Laboratoire des Biomolécules, Université P et M Curie, UMR 7203 UPMC-CNRS-ENS, Paris, France.
J Am Soc Mass Spectrom. 2012 Nov;23(11):1981-90. doi: 10.1007/s13361-012-0467-y. Epub 2012 Sep 7.
This study aims at improving the MALDI-TOF detection of a phosphorylated peptide containing a cysteine residue by β-elimination of H(3)PO(4) hardly enriched by classical methods. The experimental conditions were optimized on this phosphopeptide (biot-pAdd) and its nonphosphorylated counterpart (biot-Add). The major side-reactions were H(2)S elimination on the cysteine residues and H(2)O elimination on the non phosphorylated serine residue of biot-Add. The former dilutes the MALDI-TOF signal for the desired species. The latter gives a product similar to what is obtained by H(3)PO(4) elimination and should prompt to caution when working with a mixture between phosphorylated and non phosphorylated peptides. Modifications on the solvent, the reaction temperature and time, the nature, and concentration of the base were made. Major improvement of the selectivity of the reaction was observed in 30 % ACN, at room temperature for 4 h. However, these optimizations are specific to these sequences and should be performed anew for different peptides. The selectivity of the reaction towards H(3)PO(4) elimination is improved, but the persistence of side-reactions renders a previous sample fractionation necessary. In these optimized conditions, the ionization enhancement is 3-fold and the detection limits for biot-pAdd are similar to biot-Add (100 fmol).
本研究旨在通过β-消除 H3PO4来改善 MALDI-TOF 对含有半胱氨酸残基的磷酸化肽的检测,而 H3PO4很难用经典方法富集。在该磷酸肽(biot-pAdd)及其非磷酸化对应物(biot-Add)上优化了实验条件。主要的副反应是半胱氨酸残基上的 H2S 消除和非磷酸化丝氨酸残基上的 H2O 消除。前者稀释了所需物种的 MALDI-TOF 信号。后者产生的产物与通过 H3PO4消除获得的产物相似,并且在用磷酸化和非磷酸化肽混合物工作时应引起注意。对溶剂、反应温度和时间、碱的性质和浓度进行了修改。在 30%ACN 中,在室温下反应 4 小时,观察到反应选择性的显著提高。然而,这些优化是针对这些序列的,对于不同的肽应重新进行。反应对 H3PO4消除的选择性得到了改善,但副反应的持续存在使得需要对先前的样品进行分级。在这些优化条件下,biot-pAdd 的离子化增强了 3 倍,检测限与 biot-Add 相似(100 fmol)。