The effectiveness of coagulation sink of 3–10 nm atmospheric particles DOI Creative Commons
Runlong Cai, Ella Häkkinen, Chao Yan

et al.

Published: April 14, 2022

Abstract. As a major source of ultrafine particles, new particle formation (NPF) occurs frequently in various environments. However, the survival particles and frequent occurrence NPF events polluted environments have long been perplexing, since are expected to be scavenged by high coagulation sinks. Towards solving these problems, we establish an experimental method directly measure effectiveness size-dependent sink monodisperse 3–10 nm well-controlled chamber experiments. Based on experiments long-term atmospheric measurements from Beijing, then discuss In experiments, measured coefficient increases significantly with decreasing size, whereas it is not sensitive compositions test particles. Comparison between theoretical predictions shows that almost every leads scavenging one particle, exceeds hard-sphere kinetic limit due van der Waals attractive force. For urban moderate or (e.g., > 3 h-1) growth rate can explain events; further implies addition gaseous sulfuric acid, other precursors also contribute

Language: Английский

The missing base molecules in atmospheric acid–base nucleation DOI Creative Commons
Runlong Cai, Rujing Yin, Chao Yan

et al.

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
Significant contributions of trimethylamine to sulfuric acid nucleation in polluted environments DOI Creative Commons
Runlong Cai, Rujing Yin, Xue Li

et al.

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

31
Critical Role of Iodous Acid in Neutral Iodine Oxoacid Nucleation DOI Creative Commons
Rongjie Zhang, Hong‐Bin Xie, Fangfang Ma

et al.

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
Amine-Enhanced Methanesulfonic Acid-Driven Nucleation: Predictive Model and Cluster Formation Mechanism DOI
Yu Liu, Hong‐Bin Xie, Fangfang Ma

et al.

Environmental Science & Technology, Journal Year: 2022, Volume and Issue: 56(12), P. 7751 - 7760

Published: May 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

Language: Английский

Citations

23
A dynamic parameterization of sulfuric acid–dimethylamine nucleation and its application in three-dimensional modeling DOI Creative Commons
Yuyang Li,

Jiewen Shen,

Bin Zhao

et al.

Atmospheric chemistry and physics, Journal Year: 2023, Volume and Issue: 23(15), P. 8789 - 8804

Published: Aug. 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.

Language: Английский

Citations

15
Iodine oxoacids and their roles in sub-3 nm particle growth in polluted urban environments DOI Creative Commons
Ying Zhang, Duzitian Li, Xu‐Cheng He

et al.

Atmospheric chemistry and physics, Journal Year: 2024, Volume and Issue: 24(3), P. 1873 - 1893

Published: Feb. 12, 2024

Abstract. New particle formation contributes significantly to the number concentration of ultrafine particles (UFPs, d ≤ 100 nm) and has a great impact on human health global climate. Iodine oxoacids (HIOx, including iodic acid, HIO3, iodous HIO2) have been observed in pristine regions proved dominate new (NPF) at some sites. However, knowledge HIOx polluted urban areas is rather limited. Here, we conducted long-term measurements gaseous iodine sulfuric acid Beijing from January 2019 October 2021 also Nanjing March February 2020 investigated contribution UFP both environments. HIO3 highest summer, up 2.85 × 106 2.78 cm−3 Nanjing, respectively, lowest winter by 96 % 75 %, respectively. exhibits more prominent variation than H2SO4 shows clear diurnal pattern sites with daily maximum around noontime, similar atmospheric temperature, solar radiation, ozone (O3) levels. HIO2 same seasonal trend as but overall about an order magnitude lower concentration. Back trajectory analysis suggests that sources for inland species could be mix marine terrestrial origins, having peak emission warm seasons. While growth marginal our results demonstrate enhances survival probability sub-3 nm 40 (median) occasionally NPF events, suggesting are significant contributor UFPs areas. As per-molecule basis, propose sum used estimate inorganic origin atmospheres amount HIOx.

Language: Английский

Citations

5
The effect of COVID-19 restrictions on atmospheric new particle formation in Beijing DOI Creative Commons
Chao Yan, Yicheng Shen, Dominik Stolzenburg

et al.

Atmospheric chemistry and physics, Journal Year: 2022, Volume and Issue: 22(18), P. 12207 - 12220

Published: Sept. 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.

Language: Английский

Citations

22
Measurement of atmospheric nanoparticles: Bridging the gap between gas-phase molecules and larger particles DOI Open Access
Chao Peng,

Chenjuan Deng,

Ting Lei

et al.

Journal of Environmental Sciences, Journal Year: 2022, Volume and Issue: 123, P. 183 - 202

Published: March 11, 2022

Language: Английский

Citations

17
The effectiveness of the coagulation sink of 3–10 nm atmospheric particles DOI Creative Commons
Runlong Cai, Ella Häkkinen, Chao Yan

et al.

Atmospheric chemistry and physics, Journal Year: 2022, Volume and Issue: 22(17), P. 11529 - 11541

Published: Sept. 7, 2022

Abstract. As a major source of ultrafine particles, new particle formation (NPF) occurs frequently in various environments. However, the survival particles and frequent occurrence NPF events polluted environments have long been perplexing, since are expected to be scavenged by high coagulation sinks. Towards solving these problems, we establish an experimental method directly measure effectiveness size-dependent sink monodisperse 3–10 nm well-controlled chamber experiments. Based on experiments long-term atmospheric measurements from Beijing, then discuss In experiments, measured increases significantly with decreasing size, whereas it is not sensitive compositions test particles. Comparison between coefficient theoretical predictions shows that almost every leads scavenging one particle, exceeds hard-sphere kinetic limit due van der Waals attractive force. For urban moderate or (e.g., > 3 h−1) growth rate can explain events; further implies that, addition gaseous sulfuric acid, other precursors also contribute

Language: Английский

Citations

12
Temporal and spatial shifts in the chemical composition of urban coastal rainwaters of Kuwait: The role of air mass trajectory and meteorological variables DOI

Dhanu Radha SVV,

Amjad Al‐Rashidi,

S. Chidambaram

et al.

The Science of The Total Environment, Journal Year: 2023, Volume and Issue: 899, P. 165649 - 165649

Published: July 20, 2023

Language: Английский

Citations

7