On the benefits of using multivariate analysis in mass spectrometric studies of combustion-generated aerosols

Duca, Dumitru; Irimiea, Cornélia; Faccinetto, Alessandro; Noble, J. A.; Vojković, Marin; Carpentier, Y.; Ortega, Ismael‐Kenneth; Pirim, Claire; Focşa, Cristian

doi:10.1039/c8fd00238j

Cited by 17 publications

(24 citation statements)

References 64 publications

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“…PAHs comprising more than four rings were classified as non-volatile as they were observed in the PM in their study. Note that slightly different classes have also been defined elsewhere in the literature Elghawi et al, 2010;Sun et al, 2006). In our study, we largely found compounds consisting of one and two aromatic rings on back filters, while PAHs of m/z 176-242 were found on both back and front filters and those of m/z ≥ 252 predominantly on front filters.…”

Section: Multivariate Data Analysis: Principal Component Analysis (Pca)supporting

confidence: 59%

“…The sorbents are placed in series, i.e., one after the other in the exhaust line. The soluble organic fraction is then extracted off-line from the sorbent (filter and/or resin) for subsequent gas chromatography-mass spectrometry (GC-MS) analyses Elghawi et al, 2010;Sun et al, 2006). However, such solvent extraction methods exhibit recovery rates that are highly dependent upon the technique applied and the nature of PAHs a priori present.…”

Section: Introductionmentioning

confidence: 99%

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Chemical discrimination of the particulate and gas phases of miniCAST exhausts using a two-filter collection method

et al. 2020

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Abstract. Combustion of hydrocarbons produces both particulate- and gas-phase emissions responsible for major impacts on atmospheric chemistry and human health. Ascertaining the impact of these emissions, especially on human health, is not straightforward because of our relatively poor knowledge of how chemical compounds are partitioned between the particle and gas phases. Accordingly, we propose coupling a two-filter sampling method with a multi-technique analytical approach to fully characterize the particulate- and gas-phase compositions of combustion by-products. The two-filter sampling method is designed to retain particulate matter (elemental carbon possibly covered in a surface layer of adsorbed molecules) on a first quartz fiber filter while letting the gas phase pass through and then trap the most volatile components on a second black-carbon-covered filter. All samples thus collected are subsequently subjected to a multi-technique analytical protocol involving two-step laser mass spectrometry (L2MS), secondary ion mass spectrometry (SIMS), and micro-Raman spectroscopy. Using the combination of this two-filter sampling–multi-technique approach in conjunction with advanced statistical methods, we are able to unravel distinct surface chemical compositions of aerosols generated with different set points of a miniCAST burner. Specifically, we successfully discriminate samples by their volatile, semi-volatile, and non-volatile polycyclic aromatic hydrocarbon (PAH) contents and reveal how subtle changes in combustion parameters affect particle surface chemistry.

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Section: Multivariate Data Analysis: Principal Component Analysis (Pca)supporting

confidence: 59%

Section: Introductionmentioning

confidence: 99%

Chemical discrimination of the particulate and gas phases of miniCAST exhausts using a two-filter collection method

et al. 2020

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“…CC BY 4.0 License. and 2 SIMS polarities) following the procedure detailed in Popovicheva et al (2017), Irimiea et al (2018), and Duca et al (2019). Further information can also be found in Sect.…”

Section: Multivariate Data Analysis: Principal Component Analysis (Pca)mentioning

confidence: 99%

“…7. Cnfragments are commonly considered as markers of the EC content (Duca et al, 2019;Pagels et al, 2013;Popovicheva et al, 2017). For instance, Pagels et al (2013) used the sum of Cn -(n = 2-4) fragment signals as a marker of EC in aerosol time-of-flight mass spectrometer (ATOFMS) measurements for wood stove PM emissions and the same marker ions have been used to discriminate diesel from biodiesel PM emissions by Popovicheva et al (2017).…”

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confidence: 99%

Chemical discrimination of the particulate and gas phases of miniCAST exhausts using a two-filter collection method

Ngo¹,

Duca²,

Carpentier³

et al. 2019

Preprint

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Abstract. Combustion of hydrocarbons produces both particulate and gas phase emissions responsible for major impacts on atmospheric chemistry and human health. Ascertaining the impact of these emissions, especially on human health, is not straightforward because of our relatively poor knowledge of how chemical compounds are partitioned between the particle and gas phases. Accordingly, we propose to couple a two-filter sampling method with a multi-technique analytical approach to fully characterize the particulate and gas phase compositions of combustion by-products. The two-filter sampling method is designed to retain particulate matter (elemental carbon possibly covered in a surface layer of adsorbed molecules) on a first quartz fiber filter while letting the gas phase pass through, and then trap the most volatile components on a second black carbon-covered filter. All samples thus collected are subsequently subjected to a multi-technique analytical protocol involving two-step laser mass spectrometry (L2MS), secondary ion mass spectrometry (SIMS), and micro-Raman spectroscopy. Using the combination of this two-filter sampling/multi-technique approach in conjunction with advanced statistical methods we are able to unravel distinct surface chemical compositions of aerosols generated with different set points of a miniCAST burner. Specifically, we successfully discriminate samples by their volatile, semi-volatile and non-volatile polycyclic aromatic hydrocarbon (PAH) contents and reveal how subtle changes in combustion parameters affect particle surface chemistry.

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“…We recently showcased the advantages of using advanced statistical techniques (Duca et al, 2019;Irimiea et al, 2018Irimiea et al, , 2019 to highlight subtle differences in the chemical composition of various samples. It is also very useful to confirm initial trends deduced from a descriptive approach of the mass spectra with a more quantitative approach such as that provided by the statistical analyses.…”

Section: ) Poormentioning

confidence: 99%

Authors' response to reviewer's comments

Carpentier¹

2019

Preprint

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We would like to thank the referee for his/her careful reading of the manuscript and the detailed comments that were provided. We think we addressed all the referee's concerns and we edited our manuscript when further details or clarifications were needed. 1) Collection system and experimental setup. The collection system poses some serious problems. Positive artefacts are well known on quartz filters. Some of the filters were highly charged (PF1, PF2, PF3). We could expect that C1 AMTD Interactive comment Printer-friendly version Discussion paper a kind of "soot cake" is formed on the front filters increasing the filtration efficiency and causing more adsorption of the gaseous compounds onto the deposited particles (see Fig. 1 images front filters).

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On the benefits of using multivariate analysis in mass spectrometric studies of combustion-generated aerosols

Abstract: Building on a recently proposed comprehensive methodology, we propose herein a comparative analysis of soot particles produced by three different sources.

Cited by 17 publications

References 64 publications

Chemical discrimination of the particulate and gas phases of miniCAST exhausts using a two-filter collection method

Chemical discrimination of the particulate and gas phases of miniCAST exhausts using a two-filter collection method

Chemical discrimination of the particulate and gas phases of miniCAST exhausts using a two-filter collection method

Authors' response to reviewer's comments

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