Sheldon G. Shore
Ohio State University
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Featured researches published by Sheldon G. Shore.
Science | 1993
Ewan J. M. Hamilton; Shawn E. Dolan; Charles Mann; Hendrik O. Colijn; Clare A. McDonald; Sheldon G. Shore
Amorphous boron nitride, BN, is obtained from the reaction of B-trichloroborazine, (BCINH)3, with cesium metal. The amorphous product is converted to a turbostratic form upon heating to 1100�C. Scanning electron microscopy reveals a previously unreported morphology composed of hollow tubular structures. The largest of these appear to be approximately 3 micrometers in external diameter and 50 to 100 micrometers in length. Transmission electron microscopy and selected-area electron diffraction also indicate the tube walls to be turbostratic in nature. The mechanism by which the tubes form is not known, although apparent sites of incipient tube growth have been observed.
Catalysis Communications | 2002
Sheldon G. Shore; Errun Ding; Colin Park; Mark A. Keane
Abstract The catalytic activity/selectivity of a 5% w/w Pd/SiO 2 catalyst prepared by Pd(NO 3 ) 2 impregnation has been compared with that delivered by 5% w/w Pd/SiO 2 and PdYb/SiO 2 prepared from Pd(C 2 H 3 O 2 ) 2 and {(DMF) 10 Yb 2 [Pd(CN) 4 ] 3 } ∞ precursors, respectively; phenol hydrogenation (T=423 K ) was used as a test reaction. The activated catalysts have been characterized by HRTEM/EDX; differences in activity are related to the TEM derived Pd particle size distribution. Incorporation of Yb resulted in an appreciable enhancement of both phenol conversion and the overall yield of cyclohexanone, an effect that is attributed to electron donation from Yb to the active Pd centers.
Journal of the American Chemical Society | 2010
Xuenian Chen; Ji-Cheng Zhao; Sheldon G. Shore
A new ambient-temperature, catalyst-free reaction between ammonia borane and tetrahydrofuran borane produces aminodiborane via the formation of a dihydrogen bond and subsequent molecular hydrogen elimination. The facile synthesis of aminodiborane will make this long-sought active chemical reagent readily available for both inorganic and organic reactions. From aminodiborane, an inorganic butane analogue, NH(3)BH(2)NH(2)BH(3), was prepared, and its single-crystal structure displayed a gauche rather than an anti form conformation.
Accounts of Chemical Research | 2013
Xuenian Chen; Ji-Cheng Zhao; Sheldon G. Shore
A dihydrogen bond (DHB) is an electrostatic interaction between a protonic hydrogen and a hydridic hydrogen. Over the past two decades, researchers have made significant progress in the identification and characterization of DHBs and their properties. In comparison with conventional hydrogen bonds (HBs), which have been widely used in catalysis, molecular recognition, crystal engineering, and supramolecular synthesis, chemists have only applied DHBs in very limited ways. Considering that DHBs and conventional HBs have comparable strength, DHBs could be more widely applied in chemistry. Over the past several years, we have explored the impact of DHBs on amine borane chemistry and the syntheses and characterization of amine boranes and ammoniated metal borohydrides for hydrogen storage. Through systematic computational and experimental investigations, we found that DHBs play a dominant role in dictating the reaction pathways (and thus different products) of amine boranes where oppositely charged hydrogens coexist for DHB formation. Through careful experiments, we observed, for the first time, a long-postulated reaction intermediate, ammonia diborane (AaDB), whose behavior is essential to mechanistic understanding of the formation of the diammoniate of diborane (DADB) in the reaction of ammonia (NH3) with tetrahydrofuran borane (THF·BH3). The formation of DADB has puzzled the boron chemistry community for decades. Mechanistic insight enabled us to develop facile syntheses of aminodiborane (ADB), ammonia borane (AB), DADB, and an inorganic butane analog NH3BH2NH2BH3 (DDAB). Our examples, together with those in the literature, reinforce the fact that DHB formation and subsequent molecular hydrogen elimination are a viable approach for creating new covalent bonds and synthesizing new materials. We also review the strong effects of DHBs on the stability of conformers and the hydrogen desorption temperatures of boron-nitrogen compounds. We hope that this Account will encourage further applications of DHBs in molecular recognition, host-guest chemistry, crystal engineering, supramolecular chemistry, molecular self-assembly, chemical kinetics, and the syntheses of new advanced materials.
Journal of the American Chemical Society | 2011
Xuenian Chen; Xiaoguang Bao; Ji-Cheng Zhao; Sheldon G. Shore
The mechanism of formation of ammonia borane (NH(3)BH(3), AB) and the diammoniate of diborane ([H(2)B(NH(3))(2)][BH(4)], DADB) in the reaction between NH(3) and THF·BH(3) was explored experimentally and computationally. Ammonia diborane (NH(3)BH(2)(μ-H)BH(3), AaDB), a long-sought intermediate proposed for the formation of DADB, was directly observed in the reaction using (11)B NMR spectroscopy. The results indicate that dihydrogen bonds between the initially formed AB and AaDB accelerate the formation of DADB in competition with the formation of AB.
Inorganic Chemistry | 2011
Zhenguo Huang; Xuenian Chen; Teshome B. Yisgedu; Edward A. Meyers; Sheldon G. Shore; Ji-Cheng Zhao
A metathesis reaction between unsolvated NaB(3)H(8) and NH(4)Cl provides a simple and high-yield synthesis of NH(4)B(3)H(8). Structure determination through X-ray single crystal diffraction analysis reveals weak N-H(δ+)---H(δ-)-B interaction in NH(4)B(3)H(8) and strong N-H(δ+)---H(δ-)-B interaction in NH(4)B(3)H(8)·18-crown-6·THF adduct. Pyrolysis of NH(4)B(3)H(8) leads to the formation of hydrogen gas with appreciable amounts of other volatile boranes below 160 °C. Hydrolysis experiments show that upon addition of catalysts, NH(4)B(3)H(8) releases up to 7.5 materials wt % hydrogen.
Journal of Organometallic Chemistry | 1978
K. Inkrott; R. Goetze; Sheldon G. Shore
Abstract Reductive cleavage of [Mn(CO) 5 ] 2 , [Co(CO) 4 ] 2 , [(Ph 3 P)Co(CO) 3 ] 2 , [(C 5 H 5 )Mo(CO) 3 ] 2 , and [(C 5 H 5 )Fe(CO) 2 ] 2 by KH in THF or HMPA/THF affords KMn(CO) 5 , KCo(CO) 4 , K(Ph 3 P)Co(CO) 3 , K(C 5 H 5 )Mo(CO) 3 , and K(C 5 H 5 )Fe(CO) 2 , respectively, in near quantitative yields.
Journal of Materials Chemistry | 2010
Zhenguo Huang; Judith C. Gallucci; Xuenian Chen; Teshome B. Yisgedu; Hima Kumar Lingam; Sheldon G. Shore; Ji-Cheng Zhao
A new ammine complex, Li2B12H12·7NH3, that can reversibly release all the NH3 at below 200 °C and reabsorb NH3 at room temperature and 0.5 bar was synthesized and investigated for reversible ammonia storage or indirect hydrogen storage.
Inorganic Chemistry | 2010
Zhenguo Huang; Graham King; Xuenian Chen; Jason Michael Hoy; Teshome B. Yisgedu; Hima Kumar Lingam; Sheldon G. Shore; Patrick M. Woodward; Ji-Cheng Zhao
A simple and efficient way to synthesize unsolvated sodium octahydrotriborate has been developed. This method avoids the use of dangerous starting materials and significantly simplifies the reaction setup, thus enabling convenient large-scale synthesis. The structure of the unsolvated compound has been determined through powder X-ray diffraction.
Inorganic Chemistry | 2009
Duane C. Wilson; Shengming Liu; Xuenian Chen; Edward A. Meyers; Xiaoguang Bao; Andrey V. Prosvirin; Kim R. Dunbar; Christopher M. Hadad; Sheldon G. Shore
Water-free rare earth(III) hexacyanoferrate(III) complexes, {Ln(DMF)(6)(mu-CN)(2)Fe(CN)(4)}(infinity) (DMF = N,N-dimethylformamide; Ln = Sm, 1; Eu, 2; Gd, 3; Tb, 4; Dy, 5; Ho, 6; Er, 7; Tm, 8; Yb, 9; Lu, 10; Y, 11; La, 12; Ce, 13; Pr, 14; Nd, 15), were synthesized in dry DMF through the metathesis reactions of [(18-crown-6)K](3)Fe(CN)(6) with LnX(3)(DMF)(n) (X = Cl or NO(3)). Anhydrous DMF solutions of LnX(3)(DMF)(n) were prepared at room temperature from LnCl(3) or LnX(3).nH(2)O under a dynamic vacuum. All compounds were characterized by IR, X-ray powder diffraction (except for 10), and single crystal X-ray diffraction (except for 2, 7, 10). Infrared spectra reveal that a monotonic, linear relationship exists between the ionic radius of the lanthanide and the nu(mu-CN) stretching frequency of 1-10, 12-15 while 11 deviates slightly from the ionic radius relationship. X-ray powder diffraction data are in agreement with powder patterns calculated from single crystal X-ray diffraction results, a useful alternative for bulk sample confirmation when elemental analysis data are difficult to obtain. Eight-coordinate Ln(III) metal centers are observed for all structures. trans-cyanide units of [Fe(CN)(6)](3-) formed isocyanide linkages to Ln(III) resulting in one-dimensional polymeric chains. Structures of compounds 1-9 and 11 are isomorphous, crystallizing in the space group C2/c. Structures of compounds 12-15 are also isomorphous, crystallizing in the space group P2/n. One unique polymeric chain exists in the structures of 1-9 and 11 while two unique polymeric chains exist in structures of 12-15. One of the polymeric chains of 12-15 is similar to that observed for 1-9, 11 while the other is more distorted and has a shorter Ln-Fe distance. Magnetic susceptibility measurements for compounds 3-6, 8, 11 were performed on polycrystalline samples of the compounds.