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431.
Keisuke Fujimoto Tomoki Yoneda Prof. Dr. Hideki Yorimitsu Prof. Dr. Atsuhiro Osuka 《Angewandte Chemie (International ed. in English)》2014,53(4):1127-1130
2,18‐Bis(diphenylphosphino)porphyrins undergo peripheral cyclometalation with group 10 transition‐metal salts to afford the corresponding porphyrin‐based PCP pincer complexes. The porphyrinic plane and the PCP‐pincer unit are apparently coplanar, with small strain. The catalytic activities of the porphyrin‐based pincer complexes at the periphery were investigated in the allylation of benzaldehyde with allylstannane and in the 1,4‐reduction of chalcone to discover the electronic interplay between the inner metal and the outer metal in catalysis. 相似文献
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434.
Fengkun Chen Dr. Takayuki Tanaka Yongseok Hong Woojae Kim Prof. Dr. Dongho Kim Prof. Dr. Atsuhiro Osuka 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(30):10597-10606
ortho‐Phenylene‐bridged cyclic trimeric oligopyrrole C3 and hexameric oligopyrrole C6 were synthesized by Suzuki–Miyaura coupling reactions. The twisted structures of C3 and C6 were unambiguously revealed by X‐ray diffraction analysis. The optical properties of these cyclic oligopyrroles were compared with linear oligopyrrole L3 and cyclic tetramer C4 . The cyclic oligopyrroles exhibited large Stokes shifts and blue fluorescence with high quantum yields in solution and in the solid state. In addition, selective N‐methylation and N‐tolylation of C3 were used to tune the optical and electrochemical properties by changing the molecular twists and conformational flexibilities. Throughout these studies, the structure–property relationship of these cyclic strained oligopyrroles has been illustrated as an interesting molecular motif for novel cyclic π‐conjugated systems. 相似文献
435.
Bismetal Complexes of 5,20‐Bis(5‐formyl‐2‐pyrrolyl)‐[26]hexaphyrin(1.1.1.1.1.1) Exhibiting Strong Near‐Infrared Region Absorptions 下载免费PDF全文
Hirotaka Mori Prof. Dr. Atsuhiro Osuka 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(19):7007-7011
[26]Hexaphyrin(1.1.1.1.1.1) bearing two 5‐formyl‐2‐pyrrolyl groups at the 5‐ and 20‐positions was prepared by cross‐condensation of 5,10‐bis(pentafluorophenyl)‐substituted tripyrrane with 2,5‐diformylpyrrole as an effective binuclear metal‐coordinating ligand, owing to the two hemiporphyrin‐like NNNN pockets. In fact, metalation of this hexaphyrin with ZnII, CuII, and PdII salts proceed smoothly at room temperature to give the corresponding bismetal complexes that displayed remarkably redshifted absorption spectra reaching deep into near infrared region. These redshifted absorption bands are ascribed, through electrochemical investigations and DFT calculations, to two structural motifs: the N‐metalopyrrole substructure that elevates the HOMO level due to the electron‐donating property and the two coordinated metal ions that serve as Lewis acids to lower the LUMO level. 相似文献
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Inside Cover: A Description of Vibrational Modes in Hexaphyrins: Understanding the Aromaticity Reversal in the Lowest Triplet State (Angew. Chem. Int. Ed. 39/2016) 下载免费PDF全文
438.
Stable [48]‐, [50]‐, and [52]Dodecaphyrins(1.1.0.1.1.0.1.1.0.1.1.0): The Largest Hückel Aromatic Molecules 下载免费PDF全文
Takanori Soya Woojae Kim Prof. Dr. Dongho Kim Prof. Dr. Atsuhiro Osuka 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(23):8341-8346
[52]Dodecaphyrin(1.1.0.1.1.0.1.1.0.1.1.0) was quantitatively oxidized with 2,3‐dichloro‐5,6‐dicyano‐1,4‐benzoquinone (DDQ) to the corresponding [50]dodecaphyrin. Further oxidation of [50]dodecaphyrin with MnO2 quantitatively afforded [48]dodecaphyrin. Of the three, [50]dodecaphyrin showed Hückel aromatic character as the largest aromatic molecule reported to date. Protonation of [50]dodecaphyrin with methanesulfonic acid (MSA) led to the formation of a planar tetraprotonated species that displayed a sharp and intense Soret‐like band at 906 nm with ε=6.5×105 M ?1 cm?1 and Q‐band‐like bands at 1346 and 1600 nm. 相似文献
439.
Keisuke Fujimoto Prof. Dr. Hideki Yorimitsu Prof. Dr. Atsuhiro Osuka 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(32):11311-11314
As the most nucleophilic porphyrins, meso‐ or β‐lithiated porphyrins were generated by iodine–lithium exchange reactions of the corresponding iodoporphyrins with n‐butyllithium at ?98 °C. Porphyrinyllithiums thus prepared were used for synthesis of dimesitylporphyrinylboranes through reactions with fluorodimesitylborane. The boryl groups proved to serve as an electron‐accepting unit to alter the photophysical and electrochemical properties. In addition, 5‐diarylamino‐15‐dimesitylboryl‐substituted donor–accepter porphyrins showed increased intramolecular charge‐transfer character in the S1 state. Furthermore, the reaction of β‐lithiated porphyrin with dichloromesitylborane provided a boron‐bridged porphyrin dimer, which exhibited a conjugative interaction between two porphyrin units through the vacant p‐orbital on the boron center. 相似文献
440.
Inside Back Cover: Stable [48]‐, [50]‐, and [52]Dodecaphyrins(1.1.0.1.1.0.1.1.0.1.1.0): The Largest Hückel Aromatic Molecules (Chem. Eur. J. 23/2015) 下载免费PDF全文