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1.
Angew Chem Int Ed Engl ; 61(14): e202115087, 2022 Mar 28.
Artigo em Inglês | MEDLINE | ID: mdl-35098633

RESUMO

The structure of zeolite SSZ-43 was determined by 3D electron diffraction, synchrotron X-ray powder diffraction, and high-resolution transmission electron microscopy. The SSZ-43 framework forms one-dimensional, sinusoidal 12-ring channels from 54 61 butterfly units commonly found in other zeolites, but with unique 6.5×6.5 Šapertures and 12-ring 6.5×8.9 Šwindows perpendicular to the channels. SSZ-43 crystals are intergrowths of two polytypes: ≈90 % orthorhombic polytype A with ABAB stacking of the 12-rings, and ≈10 % monoclinic polytype B with ABCABC stacking. Molecular modeling performed on the idealized Si-SSZ-43 structure along with empirical relationships for zeolite selectivity in boron- and aluminum-containing synthesis gels were used in a combined approach to design new di-quaternary ammonium organic structure-directing agents (OSDAs). Experimental trials demonstrated that the new OSDAs produced SSZ-43 over a broader range of compositions than previous mono-quaternary OSDAs.

2.
Angew Chem Int Ed Engl ; 57(18): 4926-4930, 2018 04 23.
Artigo em Inglês | MEDLINE | ID: mdl-29490110

RESUMO

A metal-organic framework (MOF)-based catalyst, chromium hydroxide/MIL-101(Cr), was prepared by a one-pot synthesis method. The combination of chromium hydroxide particles on and within Lewis acidic MIL-101 accomplishes highly selective conversion of glucose to fructose in the presence of ethanol, matching the performance of optimized Sn-containing Lewis acidic zeolites. Differently from zeolites, NMR spectroscopy studies with isotopically labeled molecules demonstrate that isomerization of glucose to fructose on this catalyst, proceeds predominantly via a proton transfer mechanism.

3.
Rev Sci Instrum ; 87(10): 103101, 2016 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-27802763

RESUMO

A design is presented for a versatile transmission infrared cell that can interface with an external vacuum manifold to undergo in situ gas treatments and receive controlled doses of various adsorbates and probe molecules, allowing characterization of heterogeneous catalyst surfaces in order to identify and quantify active sites and adsorbed surface species. Critical design characteristics include customized temperature control for operation between cryogenic and elevated temperatures (100-1000 K) and modified Cajon fittings for operation over a wide pressure range (10-2-103 Torr) that eliminates the complications introduced when using sealants or flanges to secure cell windows. The customized, hand-tightened Cajon fittings simplify operation of the cell compared to previously reported designs, because they allow for rapid cell assembly and disassembly and, in turn, replacement of catalyst samples. In order to validate the performance of the cell, transmission infrared spectroscopic experiments are reported to characterize the Brønsted and Lewis acid sites present in H-beta and H-mordenite zeolites using cryogenic adsorption of CO (<150 K).

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