Formation Of Nucleation Mode Particles Research Articles

New Insights on the Formation of Nucleation Mode Particles in a Coastal City Based on a Machine Learning Approach.

Atmospheric particles have profound implications for the global climate and human health. Among them, ultrafine particles dominate in terms of the number concentration and exhibit enhanced toxic effects as a result of their large total surface area. Therefore, understanding the driving factors behind ultrafine particle behavior is crucial. Machine learning (ML) provides a promising approach for handling complex relationships. In this study, three ML models were constructed on the basis of field observations to simulate the particle number concentration of nucleation mode (PNCN). All three models exhibited robust PNCN reproduction (R2 > 0.80), with the random forest (RF) model excelling on the test data (R2 = 0.89). Multiple methods of feature importance analysis revealed that ultraviolet (UV), H2SO4, low-volatility oxygenated organic molecules (LOOMs), temperature, and O3 were the primary factors influencing PNCN. Bivariate partial dependency plots (PDPs) indicated that during nighttime and overcast conditions, the presence of H2SO4 and LOOMs may play a crucial role in influencing PNCN. Additionally, integrating additional detailed information related to emissions or meteorology would further enhance the model performance. This pilot study shows that ML can be a novel approach for simulating atmospheric pollutants and contributes to a better understanding of the formation and growth mechanisms of nucleation mode particles.

The influence of alcohol, carbonate and polyethers as oxygenated fuels on the soot characteristics from a CI engine

Dimethyl carbonate (DMC), ethanol (EtOH), polyoxymethylene dimethyl ether 1 (PODE1) and polyoxymethylene dimethyl ether 4 (PODE4) were blended with Jet A1 into fuel blends with 5 % oxygen content to investigate the effect of the oxygenated fuels on the soot produced by a compression ignition engine. Particle size distribution (PSD) was measured using a differential mobility spectrometer. Thermogravimetric analysis (TGA), Raman spectroscopy, ultraviolet–visible spectroscopy (UV–Vis) and Fourier transform infrared (FT-IR) spectroscopy were performed on the soot collected from the engine. The addition of EtOH, PODE1 improves brake thermal efficiency (BTE) by up to 4.5 %, while DMC reduces BTE by 0.9–1.5 % compared to Jet A1. EtOH fuel blends have the shortest combustion duration (10.0 deg), followed by PODE1, DMC and PODE4. EtOH blends also have the highest heat release rate peak (4–14 % higher than Jet A1). This, combined with improved premixing of EtOH fuel blend in the engine improves the combustion and reduces soot growth. PSD measurements showed that the addition of EtOH significantly reduces accumulation mode particle number concentrations by up to 70 % but promotes the formation of nucleation mode particles. Meanwhile, TGA revealed that the soot from oxygenated fuel blends oxidises at a lower temperature than Jet A1. Notably, PODE1 exhibited a reduction of 54 °C in the starting oxidation temperature, which is the largest reduction among the oxygenated fuel blends. Lastly, the conjugation length of the soot aromatic structure for the organic carbons (derived from the optical band gap of UV–Vis) is up to 11 % greater for the oxygenated fuel blends, indicating that oxygenated fuel blends promote organic carbon formation. The blending of oxygenated fuels in influencing the soot properties through the dilution effect, combustion condition effect and chemical effect is then critically assessed.

Revisiting Total Particle Number Measurements for Vehicle Exhaust Regulations

Road transport significantly contributes to air pollution in cities. Emission regulations have led to significantly reduced emissions in modern vehicles. Particle emissions are controlled by a particulate matter (PM) mass and a solid particle number (SPN) limit. There are concerns that the SPN limit does not effectively control all relevant particulate species and there are instances of semi-volatile particle emissions that are order of magnitudes higher than the SPN emission levels. This overview discusses whether a new metric (total particles, i.e., solids and volatiles) should be introduced for the effective regulation of vehicle emissions. Initially, it summarizes recent findings on the contribution of road transport to particle number concentration levels in cities. Then, both solid and total particle emission levels from modern vehicles are presented and the adverse health effects of solid and volatile particles are briefly discussed. Finally, the open issues regarding an appropriate methodology (sampling and instrumentation) in order to achieve representative and reproducible results are summarized. The main finding of this overview is that, even though total particle sampling and quantification is feasible, details for its realization in a regulatory context are lacking. It is important to define the methodology details (sampling and dilution, measurement instrumentation, relevant sizes, etc.) and conduct inter-laboratory exercises to determine the reproducibility of a proposed method. It is also necessary to monitor the vehicle emissions according to the new method to understand current and possible future levels. With better understanding of the instances of formation of nucleation mode particles it will be possible to identify its culprits (e.g., fuel, lubricant, combustion, or aftertreatment operation). Then the appropriate solutions can be enforced and the right decisions can be taken on the need for new regulatory initiatives, for example the addition of total particles in the tailpipe, decrease of specific organic precursors, better control of inorganic precursors (e.g., NH3, SOx), or revision of fuel and lubricant specifications.

Sources and formation of nucleation mode particles in remote tropical marine atmospheres over the South China Sea and the Northwest Pacific Ocean

A fast mobility particle sizer operating at a one-second time resolution was used to measure aerosol particle number size distribution (5.6–560 nm) in marine conditions over the South China Sea (SCS) from 29 March to 2 May 2017 and in the tropic zone of the Northwest Pacific Ocean (NWPO) from 10 to 29 October 2018. The clean background number concentration of nucleation mode atmospheric particles (<30 nm) was approximately 0.6 × 103 cm−3 in these areas. Two nighttime and five daytime strong new particle formation (NPF) events were observed to occur extending over a spatial scale from 2 to 140 km in the SCS, with a net increase of nucleation mode particles of 4.5 × 104 cm−3 ± 3.4 × 104 cm−3 during five of the seven events. Nighttime NPF events were unlikely associated with sulfuric acid vapor because of lack of photochemical reactions. Daytime NPF events share several common features with nighttime NPF events, e.g., dramatic spatiotemporal variations in the number concentration of the nucleation mode particles. Without aerosol precursor measurements we cannot address the vapors driving the formation process. However, our results show no banana-shaped growth of the particles. The growth into larger particle sizes seems to be restricted by the availability of condensable components in the gas phase. The nucleation mode was observed and sometimes even dominated the number concentration over other particle modes in the marine atmosphere over the tropic zone of the NWPO. In addition, more data obtained during the two campaigns and other campaigns were also applied to strengthen the analysis in terms of origins, formation and absent growth of nucleation mode particles in the marine atmospheres over the two tropic zones.

Modeling of the Concentrations of Ultrafine Particles in the Plumes of Ships in the Vicinity of Major Harbors.

Marine traffic in harbors can be responsible for significant atmospheric concentrations of ultrafine particles (UFPs), which have widely recognized negative effects on human health. It is therefore essential to model and measure the time evolution of the number size distributions and chemical composition of UFPs in ship exhaust to assess the resulting exposure in the vicinity of shipping routes. In this study, a sequential modelling chain was developed and applied, in combination with the data measured and collected in major harbor areas in the cities of Helsinki and Turku in Finland, during winter and summer in 2010–2011. The models described ship emissions, atmospheric dispersion, and aerosol dynamics, complemented with a time–microenvironment–activity model to estimate the short-term UFP exposure. We estimated the dilution ratio during the initial fast expansion of the exhaust plume to be approximately equal to eight. This dispersion regime resulted in a fully formed nucleation mode (denoted as Nuc2). Different selected modelling assumptions about the chemical composition of Nuc2 did not have an effect on the formation of nucleation mode particles. Aerosol model simulations of the dispersing ship plume also revealed a partially formed nucleation mode (Nuc1; peaking at 1.5 nm), consisting of freshly nucleated sulfate particles and condensed organics that were produced within the first few seconds. However, subsequent growth of the new particles was limited, due to efficient scavenging by the larger particles originating from the ship exhaust. The transport of UFPs downwind of the ship track increased the hourly mean UFP concentrations in the neighboring residential areas by a factor of two or more up to a distance of 3600 m, compared with the corresponding UFP concentrations in the urban background. The substantially increased UFP concentrations due to ship traffic significantly affected the daily mean exposures in residential areas located in the vicinity of the harbors.

Impact of straight vegetable oil–diesel blends application on vehicle regulated and non-regulated emissions over legislated and real world driving cycles

Straight vegetable oil (SVO) has been considered as a possible alternative to fossil diesel-engine fuel since the development of diesel engines. In Europe, SVOs achieved a measurable share in biofuels market reaching 4%. This study attempts to identify the impact of untreated SVO application on fuel consumption and emissions, regulated and non-regulated, on a Euro 3 common rail diesel passenger car. Three different vegetable oils (cottonseed, sunflower, and rapeseed) were blended with diesel fuel, on a 10–90% v/v ratio each. Chassis dynamometer measurements were conducted including both regulated and non-regulated pollutants. In the case of rapeseed oil–diesel blend, carbonyl compounds (10 aldehydes and ketones) were investigated. In addition to the legislated procedure (NEDC), the Artemis driving cycles were used for quantifying the fuels’ impact over realistic driving conditions. Results indicate that all blends have limited effects on gaseous pollutants and vehicle performance. Statistically significant increases on CO2, CO and HC were recorded over NEDC in the order of 3, 39 and 31%. Reductions were observed on PM emissions particularly for the sunflower oil blends, while NOx remained at baseline levels. Comparison with the emission levels measured when using esterified fuels of the same feedstocks suggests that SVO presence does not affect engine exhaust in the same way as biodiesel. The vegetable oil presence in the fuel appeared to suppress the formation of nucleation mode particles. Straight rapeseed oil increased carbonyl compound emissions over all cycles tested and resulted in higher acroleine/acetone presence in the carbonyl compound composition.

Size distribution and new particle formation in subtropical eastern Australia

Environmental context. Atmospheric submicrometre particles have a significant impact on human health, visibility impairment, acid deposition and global climate. This study aims to understand the size distribution of submicrometre particles and new particle formation in eastern Australia and the results indicate that photochemical reactions of airborne pollutants are the main mechanism of new particle formation. The findings will contribute to a better understanding of the effects of aerosols on climate and the reduction of submicrometre particles in the atmosphere. Abstract. An intensive measurement campaign of particle concentrations, nitrogen oxides and meteorological parameters was conducted at a rural site in subtropical eastern Australia during September 2006. The aim of this work was to develop an understanding of the formation and growth processes of atmospheric aerosols, and the size distributions under various meteorological conditions. In order to achieve this, the origins of air arriving at the site were explored using back trajectories cluster analysis and the diurnal patterns of particle number concentration and size distribution for the classified air masses were investigated. The study showed that the photochemical formation of nucleation mode particles and their consequent growth was often observed. Furthermore, the nucleation mode usually dominated the size distribution and concentration of the photochemical event in the first 3–4 h with a geometric mean diameter of 26.9 nm and a geometric standard deviation of 1.28. The average particle growth rate was estimated to be 1.6 nm h–1, which is lower than that observed at urban sites, but comparable to the values reported in clean environments. The potential precursors of the photochemical events are also discussed.

Condensation and coagulation sinks and formation of nucleation mode particles in coastal and boreal forest boundary layers

The formation and growth of new particles has been evaluated using a revised version of a simple, but novel, theoretical tool. The concentration of condensable vapors and their source rates has been estimated using the aerosol condensation sink together with the measured particle growth rate. Also, by adding the coagulation sink and the measured formation rate of 3 nm particles, the formation rate of 1 nm particles and their concentration can be estimated. Condensation and coagulation sinks can be obtained from ambient aerosol size distribution data. The method has been applied to analyze the particle formation and growth rates observed during coastal and boreal forest nucleation events. The condensation sinks are typically 4–7 × 10−3 s−1 in the forest and 2 × 10−3 s−1 under coastal conditions, while the coagulation sinks for 1, 2, and 3 nm particles are typically smaller by factors 1.5–2, 5–7, and 11–15, respectively. The measured growth rates are 2–10 nm/h for the boreal forest and range from 15 to 180 nm/h at the coast, corresponding to a vapor concentration of 2–13 × 107 cm−3 and 108 cm−3 to 109 cm−3, respectively. The vapor source rate was 1–2 × 105 cm−3s−1 in the boreal forest and 2–5 × 106 cm−3s−1 in the coastal environment. The estimated formation rate of 1 nm particles in the forest environment was 8–20 cm−3s−1 and 300–10,000 cm−3s−1 at the coast. The concentration of 1 nm particles was estimated to be 2000–5000 and 4 × 104–7 × 106 particles cm−3 in forest and at coast, respectively.