van den Heuvel Robert H H, van Duijn Esther, Mazon Hortense, Synowsky Silvia A, Lorenzen Kristina, Versluis Cees, Brouns Stan J J, Langridge Dave, van der Oost John, Hoyes John, Heck Albert J R
Department of Biomolecular Mass Spectrometry, Bijvoet Center for Biomolecular Research and Utrecht Institute for Pharmaceutical Sciences, Utrecht University, Sorbonnelaan 16, 3584 CA Utrecht, The Netherlands.
Anal Chem. 2006 Nov 1;78(21):7473-83. doi: 10.1021/ac061039a.
We modified and optimized a first generation quadrupole time-of-flight (Q-TOF) 1 to perform tandem mass spectrometry on macromolecular protein complexes. The modified instrument allows isolation and subsequent dissociation of high-mass protein complexes through collisions with argon molecules. The modifications of the Q-TOF 1 include the introduction of (1) a flow-restricting sleeve around the first hexapole ion bridge, (2) a low-frequency ion-selecting quadrupole, (3) a high-pressure hexapole collision cell, (4) high-transmission grids in the multicomponent ion lenses, and (5) a low repetition rate pusher. Using these modifications, we demonstrate the experimental isolation of ions up to 12 800 mass-to-charge units and detection of product ions up to 38 150 Da, enabling the investigation of the gas-phase stability, protein complex topology, and quaternary structure of protein complexes. Some of the data reveal a so-far unprecedented new mechanism in gas-phase dissociation of protein oligomers whereby a tetramer complex dissociates into two dimers. These data add to the current debate whether gas-phase structures of protein complexes do retain some of the structural features of the corresponding species in solution. The presented low-cost modifications on a Q-TOF 1 instrument are of interest to everyone working in the fields of macromolecular mass spectrometry and more generic structural biology.
我们对第一代四极杆飞行时间质谱仪(Q-TOF)1进行了改进和优化,以对大分子蛋白质复合物进行串联质谱分析。改进后的仪器允许通过与氩分子碰撞来分离高质量蛋白质复合物并使其随后解离。Q-TOF 1的改进包括:(1)在第一个六极杆离子桥周围引入限流套管;(2)一个低频离子选择四极杆;(3)一个高压六极杆碰撞池;(4)在多组分离子透镜中采用高透射率栅极;(5)一个低重复率推斥极。通过这些改进,我们展示了对高达12800质荷比的离子进行实验分离以及对高达38150 Da的产物离子进行检测,从而能够研究蛋白质复合物的气相稳定性、蛋白质复合物拓扑结构和四级结构。一些数据揭示了蛋白质寡聚体气相解离中一种迄今为止前所未有的新机制,即四聚体复合物解离成两个二聚体。这些数据为当前关于蛋白质复合物的气相结构是否确实保留了溶液中相应物种的一些结构特征的争论增添了内容。在Q-TOF 1仪器上所展示的低成本改进对于在大分子质谱和更通用的结构生物学领域工作的每个人都具有吸引力。