HELIOS/SICRIT/mass spectrometry for analysis of aerosols in engine exhaust

Thaler, Klemens M.; Gilardi, Lorenza; Weber, Markus; Vohburger, Andreas; Toumasatos, Zisimos; Kontses, Anastasios; Samaras, Zissis; Kalliokoski, Joni; Simonen, Pauli; Timonen, Hilkka; Aurela, Minna; Saarikoski, Sanna; Martikainen, Sampsa; Karjalainen, Panu; Maso, Miikka Dal; Keskinen, Jorma; Pang, Genny A.; Haisch, Christoph

doi:10.1080/02786826.2021.1909699

Cited by 12 publications

(8 citation statements)

References 38 publications

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“…In addition to the FT-IR, the exhaust from the two sampling points was analyzed using the custom-built Mass spectrometer (MS) system described by Thaler et al 46 In short, the MS was composed of a Thermo Fin Finnigan LTQ ion trap mass spectrometer by Thermo Fisher Scientific Inc. (Germany) with a commercially available highly efficient atmospheric ionization source named “soft-ionization by chemical reaction in transfer (SICRIT)” by Plasmion GmbH (Germany). 47 Directly upstream of the SICRIT ion source, a custom-built “high efficient light source for optical surface desorption (HELIOS)” infrared oven was used for evaporation of volatile particle components, thus enabling online detection of both gaseous exhaust species and volatile and semi-volatile aerosols or species absorbed on solid particles.…”

Section: Methodsmentioning

confidence: 99%

Gaseous emissions of a heavy-duty engine fueled with polyoxymethylene dimethyl ethers (OME) in transient cold-start operation and methods for after-treatment system heating

Gelner

Pang

Weber

et al. 2022

Environ. Sci.: Adv.

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Section: Methodsmentioning

confidence: 99%

Gaseous emissions of a heavy-duty engine fueled with polyoxymethylene dimethyl ethers (OME) in transient cold-start operation and methods for after-treatment system heating

Gelner

Pang

Weber

et al. 2022

Environ. Sci.: Adv.

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“…Analytes are ionized within the ambient atmosphere while passing through the source without requiring additional makeup gas. This allows to freely choose the atmosphere for ionization while coupling the system to separation techniques such as liquid chromatography (LC), gas chromatography (GC), , or performing chemical imaging. − Furthermore, the source can be used for direct measurements, e.g., in engine exhaust, where external factors determine the ionization atmosphere, and knowledge about the makeup gas dependency of ionization is critical for spectra interpretation . To our best knowledge, the influence of makeup gas and dopants on ionization has only been investigated for individual compounds or compound groups such as PAHs with nitrogen-/air-based DBDI.…”

Section: Introductionmentioning

confidence: 99%

“…24−26 Furthermore, the source can be used for direct measurements, e.g., in engine exhaust, where external factors determine the ionization atmosphere, and knowledge about the makeup gas dependency of ionization is critical for spectra interpretation. 27 To our best knowledge, the influence of makeup gas and dopants on ionization has only been investigated for individual compounds or compound groups such as PAHs 28 with nitrogen-/air-based DBDI.…”

Section: ■ Introductionmentioning

confidence: 99%

Effect of Dopants and Gas-Phase Composition on Ionization Behavior and Efficiency in Dielectric Barrier Discharge Ionization

Weber

Wolf²,

Haisch

2023

J. Am. Soc. Mass Spectrom.

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Cold plasma-based ionization techniques allow for soft ionization of a wide variety of chemical compounds. In this chemical ionization mechanism, the atmosphere plays a crucial role in ionization. Knowing its influence is critical for the optimization of analysis conditions and interpretation of resulting spectra. This study uses soft ionization by chemical reaction in transfer (SICRIT), a variant of dielectric barrier discharge ionization (DBDI), that allows for a controlled atmosphere to investigate atmosphere and dopant effects. The influence of eight makeup gas compositions (dry nitrogen, room air, and nitrogen-enriched with either water, HCl, MeOH, hexane, NH 3 , and fluorobenzene) on the ionization with SICRIT was investigated. Fifteen compound classes, comprising alkanes, polyaromatic hydrocarbons (PAHs), terpenes, oxygen-containing terpenes, alkylphenols, chlorophenols, nitrophenols, trialkylamines, triazines, phthalates with or without ether groups, aldehydes, ketones, fatty acid methyl esters (FAMEs), and polyoxy-methylene ethers (OMEs) were measured via gas chromatography SICRIT high-resolution mass spectrometry (GC-SICRIT-HRMS). The different atmospheres were compared in terms of generated ions, ion intensities and fragmentation during ionization. Measurements of reactant ions were performed for a better understanding of the underlying mechanisms. All 15 compound classes were mostly softly ionized. For most compound classes and atmospheres, protonation is the dominant ionization mode. The highest number of compounds ionized via protonation was observed in dry nitrogen, followed by room air and humid nitrogen. The study should work as a guideline for the choice of atmosphere for specific compound classes and the interpretation of spectra generated under a specific atmosphere.

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“…The DBDI source is small, affordable and enables real‐time analysis of aromatic hydrocarbons. It can be coupled to GC 21 and has been used for the analysis of polycyclic aromatic hydrocarbons (PAHs) in wastewater 22 or in the real‐time analysis of engine exhaust 23 . While these studies focus on generating intact molecular ions, N‐addition product ions [M + N] + of alkylbenzenes have been reported in APCI 24 and for volatile saturated hydrocarbons in electric fields 25 .…”

Section: Introductionmentioning

confidence: 99%

Discriminating alkylbenzene isomers with tandem mass spectrometry using a dielectric barrier discharge ionization source

2023

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Soft ambient ionization sources generate reactive species that interact with analyte molecules to form intact molecular ions, which allows rapid, sensitive, and direct identification of the molecular mass. We used a dielectric barrier discharge ionization (DBDI) source with nitrogen at atmospheric pressure to detect alkylated aromatic hydrocarbon isomers (C 8 H 10 or C 9 H 12 ). Intact molecular ions [M] •+ were detected at 2.4 kV pp , but at increased voltage (3.4 kV pp ), [M + N] + ions were formed, which could be used to differentiate regioisomers by collision-induced dissociation (CID). At 2.4 kV pp , alkylbenzene isomers with different alkyl-substituents could be identified by additional product ions: ethylbenzene and -toluene formed [M-2H] + , isopropylbenzene formed abundant [M-H] + , and propylbenzene formed abundant C 7 H 7 + . At an operating voltage of 3.4 kV pp , fragmentation of [M + N] + by CID led to neutral loss of HCN and CH 3 CN, which corresponded to steric hindrance for excited state N-atoms approaching the aromatic ring (C-H). The ratio of HCN to CH 3 N loss (interday relative standard deviation [RSD] < 20%) was distinct for ethylbenzene and ethyltoluene isomers. The greater the number of alkyl-substituents (C-CH 3 ) and the more sterically hindered (meta > para > ortho) the aromatic core, the greater the loss of CH 3 CN relative to HCN was.

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HELIOS/SICRIT/mass spectrometry for analysis of aerosols in engine exhaust

Cited by 12 publications

References 38 publications

Gaseous emissions of a heavy-duty engine fueled with polyoxymethylene dimethyl ethers (OME) in transient cold-start operation and methods for after-treatment system heating

Gaseous emissions of a heavy-duty engine fueled with polyoxymethylene dimethyl ethers (OME) in transient cold-start operation and methods for after-treatment system heating

Effect of Dopants and Gas-Phase Composition on Ionization Behavior and Efficiency in Dielectric Barrier Discharge Ionization

Discriminating alkylbenzene isomers with tandem mass spectrometry using a dielectric barrier discharge ionization source

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