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131.
132.
Andreas F. G. Glawar Dr. Daniel Best Benjamin J. Ayers Saori Miyauchi Shinpei Nakagawa Matilde Aguilar‐Moncayo Prof. José M. García Fernández Prof. Carmen Ortiz Mellet Dr. Elizabeth V. Crabtree Dr. Terry D. Butters Dr. Francis X. Wilson Prof. Atsushi Kato Prof. George W. J. Fleet 《Chemistry (Weinheim an der Bergstrasse, Germany)》2012,18(30):9341-9359
The efficient scalable syntheses of 2‐acetamido‐1,2‐dideoxy‐D ‐galacto‐nojirimycin (DGJNAc) and 2‐acetamido‐1,2‐dideoxy‐D ‐gluco‐nojirimycin (DNJNAc) from D ‐glucuronolactone, as well as of their enantiomers from L ‐glucuronolactone, are reported. The evaluation of both enantiomers of DNJNAc and DGJNAc, along with their N‐alkyl derivatives, as glycosidase inhibitors showed that DGJNAc and its N‐alkyl derivatives were all inhibitors of α‐GalNAcase but that none of the epimeric DNJNAc derivatives inhibited this enzyme. In contrast, both DGJNAc and DNJNAc, as well as their alkyl derivatives, were potent inhibitors of β‐GlcNAcases and β‐GalNAcases. Neither of the L ‐enantiomers showed any significant inhibition of any of the enzymes tested. Correlation of the in vitro inhibition with the cellular data, by using a free oligosaccharide analysis of the lysosomal enzyme inhibition, revealed the following structure–property relationship: hydrophobic side‐chains preferentially promoted the intracellular access of iminosugars to those inhibitors with more‐hydrophilic side‐chain characteristics. 相似文献
133.
Glawar AF Best D Ayers BJ Miyauchi S Nakagawa S Aguilar-Moncayo M García Fernández JM Ortiz Mellet C Crabtree EV Butters TD Wilson FX Kato A Fleet GW 《Chemistry (Weinheim an der Bergstrasse, Germany)》2012,18(30):9341-9359
The efficient scalable syntheses of 2-acetamido-1,2-dideoxy-D-galacto-nojirimycin (DGJNAc) and 2-acetamido-1,2-dideoxy-D-gluco-nojirimycin (DNJNAc) from D-glucuronolactone, as well as of their enantiomers from L-glucuronolactone, are reported. The evaluation of both enantiomers of DNJNAc and DGJNAc, along with their N-alkyl derivatives, as glycosidase inhibitors showed that DGJNAc and its N-alkyl derivatives were all inhibitors of α-GalNAcase but that none of the epimeric DNJNAc derivatives inhibited this enzyme. In contrast, both DGJNAc and DNJNAc, as well as their alkyl derivatives, were potent inhibitors of β-GlcNAcases and β-GalNAcases. Neither of the L-enantiomers showed any significant inhibition of any of the enzymes tested. Correlation of the in vitro inhibition with the cellular data, by using a free oligosaccharide analysis of the lysosomal enzyme inhibition, revealed the following structure-property relationship: hydrophobic side-chains preferentially promoted the intracellular access of iminosugars to those inhibitors with more-hydrophilic side-chain characteristics. 相似文献
134.
Kishi R Fujii H Kishimoto S Murata Y Ito S Okuno K Shigeta Y Nakano M 《The journal of physical chemistry. A》2012,116(17):4371-4380
We develop novel calculation and analysis methods for the dynamic first hyperpolarizabilities β [the second-order nonlinear optical (NLO) properties at the molecular level] in the second-harmonic generation based on the quantum master equation method combined with the ab initio molecular orbital (MO) configuration interaction method. As examples, we have evaluated off-resonant dynamic β values of donor (NH(2))- and/or acceptor (NO(2))-substituted benzenes using these methods, which are shown to reproduce those by the conventional summation-over-states method well. The spatial contributions of electrons to the dynamic β of these systems are also analyzed using the dynamic β density and its partition into the MO contributions. The present results demonstrate the advantage of these methods in unraveling the mechanism of dynamic NLO properties and in building the structure-dynamic NLO property relationships of real molecules. 相似文献
135.
136.
By using the IRMS-TPD method in which IR (infrared) and MS (mass spectroscopy) worked together, acid sites of USY (ultrastable Y) zeolite were studied. A new band of OH playing a role of Br?nsted acid was clearly detected on Na2H2-ethylenediaminetetraacetic acid (EDTA)-treated USY at 3595 cm(-1) during an elevation in temperature after the adsorption of ammonia. MS-measured TPD (temperature-programmed desorption) of NH3 and IR-measured TPD of the NH4+ cation coincided well to show that this zeolite consisted of the Br?nsted acid sites. The MS-TPD profile at higher temperatures corresponded to the IR-TPD of the 3595-cm(-1) band, and therefore, this OH was identified as a strong acid site. From comparison between IR-TPD of OH and MS-TPD, numbers of three kinds of Br?nsted OH (i.e., those in super and sodalite cages of a Y zeolite structure) and created strong Br?nsted acid site were quantified. On the other hand, strength of the Br?nsted acid site DeltaH was determined individually by a simulation method, where the corrected IR-TPD of OH was simulated based on the proposed equation. Thus, a new strong Br?nsted acid site was identified in the EDTA-treated USY, and the amount and strength was measured quantitatively. 相似文献
137.
Total synthesis of ent-dihydrocorynantheol by using a proline-catalyzed asymmetric addition reaction
[reaction: see text] 9-Tosyl-3,4-dihydro-beta-carboline reacted with 3-ethyl-3-buten-2-one in the presence of (S)-proline to give (3R,12bR)-3-ethyl-12-tosyl-3,4,6,7,8,9,10,11,12,12b-decahydro-1H-indolo[2,3-a]quinolizin-2-one in complete enantio- and diastereoselectivity. The compound thus obtained was readily transformed to ent-dihydrocorynantheol in three steps. 相似文献
138.
139.
Gyung-Min Choi Mamoru Tanahashi Toshio Miyauchi 《Proceedings of the Combustion Institute》2005,30(2):1807-1814
To control combustion oscillations, the characteristics of an oscillating swirl injection premixed flame have been investigated, and control of oscillating combustion and noise based on local flame structure has been conducted. The r.m.s. value of pressure fluctuations and noise level show significantly large values between = 0.8 and 1.1. The beating of pressure fluctuations is observed for the large oscillating flame conditions in this combustor. Relationship between beating of pressure fluctuations and local flame structure was observed by the simultaneous measurement of CH/OH planar laser induced fluorescence and pressure fluctuations. The local flame structure and beating of pressure fluctuations are related and the most complicated flame is formed in the middle pressure fluctuating region of beating. The beating of pressure fluctuations, which plays important roles in noise generation and nitric oxide emission in this combustor, could be controlled by injecting secondary fuel into the recirculating region of oscillating flames. Injecting secondary fuel prevented lean blowout, and low NOx combustion was also achieved even for the case of pure methane injection as a secondary fuel. By injecting secondary fuel into the recirculating region near the swirl injector, the flame lifted from the swirl injector and its reaction region became uniform and widespread, hence resulting in low nitric oxide emission. Secondary mixture injection, fuel diluted with air, is not effective for control of combustion oscillations suppression and lean blowout prevention. 相似文献
140.
Mitsuru Akashi Koichi Beppu Ikuo Kikuchi Noriyuki Miyauchi 《高分子科学杂志,A辑:纯化学与应用化学》2013,50(10):1233-1249
Hydrophilic copolymers containing 5-fluorouracil (5-FU), thymine, or adenine were prepared by the free-radical copolymerization of methacryloyl-type monomers containing them with water-soluble vinyl monomers such as acrylic acid, methacrylic acid, vinylpyrroli-done, acrylamide, and 4(5)-vinylimidazole with AIBN as initiator. Complex formation between the copolymers and RNA and between the copolymers having complementary nucleic acid bases in aqueous solution and a DMSO-ethylene glycol was studied by means of UV spectroscopy. These copolymers were found to release the N-hydroxyethyl derivatives of 5-FU, thymine, or adenine by hydrolysis of the ester of the polymer side chain under mild conditions. The effects of the kind of water-soluble comonomer, temperature, pH, and the imidazole group as catalyst on the hydrolysis of the ester are discussed. 相似文献