National High Magnetic Field Laboratory, Florida State University, 1800 East Paul Dirac Drive, Tallahassee, Florida 32310-4005, USA.
Anal Chem. 2011 Sep 1;83(17):6907-10. doi: 10.1021/ac201546d. Epub 2011 Aug 12.
Complex natural organic mixtures such as petroleum require ultrahigh mass spectral resolution to separate and identify thousands of elemental compositions. Here, we incorporate a custom-built, voltage-compensated ICR cell for Fourier transform ion cyclotron resonance mass spectrometry (FTICR MS), based on a prior design by Tolmachev to produce optimal mass resolution. The compensated ICR cell installed in a custom-built 9.4 T FTICR mass spectrometer consists of seven cylindrical segments with axial proportions designed to generate a dc trapping potential that approaches an ideal three-dimensional axial quadrupolar potential. However, the empirically optimized compensation voltages do not correspond to the most quadrupolar trapping field. The compensation electrodes minimize variation in the reduced cyclotron frequency by balancing imperfections in the magnetic and electric field. The optimized voltages applied to compensation electrodes preserve ion cloud coherence for longer transient duration by approximately a factor of 2, enabling separation and identification of isobaric species (compounds with the same nominal mass but different exact mass) common in petroleum, such as C(3) vs SH(4) (separated by 3.4 mDa) and SH(3)(13)C vs (12)C(4) (separated by 1.1 mDa). The improved performance of the ICR cell provides more symmetric peak shape and better mass measurement accuracy. A positive ion atmospheric pressure photoionization (APPI) petroleum spectrum yields more than 26,000 assigned peaks, Fourier-limited resolving power of 800,000 at m/z 500 (6.6 s transient duration), and 124 part per billion root mean square (rms) error. The tunability of the compensation electrodes is critical for optimal performance.
复杂的天然有机混合物,如石油,需要超高的质谱分辨率来分离和识别数千种元素组成。在这里,我们结合了一种基于 Tolmachev 先前设计的定制、电压补偿 ICR 细胞,用于傅里叶变换离子回旋共振质谱 (FTICR MS),以产生最佳的质量分辨率。安装在定制 9.4 T FTICR 质谱仪中的补偿 ICR 细胞由七个圆柱形部分组成,轴向比例设计旨在产生接近理想三维轴向四极电位的直流捕获电位。然而,经验优化的补偿电压与最四极捕获场不对应。补偿电极通过平衡磁场和电场的不完美来最小化回旋频率的降低。优化施加到补偿电极上的电压通过将离子云相干性延长约 2 倍来保持更长的瞬态持续时间,从而能够分离和识别石油中常见的等压物种(具有相同名义质量但不同精确质量的化合物),例如 C(3)与 SH(4)(分离度为 3.4 mDa)和 SH(3)(13)C 与 (12)C(4)(分离度为 1.1 mDa)。ICR 细胞的改进性能提供了更对称的峰形和更好的质量测量精度。正离子大气压光解(APPI)石油谱产生超过 26,000 个分配的峰,在 m/z 500 处的傅里叶限制分辨率为 800,000(6.6 s 瞬态持续时间),以及 124 个 ppm rms 误差。补偿电极的可调性对于最佳性能至关重要。