Significant contributions of trimethylamine to sulfuric acid nucleation in polluted environments

npj Climate and Atmospheric Science, Год журнала: 2023, Номер 6(1)

Опубликована: Июнь 27, 2023

Abstract As one of the least understood aerosol processes, nucleation can be a dominant source atmospheric aerosols. Sulfuric acid (SA)-amine binary with dimethylamine (DMA) has been recognized as governing mechanism in polluted continental boundary layer. Here we demonstrate importance trimethylamine (TMA) for complex atmosphere and propose molecular-level SA-DMA-TMA ternary an improvement upon conventional mechanism. Using proposed mechanism, could connect gaseous amines to SA-amine cluster signals measured urban Beijing. Results show that TMA accelerate SA-DMA-based new particle formation Beijing by 50–100%. Considering global abundance DMA, our findings imply comparable DMA layer, probably higher contributions from rural environments future controlled emissions.

Язык: Английский

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Enhancement of Atmospheric Nucleation Precursors on Iodic Acid-Induced Nucleation: Predictive Model and Mechanism

Environmental Science & Technology, Год журнала: 2023, Номер 57(17), С. 6944 - 6954

Опубликована: Апрель 21, 2023

Iodic acid (IA) has recently been recognized as a key driver for new particle formation (NPF) in marine atmospheres. However, the knowledge of which atmospheric vapors can enhance IA-induced NPF remains limited. The unique halogen bond (XB)-forming capacity IA makes it difficult to evaluate enhancing potential (EP) target compounds on based widely studied sulfuric systems. Herein, we employed three-step procedure EP nucleation precursors NPF. First, evaluated 63 by simulating free energies (ΔG) IA-containing dimer clusters. Among all clusters, 44 contained XBs, demonstrating that XBs are frequently formed. Based calculated ΔG values, quantitative structure–activity relationship model was developed evaluating other precursors. Second, amines and O/S-atom-containing acids were found have high EP, with diethylamine (DEA) yielding highest combining both concentration considered Finally, studying larger (IA)1–3(DEA)1–3 IA-DEA system merely 0.1 ppt (2.5×106 cm–3) DEA yields comparable rates IA–iodous system.

Язык: Английский

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Aqueous-Phase Reactions of Anthropogenic Emissions Lead to the High Chemodiversity of Atmospheric Nitrogen-Containing Compounds during the Haze Event

Environmental Science & Technology, Год журнала: 2023, Номер 57(43), С. 16500 - 16511

Опубликована: Окт. 16, 2023

Nitrogen-containing organic compounds (NOCs), a type of important reactive-nitrogen species, are abundant in aerosols haze events observed Northern China. However, due to the complex nature NOCs, sources, formation, and influencing factors still ambiguous. Here, molecular composition matters (OMs) hourly PM2.5 samples collected during event China was characterized using Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS). We found that CHON (formulas containing C, H, O, N atoms) dominated OM fractions showed high chemodiversity transformability. Relying on newly developed revised-workflow oxidation-hydrolyzation knowledge for compounds, 64% major aromatic (>80%) could be derived from oxidization or hydrolyzation processes. Results FT-ICR MS data analysis further aerosol liquid water (ALW)-involved aqueous-phase reactions distribution aromatic-CHON besides coal combustion, ALW-involved compound formation daytime nighttime different. Our results improve understanding composition, potential which can help advance evolution, control haze.

Язык: Английский

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A new advance in the pollution profile, transformation process, and contribution to aerosol formation and aging of atmospheric amines

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

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Aqueous‐Phase Secondary Processes and Meteorological Change Promote the Brown Carbon Formation and Transformation During Haze Events

Journal of Geophysical Research Atmospheres, Год журнала: 2023, Номер 128(16)

Опубликована: Авг. 20, 2023

Abstract The evolution and the impacts of meteorological conditions on brown carbon (BrC) absorption are not understood, which hinders assessment BrC radiative forcing. To address this issue, 1‐hr time‐resolved PM 2.5 samples collected during three haze events in North China Plain prior to COVID‐19 pandemic were used measure optical properties BrC. By coupling excitation‐emission matrix spectroscopy, chemical tracer analysis with multiple model including positive factorization (PMF) a deweather‐random forest model, we found that higher proportion highly oxidized chromophoric components was present water‐soluble than methanol‐soluble BrC, indicating conversion low‐oxidized water‐insoluble into day. results PMF showed aqueous secondary processes major contributor (68% ± 38%), changes such as relative humidity (RH) could significantly lead light‐absorbing capacity especially enhancement for bleaching noon afternoon. We further increased RH increases maximum ∼65%, then decreased when >65%, highlighting important role generation

Язык: Английский

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Biomass Burning Is a Non‐Negligible Source for Ammonium During Winter Haze Episodes in Rural North China: Evidence From High Time Resolution ¹⁵N‐Stable Isotope

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

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Characteristics and origins of fine particulate amines at a coastal mountain site in northern China in spring

Atmospheric Environment, Год журнала: 2024, Номер 321, С. 120365 - 120365

Опубликована: Янв. 22, 2024

Язык: Английский

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Measurement report: Occurrence of aminiums in PM_2.5 during winter in China – aminium outbreak during polluted episodes and potential constraints

Atmospheric chemistry and physics, Год журнала: 2024, Номер 24(18), С. 10531 - 10542

Опубликована: Сен. 23, 2024

Abstract. Amines and aminiums play an important role in particle formation, liquid-phase reactions, climate change have attracted considerable attention over the years. Here, we investigated concentrations compositions of PM2.5 11 Chinese cities during winter, focusing on characteristics polluted days key factors influencing aminium outbreak. Monomethylaminium was dominant species most cities, except Taiyuan Guangzhou, followed by dimethylaminium. Diethylaminium dominated total Guangzhou. Thus, main amine sources Guangzhou were significantly different from those other cities. The (TAs) increased days, while relatively weak outbreaks occurred Xi'an Beijing. Additionally, TAs Beijing insignificantly correlated with major acidic aerosol components, opposite pattern observed nine acid–base chemistry associated formation all Based sensitivity analysis : ammonium ratio to changes, as well excluding effects relative humidity atmospheric oxidation, proposed possibility competitive uptake ammonia versus amines aerosols or displacement (constraining outbreaks). Overall, this study deepens understanding spatiotemporal differences characteristic China. However, particles form relevant require further mechanistic research.

Язык: Английский

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Organosulfur Compounds: A Non‐Negligible Component Affecting the Light Absorption of Brown Carbon During North China Haze Events

Journal of Geophysical Research Atmospheres, Год журнала: 2025, Номер 130(1)

Опубликована: Янв. 4, 2025

Abstract The roles of organosulfur compounds (OSCs), an important component in organic matter, brown carbon (BrC) aerosol absorption is often overlooked. Here, the molecular composition OSCs and its associations with methanol‐soluble BrC (MS‐BrC) during a haze event North China were revealed using Fourier transform ion cyclotron resonance mass spectrometry analysis. By combining aggregated boosted tree model partial least squares regression estimation, our results suggested that mainly composed potential aromatic structures, MS‐BrC was closely related to OSCs. Specifically, contribute notable 26% total number upper limit 10.4% absorption. Furthermore, we found influenced by coal combustion, desulfurization reactions showed variations Since residential combustion (an primary source OSs) major energy China, research underscores as tracers for assessing impact fossil fuel on highlights atmospheric influences (e.g., light health), which need more works uncover origins, fates, environmental effects

Язык: Английский

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Atmospheric amines are a crucial yet missing link in Earth’s climate via airborne aerosol production

Communications Earth & Environment, Год журнала: 2025, Номер 6(1)

Опубликована: Фев. 10, 2025

Atmospheric amines, derivatives of ammonia, play a unique yet not fully understood role in air quality, climate and public health. Sub-5 parts per trillion Volume (pptV, <10-12 volume) mixing ratios amines facilitate the physical and/or chemical transformation aerosols atmosphere, enhancing aerosol formation growth rates, hygroscopicity, activation cloud condensation nuclei. This serves as initial step for droplet and, consequently, influences properties hydrological cycle. Ambient observations demonstrate more than thousand-fold particle rates presence compared to ammonia. Yet, challenges related detecting minute levels paucity ambient amine measurements, limited process-based understanding airborne production have resulted being underrepresented global models. Therefore, advanced techniques with extremely low detection limits highly spatially temporally resolved measurements globally diverse environments are essential. Amines, ubiquitous atmospheric compounds that emitted from range natural anthropogenic sources, key activating nuclei, under-represented models require future high-precision measurement.

Язык: Английский

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