Atmospheric Environment, Journal Year: 2023, Volume and Issue: 311, P. 120001 - 120001
Published: Aug. 5, 2023
Language: Английский
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
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
Environmental Science & Technology, Journal Year: 2023, Volume and Issue: 57(17), P. 6944 - 6954
Published: April 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.
Language: Английский
Citations
30
ACS Omega, Journal Year: 2023, Volume and Issue: 8(10), P. 9621 - 9629
Published: Feb. 28, 2023
Formic acid (FA) is a prominent candidate for organic enhanced nucleation due to its high abundance and stabilizing effect on smaller clusters. Its role in new particle formation studied through the use of state-of-the-art quantum chemical methods cluster systems (acid)1–2(FA)1(base)1–2 with acids being sulfuric (SA)/methanesulfonic (MSA) bases consisting ammonia (A), methylamine (MA), dimethylamine (DMA), trimethylamine (TMA), ethylenediamine (EDA). A funneling approach used determine structures initial configurations generated ABCluster program, followed by semiempirical PM7 ωB97X-D/6-31++G(d,p) calculations. The final binding free energy calculated at DLPNO-CCSD(T0)/aug-cc-pVTZ//ωB97X-D/6-31++G(d,p) level theory using quasi-harmonic approximation. Cluster dynamics simulations show that FA has minuscule or negligible MSA–FA–base as well most SA–FA–base systems. SA–FA–DMA system shows highest influence from an enhancement 21%, compared non-FA counterpart.
Language: Английский
Citations
24
ACS Omega, Journal Year: 2021, Volume and Issue: 6(26), P. 17035 - 17044
Published: June 23, 2021
The role of methanesulfonic acid (MSA) in atmospheric new particle formation remains highly uncertain. Using state-of-the-art computational methods, we study the electrically neutral
Language: Английский
Citations
55
ACS Omega, Journal Year: 2021, Volume and Issue: 6(11), P. 7804 - 7814
Published: March 12, 2021
We recently coined the term clusteromics as a holistic approach for obtaining insight into chemical complexity of atmospheric molecular cluster formation and at same time providing foundation thermochemical databases that can be utilized developing machine learning models. Here, we present first paper in series applies state-of-the-art computational methods to study multicomponent (SA)
Language: Английский
Citations
49
ACS Omega, Journal Year: 2022, Volume and Issue: 7(17), P. 15206 - 15214
Published: April 20, 2022
Acid-base molecular clusters are an important stage in atmospheric new particle formation. While such most likely multicomponent nature, there very few reports on consisting of multiple acid molecules and base molecules. By applying state-of-the-art quantum chemical methods, we herein study electrically neutral (SA)1(MSA)1(base)0-2 with = ammonia (A), methylamine (MA), dimethylamine (DMA), trimethylamine (TMA) ethylenediamine (EDA). The cluster structures obtained using a funneling approach employing the ABCluster program, semiempirical PM7 calculations ωB97X-D/6-31++G(d,p) calculations. final binding free energies calculated at DLPNO-CCSD(T0)/aug-cc-pVTZ//ωB97X-D/6-31++G(d,p) level theory quasi-harmonic approximation. Based geometries thermochemistry (at 298.15 K 1 atm), find that mixed (SA)1(MSA)1(base)1-2 more resemble (SA)2(base)1-2 compared to (MSA)2(base)1-2 clusters. Hence, some steric hindrance lack hydrogen bond capacity previously observed is diminished corresponding Cluster kinetics simulations reveal presence MSA molecule enhances formation potential by up factor 20. We SA-MSA-DMA have highest potential, thus, this system should be further extended larger sizes future studies.
Language: Английский
Citations
36
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
npj Climate and Atmospheric Science, Journal Year: 2022, Volume and Issue: 5(1)
Published: Nov. 17, 2022
Abstract Marine new particle formation (NPF) can affect cloud condensation nuclei (CCN) in the global atmosphere. Recently, iodic acid (IA) has been identified as a critical driver for marine NPF. However, atmospheric observations of IA cannot be associated with predicted rates. Given complexity components, other species may promote formation. As an efficient stabilizer acidic precursors, dimethylamine (DMA) wide distribution over oceans. Hence, we investigated nucleation process DMA and under different conditions uncovered corresponding nucleating mechanism using quantum chemical approach Atmospheric Cluster Dynamics Code (ACDC). The findings show that structurally stabilize via hydrogen halogen bonds, clustering is energy barrierless. Moreover, enhance rate clusters by five orders magnitude, its efficiency promoting cluster much higher than NH 3 . Compared to sequential addition IA, IA-DMA plays more dominant role kinetic. Thus, effect on enhancing stability ignored, especially regions near source emissions. Broadly, proposed help explain some missing sources particles and, thus intensive NPF events.
Language: Английский
Citations
29
Reviews of Modern Physics, Journal Year: 2023, Volume and Issue: 95(4)
Published: Nov. 9, 2023
Atmospheric nanoparticles can serve as nuclei for cloud droplets, thereby inducing significant but uncertain effects on the radiative forcing of climate system. This article focuses physicochemical processes that govern growth these particles from formation molecular clusters until reach sizes where they act condensation nuclei. The review describes latest developments in measurement and modeling connects domains to large-scale simulations such Earth system models. authors recommend closer coordination among laboratory studies, atmospheric measurements, understand importance
Language: Английский
Citations
22