The Science of The Total Environment, Год журнала: 2022, Номер 821, С. 153336 - 153336
Опубликована: Янв. 22, 2022
Язык: Английский
Environmental Science Atmospheres, Год журнала: 2023, Номер 3(3), С. 444 - 473
Опубликована: Янв. 1, 2023
Atmospheric amines from various sources undergo a variety of homogeneous and heterogeneous reactions to contribute the overall process aerosol particle formation further affect climate.
Язык: Английский
Процитировано
22
Current Pollution Reports, Год журнала: 2024, Номер 10(1), С. 40 - 53
Опубликована: Янв. 19, 2024
Язык: Английский
Процитировано
8
Environmental Science & Technology, Год журнала: 2022, Номер 56(12), С. 7751 - 7760
Опубликована: Май 20, 2022
Atmospheric amines are considered to be an effective enhancer for methanesulfonic acid (MSA)-driven nucleation. However, out of the 195 detected atmospheric amines, enhancing potential (EP) has so far only been studied five amines. This severely hinders understanding contribution MSA-driven Herein, a two-step procedure was employed probe EP various on Initially, formation free energies (ΔG) 50 MSA-amine dimer clusters were calculated. Based calculated ΔG values, robust quantitative structure-activity relationship (QSAR) model built and utilized predict values remaining 145 The QSAR identified two guanidino-containing compounds as potentially strongest Second, by employing larger selecting guanidine (Gud) representative. results indicate that Gud indeed EP. Gud-MSA system presents unique clustering mechanism, proceeding via initial (Gud)1(MSA)1 cluster, subsequently cluster collisions with either or (Gud)2(MSA)2 cluster. developed identification provide foundation comprehensively evaluating
Язык: Английский
Процитировано
24
Atmospheric chemistry and physics, Год журнала: 2023, Номер 23(15), С. 8789 - 8804
Опубликована: Авг. 9, 2023
Abstract. Sulfuric acid (SA) is a governing gaseous precursor for atmospheric new particle formation (NPF), major source of global ultrafine particles, in environments studied around the world. In polluted urban atmospheres with high condensation sinks (CSs), stable SA–amine clusters, such as SA–dimethylamine (DMA) usually initializes intense NPF events. Coagulation scavenging and cluster evaporation are dominant sink processes clusters atmospheres, yet these loss not quantitatively included present parameterizations nucleation. We herein report parameterization SA–DMA nucleation, based on dynamic simulations quantum chemistry calculations, certain simplifications to greatly reduce computational costs. Compared previous nucleation parameterizations, this was able reproduce dependences rates temperature CSs. then incorporated it three-dimensional (3-D) chemical transport model simulate evolution number size distributions. Simulation results showed good consistency observations occurrence events distributions wintertime Beijing represented significant improvement compared that using without coagulation scavenging. Quantitative analysis shows contributes significantly aerosol population during 3-D (>99 % >60 %, respectively). These broaden understanding stress necessity including effects stability simulating simulations. Representing thus likely improve performance apportionment quantification air quality, human health, climate.
Язык: Английский
Процитировано
15
Environmental Science & Technology Letters, Год журнала: 2022, Номер 9(4), С. 306 - 311
Опубликована: Март 22, 2022
Amines, as the vital precursors of new particle formation (NPF), have received considerable attention because their outbreak characteristics and sources haze episodes. During hourly resolution observations conducted in Hebei Province, a significant amine concentrations, four times higher burst periods (BPs, 625 ± 383 ng m–3) than that nonburst (NBPs, 164 62.1 m–3), was observed. Especially for ethyl-amines (sum diethylamine triethylamine), its ratio to methyl-amines monomethylamine, dimethylamine, trimethylamine) increased from 0.62 0.35 (NBPs) 3.28 2.04 (BPs). This is first study determine composition profiles three types sources, namely, mobile residential solid fuel combustion (RSFC), biological (BS), exploring ethyl-amines. The widely used ethanol gasoline vehicles (EGVs) Province were found primarily emit ethyl-amines, methyl-amine emitted EGVs (2.82 1.1) much larger RSFC (0.94 0.4) BS (0.87 0.4). Considering widespread application China, role EGV emissions outbreaks requires urgent attention.
Язык: Английский
Процитировано
23
Atmospheric chemistry and physics, Год журнала: 2022, Номер 22(18), С. 12207 - 12220
Опубликована: Сен. 19, 2022
Abstract. During the COVID-19 lockdown, dramatic reduction of anthropogenic emissions provided a unique opportunity to investigate effects reduced activity and primary on atmospheric chemical processes consequent formation secondary pollutants. Here, we utilize comprehensive observations examine response new particle (NPF) changes in cocktail. We find that main clustering process was unaffected by drastically traffic emissions, rate 1.5 nm particles remained unaltered. However, survival probability enhanced due an increased growth (GR) during lockdown period, explaining NPF earlier studies. For GR at 1.5–3 nm, sulfuric acid (SA) contributor high temperatures, whilst there were unaccounted contributing vapors low temperatures. 3–7 7–15 oxygenated organic molecules (OOMs) played major role. Surprisingly, OOM composition volatility insensitive large change NOx concentration; instead associated rates concentration period mostly caused oxidative capacity. Overall, our findings suggest limited role NPF.
Язык: Английский
Процитировано
22
Journal of Geophysical Research Atmospheres, Год журнала: 2023, Номер 128(3)
Опубликована: Янв. 26, 2023
Abstract The refined source apportionment of ammonium (NH 4 + ), especially for biomass burning emissions, is unclear. Hourly resolution δ 15 N‐NH values three winter haze episodes (EP1–EP3) were determined in the North China Plain (NCP) 2019 to identify and quantify contribution burning. A reasonable source‐resolved structure NH was obtained after using corrected signatures N considering emissions. time‐series variation vehicle sources identified by more matched better with their tracers (e.g., levoglucosan). non‐negligible NCP found contributed 13.0% ± 11.4% episodes, but special stages as high 29% 11% local emission EP1 23% 15% southwest transportation EP2. redistribution further emphasize its PM 2.5 increased up 5% (without SO 2− NO 3 − ). Considering uniqueness formation new particles, role during should be considered. This study indicates that studies need conducted reduce emissions NCP.
Язык: Английский
Процитировано
12
Journal of Environmental Sciences, Год журнала: 2022, Номер 123, С. 183 - 202
Опубликована: Март 11, 2022
Язык: Английский
Процитировано
17
International Journal of Quantum Chemistry, Год журнала: 2025, Номер 125(8)
Опубликована: Апрель 10, 2025
ABSTRACT The study investigated the contribution of hydroxymethanesulfonic acid (HMSA) to formation new particles in presence atmospheric bases such as ammonia (A), methylamine (MA), dimethylamine (DMA) and water (W) by DLPNO‐CCSD(T)/aug‐cc‐pVTZ//B3LYP‐D3/aug‐cc‐pVTZ(aug‐cc‐pV(T+d)Z for sulfur) level. Clusters containing HMSA were found easily form six− or eight−membered ring structures via SO—H⋯O (HMSA donor), O—H⋯O/N (W N—H⋯O/N (A/MA/DMA C—H⋯O (MA/DMA donor) hydrogen bonds. Due synergistic interaction between X Y molecules, stability HMSA−X−Y trimers is thermodynamically more favorable than HMSA−X dimers, proton transfer was be exothermic barrier−free trimers. Moreover, increased with higher alkalinity Y, leading decreased evaporation rates. highlights significance HMSA−containing nucleation processes particle formation, suggesting their potential role centers conditions.
Язык: Английский
Процитировано
0
Опубликована: Май 1, 2025
Abstract New particle formation (NPF) is a key source of atmospheric particles and cloud condensation nuclei (CCN). In polluted regions, the nucleation mechanism sulfuric acid (H 2 SO 4 )-dimethylamine (DMA) thought to play crucial role in NPF. However, it still remains unclear about sources DMA their contributions regional number concentrations (PNC) CCN. this study, we incorporated H -DMA into aerosol module WRF-Chem model improve model’s simulation ability for NPF events. The default 8 size bins covering 39 nm 10 μm were extended 12 ranging from 1 better capture growth small particles. modified was applied Beijing its surrounding areas an observation episode March 18 2017. results show that revised significantly improves capability simulating smaller range (<20 nm), reducing standardized bias over 58% 10%. contributes 46–78% PNC surface layer (from ~300 m) 22–36% CCN at 0.5% supersaturation (CCN ). are notably higher on days than those non-NPF days. High zones correspond with elevated , suggesting process leads increased concentrations, these regions also exhibit levels DMA. Agricultural residential activities identified as main study area. contribution particularly significant urban Beijing, reaching up 70%. This enhances our understanding how events induced by affect intensive anthropogenic emission regions.
Язык: Английский
Процитировано
0