2D Liquid Chromatographic Fractionation with Ultra-high Resolution MS Analysis Resolves a Vast Molecular Diversity of Tropospheric Particle Organics

Environmental Science & Technology, Journal Year: 2019, Volume and Issue: 53(19), P. 11353 - 11363

Published: Sept. 3, 2019

A 2D-liquid chromatographic fractionation method was combined with direct infusion electrospray ionization Fourier transform-ion cyclotron resonance mass spectrometry to better resolve the high complexity of organic material in atmospheric particles. The number assigned molecular formulas increased by a factor 2.3 for fractionated sample (18 144) compared bulk analysis without (7819), while simultaneously allowing identification 71 240 isomeric compounds. Accounting these isomers has an impact on means and distributions different descriptive parameters. More than 15 000 compounds were exclusively identified providing insights regarding formation organosulfates, reduced N-containing compounds, polyaromatic Further, new assigning organonitrates poly-organonitrates based Kendrick defect is presented. current study implicates that analytical separation leads much more detailed into particle organics composition, commonly applied MS studies can strongly underestimate composition lead biased assignments properties. Overall, far complex previously shown, through techniques helps understand processes constituents.

Language: Английский

---

Research progress on secondary formation, photosensitive reaction mechanism and human health effects of chromophoric brown carbon

Journal of Environmental Sciences, Journal Year: 2024, Volume and Issue: 151, P. 310 - 330

Published: April 14, 2024

Language: Английский

---

Modeling Photosensitized Secondary Organic Aerosol Formation in Laboratory and Ambient Aerosols

Environmental Science & Technology, Journal Year: 2017, Volume and Issue: 51(13), P. 7496 - 7501

Published: June 12, 2017

Photosensitized reactions involving imidazole-2-carboxaldehyde (IC) have been experimentally observed to contribute secondary organic aerosol (SOA) growth. However, the extent of photosensitized in ambient aerosols remains poorly understood and unaccounted for atmospheric models. Here we use GAMMA 4.0, a photochemical box model that couples gas-phase aqueous-phase chemistry, along with recent laboratory measurements kinetics IC photochemistry, analyze IC-photosensitized SOA formation settings. Analysis results Aregahegn et al. (2013) suggests production from limonene, isoprene, α-pinene, β-pinene, toluene by 3IC* occurs at or near surface particle. Reactive uptake coefficients were derived experimental data using 4.0. Simulations aqueous remote conditions including photosensitizer chemistry indicate less than 0.3% contribution growth direct toluene, an enhancement 0.04% other precursors due radicals bulk phase. Other, more abundant species, such as humic-like substances (HULIS), may significantly production.

Language: Английский

---

Modeling Secondary Organic Aerosol Production from Photosensitized Humic-like Substances (HULIS)

Environmental Science & Technology Letters, Journal Year: 2018, Volume and Issue: 5(5), P. 255 - 259

Published: April 3, 2018

Humic-like substances (HULIS) are ubiquitous in atmospheric aerosols. Despite experimental evidence that HULIS can catalyze secondary organic aerosol (SOA) formation through photosensitizer chemistry, the potential contribution of this pathway to ambient SOA has not been quantified. In study, GAMMA, a photochemical box model, was used analyze data Monge et al. ( Proc. Natl. Acad. Sci. U. S. A. 2012, 109, 6840−6844) quantify kinetics uptake limonene by particles containing humic acid, laboratory proxy for HULIS. The results indicate is taken up irradiated acid efficiently, with reactive coefficient 1.6 × 10–4. Consequently, simulations limonene–HULIS chemistry under conditions, simultaneously other aqueous processes, show could contribute 65% total at pH 4. importance warrants further studies and representation source models.

Language: Английский

---

Formation of highly oxygenated multifunctional compounds from cross-reactions of carbonyl compounds in the atmospheric aqueous phase

Atmospheric Environment, Journal Year: 2019, Volume and Issue: 219, P. 117046 - 117046

Published: Oct. 10, 2019

Language: Английский

---