Yang Dan, Zhang Yu-Hui, Li Bing, Zhang Dan-Wei, Chan Jenny Chun-Yu, Zhu Nian-Yong, Luo Shi-Wei, Wu Yun-Dong
Department of Chemistry, The University of Hong Kong, Pokfulam Road, Hong Kong, China.
J Am Chem Soc. 2004 Jun 9;126(22):6956-66. doi: 10.1021/ja049976s.
We have investigated, using NMR, IR, and CD spectroscopy and X-ray crystallography, the conformational properties of peptides 1-10 of beta(3)-aminoxy acids (NH(2)OCHRCH(2)COOH) having different side chains on the beta carbon atom (e.g., R = Me, Et, COOBn, CH(2)CH(2)CH=CH(2), i-Bu, i-Pr). The beta N-O turns and beta N-O helices that involve a nine-membered-ring intramolecular hydrogen bond between NH(i)(+2) and CO(i), which have been found previously in peptides of beta(2,2)-aminoxy acids (NH(2)OCH(2)CMe(2)COOH), are also present in those beta(3)-aminoxy peptides. X-ray crystal structures and NMR spectral analysis reveal that, in the beta N-O turns and beta N-O helices induced by beta(3)-aminoxy acids, the N-O bond could be either anti or gauche to the C(alpha)-C(beta) bond depending on the size of the side chain; in contrast, only the anti conformation was found in beta(2,2)-aminoxy peptides. Both diamide 1 and triamide 9 exist in different conformations in solution and in the solid state: parallel sheet structures in the solid state and predominantly beta N-O turn and beta N-O helix conformations in nonpolar solvents. Theoretical studies on a series of model diamides rationalize very well the experimentally observed conformational features of these beta(3)-aminoxy peptides.
我们使用核磁共振(NMR)、红外(IR)和圆二色(CD)光谱以及X射线晶体学,研究了β(3)-氨基氧基酸(NH(2)OCHRCH(2)COOH)的肽1-10在β碳原子上具有不同侧链(例如,R = 甲基、乙基、苄氧羰基、CH(2)CH(2)CH=CH(2)、异丁基、异丙基)时的构象性质。先前在β(2,2)-氨基氧基酸(NH(2)OCH(2)CMe(2)COOH)的肽中发现的涉及NH(i)(+2)和CO(i)之间九元环分子内氢键的β N-O转角和β N-O螺旋,在这些β(3)-氨基氧基肽中也存在。X射线晶体结构和NMR光谱分析表明,在由β(3)-氨基氧基酸诱导的β N-O转角和β N-O螺旋中,N-O键相对于C(α)-C(β)键可以是反式或gauche式,这取决于侧链的大小;相比之下,在β(2,2)-氨基氧基肽中仅发现了反式构象。二酰胺1和三酰胺9在溶液和固态中均以不同构象存在:固态中为平行片层结构,在非极性溶剂中主要为β N-O转角和β N-O螺旋构象。对一系列模型二酰胺的理论研究很好地解释了这些β(3)-氨基氧基肽的实验观察到的构象特征。
J Am Chem Soc. 2004-6-9
Chem Commun (Camb). 2006-8-28
J Am Chem Soc. 2004-12-15
J Am Chem Soc. 2008-1-16