Brown carbon in fine particles in four typical cities in Northwest China during wintertime: coupling optical properties with chemical processes DOI Creative Commons
Miao Zhong, Jianzhong Xu, Huiqin Wang

et al.

Published: May 12, 2023

Abstract. Brown carbon (BrC) aerosol could impact atmospheric radiative forcing and play a crucial role in photochemistry. Most previous studies have predominantly focused on bulk optical properties of ambient BrC from biomass burning emitted primary or secondary aerosol. Few fossil-fuel-influenced aerosol, especially coal combustion emissions. In this study, fine particulate matter (PM2.5) filter samples were collected synchronously four capital cities Northwest China during the winter season (December 2019–January 2020): Lan-zhou (LZ), Xining (XN), Yinchuan (YC), Urumqi (UR), which are represented as energy-producing heavy manufacturing China. The aim study was to explore opti-cal properties, sources, chemical processes water-soluble (WS-BrC). average mass absorption efficiency at 365 nm (MAE365) WS-BrC these 1.24 ± 0.19 m2/g 1.19 0.12 1.07 0.23 0.78 0.16 respectively. investigated by an acid-base titration experiment. MAE365 values all increased with increasing pH (2–11), while fluorescent intensities water extracts fluctuated corresponding values, being stronger higher acidic basic conditions. YC LZ two most sensitive sites variation, suggest-ing important contribution acid/base functional groups. Furthermore, significant photo-enhancement (LZ) photo-bleaching (YC UR) phenomena based coupling light observed different cities, indicating their sources and/or among each other. further explored combination par-allel factor analysis (PARAFAC) excitation-emission matrix positive factorization (PMF) high-resolution spectra organic (OA). Six PARAFAC components including three humic-like substances (LO-HULIS, HO-HULIS1, HO-HULIS2), protein-like (PLS) phenol-like substances, one undefined substance obtained. Four PMF factors OA (WS-POA), less oxi-dized oxygenated that associated combustion-induced WSOA (LO-OOA), highly oxidized OAs respectively photochemical oxidation aqueous-phase transformations (HO-OOA1 HO-OOA2) identified. WS-POA source accounting for 30 %–60 % multiple linear regression model significantly correlated PLS LO-HULIS components. loss is accomplished conversion LO-OOA HO-OOAs through photo- aqueous reactions, where HO-HULIS component. potential precursors reaction pathways city proposed.

Language: Английский

Brown carbon absorption and radiative effects under intense residential wood burning conditions in Southeastern Europe: New insights into the abundance and absorptivity of methanol-soluble organic aerosols DOI
Despina Paraskevopoulou, Dimitris G. Kaskaoutis, Georgios Grivas

et al.

The Science of The Total Environment, Journal Year: 2022, Volume and Issue: 860, P. 160434 - 160434

Published: Nov. 24, 2022

Language: Английский

Citations

41
Enhanced Light Absorption and Elevated Viscosity of Atmospheric Brown Carbon through Evaporation of Volatile Components DOI
Diego Calderon‐Arrieta, Ana C. Morales, Anusha P. S. Hettiyadura

et al.

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: 58(17), P. 7493 - 7504

Published: April 18, 2024

Samples of brown carbon (BrC) material were collected from smoke emissions originating wood pyrolysis experiments, serving as a proxy for BrC representative biomass burning emissions. The acquired samples, referred to "pyrolysis oil (PO

Language: Английский

Citations

10
Phase Behavior and Viscosity in Biomass Burning Organic Aerosol and Climatic Impacts DOI
Florence K. A. Gregson, Nealan G. A. Gerrebos, Meredith Schervish

et al.

Environmental Science & Technology, Journal Year: 2023, Volume and Issue: 57(39), P. 14548 - 14557

Published: Sept. 20, 2023

Smoke particles generated by burning biomass consist mainly of organic aerosol termed (BBOA). BBOA influences the climate scattering and absorbing solar radiation or acting as nuclei for cloud formation. The viscosity phase behavior (i.e., number type phases present in a particle) are properties that expected to impact several climate-relevant processes but remain highly uncertain. We studied using fluorescence microscopy showed comprise two (a hydrophobic hydrophilic phase) across wide range atmospheric relative humidity (RH). determined at room temperature photobleaching method possess different RH-dependent viscosities. is largely independent RH from 0 95%. use Vogel–Fulcher–Tamman equation extrapolate our results colder warmer temperatures, based on extrapolation, predicted be glassy (viscosity >1012 Pa s) temperatures less than 230 K RHs below 95%, with possible implications heterogeneous reaction kinetics formation atmosphere. Using kinetic multilayer model (KM-GAP), we investigated effect lifetime brown carbon within BBOA, which climate-warming agent. presence can increase planetary boundary layer polar regions compared previous modeling studies. Hence, lead an warming climate.

Language: Английский

Citations

18
Unraveling the Light‐Absorbing Properties of Brown Carbon at a Molecular Level DOI Creative Commons
Nan Xu, Min Hu, Xiao Li

et al.

Geophysical Research Letters, Journal Year: 2024, Volume and Issue: 51(10)

Published: May 15, 2024

Abstract Brown carbon (BrC) exhibits a highly complex chemical composition with diverse light‐absorbing properties, which complicates our understanding of its climate impacts. This study examined the impact molecular characteristics (including mass, unsaturation, oxidation state, and polarity) heteroatoms on properties (absorptivity wavelength dependence) BrC from perspective, based ultraviolet‐visible spectra over 40,000 substances in aerosol different sources ambience. Our findings reveal that light‐absorptivity molecules increases decreasing polarity O/C ratio, while it rises higher mass unsaturation. We developed predictive models for absorptivity double bond equivalent ratio. In addition, we observed an inverse correlation between dependence at level, as determined through mathematical analysis. molecular‐level provides valuable insights into absorbing mechanisms, facilitating more accurate characterization atmospheric models.

Language: Английский

Citations

8
Concurrent photochemical whitening and darkening of ambient brown carbon DOI Creative Commons
Qian Li, Dantong Liu, Xiaotong Jiang

et al.

Atmospheric chemistry and physics, Journal Year: 2023, Volume and Issue: 23(16), P. 9439 - 9453

Published: Aug. 25, 2023

Abstract. The light-absorbing organic aerosol (OA), known as brown carbon (BrC), has important radiative impacts; however, its sources and evolution after emission remain to be elucidated. In this study, the light absorption at multiple wavelengths, mass spectra of OA microphysical properties black (BC) were characterized a typical suburban environment in Beijing. BC is constrained by size distribution mixing state, BrC obtained subtracting from total absorption. Aerosol was further apportioned BC, primary secondary applying least correlation between BC. multilinear regression analysis on factorized indicated that traffic biomass burning contributed BrC. Importantly, moderately oxygenated (O / C = 0.62) revealed highly correlate with These had higher nitrogen content, line nitrogen-containing functional groups detected Fourier transform infrared spectrometer. photochemical processes found reduce cross section (MAC) OA, reducing contribution 20 %, same time increasing MAC for which showed 30 % enhancement absorbance, implying concurrent whitening darkening This provides field evidence photochemically produced can considerably compensate some bleaching effect BrC, hereby causing impacts.

Language: Английский

Citations

14
Enhancing characterization of organic nitrogen components in aerosols and droplets using high-resolution aerosol mass spectrometry DOI Creative Commons
Xinlei Ge, Yele Sun, Justin Trousdell

et al.

Atmospheric measurement techniques, Journal Year: 2024, Volume and Issue: 17(2), P. 423 - 439

Published: Jan. 22, 2024

Abstract. This study aims to enhance the understanding and application of Aerodyne high-resolution aerosol mass spectrometer (HR-AMS) for comprehensive characterization organic nitrogen (ON) compounds in particles atmospheric droplets. To achieve this goal, we analyzed 75 N-containing compounds, representing a diverse range ambient non-organonitrate ON (NOON) types, including amines, amides, amino acids, N heterocycles, protein, humic acids. Our results show that NOON can produce significant levels NHx+ NOx+ ion fragments, which are typically recognized as ions representative inorganic species. We also identified presence CH2N+ at m/z = 28.0187, an fragment rarely quantified datasets due substantial interference from N2+. As result, utilization updated calibration factor 0.79 is necessary accurate quantification via HR-AMS. assessed relative ionization efficiencies (RIEs) various species found average RIE (1.52 ± 0.58) aligns with commonly used default value 1.40 aerosol. Moreover, through careful examination HR-AMS spectral features propose fingerprint series aid speciation analysis. For instance, CnH2n+2N+ closely linked CH4N+ indicating primary C2H6N+ suggesting secondary C3H8N+ tertiary amines. CnH2nNO+ (especially n values 1–4) very likely derived amides. The co-existence three ions, C2H4NO2+, C2H3NO+, CH4NO+, serves indicator Additionally, CxHyN2+ indicates occurrence 2N-heterocyclic compounds. Notably, elevated abundance NH4+ distinct signature amines ammonium salts only negligible amounts Finally, contents submicron (PM1) fog water Fresno, California, PM1 New York City (NYC). revealed both Fresno NYC aerosols, whereas concurrently collected contained broader species, aromatic heterocycle (e.g., imidazoles) These findings highlight potential employing widespread measurements aerosols droplets our sources, transformation processes, environmental impacts associated atmosphere.

Language: Английский

Citations

6
Seasonal characterization of chemical and optical properties of water-soluble organic aerosol in Beijing DOI
Bo You, Zhi‐Qiang Zhang,

Aodong Du

et al.

The Science of The Total Environment, Journal Year: 2024, Volume and Issue: 930, P. 172508 - 172508

Published: April 18, 2024

Language: Английский

Citations

6
Significant N-containing brown carbon emission from heavy-duty diesel vehicles revealed by the molecular and chromophore analysis using ultra-high resolution mass spectrometry DOI Creative Commons
Xiao He, Xuan Zheng, Bin Jiang

et al.

Research Square (Research Square), Journal Year: 2025, Volume and Issue: unknown

Published: March 29, 2025

Abstract Brown carbon (BrC) holds scientific significance by influencing radiative balance, cloud condensation dynamics, and regional air quality. This study demonstrated that heavy-duty diesel vehicles (HDDVs) emit substantially higher levels of light-absorbing carbonaceous aerosols under aggressive conditions, such as frequent acceleration high-speed phases investigating the emission profiles, formula distribution, chromophore characteristics various driving conditions. A non-targeted analysis BrC was performed using Fourier-transform ion cyclotron resonance mass spectrometry coupled with a soft electrospray ionization source. The light absorption properties were assessed revealed significantly during compared to low-speed phases. Formula distribution highlighted substantial presence nitrogen-containing species, constituting 53-65% identified peaks, high O/N ratios (≥ 3), double bond equivalent values (DBE > 10), aromaticity (Xc ≥ 2.5), which indicated contribution aromatic structures, condensed aromatics, nitrooxy functionalities chromophores.

Language: Английский

Citations

0
Significant N-containing brown carbon emission from heavy-duty diesel vehicles revealed by the molecular and chromophore analysis using ultra-high resolution mass spectrometry DOI Creative Commons
Xiao He, Xuan Zheng, Bin Jiang

et al.

npj Climate and Atmospheric Science, Journal Year: 2025, Volume and Issue: 8(1)

Published: May 27, 2025

Language: Английский

Citations

0
Organic Matrix Effect on the Molecular Light Absorption of Brown Carbon DOI Creative Commons

Antai Zhang,

Yaling Zeng,

Xin Yang

et al.

Geophysical Research Letters, Journal Year: 2023, Volume and Issue: 50(24)

Published: Dec. 21, 2023

Abstract Brown carbon (BrC) absorption impacts radiative forcing and climate change. Quantifying of BrC requires understanding its molecular composition characteristics. While organic molecules surrounding may impact absorption, their effects have not yet been investigated. This research determined matrix effect on by comparing individual within an matrix. Over 20,000 water‐soluble constituted the associated The enhanced aliphatic but suppressed aromatic BrC, especially with higher O/C ratios indicating greater polarity acidity. By directly measuring modeling we can improve prediction precision aerosol‐radiation interaction comprehension.

Language: Английский

Citations

7