amorphous B 2 (OH) x O (3− /2) ( x= 0–6) layer. Yet, precise nature active site(s) remains elusive. In this Communication, we provide a detailed zeolite...

Cu/AlO(OH) has been found to be an efficient catalyst for the formation of β-enamino ketones/esters under solvent, ligand and base free conditions. The is prepared from CuCl2·2H2O, pluronic P123 Al(O-sec-Bu)3. characterized by HR-TEM, SEM-EDX, XPS FT-IR spectra. β-ketoenamine using as mild environmentally benign reaction conditions are optimized with different amounts temperatures acetylacetone aniline system a model. scope extended types diketones amines. Solvent, room temperature make...

Abstract Hybrid magic‐angle spinning (MAS) NMR spectroscopy and TEM were demonstrated for de novo structure determination of para ‐crystalline materials with a bioinspired fused naphthalene diimide (NDI)–salphen–phenazine prototype light‐harvesting compound. Starting from chiral building blocks C 2 molecular symmetry, the asymmetric unit was determined by MAS spectroscopy, index low‐resolution diffraction data, resolve reflection conditions, first time ability to determine space group...

Abstract Controlling complexity, flexibility, and functionality of synthetic biomimetic materials requires insight into how molecular functionalities can be exploited for steering their packing. A fused NDI‐salphen (NDI=naphthalene diimide) prototypic artificial photosynthesis material, DATZnS, is shown to comprised a phenazine motif, in which the alignment electric dipole moments P 2/ c supramolecular scaffold modulated with bulky substituents. They also switched between parallel stacks...

Abstract The molecular geometry and supramolecular packing of two bichromophoric prototypic light harvesting compounds D1A2 D2A2 , consisting naphthylimide energy donors that were attached to the 1,7 bay positions a perylene monoimide diester acceptor, have been determined by hybrid approach using magic angle spinning NMR spectroscopy electron nano‐crystallography (ENC), followed modelling. shift constraints, combined with P space group obtained from ENC, used generate centrosymmetric dimer...

The combination of advanced solid-state NMR spectroscopy, powder X-ray diffraction (PXRD), structure refinement, and quantum chemical calculations was used to determine the three-dimensional molecular structures self-assembled, one-dimensional (1D) metal coordination polymers. methodology is based on partial indexing PXRD patterns followed by modeling using constraints and, finally, Rietveld refinement density functional theory (DFT) optimization. protocol first demonstrated scandium...

Structural analysis by XRD still remains a considerable challenge for materials that can't be isolated as single crystals.In NMR crystallography structural constraints are extracted from the modern solid-state techniques, and along with DFT (density functional theory) calculations.[1-4]NMR has been used to derive de novo structures aid refinement of Xray powder diffraction data.[1][2][3][4] In this work, computational integration advanced PXRD (powder X-ray diffraction) modelling is...

Abstract The largest light-harvesting antenna in nature, the chlorosome, is a heterogeneous helical BChl self-assembly that has evolved green bacteria to harvest light for performing photosynthesis low-light environments. Guided by NMR chemical shifts and distance constraints Chlorobaculum tepidum wild-type chlorosomes, two contrasting packing modes syn-anti parallel stacks of c form polar 2D arrays, with dipole moments adding up, are explored. Layered assemblies were optimized using local...

Perylenediimides (PDI(s)) are one of the most fascinating classes dyes in vast plethora perylene families.PDIs robust, and have good photochemical thermal stability, making them suitable candidates for multiple optoelectronic applications.4] The importance a definitive crystal packing solid state efficient electron transfer charge separation was unraveled above-mentioned work.Among PDIs, nitro-perylenediimide(s) (NO2-PDI(s)) previously reported to exhibit light-induced excited-state...