Pushing the analytical limits: new insights into complex mixtures using mass spectra segments of constant ultrahigh resolving power

Lozano, Diana Catalina Palacio; Gavard, Remy; Arenas-Diaz, Juan P.; Thomas, Mary J.; Stranz, David D.; Mejía-Ospino, Enrique; Guzmán, Alexander; Spencer, Simon E. F.; Rossell, David; Barrow, Mark P.

doi:10.1039/c9sc02903f

Cited by 85 publications

(68 citation statements)

References 78 publications

(67 reference statements)

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“…Research that focusses on broad geochemical trends can often be achieved with lower resolving power, e.g., when determining presence and absence of specific chemical compositions or easily resolved ions, and when determining the abundance changes of the most prominent ions is sufficient (Hawkes et al 2016;Simon et al 2018). However, some research applications may benefit from maximizing resolving power and extending dynamic range to enable a more thorough assignment of compound classes (Pohlabeln and Dittmar 2015;Smith et al 2018;Palacio Lozano et al 2019).…”

Section: Discussionmentioning

confidence: 99%

“…Formula assignment continues to be debated in the ESI-HRMS community, and here the conservative approach was taken to more severely constrain assigned formulas as compared to many other studies, bearing in mind that the samples chosen are not among the most complex examples, such as petroleum or mixtures containing fresh metabolites (Gonsior et al 2019;Palacio Lozano et al 2019). Rates of formula assignment heavily depend on the resolving power of the chosen instrument.…”

Section: Theoretical Formula Listmentioning

confidence: 99%

“…S8). It is unlikely that any instrument at any particular tune setting can capture the full representative distribution of ionizable compounds in these complex DOM mixtures in a single broadband analysis (Southam et al 2007;Hawkes et al 2019;Palacio Lozano et al 2019). Indeed, the various instruments produced a relatively broad range in O/C wa in both ionization modes (Fig.…”

Section: Bias Due To Ionizationmentioning

confidence: 99%

See 2 more Smart Citations

An international laboratory comparison of dissolved organic matter composition by high resolution mass spectrometry: Are we getting the same answer?

Hawkes

D’Andrilli

Agar

et al. 2020

Limnology & Ocean Methods

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132

153

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High-resolution mass spectrometry (HRMS) has become a vital tool for dissolved organic matter (DOM) characterization. The upward trend in HRMS analysis of DOM presents challenges in data comparison and interpretation among laboratories operating instruments with differing performance and user operating conditions. It is therefore essential that the community establishes metric ranges and compositional trends for data comparison with reference samples so that data can be robustly compared among research groups. To this end, four identically prepared DOM samples were each measured by 16 laboratories, using 17 commercially purchased instruments, using positive-ion and negative-ion mode electrospray ionization (ESI) HRMS analyses. The instruments identified~1000 common ions in both negative-and positive-ion modes over a wide range of m/z values and chemical space, as determined by van Krevelen diagrams. Calculated metrics of abundance-weighted average indices (H/C, O/C, aromaticity, and m/z) of the commonly detected ions showed that hydrogen saturation and aromaticity were consistent for each reference sample across the instruments, while average mass and oxygenation were more affected by differences in instrument type and settings. In this paper we present 32 metric values for future benchmarking. The metric values were obtained for the four different parameters from four samples in two ionization modes and can be used in future work to evaluate the performance of HRMS instruments.

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Section: Discussionmentioning

confidence: 99%

Section: Theoretical Formula Listmentioning

confidence: 99%

Section: Bias Due To Ionizationmentioning

confidence: 99%

See 1 more Smart Citation

An international laboratory comparison of dissolved organic matter composition by high resolution mass spectrometry: Are we getting the same answer?

Hawkes

D’Andrilli

Agar

et al. 2020

Limnology & Ocean Methods

Self Cite

132

153

View full text Add to dashboard Cite

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“…Fourier transform ion cyclotron resonance (FT-ICR) and Orbitrap mass spectrometry with their ultrahigh mass resolution and mass accuracy ensure an unambiguous assignment of each detected signal in complex mixtures such as crude oil, bio oils, tar oils or lignin derivatives. [14][15][16][17][18][19][20] A combination of various atmospheric pressure ionization (API) methods, such as electrospray ionization (ESI), atmospheric pressure chemical and photo ionization (APCI/APPI), enables a comprehensive view of the sample. 21 Negative mode ESI coupled to FT MS opens the possibility for detailed characterization of acidic compounds especially oxygenated classes.…”

Section: Introductionmentioning

confidence: 99%

Development of a Non-Targeted Method to Study Petroleum Polyaromatic Hydrocarbons in Soil by Ultrahigh Resolution Mass Spectrometry Using Multiple Ionization Methods

Luo

Schräder

2020

Polycyclic Aromatic Compounds

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A non-targeted method for analyzing petroleum hydrocarbons in soil was established by extracting a wide range of PAC compounds using a model system. Here, sand was spiked with a heavy crude oil, which simulated a hydrocarbon contaminated soil of low soil organic matter (SOM). Soxhlet and supercritical fluid extraction (SFE) was optimized for PAXHs analysis in soil. A concept of using multidimensional ionization for ultrahigh resolution mass spectrometry was employed for detection using electrospray ionization (ESI), atmospheric pressure chemical ionization (APCI) and atmospheric pressure photo ionization (APPI) for the analysis of polycyclic aromatic hydrocarbons (PAHs) and polycyclic aromatic heterocycles. Fourier transform mass spectrometry (FT-MS) with its ultrahigh mass resolution and high mass accuracy enables an unambiguous assignment of the detected ions obtained from different ionization methods, which provides a secure and comprehensive view of contaminants in soil on a molecular level. Over 95% of the spiked crude oil could be recovered by Soxhlet extraction using toluene, dichloromethane and acetone:n-hexane (1:1, v:v). In comparison, when using SFE with supercritical CO 2 the recovery was only about 50% but showed more polar compounds. Detailed analyses showed that besides 16 PAHs, a wide range with more than 10,000 PAXHs could also be successfully extracted.

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“…Ultrahigh resolution mass spectrometry (UHRMS) is the method of choice for investigation of complex mixtures [2,[19][20][21][22][23][24][25]. Thanks to the ultrahigh resolving power and based on accurate mass measurements, UHRMS provides unique elemental compositions (C c H h N n O o S s ) for the detected compounds [11,22].…”

Section: Introductionmentioning

confidence: 99%

A Detailed Look at the Saturate Fractions of Different Crude Oils Using Direct Analysis by Ultrahigh Resolution Mass Spectrometry (UHRMS)

Farmani

Schräder

2019

Energies

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SARA (Saturates, Aromatics, Resins, Asphaltenes) fractionation is a common simplification technique used for decades in petrochemical analysis. A large number of studies are dealing with the different fractions, but overall, the saturate fraction is strongly neglected. Of the very few available studies on the saturates fraction, almost all have been performed using gas chromatographic (GC) techniques. This discriminates the results of the saturate fraction especially since non-volatile, high molecular weight and polar constituents are mostly excluded. Here, for the first time, saturate fractions of different crude oils from different origins are analyzed using direct infusion ultrahigh resolution mass spectrometry (UHRMS), to study the compositions on a molecular level. Electrospray (ESI), atmospheric pressure chemical ionization (APCI) and atmospheric pressure photoionization (APPI) are used in positive mode. The observed results show the presence of different heteroatom containing classes, with different chemical identities (i.e., presence of thiophenes, mercaptans and cyclic-sulfides in case of S-containing compounds). These results show the high affinity of some specific compounds towards different ionization techniques. Finally, the saturate fraction is shown to include much more than only volatile, saturated and aliphatic compounds. The detected compounds in this fraction present a very wide variety, not only in terms of their carbon atoms per molecule and their aromaticity, but also with regard to their functional groups and structural arrangements.

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Pushing the analytical limits: new insights into complex mixtures using mass spectra segments of constant ultrahigh resolving power

Abstract: A new strategy has been developed for characterization of the most challenging complex mixtures to date, using a combination of custom-designed experiments and a new data pre-processing algorithm.

Cited by 85 publications

References 78 publications

An international laboratory comparison of dissolved organic matter composition by high resolution mass spectrometry: Are we getting the same answer?

An international laboratory comparison of dissolved organic matter composition by high resolution mass spectrometry: Are we getting the same answer?

Development of a Non-Targeted Method to Study Petroleum Polyaromatic Hydrocarbons in Soil by Ultrahigh Resolution Mass Spectrometry Using Multiple Ionization Methods

A Detailed Look at the Saturate Fractions of Different Crude Oils Using Direct Analysis by Ultrahigh Resolution Mass Spectrometry (UHRMS)

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