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11.
Total Synthesis and Biological Evaluation of the Antibiotic Lysocin E and Its Enantiomeric,Epimeric, and N‐Demethylated Analogues
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Dr. Motoki Murai Takuya Kaji Dr. Takefumi Kuranaga Dr. Hiroshi Hamamoto Prof. Dr. Kazuhisa Sekimizu Prof. Dr. Masayuki Inoue 《Angewandte Chemie (International ed. in English)》2015,54(5):1556-1560
Lysocin E, a macrocyclic peptide, exhibits potent antibacterial activity against methicillin‐resistant Staphylococcus aureus (MRSA) through a novel mechanism. The first total synthesis of lysocin E was achieved by applying a full solid‐phase strategy. The developed approach also provides rapid access to the enantiomeric, epimeric, and N‐demethylated analogues of lysocin E. Significantly, the antibacterial activity of the unnatural enantiomer was comparable to that of the natural isomer, suggesting the absence of chiral recognition in its mode of action. 相似文献
12.
Elgeti M Kazmin R Heck M Morizumi T Ritter E Scheerer P Ernst OP Siebert F Hofmann KP Bartl FJ 《Journal of the American Chemical Society》2011,133(18):7159-7165
Rhodopsin, a seven transmembrane helix (TM) receptor, binds its ligand 11-cis-retinal via a protonated Schiff base. Coupling to the G-protein transducin (G(t)) occurs after light-induced cis/trans-retinal isomerization, which leads through photoproducts into a sequence of metarhodopsin (Meta) states: Meta I ? Meta IIa ? Meta IIb ? Meta IIbH(+). The structural changes behind this three-step activation scheme are mediated by microswitch domains consisting of conserved amino acids. Here we focus on Tyr223(5.58) as part of the Y(5.58)X(7)K(R)(5.66) motif. Mutation to Ala, Phe, or Glu results in specific impairments of G(t)-activation measured by intrinsic G(t) fluorescence. UV-vis/FTIR spectroscopy of rhodopsin and its complex with a C-terminal G(t)α peptide allows the assignment of these deficiencies to specific steps in the activation path. Effects of mutation occur already in Meta I but do not directly influence deprotonation of the Schiff base during formation of Meta IIa. Absence of the whole phenol ring (Y223A) allows the activating motion of TM6 in Meta IIb but impairs the coupling to G(t). When only the hydroxyl group is lacking (Y223F), Meta IIb does not accumulate, but the activity toward G(t) remains substantial. From the FTIR features of Meta IIbH(+) we conclude that proton uptake to Glu134(3.49) is mandatory for Tyr223(5.58) to engage in the interaction with the key player Arg135(3.50) predicted by X-ray analysis. This polar interaction is partially recovered in Y223E, explaining its relatively high activity. Only the phenol side chain of tyrosine provides all characteristics for accumulation of the active state and G-protein activation. 相似文献
13.
Takefumi Nosaka 《Topology and its Applications》2011,158(8):996-1011
For a quandle X, the quandle space BX is defined, modifying the rack space of Fenn, Rourke and Sanderson (1995) [13], and the quandle homotopy invariant of links is defined in Z[π2(BX)], modifying the rack homotopy invariant of Fenn, Rourke and Sanderson (1995) [13]. It is known that the cocycle invariants introduced in Carter et al. (2005) [3], Carter et al. (2003) [5], Carter et al. (2001) [6] can be derived from the quandle homotopy invariant.In this paper, we show that, for a finite quandle X, π2(BX) is finitely generated, and that, for a connected finite quandle X, π2(BX) is finite. It follows that the space spanned by cocycle invariants for a finite quandle is finitely generated. Further, we calculate π2(BX) for some concrete quandles. From the calculation, all cocycle invariants for those quandles are concretely presented. Moreover, we show formulas of the quandle homotopy invariant for connected sum of knots and for the mirror image of links. 相似文献
14.
Takefumi Yano Shigeru Ikai Katsutoshi Washio 《Journal of polymer science. Part A, Polymer chemistry》1985,23(12):3069-3080
The catalyst system comprised of a heptane solution of magnesiumoctoate-H2O-Tetrabutoxytitanium/diethylaluminumchloride was highly active for ethylene polymerization at a high temperature. High productivity for the catalyst system at a low temperature was achieved by the aging of the catalyst components. The effect of different orders of addition of the catalyst components on productivity was investigated to assume the role of each components in the formation of active species. 相似文献
15.
Takefumi Kondo 《Differential Geometry and its Applications》2005,22(2):121-130
In this paper we are going to generalize Gromov's mm-Reconstruction theorem (cf. [Metric Structures for Riemannian and Non-Riemannian Spaces, Birkhäuser, Basel, 1999] ) to a probability measures on the spaces of mm-spaces. And for this purpose, we give alternative proof of mm-Reconstruction theorem. 相似文献
16.
Total Synthesis of the Nonribosomal Peptide Surugamide B and Identification of a New Offloading Cyclase Family
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Prof. Takefumi Kuranaga Prof. Kenichi Matsuda Ayae Sano Masakazu Kobayashi Dr. Akihiro Ninomiya Prof. Kentaro Takada Prof. Shigeki Matsunaga Prof. Toshiyuki Wakimoto 《Angewandte Chemie (International ed. in English)》2018,57(30):9447-9451
The cathepsin B inhibitor surugamide B ( 2 ), along with structurally related derivatives (A and C–E), has previously been isolated from the marine actinomycete Streptomyces sp. JAMM992. The biosynthetic genes are unexpectedly part of a cluster of four non‐ribosomal peptide synthetase (NRPS) genes, two of which are responsible for the biosynthesis of the additional linear decapeptide surugamide F. However, the thioesterase domain required for the later stage of the biosynthesis of the cyclic peptides surugamides A–E is not present in any module architecture of the surugamide NRPSs. Herein, we report the first total synthesis of surugamide B ( 2 ) through the macrocyclization at the biomimetic position, which not only alleviated the Cα epimerization in the macrolactamization process, but also efficiently provided 2 in 34 % yield for 18 steps. Furthermore, both the chemical and enzymatic studies with the biosynthetic precursor mimics revealed that the stand‐alone enzyme SurE, which belongs to the penicillin‐binding protein family, is responsible for macrocyclization of the tethered octapeptidyl intermediate. 相似文献
17.
Direct Observation of Ordered High‐Spin–Low‐Spin Intermediate States of an Iron(III) Three‐Step Spin‐Crossover Complex
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Dr. Zhao‐Yang Li Dr. Hiroyoshi Ohtsu Dr. Tatsuhiro Kojima Dr. Jing‐Wei Dai Takefumi Yoshida Dr. Brian K. Breedlove Dr. Wei‐Xiong Zhang Dr. Hiroaki Iguchi Prof. Osamu Sato Prof. Masaki Kawano Prof. Masahiro Yamashita 《Angewandte Chemie (International ed. in English)》2016,55(17):5184-5189
A neutral mononuclear FeIII complex [FeIII(H‐5‐Br‐thsa‐Me)(5‐Br‐thsa‐Me)]?H2O ( 1 ; H2‐5‐Br‐thsa‐Me=5‐bromosalicylaldehyde methylthiosemicarbazone) was prepared that exhibited a three‐step spin‐crossover (SCO) with symmetry breaking and a 14 K hysteresis loop owing to strong cooperativity. Two ordered intermediate states of 1 were observed, 4HS–2LS and 2HS–4LS, which exhibited reentrant phase‐transition behavior. This study provides a new platform for examining multistability in SCO complexes. 相似文献
18.
Naoki Toyooka Yasuhito Yotsui Yasuko Yoshida Takefumi Momose Hideo Nemoto 《Tetrahedron》1999,55(52):1189-15224
The enantioselective total synthesis of the marine alkaloids clavepictines A, B and pictamine has been achieved through the highly stereocontrolled quinolizidine ring closure of the conformationally constrained piperidine ring system (2), which bears the chiral centers and appropriate functionality needed for the synthesis of target alkaloids. The absolute stereochemistry of clavepictines and pictamine was verified to be 3R, 4S, 6S, 9aS by the present synthesis. 相似文献
19.
Yasuhiro Matsuda Takefumi Kawata Shinji Sugihara Sadahito Aoshima Takahiro Sato 《Journal of Polymer Science.Polymer Physics》2006,44(8):1179-1187
The aqueous solution of a thermoresponsive polymer, poly[2‐(2‐ethoxy) ethoxyethyl vinyl ether] poly(EOEOVE), contains a tiny amount of large polymer aggregates at low polymer concentrations far below the lower critical solution temperature (~40 °C). The molar mass Mw,slow, radius of gyration 〈S2〉, and hydrodynamic radius RH,slow of the aggregating component of poly(EOEOVE) were obtained by simultaneous static and dynamic light scattering as functions of the polymer concentration and temperature, while the weight fraction wslow of the component was estimated by size‐exclusion chromatography. The Mw,slow dependencies of 〈S2〉 and RH,slow, as well as the ratio 〈S2〉/RH,slow, indicated that the poly(EOEOVE) aggregate takes a sparsely branched polymer‐like conformation. We have analyzed the structure of the aggregate, using the branched polymer model of random type. The Mw,slow dependence of 〈S2〉 obtained was favorably compared with this model with reasonable structural parameters. © 2006 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 44: 1179–1187, 2006 相似文献
20.
Yongbing Shen Hiroshi Ito Haitao Zhang Hideki Yamochi Seiu Katagiri Shinji K. Yoshina Akihiro Otsuka Manabu Ishikawa Goulven Cosquer Kaiji Uchida Carmen Herrmann Takefumi Yoshida Brian K. Breedlove Masahiro Yamashita 《Chemical science》2020,11(41):11154
Single-molecule magnets (SMMs) show superparamagnetic behaviour below blocking temperature at the molecular scale, so they exhibit large magnetic density compared to the conventional magnets. Combining SMMs and molecular conductors in one compound will bring about new physical phenomena, however, the synergetic effects between them still remain unexplored. Here we present a layered molecule-based compound, β′′-(BEDO-TTF)4 [Co(pdms)2]·3H2O (BO4), (BEDO-TTF (BO) and H2pdms are bis(ethylenedioxy)tetrathiafulvalene and 1,2-bis(methanesulfonamido)benzene, respectively), which was synthesized by using an electrochemical approach and studied by using crystal X-ray diffraction. This compound simultaneously exhibited metallic conductivity and SMM behaviour up to 11 K for the first time. The highest electrical conductivity was 400–650 S cm−1 at 6.5 K, which is the highest among those reported so far for conducting SMM materials. Furthermore, antiferromagnetic ordering occurred below 6.5 K, along with a decrease in conductivity, and the angle-independent negative magnetoresistance suggested an effective electron correlation between the conducting BO and Co(pdms)2 SMM layers (d–π interactions). The strong magnetic anisotropy and two-dimensional conducting plane play key roles in the low-temperature antiferromagnetic semiconducting state. BO4 is the first compound exhibiting antiferromagnetic ordering among SMMs mediated by π-electrons, demonstrating the synergetic effects between SMMs and molecular conductors.A metallic single-molecule magnet was synthesised demonstrating simultaneous metallic conduction and excellent SMM properties at the same temperature range for the first time, with potential applications in molecule-based quantum spintronics. 相似文献