Tandem Mass Spectrometry and Ion Mobility Reveals Structural Insight into Eicosanoid Product Ion Formation.
Tandem Mass Spectrometry and Ion Mobility Reveals Structural Insight into Eicosanoid Product Ion Formation.
复制标题
串联质谱法和离子迁移率揭示了对类花生酸产物离子形成的结构洞察力。
DOI：
10.1007/s13361-018-1927-9
复制
发表时间：
2018-06
影响因子：
3.2
通讯作者：
Murphy RC
中科院分区：
文献类型：
--
作者：
Di Giovanni JP;Barkley RM;Jones DNM;Hankin JA;Murphy RC
产品离子的离子迁移率测量已被用于使用行波离子迁移率质谱（TWIMS）表征各种复杂脂质[M-H]−离子的碰撞截面（CCS）。TWIMS分析后，碰撞激活的单和二羟基花生四烯酸代谢产物的各种产物离子被发现是更复杂的分析比完整的分子离子，并提供了一些深入了解参与产物离子形成的分子机制。观察到的分子离子[M-H]−和某些子离子的CCS与折叠离子结构一致，后者是通过提出的子离子形成机制预测的。出乎意料的是，[M-H-H2O - CO2]−和[M-H-H2O]−的产物离子显示出复杂的离子迁移率曲线，表明离子形成的多种机制。使用氮气和氦气作为离子迁移池中的漂移气体，更详细地研究了来自LTB 4的[M-H-H2O]−离子。来自LTB 4的[M-H-H2O]−产物离子的一个群体与共价环结构的形成一致，而显示出更高CCS的离子与更开链的结构一致。使用分子动力学和理论CCS计算，能量最小化结构的那些开链结构的子离子被发现有一个较高的CCS比折叠分子离子结构。产物离子迁移率的测量可以是通过LC-MS/MS技术测量的类二十烷酸的额外且独特的特征。
Ion mobility measurements of product ions has been used characterize the collisional cross-section (CCS) of various complex lipid [M-H]− ions using traveling wave ion mobility mass spectrometry (TWIMS). TWIMS analysis of various product ion derived after collisional activation of mono-and di-hydroxy arachidonate metabolites was found to be more complex than the analysis of intact molecular ions and provided some insight into molecular mechanisms involved in product ion formation. The CCS observed for the molecular ion [M-H]− and certain product ions were consistent with a folded ion structure, the latter predicted by the proposed mechanisms of product ion formation. Unexpectedly, product ions from [M-H-H2O - CO2]− and [M-H-H2O]− displayed complex ion mobility profiles suggesting multiple mechanisms of ion formation. The [M-H-H2O]− ion from LTB4 was studied in more detail using both nitrogen and helium as the drift gas in the ion mobility cell. One population of [M-H-H2O]− product ions from LTB4 was consistent with formation of covalent ring structures, while the ions displaying a higher CCS were consistent with a more open-chain structure. Using molecular dynamics and theoretical CCS calculations, energy minimized structures of those product ions with the open-chain structures were found to have a higher CCS than a folded molecular ion structure. The measurement of product ion mobility can be an additional and unique signature of eicosanoids measured by LC-MS/MS techniques.
登录
查看更多内容
影响因子：
2.3
作者：
Lalli, Priscila M.;Corilo, Yuri E.;Campuzano, Iain D. G.
通讯作者：
Campuzano, Iain D. G.
DOI：
10.1016/j.bbalip.2014.10.002
发表时间：
2015-04
期刊：
Biochimica et biophysica acta
影响因子：
--
作者：
Kuhn H;Banthiya S;van Leyen K
通讯作者：
van Leyen K
影响因子：
7.4
作者：
Paglia, Giuseppe;Angel, Peggi;Williams, Jonathan P.;Richardson, Keith;Olivos, Hernando J.;Thompson, J. Will;Menikarachchi, Lochana;Lai, Steven;Walsh, Callee;Moseley, Arthur;Plumb, Robert S.;Grant, David F.;Palsson, Bernhard O.;Langridge, James;Geromanos, Scott;Astarite, Giuseppe
通讯作者：
Astarite, Giuseppe
影响因子：
7.4
作者：
Kim, Hugh I.;Kim, Hyungjun;Pang, Eric S.;Ryu, Ernest K.;Beegle, Luther W.;Loo, Joseph A.;Goddard, William A.;Kanik, Isik
通讯作者：
Kanik, Isik
影响因子：
1.8
作者：
VON HELDEN, G;WYTTENBACH, T;BOWERS, MT
通讯作者：
BOWERS, MT