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2.
Reconstitution of Biosynthetic Machinery for the Synthesis of the Highly Elaborated Indole Diterpene Penitrem 下载免费PDF全文
Dr. Chengwei Liu Koichi Tagami Dr. Atsushi Minami Tomoyuki Matsumoto Jens Christian Frisvad Hideyuki Suzuki Jun Ishikawa Katsuya Gomi Prof. Dr. Hideaki Oikawa 《Angewandte Chemie (International ed. in English)》2015,54(19):5748-5752
Penitrem A is one of the most elaborated members of the fungal indole diterpenes. Two separate penitrem gene clusters were identified using genomic and RNA sequencing data, and 13 out of 17 transformations in the penitrem biosynthesis were elucidated by heterologous reconstitution of the relevant genes. These reactions involve 1) a prenylation‐initiated cationic cyclization to install the bicyclo[3.2.0]heptane skeleton (PtmE), 2) a two‐step P450‐catalyzed oxidative processes forming the unique tricyclic penitrem skeleton (PtmK and PtmU), and 3) five sequential oxidative transformations (PtmKULNJ). Importantly, without conventional gene disruption, reconstitution of the biosynthetic machinery provided sufficient data to determine the pathway. It was thus demonstrated that the Aspergillus oryzae reconstitution system is a powerful method for studying the biosynthesis of complex natural products. 相似文献
3.
Cover Picture: Reconstitution of Biosynthetic Machinery for the Synthesis of the Highly Elaborated Indole Diterpene Penitrem (Angew. Chem. Int. Ed. 19/2015) 下载免费PDF全文
4.
Fe K‐Edge X‐ray Absorption Fine Structure Determination of γ‐Al2O3‐Supported Iron‐Oxide Species 下载免费PDF全文
Dr. Atsuko Tomita Dr. Takeshi Miki Takeru Tango Tatsuro Murakami Hideyuki Nakagawa Dr. Yutaka Tai 《Chemphyschem》2015,16(9):2015-2020
The structure of FeOx species supported on γ‐Al2O3 was investigated by using Fe K‐edge X‐ray absorption fine structure (XAFS) and X‐ray diffraction (XRD) measurements. The samples were prepared through the impregnation of iron nitrate on Al2O3 and co‐gelation of aluminum and iron sulfates. The dependence of the XRD patterns on Fe loading revealed the formation of α‐Fe2O3 particles at an Fe loading of above 10 wt %, whereas the formation of iron‐oxide crystals was not observed at Fe loadings of less than 9.0 wt %. The Fe K‐edge XAFS was characterized by a clear pre‐edge peak, which indicated that the Fe?O coordination structure deviates from central symmetry and that the degree of Fe?O?Fe bond formation is significantly lower than that in bulk samples at low Fe loading (<9.0 wt %). Fe K‐edge extended XAFS oscillations of the samples with low Fe loadings were explained by assuming an isolated iron‐oxide monomer on the γ‐Al2O3 surface. 相似文献
5.
A new method for constructing the polycyclic skeleton of psiguadial B (1), a meroterpenoid isolated from an evergreen shrub of Myrtaceae, was developed. The terpenoid substructure of 1 was constructed on the basis of a cascade double cyclization reaction of an alkyne dicobalt complex, which afforded the bicyclo[4.3.1]decane derivative having a benzyl group with the correct configuration. The substituted aromatic ring was introduced to the bridgehead position of the intermediate, and bromination under radical conditions followed by intramolecular cyclization reaction resulted in formation of the benzopyran moiety in a stereoselective manner. 相似文献
6.
Morphological studies of a hydrogen-bonded LC polymer obtained by photopolymerization in LC solvents
Hideyuki Kihara Corresponding author Toshiaki Miura Ryoichi Kishi Takashi Yoshida Mitsuhiro Shibata Ryutoku Yosomiya 《Liquid crystals》2013,40(7):799-809
Anisotropic morphologies and the phase behaviour of a hydrogen-bonded LC polymer obtained by photopolymerization in two kinds of LC solvent are discussed. The hydrogen-bonded LC monomer, 4-(6-acryloyloxyhexyloxy) benzoic acid (A6OBA), was photopolymerized in 4-cyano-4′-hexyloxybiphenyl (6OCB) and in 4-cyano-4′-undecyloxybiphenyl (11OCB), which show a nematic phase and a smectic A phase, respectively. After photo-polymerization, the LC media were removed by extraction and the pure polymer was observed by scanning electron microscopy. SEM images showed that the polymer possessed fibrous morphology with a fibre diameter of a few micrometers, based on polymerization-induced phase separation. The overall geometries reflected typical LC characteristics such as schlieren and focal-conic fan textures. It was found that the hydrogen bond between benzoic acid groups in the monomer was rigid enough to fix the anisotropic phase-separated structure forming during the early stage of phase separation; however, it could not permanently maintain the fibre structure due to dissociation at elevated temperature. X-ray measurements revealed that a well developed layer structure of the hydrogen-bonded mesogen existed in the polymer obtained from the smectic phase of 11OCB, whereas a polymer layer structure could develop only partially from the nematic phase of 6OCB. 相似文献
7.
Fujiko Iwasaki Hideyuki Nishiyama Noriko Manabe Masanori Yasui Noboru Matsumura 《Phosphorus, sulfur, and silicon and the related elements》2013,188(1):429-430
Abstract Novel metal-carbene complexes (4) with a metallapentalene framework have been obtained from hypervalent diazadiselenathiapentalenes (3) by treating with Pt(PPh3)4, Pd(PPh3)4 and RhCl(PPh3)3. X-Ray investigations revealed that the central hypervalent sulfur atom in 3 was substituted by a metal atom to form M-Se bonds in the resultant metallapentalene framework. 相似文献
8.
Effects of polyethylene spacer length in polymeric electrolytes on gelation of ionic liquids and ionogel properties 下载免费PDF全文
Jun'ichi Nagasawa Sonoko Wakahara Hajime Matsumoto Hideyuki Kihara Masaru Yoshida 《Journal of polymer science. Part A, Polymer chemistry》2015,53(2):249-255
Polymer electrolytes containing N,N′-(trans-cyclohexane-1,4-diyl)dibenzamide linkages, polyethylene ((CH2)m, m = 2, 4, 10) spacers, and bis(trifluoromethanesulfonyl)amide (TFSA) or bis(fluorosulfonyl)amide (FSA) counteranions (polymer abbreviation: CDBAm•X; m = 2, 4, 10; X = TFSA, FSA) have been synthesized, adding to our previous report (m = 6). In addition, their ability to effect the gelation of six ionic liquids and the properties of the resulting ionogels have been examined. The polymers, except for CDBA10•TFSA, effect the gelation for all ionic liquids used in this study at fairly low concentrations (0.9–50 g/L). Ionogel ionic conductivity is not dependent on the spacer length, but does decrease slightly as increasing amounts of the gelatinizer are introduced. In contrast to ionic conductivity, the temperatures at which these ionogels transition into isotropic fluids is dependent on the spacer length; the gel composed of [EMI][FSA] and 100 g/L of CDBA6•FSA transforms at 120 °C, while the gel composed of [EMI][FSA] and 5 g/L of CDBA2•FSA does not transform into a sol even when temperatures become 155 °C. In brief, ionogel heat resistance can be improved by changing the spacer length of the polyelectrolyte. Finally, it has been determined using cyclic voltammetry that the potential window of the polyelectrolytes is particularly wide, ranging from −1.6 to 2.5 V. © 2014 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2015 , 53, 249–255 相似文献
9.
Hiromichi Aono Hiroki Ebara Ryota Senba Takashi Naohara Tsunehiro Maehara Hideyuki Hirazawa Yuji Watanabe 《Journal of magnetism and magnetic materials》2012
Nano-sized magnetic Y3Fe5O12 ferrite having a high heat generation ability in an AC magnetic field was prepared by bead milling. A commercial powder sample (non-milled sample) of ca. 2.9 μm in particle size did not show any temperature enhancement in the AC magnetic field. The heat generation ability in the AC magnetic field improved with a decrease in the average crystallite size for the bead-milled Y3Fe5O12 ferrites. The highest heat ability in the AC magnetic field was for the fine Y3Fe5O12 powder with a 15-nm crystallite size (the samples were milled for 4 h using 0.1 mm? beads). The heat generation ability of the excessively milled Y3Fe5O12 samples decreased. The main reason for the high heat generation property of the milled samples was ascribed to an increase in the Néel relaxation of the superparamagnetic material. The heat generation ability was not influenced by the concentration of the ferrite powder. For the samples milled for 4 h using 0.1 mm? beads, the heat generation ability (W g−1) was estimated using a 3.58×10−4 fH2 frequency (f/kHz) and the magnetic field (H/kA m−1), which is the highest reported value of superparamagnetic materials. 相似文献
10.
Tetsuya Uematsu 《Mathematische Zeitschrift》2015,279(3-4):1047-1066