Hyphenation of Thermal Analysis to Ultrahigh-Resolution Mass Spectrometry (Fourier Transform Ion Cyclotron Resonance Mass Spectrometry) Using Atmospheric Pressure Chemical Ionization For Studying Composition and Thermal Degradation of Complex Materials.

Hyphenation of Thermal Analysis to Ultrahigh-Resolution Mass Spectrometry (Fourier Transform Ion Cyclotron Resonance Mass Spectrometry) Using Atmospheric Pressure Chemical Ionization For Studying Composition and Thermal Degradation of Complex Materials.
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热分析与超高分辨率质谱(傅里叶变换离子回旋共振质谱)的联用,利用大气压化学电离研究复杂材料的成分和热降解

DOI:
10.1021/acs.analchem.5b00785
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发表时间:
2015
影响因子:
7.4
通讯作者:
Zimmermann R
Zimmermann R
中科院分区:
化学1区
文献类型:
--
作者:
Rüger CP;Miersch T;Schwemer T;Sklorz M;Zimmermann R

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在这项研究中,热天平的联用超高分辨率傅里叶变换离子回旋共振质谱仪(UHR FTICR MS)。大气压化学电离(APCI)用于有效电离。逸出气体分析(EGA)使用高分辨率质谱法,可对复杂材料或混合物(如生物质或原油)中的热诱导过程进行时间分辨分子表征。该装置最关键的部分是热天平和APCI源之间的连接。通过在连字符的热天平侧施加轻微的超压,迫使逸出气体进入MS的大气压电离界面。使用FTICR精确质量数据,通过计算有机物质的元素组成获得详细的化学信息,从而能够对演化的物质进行时间和温度分辨的高选择性检测。通过APCI电离获得额外的选择性,其对极性化合物特别敏感。这种选择性一方面错过了石油样品的大宗组分,如烷烃,并没有提供一个全面的看法,但另一方面,特别侧重于从生物质样品的典型演变组分。作为原理的证明,研究了不同化石燃料的热行为:重燃料油、轻燃料油和原油,以及不同木质纤维素生物质,即山毛榉、桦树、云杉、白蜡、橡树和松树,以及市售软木和桦树皮颗粒。结果清楚地显示了通过其分子模式和化合物类别区分某些木材类型的能力。此外,典型文献已知的热解生物质标记物通过它们的元素组成来确认,例如松柏醛(C10H10O3)、芥子醛(C11H12O4)、retene(C18H18)和松香酸(C20H30O2)。
In this study, the hyphenation of a thermobalance to an ultrahigh-resolution Fourier transform ion cyclotron resonance mass spectrometer (UHR FTICR MS) is presented. Atmospheric pressure chemical ionization (APCI) is used for efficient ionization. The evolved gas analysis (EGA), using high-resolution mass spectrometry allows the time-resolved molecular characterization of thermally induced processes in complex materials or mixtures, such as biomass or crude oil. The most crucial part of the setup is the hyphenation between the thermobalance and the APCI source. Evolved gases are forced to enter the atmospheric pressure ionization interface of the MS by applying a slight overpressure at the thermobalance side of the hyphenation. Using the FTICR exact mass data, detailed chemical information is gained by calculation of elemental compositions from the organic species, enabling a time and temperature resolved, highly selective detection of the evolved species. An additional selectivity is gained by the APCI ionization, which is particularly sensitive toward polar compounds. This selectivity on the one hand misses bulk components of petroleum samples such as alkanes and does not deliver a comprehensive view but on the other hand focuses particularly on typical evolved components from biomass samples. As proof of principle, the thermal behavior of different fossil fuels: heavy fuel oil, light fuel oil, and a crude oil, and different lignocellulosic biomass, namely, beech, birch, spruce, ash, oak, and pine as well as commercial available softwood and birch-bark pellets were investigated. The results clearly show the capability to distinguish between certain wood types through their molecular patterns and compound classes. Additionally, typical literature known pyrolysis biomass marker were confirmed by their elemental composition, such as coniferyl aldehyde (C10H10O3), sinapyl aldehyde (C11H12O4), retene (C18H18), and abietic acid (C20H30O2).
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在外部离子源傅里叶变换离子回旋共振质谱仪上通过源内 PyMS 直接温度分辨阻燃聚合物的 HRMS
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