The Science of The Total Environment, Journal Year: 2022, Volume and Issue: 821, P. 153336 - 153336
Published: Jan. 22, 2022
Language: Английский
Nature, Journal Year: 2024, Volume and Issue: 631(8019), P. 98 - 105
Published: June 12, 2024
A key challenge in aerosol pollution studies and climate change assessment is to understand how atmospheric particles are initially formed
Language: Английский
Citations
26
Atmospheric chemistry and physics, Journal Year: 2022, Volume and Issue: 22(4), P. 2639 - 2650
Published: Feb. 25, 2022
Abstract. Atmospheric organic acids (OAs) are expected to enhance methanesulfonic acid (MSA)-driven new particle formation (NPF). However, the exact role of OAs in MSA-driven NPF remains unclear. Here, we employed a two-step strategy probe MSA–methylamine (MA) NPF. Initially, evaluated enhancing potential 12 commonly detected ternary MA–MSA–OA cluster by considering free energies (MSA)1(MA)1(OA)1 clusters and atmospheric concentrations OAs. It was found that formic (ForA) has highest stabilize MA–MSA clusters. The high ForA results from its acidity, structural factors such as no intramolecular H bonds, abundance. second step is extend MSA–MA–ForA system larger sizes. indicate can indeed MSA–MA at conditions (the upper limited temperature 258.15 K), indicating might have an important effect mainly caused increased (MSA)2(MA)1 cluster, which involved pathway binary nucleation. Hence, our be required facilitate atmosphere.
Language: Английский
Citations
50
National Science Review, Journal Year: 2022, Volume and Issue: 9(10)
Published: July 25, 2022
Transformation of low-volatility gaseous precursors to new particles affects aerosol number concentration, cloud formation and hence the climate. The clustering acid base molecules is a major mechanism driving fast nucleation initial growth in atmosphere. However, acid-base cluster composition, measured using state-of-the-art mass spectrometers, cannot explain high rate particles. Here we present strong evidence for existence such as amines smallest atmospheric sulfuric clusters prior their detection by spectrometers. We demonstrate that forming (H2SO4)1(amine)1 rate-limiting step H2SO4-amine uptake pathway H2SO4 clusters. proposed very consistent with particle urban Beijing, which dimethylamine key while other bases ammonia may contribute larger Our findings further underline fact amines, even at low concentrations when undetected clusters, can be crucial planetary boundary layer.
Language: Английский
Citations
48
Environmental Science & Technology, Journal Year: 2022, Volume and Issue: 56(9), P. 5440 - 5447
Published: April 11, 2022
Emissions of NH3 and nine nitrogen-containing volatile organic compounds (NVOCs) (C1–3-amines, C1–3-amides, C1–3-imines) from motor vehicles powered by gasoline, diesel, natural gas under low-speed driving conditions roadside in situ measurements were characterized using a water-cluster chemical ionization mass spectrometer trace monitors. The total emission strength diesel trucks was the greatest followed those gasoline cars cars. per vehicle found to be 2–3 orders magnitude greater than that all NVOCs, regardless type vehicle. Although much lower emissions amides or imines, amines sufficient produce atmospheric concentrations exceeding threshold level for enhance nucleation several magnitude. Different engine reduction technologies (e.g., three-way catalytic converter vs selective reduction) can lead different NVOC profiles. During lifetime vehicle, its most likely increase with mileage. Source profiles three types also obtained measurements. These valuable contribution air pollution management system terms source apportionment, elucidating contributions specific
Language: Английский
Citations
42
npj Climate and Atmospheric Science, Journal Year: 2023, Volume and Issue: 6(1)
Published: June 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.
Language: Английский
Citations
32
Nature Geoscience, Journal Year: 2023, Volume and Issue: 16(11), P. 948 - 957
Published: Nov. 1, 2023
Language: Английский
Citations
29
Journal of Geophysical Research Atmospheres, Journal Year: 2023, Volume and Issue: 128(14)
Published: July 9, 2023
Abstract Amines affect particle formation, aerosol acidity, nitrogen cycle, and climate change. However, little is known about the temporal spatial differences in composition, source, formation process of amines fine particulate matter (PM 2.5 ) different regions China. Seven (amine salts) were investigated PM collected Yangtze River Delta (YRD, Shanghai Nanjing), Pearl (PRD, Guangzhou), northern China (Xi'an Haerbin), background (Puding) areas winter 2017–2018. Methylamine was dominant amine species at YRD, China, sites, while diethylamine dominated PRD site; moreover, mass concentration fraction lowest site. These results could be attributed to changes sources atmospheric processes. Further, coal combustion biomass burning found important contributors cities winter. The contribution weakened other urban sites. In contrast, abundance site largely controlled by biogenic sources. Acid‐base chemistry displacement mechanism tightly associated with salts all particular, degradation hydroxyl radical (•OH) significant Nanjing, Guangzhou, Xi'an, Haerbin insignificant photochemical sites can explained differentiated sources, meteorological conditions, •OH levels. Overall, our findings deepen understanding origins processes amines.
Language: Английский
Citations
26
Proceedings of the National Academy of Sciences, Journal Year: 2024, Volume and Issue: 121(31)
Published: July 24, 2024
New particle formation (NPF) substantially affects the global radiation balance and climate. Iodic acid (IA) is a key marine NPF driver that recently has also been detected inland. However, its impact on continental nucleation remains unclear. Here, we provide molecular-level evidence IA greatly facilitates clustering of two typical land-based nucleating precursors: dimethylamine (DMA) sulfuric (SA), thereby enhancing nucleation. Incorporating this mechanism into an atmospheric chemical transport model, show IA-induced enhancement could realize increase over 20% in SA–DMA rate iodine-rich regions China. With declining anthropogenic pollution driven by carbon neutrality clean air policies China, enhance rates 1.5 to 50 times 2060. Our results demonstrate overlooked role highlight necessity for considering synergistic SA-IA-DMA modeling correct representation climatic impacts aerosols.
Language: Английский
Citations
10
Environmental Science & Technology, Journal Year: 2022, Volume and Issue: 56(19), P. 14166 - 14177
Published: Sept. 20, 2022
Nucleation of neutral iodine particles has recently been found to involve both iodic acid (HIO3) and iodous (HIO2). However, the precise role HIO2 in oxoacid nucleation remains unclear. Herein, we probe such a by investigating cluster formation mechanisms kinetics (HIO3)m(HIO2)n (m = 0-4, n 0-4) clusters with quantum chemical calculations atmospheric dynamics modeling. When compared HIO3, find that binds more strongly HIO3 also HIO2. After accounting for ambient vapor concentrations, fastest rate is predicted mixed HIO3-HIO2 rather than pure or ones. Our reveal strong binding results from exhibiting base behavior (accepting proton HIO3) forming stronger halogen bonds. Moreover, energies show far tolerant choice growth paths when strict stoichiometry required sulfuric acid-base nucleation. rates dimer concentrations are acceptably consistent those measured Cosmic Leaving Outdoor Droplets (CLOUD) experiment. This study suggests could facilitate other acids beyond regions where vapors as ammonia amines scarce.
Language: Английский
Citations
35
Environmental Science & Technology, Journal Year: 2022, Volume and Issue: 56(24), P. 17545 - 17555
Published: Nov. 28, 2022
Alkaline gases, including NH3, C1–3-amines, C1–3-amides, and C1–3-imines, were measured in situ using a water cluster-CIMS urban Beijing during the wintertime of 2018, with campaign average 2.8 ± 2.0 ppbv, 5.2 4.3, 101.1 94.5, 5.4 pptv, respectively. Source apportionment analysis constrained by emission profiles in-use motor vehicles was performed SoFi-PMF software package, five sources identified as gasoline-powered (GV), diesel-powered (DV), septic system (SS), soil (SE), combustion-related (CS). SS dominant NH3 source (60.0%), followed DV (18.6%), SE (13.1%), CS (4.3%), GV (4.0%). responsible for 69.9 85.2% C1- C2-amines emissions, Most C3-amines emitted from nonmotor vehicular (SS = 61.3%; 17.8%; 9.1%). accounted 71.9 34.1% C2-amides mainly comprised amides imines, likely originating pyrolysis nitrogen-containing compounds. Our results suggested that vehicle exhausts can not only contribute to criteria air pollutants but also promote new particle formation, which has been well recognized considered current regulations. Urban residential predominant contributor background NH3. Enhanced emissions major cause PM2.5 buildup haze events. Combustion-related sources, together vehicles, most observed imines may be public health concern within vicinity these sources.
Language: Английский
Citations
34