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1.
Synthesis and Self‐Assembly of Cyclic 2,7‐Anthrylene Ethynylene 1,3‐Phenylene Ethynylene Trimer with a Planar Conformation 下载免费PDF全文
Yuta Takaki Ryota Ozawa Dr. Takashi Kajitani Prof. Takanori Fukushima Prof. Masaaki Mitsui Prof. Kenji Kobayashi 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(47):16760-16764
Cyclic arylene ethynylene hexamer 1 , composed of alternating 2,7‐anthrylene ethynylene units and meta‐phenylene ethynylene units, was synthesized. It shows C3 symmetry and possesses a flat and rigid conformation with a large equilateral triangle‐like cavity. Macrocycle 1 self‐associates through π–π stacking interactions between the anthracene‐containing macrocyclic aromatic cores with indefinite‐association constant KE=6980 m ?1 in CDCl3 at 303 K. Macrocycle 1 also self‐assembles into π‐stacked nanofibers in the drop‐cast film. 相似文献
2.
Total Synthesis of the 7,10‐Epimer of the Proposed Structure of Amphidinolide N,Part II: Synthesis of C17–C29 Subunit and Completion of the Synthesis 下载免费PDF全文
Dr. Koji Ochiai Dr. Sankar Kuppusamy Yusuke Yasui Kenji Harada Dr. Nishant R. Gupta Dr. Yohei Takahashi Prof. Dr. Takaaki Kubota Prof. Dr. Jun'ichi Kobayashi Prof. Dr. Yujiro Hayashi 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(10):3287-3291
The total synthesis of 7,10‐epimer of the proposed structure of amphidinolide N was accomplished. The requisite chiral C17–C29 subunit was assembled stereoselectively via Keck allylation, Shi epoxidation, diastereoselective 1,3‐reduction, and a later oxidative synthesis of the THF framework. The C1–C13 and C17–C29 subunits were successfully coupled using a Enders RAMP “linchpin” as the C14–C16 three carbon unit, thereby controlling the chirality at C14 and C16. The labile allyl epoxy moiety was successfully constructed by Grieco–Nishizawa olefination at a final stage of the synthesis. 相似文献
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Ryuto Yasui Dr. Daiki Shimizu Prof. Kenji Matsuda 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(27):e202104242
The single-molecular conductance between two π-conjugated wires with and without a radical substituent has been compared. Specifically, methyl- and iminonitroxide-substituted 4-(biphenyl-4-yl)pyridine wires bound onto a porphyrin template were subjected to scanning tunneling microscopy (STM) apparent-height measurement at the interface between highly oriented pyrolytic graphite (HOPG) and octan-1-oic acid. Statistical analysis of the STM images revealed that the radical-substituted wire has 3.2±1.7-fold higher conductance than the methyl-substituted reference. Although density functional theory (DFT) calculation suggests that only 17 % of the SOMO is distributed on the wire moiety, the effect was significant. This study presents the potential of radical substituents to achieve high conductivity in molecular wires. 相似文献
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Makoto Yonenaga Yusuke Kaiwa Dr. Kouki Oka Prof. Dr. Kenichi Oyaizu Prof. Dr. Kenji Miyatake 《Angewandte Chemie (International ed. in English)》2023,62(30):e202304366
A proof-of-concept study was conducted on an all-solid-state rechargeable air battery (SSAB) using redox-active 2,5-dihydroxy-1,4-benzoquinone (DHBQ) and its polymer (PDBM) and a proton-conductive polymer (Nafion). DHBQ functioned well in the redox reaction with the solid Nafion ionomer at 0.47 and 0.57 V vs. RHE, similar to that in acid aqueous solution. The resulting air battery exhibited an open circuit voltage of 0.80 V and a discharge capacity of 29.7 mAh gDHBQ−1 at a constant current density (1 mA cm−2). With PDBM, the discharge capacity was much higher, 176.1 mAh gPDBM−1, because of the improved utilization of the redox-active moieties. In the rate characteristics of the SSAB-PDBM, the coulombic efficiency was 84 % at 4 C, which decreased to 66 % at 101 C. In a charge/discharge cycle test, the capacity remaining after 30 cycles was 44 %, which was able to be significantly improved, to 78 %, by tuning the Nafion composition in the negative electrode. 相似文献
9.
Dr. Zhouen Zhang Dr. Takashi Niwa Dr. Kenji Watanabe Prof. Dr. Takamitsu Hosoya 《Angewandte Chemie (International ed. in English)》2023,62(22):e202302956
Aryl fluorides are expected to be useful as radiolabeling precursors due to their chemical stability and ready availability. However, direct radiolabeling via carbon-fluorine (C−F) bond cleavage is a challenging issue due to its significant inertness. Herein, we report a two-phase radiosynthetic method for the ipso-11C-cyanation of aryl fluorides to obtain [11C]aryl nitriles via nickel-mediated C−F bond activation. We also established a practical protocol that avoids the use of a glovebox, except for the initial preparation of a nickel/phosphine mixture, rendering the method applicable for general PET centers. This method enabled the efficient synthesis of diverse [11C]aryl nitriles from the corresponding aryl fluorides, including pharmaceutical drugs. Stoichiometric reactions and theoretical studies indicated a significant promotion effect of lithium chloride on the oxidative addition, affording an aryl(chloro)nickel(II) complex, which serves as a precursor for rapid 11C-cyanation. 相似文献
10.
Dr. Akihiro Takada Hiroaki Fujiwara Dr. Kenji Sugimoto Dr. Hirofumi Ueda Prof. Dr. Hidetoshi Tokuyama 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(46):16400-16403
The total synthesis of (?)‐isoschizogamine was accomplished, featuring the construction of the quaternary carbon center by the modified Johnson–Claisen rearrangement in basic media and the facile assembly of the key tetracyclic quinolone intermediate through a cascade cyclization. The characteristic cyclic aminal was constructed by late‐stage C?H functionalization at the position adjacent to the lactam nitrogen using a combination of CrO3 and nBu4NIO4 and subsequent Bi(OTf)3‐mediated cyclization. 相似文献