Physical Chemistry Chemical Physics, Journal Year: 2021, Volume and Issue: 23(5), P. 3195 - 3213
Published: Jan. 1, 2021
In this perspective, we review experiments with molecules picked up on clusters in molecular beams the focus processes atmospheric and interstellar chemistry.
Language: Английский
Geophysical Research Letters, Journal Year: 2020, Volume and Issue: 48(4)
Published: Dec. 29, 2020
Abstract New particle formation in the Arctic atmosphere is an important source of aerosol particles. Understanding processes secondary crucial due to their significant impact on cloud properties and therefore amplification. We observed molecular new particles from low‐volatility vapors at two sites with differing surroundings. In Svalbard, sulfuric acid (SA) methane sulfonic (MSA) contribute some extent condensation nuclei (CCN). This occurs via ion‐induced nucleation SA NH 3 subsequent growth by mainly MSA during springtime highly oxygenated organic molecules summertime. By contrast, ice‐covered region around Villum, we driven iodic but its concentration was insufficient grow nucleated CCN sizes. Our results provide insight about sources precursors
Language: Английский
Citations
242
Proceedings of the National Academy of Sciences, Journal Year: 2020, Volume and Issue: 117(7), P. 3427 - 3432
Published: Feb. 3, 2020
High levels of ultrafine particles (UFPs; diameter less than 50 nm) are frequently produced from new particle formation under urban conditions, with profound implications on human health, weather, and climate. However, the fundamental mechanisms remain elusive, few experimental studies have realistically replicated relevant atmospheric conditions. Previous simulated oxidation one compound or a mixture compounds, extrapolation laboratory results to chemically complex air was uncertain. Here, we show striking UFPs in combining ambient chamber measurements. By capturing conditions (i.e., temperature, relative humidity, sunlight, types abundances chemical species), elucidate roles existing particles, photochemistry, synergy multipollutants formation. Aerosol nucleation is limited by but negligibly nitrogen oxides. Photooxidation vehicular exhaust yields abundant precursors, organics, rather sulfuric acid base species, dominate Recognition this source essential assessing their impacts developing mitigation policies. Our imply that reduction primary removal without simultaneously limiting organics automobile emissions ineffective can even exacerbate problem.
Language: Английский
Citations
213
Environmental Science & Technology, Journal Year: 2021, Volume and Issue: 55(4), P. 2189 - 2207
Published: Feb. 4, 2021
Severe haze events with exceedingly high-levels of fine aerosols occur frequently over the past decades in North China Plain (NCP), exerting profound impacts on human health, weather, and climate. The development effective mitigation policies requires a comprehensive understanding formation mechanisms, including identification quantification sources, formation, transformation aerosol species. Haze evolution this region exhibits distinct physical chemical characteristics from clean to polluted periods, as evident increasing stagnation relative humidity, but decreasing solar radiation well explosive secondary formation. latter is attributed highly elevated concentrations precursor gases reflected by rapid increases particle number mass concentrations, both corresponding nonequilibrium processes. Considerable new knowledge has been acquired understand processes regulating particularly light progress elucidating mechanisms. This review synthesizes recent advances highlighting several critical chemical/physical processes, that is, growth driven photochemistry aqueous chemistry interaction between atmospheric stability. Current challenges future research priorities are also discussed.
Language: Английский
Citations
177
Atmospheric chemistry and physics, Journal Year: 2021, Volume and Issue: 21(4), P. 2457 - 2468
Published: Feb. 18, 2021
Abstract. New particle formation (NPF) is one of the major sources atmospheric ultrafine particles. Due to high aerosol and trace gas concentrations, mechanism governing factors for NPF in polluted boundary layer may be quite different from those clean environments, which however less understood. Herein, based on long-term measurements January 2018 March 2019 Beijing, nucleation influences H2SO4 concentration, amine concentration are quantified. The collision H2SO4–amine clusters found dominating initialize urban Beijing. coagulation scavenging due a factor as it limits new rates. Beijing sometimes limited by low concentrations. Summarizing synergistic effects we elucidate various conditions.
Language: Английский
Citations
149
Atmospheric chemistry and physics, Journal Year: 2021, Volume and Issue: 21(17), P. 13483 - 13536
Published: Sept. 10, 2021
Abstract. The acidity of aqueous atmospheric solutions is a key parameter driving both the partitioning semi-volatile acidic and basic trace gases their aqueous-phase chemistry. In addition, phases, e.g., deliquesced aerosol particles, cloud, fog droplets, also dictated by These feedbacks between chemistry have crucial implications for tropospheric lifetime air pollutants, composition, deposition to terrestrial oceanic ecosystems, visibility, climate, human health. Atmospheric research has made substantial progress in understanding multiphase during recent decades. This paper reviews current state knowledge on these with focus cloud systems, which involve inorganic organic Here, we describe impacts phase buffering phenomena. Next, review different regimes chemical reaction mechanisms kinetics, as well uncertainties subsystems incomplete information. Finally, discuss highlight need future investigations, particularly respect reducing emissions acid precursors changing world, advancements field laboratory measurements model tools.
Language: Английский
Citations
145
Nature Geoscience, Journal Year: 2021, Volume and Issue: 14(6), P. 383 - 388
Published: May 13, 2021
Language: Английский
Citations
132
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
Environmental Science & Technology, Journal Year: 2019, Volume and Issue: 53(24), P. 14387 - 14397
Published: Nov. 11, 2019
Amines are recognized as significant enhancing species on methanesulfonic acid (MSA)-driven new particle formation (NPF). Monoethanolamine (MEA) has been detected in the atmosphere, and its concentration could be significantly increased once MEA-based postcombustion CO2 capture technology is widely implemented. Here, we evaluated potential of MEA MSA-driven NPF by examining MEA–MSA clusters using a combination quantum chemical calculations kinetics modeling. The results indicate that −OH group can form at least one hydrogen bond with MSA or all MEA-containing clusters. higher than strongest agent known so far, methylamine (MA), for NPF. Such high ascribed to not only gas-phase basicity but also role additional increasing binding free energy forming bonds. This clarifies importance hydrogen-bonding capacity from nonamino amines main growth pathway proceeds via initial (MEA)1(MSA)1 cluster, followed alternately adding molecule, differing case MA–MSA
Language: Английский
Citations
91
Faraday Discussions, Journal Year: 2020, Volume and Issue: 226, P. 9 - 52
Published: Oct. 30, 2020
This introduction provides an overview of air quality in megacities, sources and atmospheric processing emissions, impacts on health climate, mitigation strategies, challenges COVID-19.
Language: Английский
Citations
79
Environmental Science & Technology, Journal Year: 2020, Volume and Issue: 54(21), P. 13498 - 13508
Published: Oct. 22, 2020
Atmospheric amines can enhance methanesulfonic acid (MSA)-driven new particle formation (NPF), but the mechanism is fundamentally different compared to that of extensively studied sulfuric (SA)-driven process. Generally, enhancing potentials in SA-driven NPF follow basicity, while this not case for MSA-driven NPF, where structural effects dominate, making more prominent methylamine (MA) dimethylamine (DMA). Therefore, probing factors determining on key fully understanding contribution MSA NPF. Here, we performed a comparative study DMA and MA by examining cluster using computational methods. The results indicate DMA-MSA clusters are stable than corresponding MA-MSA sizes up (DMA)2(MSA)2, indicating basicity dominates initial formation. methyl groups were found present significant steric hindrance beyond (DMA)2(MSA)2 adds lower hydrogen bonding capacity DMA, growth less favorable MA. This implies several could synergistically maximizing advantage amine-MSA stages.
Language: Английский
Citations
77