Gas phase conformations of biological molecules: The hydrogen/deuterium exchange mechanism

被引:143
作者
Wyttenbach, T [1 ]
Bowers, MT [1 ]
机构
[1] Univ Calif Santa Barbara, Dept Chem, Santa Barbara, CA 93106 USA
基金
美国国家科学基金会;
关键词
D O I
10.1016/S1044-0305(98)00121-4
中图分类号
Q5 [生物化学];
学科分类号
071010 ; 081704 ;
摘要
A model was developed to describe the deuterium uptake of gas phase polypeptide ions via H/D exchange with D2O. Ab initio calculations established, for energetic reasons, that the exchange must take place via a "relay" mechanism involving both a charged site and a nearby basic site. Molecular dynamics simulations indicated that the D2O molecule did not penetrate the core of the example peptide, protonated bradykinin (Bk+H)(+), and hence the relay mechanism must occur on the peptide surface. Two factors were deemed to be important: (1) The surface accessibility of the charged sites and the basic sites and (2) the distances between them. An algorithm was developed that accounted for these features using the absolute exchange rate as a free parameter. Excellent agreement was obtained with experiment when equal weight was given to an ensemble of low energy conformations of (Bk+H)(+), assumed to have a salt bridge primary structure. Single conformations, or other protonated forms, did not allow,good a,agreement with experiment for any value of the absolute exchange rate constant. (J Am Soc Mass Spectrom 1999, 10, 9-14) (C) 1999 American Society for Mass Spectrometry.
引用
收藏
页码:9 / 14
页数:6
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