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首页> 外文期刊>Energy & fuels >Assessing Relative Electrospray Ionization, Atmospheric Pressure Photoionization, Atmospheric Pressure Chemical Ionization, and Atmospheric Pressure Photo- and Chemical Ionization Efficiencies in Mass Spectrometry Petroleomic Analysis via Pools and Pairs of Selected Polar Compound Standards
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Assessing Relative Electrospray Ionization, Atmospheric Pressure Photoionization, Atmospheric Pressure Chemical Ionization, and Atmospheric Pressure Photo- and Chemical Ionization Efficiencies in Mass Spectrometry Petroleomic Analysis via Pools and Pairs of Selected Polar Compound Standards

机译：通过池和成对选定的极性化合物标准对质谱质谱分析中的相对电喷雾电离，大气压光电离，大气压化学电离，大气压光化学电离效率进行评估

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摘要

A total of 15 standard compounds with structures similar to those normally found in crude oils were analyzed using an ultrahigh-resolution and high-accuracy Fourier transform ion cyclotron resonance (7.2 T LTQ FT Ultra, Thermo Fisher, Bremen, Germany) mass spectrometer. Four different ionization techniques were used: electrospray ionization (ESI), atmospheric pressure chemical ionization (APCI), atmospheric pressure photoionization (APPI), and a novel technique that couples APCI and APPI, herein termed atmospheric pressure photo- and chemical ionization (APPCI). Relationships between chemical structures and ionization efficiencies were established for these techniques, which operate via different ionization mechanisms. The unsaturation level and position of the double bond were shown to be key factors on ionization efficiency for all ionization techniques. Comparisons between molecules with similar backbones but with different heteroatoms were also made. For the whole mixture, APPI showed the highest sensitivity for the positive ion mode and ESI showed the highest sensitivity for the negative ion mode. APPCI was found to be the most comprehensive ionization technique, whereas as expected, ESI preferentially ionized the most polar compounds. APPCI produced, however, more than one ionic species per molecule, a disadvantage in terms of data complexity. Such "splitting" was observed for APPI and APCI. Ions with the same molecular formula formed from different molecules were also detected by APPCI, producing composite abundances that would mislead chemical and geochemical conclusions based on petroleomic approaches. We suggest that, although less comprehensive, ESI is overall the most suitable ionization technique for petroleomic studies.
机译：使用超高分辨率和高精度傅里叶变换离子回旋共振（7.2 T LTQ FT Ultra，Thermo Fisher，Bremen，德国）质谱仪对总共15种结构与原油中通常存在的结构相似的标准化合物进行了分析。使用了四种不同的电离技术：电喷雾电离（ESI），大气压化学电离（APCI），大气压光电离（APPI），以及将APCI和APPI耦合的新技术，在本文中称为大气压光电离和化学电离（APPCI） 。为这些技术建立了化学结构与电离效率之间的关系，这些技术通过不同的电离机理进行操作。对于所有电离技术，双键的不饱和度和位置均是影响电离效率的关键因素。还对具有相似主链但具有不同杂原子的分子进行了比较。对于整个混合物，APPI对正离子模式显示出最高的灵敏度，而ESI对负离子模式显示出最高的灵敏度。发现APPCI是最全面的电离技术，而正如预期的那样，ESI优先将最极性的化合物电离。但是，APPCI每个分子产生一种以上的离子物种，这在数据复杂性方面是不利的。对于APPI和APCI观察到了这种“分裂”。 APPCI还检测到了由不同分子形成的具有相同分子式的离子，从而产生了复合丰度，这些丰度会误导基于石油学方法的化学和地球化学结论。我们建议，尽管不那么全面，但ESI总体而言是最适合于石油学研究的电离技术。

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  • 来源
    《Energy & fuels》 |2016年第9期|7125-7133|共9页
  • 作者

    Pudenzi Marcos A.; Eberlin Marcos N.;

  • 作者单位

    State Univ Campinas UNICAMP, Inst Chem, ThoMSon Mass Spectrometry Lab, BR-13083970 Campinas, SP, Brazil;

    State Univ Campinas UNICAMP, Inst Chem, ThoMSon Mass Spectrometry Lab, BR-13083970 Campinas, SP, Brazil;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);
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