Structure of Sodiated Polyglycines

被引:21
作者
Balaj, O. Petru [1 ]
Semrouni, David [1 ]
Steinmetz, Vincent [2 ]
Nicol, Edith [1 ]
Clavaguera, Carine [1 ]
Ohanessian, Gilles [1 ]
机构
[1] Ecole Polytech, CNRS, Lab Mecanismes React, F-91128 Palaiseau, France
[2] Univ Paris 11, CNRS, Lab Chim Phys, F-91405 Orsay, France
关键词
ab initio calculations; IRMPD spectroscopy; peptides; polyglycines; sodium; PHOTON DISSOCIATION SPECTROSCOPY; PHASE H/D EXCHANGE; GAS-PHASE; INFRARED-SPECTROSCOPY; VIBRATIONAL SPECTROSCOPY; IRMPD SPECTROSCOPY; MASS-SPECTROMETRY; PEPTIDES; COMPLEXES; CONFORMATIONS;
D O I
10.1002/chem.201102812
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The intrinsic folding of peptides about a sodium ion has been investigated in detail by using infrared multiple photon dissociation (IRMPD) spectroscopy and a combination of theoretical methods. IRMPD spectroscopy was carried out on sodiated polyglycines Gn-Na+ (n=28), in both the fingerprint and N-H/O-H stretching regions. Interplay between experimental and computational approaches (classical and quantum) enables us to decipher most structural details. The most stable structures of the small peptides up to G6-Na+ maximize metalpeptide interactions with all peptidic C=O groups bound to sodium. In addition, direct interactions between peptide termini are possible for G6-Na+ and larger polyglycines. The increased flexibility of larger peptides leads to more complex folding and internal peptide structuration through gamma or beta turns. A structural transition is found to occur between G6-Na+ and G7-Na+, leading to a structure with sodium coordination that becomes tri-dimensional for the latter. This transition was confirmed by H/D exchange experiments on Gn-Na+ (n=38). The most favorable hydrogen-bonding pattern in G8-Na+ involves direct interactions between the peptide termini and opens the way to salt-bridge formation; however, there is only good agreement between experimental and computational data over the entire spectral range for the charge solvation isomer.
引用
收藏
页码:4583 / 4592
页数:10
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