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991.
Alfonso I Bolte M Bru M Burguete MI Luis SV 《Chemistry (Weinheim an der Bergstrasse, Germany)》2008,14(29):8879-8891
The efficient synthesis of large-ring pseudopeptidic macrocycles through a multicomponent [2+2] reductive amination reaction is described. The reaction was entirely governed by the structural information contained in the corresponding open-chain pseudopeptidic bis(amidoamine) precursors, which have a rigid (R,R)-cyclohexane-1,2-diamine moiety. A remarkable match/mismatch relationship between the configurations of the chiral centers of the cyclic diamine and those of the peptidic frame was observed. The macrocyclic tetraimine intermediates have been studied in detail by NMR spectroscopy, circular dichroism (CD), and molecular modeling, and the results support the appropriate preorganization induced by the match combination of the chiral centers. We have also synthesized the corresponding open-chain bis(imine) model compounds. The structural studies (NMR spectroscopy, CD, modeling) of these systems showed an intrinsically lower reactivity of the mismatch combination, even when the product of the reaction was acyclic. In addition, a synergistic effect between the two chiral substructures for the correct folding of the molecules was observed. Finally, X-ray analysis of the HCl salt of one of the macrocycles showed an interesting pattern; the macrocyclic rings stack in columnar aggregates leaving large interstitial channels filled with water-solvated chloride anions. 相似文献
992.
Bojdys MJ Müller JO Antonietti M Thomas A 《Chemistry (Weinheim an der Bergstrasse, Germany)》2008,14(27):8177-8182
Herein we report the synthesis of a crystalline graphitic carbon nitride, or g-C(3)N(4), obtained from the temperature-induced condensation of dicyandiamide (NH(2)C(=NH)NHCN) by using a salt melt of lithium chloride and potassium chloride as the solvent. The proposed crystal structure of this g-C(3)N(4) species is based on sheets of hexagonally arranged s-heptazine (C(6)N(7)) units that are held together by covalent bonds between C and N atoms which are stacked in a graphitic, staggered fashion, as corroborated by powder X-ray diffractometry and high-resolution transmission electron microscopy. 相似文献
993.
The crystal and molecular structures of trans-2,4,4-trimethyl-4-silathiane 1-oxide 1 and 4,4-dimethyl-4-silathiane 1,1-dioxide 2 were determined by single crystal X-ray diffraction. Both compounds have the chair conformation with the 2-Me and the S=O
group in compound 1 occupying the equatorial positions. The DFT (B3LYP/6-311G(d,p)) and MP2 (MP2/6-311G(d,p)) theoretical calculations nicely
reproduce the X-ray experimental geometry. The obtained results are discussed in connection with the electronic and structural
properties of the compounds.
相似文献
Bagrat A. ShainyanEmail: |
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