Combining chip-ESI with APLI (cESILI) as a multimode source for analysis of complex mixtures with ultrahigh-resolution mass spectrometry

Combining chip-ESI with APLI (cESILI) as a multimode source for analysis of complex mixtures with ultrahigh-resolution mass spectrometry
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将芯片 ESI 与 APLI (cESILI) 相结合作为多模式源,用于通过超高分辨率质谱分析复杂混合物

DOI:
10.1007/s00216-008-2211-9
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发表时间:
2008
影响因子:
4.3
通讯作者:
O. Schmitz
O. Schmitz
中科院分区:
化学2区
文献类型:
--
作者:
P. Schmitt‐Kopplin;M. Englmann;R. Rosselló;R. Schiewek;K. Brockmann;T. Benter;O. Schmitz

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最近,我们建立了大气压激光电离(APLI)作为耦合飞行时间质谱检测器(TOF MS)与色谱系统(HPLC和GC)的方法,以允许非极性芳香族化合物的双光子电离。在这里,我们证明了APLI可以与芯片电喷雾电离(cESI)和傅里叶变换回旋共振质谱(FT-ICR MS)相结合,用于复杂样品的超高分辨率分析。当激光关闭时,分析物仅被ESI电离,而当激光打开时,非极性芳香族物质也被电离。结合FT-ICR MS的极高质量分辨率,极性和非极性分析物在正负两种模式下都可以同时进行定性分析,如原油样品所示。然而,观察到离子抑制(d10 -芘高达约70%),因此对目标进行定量分析需要进行色谱或电泳预分离的样品制备。此外,还首次将掺杂剂辅助APLI法与cESI (DA-cESILI)联合用于1-硝基冠烯的测定。
Recently we have established atmospheric-pressure laser ionisation (APLI) as a method for coupling time-of-flight mass spectrometric detectors (TOF MS) with chromatographic systems (HPLC and GC) to allow two-photon ionisation of non-polar aromatic compounds. Here we demonstrate that APLI can be combined with chip-electrospray ionisation (cESI) coupled to Fourier-transform-ion cyclotron resonance mass spectrometry (FT-ICR MS) for ultrahigh-resolution analysis of complex samples. With the laser turned off, the analytes are ionised only by ESI, whereas when the laser is switched on non-polar aromatic substances also are ionised. In combination with the extremely high mass resolution of an FT-ICR MS, simultaneous qualitative analysis of polar and non-polar analytes is possible in both positive and negative modes, as is exemplified with a crude oil sample. Nevertheless, ion suppression was observed (up to ca. 70% for D10-pyrene) and thus sample preparation with chromatographic or electrophoretic pre-separation is necessary for quantitative analysis of targets. In addition, for the first time, the dopant-assisted APLI method in combination with cESI (DA-cESILI) was used for determination of 1-nitrocoronene.