Cooper Helen J, Hudgins Robert R, Håkansson Kristina, Marshall Alan G
Ion Cyclotron Resonance Program, National High Magnetic Field Laboratory, Florida State University, Tallahassee 32310, USA.
J Am Soc Mass Spectrom. 2002 Mar;13(3):241-9. doi: 10.1016/S1044-0305(01)00357-9.
We have used electrospray ionization (ESI) Fourier-transform ion cyclotron resonance (FTICR) mass spectrometry to characterize amino acid side chain losses observed during electron capture dissociation (ECD) of ten 7- to 14-mer peptides. Side-chain cleavages were observed for arginine, histidine, asparagine or glutamine, methionine, and lysine residues. All peptides containing an arginine, histidine, asparagine or glutamine showed the losses associated with that residue. Methionine side-chain loss was observed for doubly-protonated bombesin. Lysine side-chain loss was observed for triply-protonated dynorphin A fragment 1-13 but not for the doubly-protonated ion. The proximity of arginine to a methoxy C-terminal group significantly enhances the extent of side-chain fragmentation. Fragment ions associated with side-chain losses were comparable in abundance to those resulting from backbone cleavage in all cases. In the ECD spectrum of one peptide, the major product was due to fragmentation within an arginine side chain. Our results suggest that cleavages within side chains should be taken into account in analysis of ECD mass spectral data. Losses from arginine, histidine, and asparigine/glutamine can be used to ascertain their presence, as in the analysis of unknown peptides, particularly those with non-linear structures.
我们利用电喷雾电离(ESI)傅里叶变换离子回旋共振(FTICR)质谱对10种7至14肽段在电子捕获解离(ECD)过程中观察到的氨基酸侧链损失进行了表征。观察到精氨酸、组氨酸、天冬酰胺或谷氨酰胺、甲硫氨酸和赖氨酸残基的侧链裂解。所有含有精氨酸、组氨酸、天冬酰胺或谷氨酰胺的肽段都显示出与该残基相关的损失。在双质子化的铃蟾肽中观察到甲硫氨酸侧链损失。在三质子化的强啡肽A片段1 - 13中观察到赖氨酸侧链损失,但在双质子化离子中未观察到。精氨酸与甲氧基C末端基团的接近程度显著增强了侧链断裂的程度。在所有情况下,与侧链损失相关的碎片离子丰度与主链裂解产生的碎片离子丰度相当。在一种肽段的ECD谱中,主要产物是由精氨酸侧链内的断裂产生的。我们的结果表明,在分析ECD质谱数据时应考虑侧链内的裂解。精氨酸、组氨酸以及天冬酰胺/谷氨酰胺的损失可用于确定它们的存在,如在分析未知肽段时,特别是那些具有非线性结构的肽段。