Formation of Frustrated Lewis Pairs in Ptx -Loaded Zeolite NaY.

The formation of a frustrated Lewis pair consisting of sodium hydride (Na(+) H(-) ) and a framework-bound hydroxy proton O(H(+) ) is reported upon H2 treatment of zeolite NaY loaded with Pt nanoparticles (Ptx /NaY). Frustrated Lewis pair formation was confirmed using in situ neutron diffraction and spectroscopic measurements. The activity of the intrazeolite NaH as a size-selective catalyst was verified by the efficient esterification of acetaldehyde (a small aldehyde) to form the corresponding ester ethyl acetate, whereas esterification of the larger molecule benzaldehyde was unsuccessful. The frustrated Lewis pair (consisting of Na(+) H(-) and O(H(+) )) generated within zeolite NaY may be a useful catalyst for various catalytic reactions which require both H(-) and H(+) ions, such as catalytic hydrogenation or dehydrogenation of organic compounds and activation of small molecules.

[1]  D. Stephan,et al.  Enabling catalytic ketone hydrogenation by frustrated Lewis pairs. , 2014, Journal of the American Chemical Society.

[2]  Ana Primo,et al.  Zeolites as catalysts in oil refining. , 2014, Chemical Society reviews.

[3]  J. Seo,et al.  In Situ Neutron Powder Diffraction and X-ray Photoelectron Spectroscopy Analyses on the Hydrogenation of MOF-5 by Pt-Doped Multiwalled Carbon Nanotubes , 2014 .

[4]  M. Leskelä,et al.  A frustrated-Lewis-pair approach to catalytic reduction of alkynes to cis-alkenes , 2013, Nature Chemistry.

[5]  Heiner Friedrich,et al.  Heterogeneities of the nanostructure of platinum/zeolite y catalysts revealed by electron tomography. , 2013, ACS nano.

[6]  S. Grimme,et al.  Metal-free catalytic olefin hydrogenation: low-temperature H2 activation by frustrated Lewis pairs. , 2012, Angewandte Chemie.

[7]  M. Conradi,et al.  NMR Studies of NaH , 2012 .

[8]  J. Weitkamp.  Catalytic Hydrocracking—Mechanisms and Versatility of the Process , 2012 .

[9]  J. Klankermayer,et al.  Enantioselective hydrogenation with chiral frustrated Lewis pairs. , 2010, Angewandte Chemie.

[10]  T. Werner,et al.  Sodium Hydride Catalyzed Tishchenko Reaction , 2010 .

[11]  W. Piers,et al.  Tandem frustrated Lewis pair/tris(pentafluorophenyl)borane-catalyzed deoxygenative hydrosilylation of carbon dioxide. , 2010, Journal of the American Chemical Society.

[12]  G. Erker,et al.  Frustrierte Lewis‐Paare: metallfreie Wasserstoffaktivierung und mehr , 2010 .

[13]  Douglas W Stephan,et al.  Frustrated Lewis pairs: metal-free hydrogen activation and more. , 2010, Angewandte Chemie.

[14]  Douglas W Stephan,et al.  "Frustrated Lewis pairs": a concept for new reactivity and catalysis. , 2008, Organic & biomolecular chemistry.

[15]  Anmin Zheng,et al.  Brønsted/Lewis acid synergy in dealuminated HY zeolite: a combined solid-state NMR and theoretical calculation study. , 2007, Journal of the American Chemical Society.

[16]  Xuefeng Wang,et al.  Sodium hydride clusters in solid hydrogen and neon: infrared spectra and theoretical calculations. , 2007, The journal of physical chemistry. A.

[17]  A. Feller,et al.  On the mechanism of catalyzed isobutane/butene alkylation by zeolites , 2004 .

[18]  P. Jacobs,et al.  Alkylcarbenium Ion Concentrations in Zeolite Pores During Octane Hydrocracking on Pt/H-USY Zeolite , 2004 .

[19]  H. Karge.  Characterization by infrared spectroscopy , 1998 .

[20]  M. Hunger.  Br⊘nsted Acid Sites in Zeolites Characterized by Multinuclear Solid-State NMR Spectroscopy , 1997 .

[21]  M. Hunger,et al.  Characterisation of sodium cations in dehydrated zeolite NaX by 23Na NMR spectroscopy. , 1996, Solid state nuclear magnetic resonance.

[22]  B. Gil,et al.  IR Spectroscopic Studies of Dealuminated and Realuminated Zeolite HY , 1996 .

[23]  John L. Falconer,et al.  Spillover in Heterogeneous Catalysis , 1995 .

[24]  R. A. Santen,et al.  Hydrocracking of n-decane over zeolite-supported metal sulfide catalysts. 1. CaY-supported transition metal sulfides , 1995 .

[25]  M. Sakata,et al.  Maximum-entropy-method analysis of neutron diffraction data , 1993 .

[26]  T. Barr.  The nature of the relative bonding chemistry in zeolites : an XPS study , 1990 .