Shipping Remains a Globally Significant Source of Anthropogenic PN Emissions Even after 2020 Sulfur Regulation.

Shipping is the main source of anthropogenic particle emissions in large areas of the globe, influencing climate, air quality, and human health in open seas and coast lines. Here, we determined, by laboratory and on-board measurements of ship engine exhaust, fuel-specific particle number (PN) emissions for different fuels and desulfurization applied in shipping. The emission factors were compared to ship exhaust plume observations and, furthermore, exploited in the assessment of global PN emissions from shipping, utilizing the STEAM ship emission model. The results indicate that most particles in the fresh ship engine exhaust are in ultrafine particle size range. Shipping PN emissions are localized, especially close to coastal lines, but significant emissions also exist on open seas and oceans. The global annual PN produced by marine shipping was 1.2 × 1028 (±0.34 × 1028) particles in 2016, thus being of the same magnitude with total anthropogenic PN emissions in continental areas. The reduction potential of PN from shipping strongly depends on the adopted technology mix, and except wide adoption of natural gas or scrubbers, no significant decrease in global PN is expected if heavy fuel oil is mainly replaced by low sulfur residual fuels. The results imply that shipping remains as a significant source of anthropogenic PN emissions that should be considered in future climate and health impact models.

Using an oxidation flow reactor to understand the effects of gasoline aromatics and ethanol levels on secondary aerosol formation.

Fuel type and composition affect tailpipe emissions and secondary aerosol production from mobile sources. This study assessed the influence of gasoline fuels with varying levels of aromatics and ethanol on the primary emissions and secondary aerosol formation from a flexible fuel vehicle equipped with a port fuel injection engine. The vehicle was exercised over the LA92 and US06 driving cycles using a chassis dynamometer. Secondary aerosol formation potential was measured using a fast oxidation flow reactor. Results showed that the high aromatics fuels led to higher gaseous regulated emissions, as well as particulate matter (PM), black carbon, and total and solid particle number. The high ethanol content fuel (E78) resulted in reductions for the gaseous regulated pollutants and particulate emissions, with some exceptions where elevated emissions were seen for this fuel compared to both E10 fuels, depending on the driving cycle. Secondary aerosol formation potential was dominated by the cold-start phase and increased for the high aromatics fuel. Secondary aerosol formation was seen in lower levels for E78 due to the lower formation of precursor emissions using this fuel. In addition, operating driving conditions and aftertreatment efficiency played a major role on secondary organic and inorganic aerosol formation, indicating that fuel properties, driving conditions, and exhaust aftertreatment should be considered when evaluating the emissions of secondary aerosol precursors from mobile sources.

Physical Characteristics of Particle Emissions from a Medium Speed Ship Engine Fueled with Natural Gas and Low-Sulfur Liquid Fuels.

Particle emissions from marine traffic affect significantly air quality in coastal areas and the climate. The particle emissions were studied from a 1.4 MW marine engine operating on low-sulfur fuels natural gas (NG; dual-fuel with diesel pilot), marine gas oil (MGO) and marine diesel oil (MDO). The emitted particles were characterized with respect to particle number (PN) emission factors, PN size distribution down to nanometer scale (1.2-414 nm), volatility, electric charge, morphology, and elemental composition. The size distribution of fresh exhaust particles was bimodal for all the fuels, the nucleation mode highly dominating the soot mode. Total PN emission factors were 2.7 × 1015-7.1 × 1015 #/kWh, the emission being the lowest with NG and the highest with MDO. Liquid fuel combustion generated 4-12 times higher soot mode particle emissions than the NG combustion, and the harbor-area-typical lower engine load (40%) caused higher total PN emissions than the higher load (85%). Nonvolatile particles consisted of nanosized fuel, and spherical lubricating oil core mode particles contained, e.g., calcium as well as agglomerated soot mode particles. Our results indicate the PN emissions from marine engines may remain relatively high regardless of fuel sulfur limits, mostly due to the nanosized particle emissions.

Traffic is a major source of atmospheric nanocluster aerosol.

In densely populated areas, traffic is a significant source of atmospheric aerosol particles. Owing to their small size and complicated chemical and physical characteristics, atmospheric particles resulting from traffic emissions pose a significant risk to human health and also contribute to anthropogenic forcing of climate. Previous research has established that vehicles directly emit primary aerosol particles and also contribute to secondary aerosol particle formation by emitting aerosol precursors. Here, we extend the urban atmospheric aerosol characterization to cover nanocluster aerosol (NCA) particles and show that a major fraction of particles emitted by road transportation are in a previously unmeasured size range of 1.3-3.0 nm. For instance, in a semiurban roadside environment, the NCA represented 20-54% of the total particle concentration in ambient air. The observed NCA concentrations varied significantly depending on the traffic rate and wind direction. The emission factors of NCA for traffic were 2.4·1015 (kgfuel)-1 in a roadside environment, 2.6·1015 (kgfuel)-1 in a street canyon, and 2.9·1015 (kgfuel)-1 in an on-road study throughout Europe. Interestingly, these emissions were not associated with all vehicles. In engine laboratory experiments, the emission factor of exhaust NCA varied from a relatively low value of 1.6·1012 (kgfuel)-1 to a high value of 4.3·1015 (kgfuel)-1 These NCA emissions directly affect particle concentrations and human exposure to nanosized aerosol in urban areas, and potentially may act as nanosized condensation nuclei for the condensation of atmospheric low-volatile organic compounds.

Strategies To Diminish the Emissions of Particles and Secondary Aerosol Formation from Diesel Engines.

Particle emissions and secondary aerosol formation from internal combustion engines deteriorate air quality and significantly affect human wellbeing and health. Both the direct particle emissions and the emissions of compounds contributing to secondary aerosol formation depend on choices made in selecting fuels, engine technologies, and exhaust aftertreatment (EAT). Here we study how catalytic EATs, particle filtration, and fuel choices affect these emissions concerning heavy-duty diesel engine. We observed that the most advanced EAT decreased the emissions of fresh exhaust particle mass as much as 98% (from 44.7 to 0.73 mg/kWh) and the formation of aged exhaust particle mass ∼100% (from 106.2 to ∼0 mg/kWh). The composition of emitted particles depended significantly on the EAT and oxidative aging. While black carbon typically dominated the composition of fresh exhaust particles, aged particles contained more sulfates and organics. The fuel choices had minor effects on the secondary aerosol formation, implicating that, in diesel engines, either the lubricant is a significant source of secondary aerosol precursors or the precursors are formed in the combustion process. Results indicate that the utilization of EAT in diesel engines would produce benefits with respect to exhaust burden on air quality, and thus their utilization should be promoted especially in geographical areas suffering from poor air quality.

Infant and Adult Inhalation Exposure to Resuspended Biological Particulate Matter.

Human-induced resuspension of floor dust is a dynamic process that can serve as a major indoor source of biological particulate matter (bioPM). Inhalation exposure to the microbial and allergenic content of indoor dust is associated with adverse and protective health effects. This study evaluates infant and adult inhalation exposures and respiratory tract deposited dose rates of resuspended bioPM from carpets. Chamber experiments were conducted with a robotic crawling infant and an adult performing a walking sequence. Breathing zone (BZ) size distributions of resuspended fluorescent biological aerosol particles (FBAPs), a bioPM proxy, were monitored in real-time. FBAP exposures were highly transient during periods of locomotion. Both crawling and walking delivered a significant number of resuspended FBAPs to the BZ, with concentrations ranging from 0.5 to 2 cm-3 (mass range: ∼50 to 600 µg/m3). Infants and adults are primarily exposed to a unimodal FBAP size distribution between 2 and 6 µm, with infants receiving greater exposures to super-10 µm FBAPs. In just 1 min of crawling or walking, 103-104 resuspended FBAPs can deposit in the respiratory tract, with an infant receiving much of their respiratory tract deposited dose in their lower airways. Per kg body mass, an infant will receive a nearly four times greater respiratory tract deposited dose of resuspended FBAPs compared to an adult.

Heavy Duty Diesel Exhaust Particles during Engine Motoring Formed by Lube Oil Consumption.

This study reports high numbers of exhaust emissions particles during engine motoring. Such particles were observed in the exhaust of two heavy duty vehicles with no diesel particle filter (DPF), driven on speed ramp tests and transient cycles. A significant fraction of these particles was nonvolatile in nature. The number-weighted size distribution peak was below 10 nm when a thermodenuder was used to remove semivolatile material, growing up to 40 nm after semivolatile species condensation. These particles were found to contribute to 9-13% of total particle number emitted over a complete driving cycle. Engine motoring particles originated from lube oil and evidence suggests that these are of heavy organic or organometallic material. Particles of similar characteristics have been observed in the core particle mode during normal fired engine operation. Their size and chemical character has implications primarily on the environmental toxicity of non-DPF diesel and, secondarily, on the performance of catalytic devices and DPFs. Lube oil formulation measures can be taken to reduce the emission of such particles.

Effects of fresh lubricant oils on particle emissions emitted by a modern gasoline direct injection passenger car.

Particle emissions from a modern turbocharged gasoline direct injection passenger car equipped with a three-way catalyst and an exhaust gas recirculation system were studied while the vehicle was running on low-sulfur gasoline and, consecutively, with five different lubrication oils. Exhaust particle number concentration, size distribution, and volatility were determined both at laboratory and on-road conditions. The results indicated that the choice of lubricant affected particle emissions both during the cold start and warm driving cycles. However, the contribution of engine oil depended on driving conditions being higher during acceleration and steady state driving than during deceleration. The highest emission factors were found with two oils that had the highest metal content. The results indicate that a 10% decrease in the Zn content of engine oils is linked with an 11-13% decrease to the nonvolatile particle number emissions in steady driving conditions and a 5% decrease over the New European Driving Cycle. The effect of lubricant on volatile particles was even higher, on the order of 20%.

Vehicle engines produce exhaust nanoparticles even when not fueled.

Vehicle engines produce submicrometer exhaust particles affecting air quality, especially in urban environments. In on-road exhaust studies with a heavy duty diesel vehicle and in laboratory studies with two gasoline-fueled passenger cars, we found that as much as 20-30% of the number of exhaust particles larger than 3 nm may be formed during engine braking conditions-that is, during decelerations and downhill driving while the engine is not fueled. Particles appeared at size ranges extending even below 7 nm and at high number concentrations. Their small size and nonvolatility, coupled with the observation that these particles contain lube-oil-derived metals zinc, phosphorus, and calcium, are suggestive of health risks at least similar to those of exhaust particles observed before. The particles' characteristics indicate that their emissions can be reduced using exhaust after-treatment devices, although these devices have not been mandated for all relevant vehicle types. Altogether, our findings enhance the understanding of the formation vehicle emissions and allow for improved protection of human health in proximity to traffic.

Sulfur driven nucleation mode formation in diesel exhaust under transient driving conditions.

Sulfur driven diesel exhaust nucleation particle formation processes were studied in an aerosol laboratory, on engine dynamometers, and on the road. All test engines were equipped with a combination of a diesel oxidation catalyst (DOC) and a partial diesel particulate filter (pDPF). At steady operating conditions, the formation of semivolatile nucleation particles directly depended on SO2 conversion in the catalyst. The nucleation particle emission was most significant after a rapid increase in engine load and exhaust gas temperature. Results indicate that the nucleation particle formation at transient driving conditions does not require compounds such as hydrocarbons or sulfated hydrocarbons, however, it cannot be explained only by the nucleation of sulfuric acid. A real-world exhaust study with a heavy duty diesel truck showed that the nucleation particle formation occurs even with ultralow sulfur diesel fuel, even at downhill driving conditions, and that nucleation particles can contribute 60% of total particle number emissions. In general, due to sulfur storage and release within the exhaust aftertreatment systems and transients in driving, emissions of nucleation particles can even be the dominant part of modern diesel vehicle exhaust particulate number emissions.

Optical and chemical characterization of aerosols emitted from coal, heavy and light fuel oil, and small-scale wood combustion.

Particle emissions affect radiative forcing in the atmosphere. Therefore, it is essential to know the physical and chemical characteristics of them. This work studied the chemical, physical, and optical characteristics of particle emissions from small-scale wood combustion, coal combustion of a heating and power plant, as well as heavy and light fuel oil combustion at a district heating station. Fine particle (PM1) emissions were the highest in wood combustion with a high fraction of absorbing material. The emissions were lowest from coal combustion mostly because of efficient cleaning techniques used at the power plant. The chemical composition of aerosols from coal and oil combustion included mostly ions and trace elements with a rather low fraction of absorbing material. The single scattering albedo and aerosol forcing efficiency showed that primary particles emitted from wood combustion and some cases of oil combustion would have a clear climate warming effect even over dark earth surfaces. Instead, coal combustion particle emissions had a cooling effect. Secondary processes in the atmosphere will further change the radiative properties of these emissions but are not considered in this study.

Effects of gaseous sulphuric acid on diesel exhaust nanoparticle formation and characteristics.

Diesel exhaust gaseous sulphuric acid (GSA) concentrations and particle size distributions, concentrations, and volatility were studied at four driving conditions with a heavy duty diesel engine equipped with oxidative exhaust after-treatment. Low sulfur fuel and lubricant oil were used in the study. The concentration of the exhaust GSA was observed to vary depending on the engine driving history and load. The GSA affected the volatile particle fraction at high engine loads; higher GSA mole fraction was followed by an increase in volatile nucleation particle concentration and size as well as increase of size of particles possessing nonvolatile core. The GSA did not affect the number of nonvolatile particles. At low and medium loads, the exhaust GSA concentration was low and any GSA driven changes in particle population were not observed. Results show that during the exhaust cooling and dilution processes, besides critical in volatile nucleation particle formation, GSA can change the characteristics of all nucleation mode particles. Results show the dual nature of the nucleation mode particles so that the nucleation mode can include simultaneously volatile and nonvolatile particles, and fulfill the previous results for the nucleation mode formation, especially related to the role of GSA in formation processes.

Size distribution, chemical composition, and hygroscopicity of fine particles emitted from an oil-fired heating plant.

Heavy fuel oil (HFO) is a commonly used fuel in industrial heating and power generation and for large marine vessels. In this study, the fine particle emissions of a 47 MW oil-fired boiler were studied at 30 MW power and with three different fuels. The studied fuels were HFO, water emulsion of HFO, and water emulsion of HFO mixed with light fuel oil (LFO). With all the fuels, the boiler emitted considerable amounts of particles smaller than 200 nm in diameter. Further, these small particles were quite hygroscopic even as fresh and, in the case of HFO+LFO emulsion, the hygroscopic growth of the particles was dependent on particle size. The use of emulsions and the addition of LFO to the fuel had a reducing effect on the hygroscopic growth of particles. The use of emulsions lowered the sulfate content of the smallest particles but did not affect significantly the sulfate content of particles larger than 42 nm and, further, the addition of LFO considerably increased the black carbon content of particulate matter. The results indicate that even the fine particles emitted from HFO based combustion can have a significant effect on cloud formation, visibility, and air quality.

Reductions in particulate and NO(x) emissions by diesel engine parameter adjustments with HVO fuel.

Hydrotreated vegetable oil (HVO) diesel fuel is a promising biofuel candidate that can complement or substitute traditional diesel fuel in engines. It has been already reported that by changing the fuel from conventional EN590 diesel to HVO decreases exhaust emissions. However, as the fuels have certain chemical and physical differences, it is clear that the full advantage of HVO cannot be realized unless the engine is optimized for the new fuel. In this article, we studied how much exhaust emissions can be reduced by adjusting engine parameters for HVO. The results indicate that, with all the studied loads (50%, 75%, and 100%), particulate mass and NO(x) can both be reduced over 25% by engine parameter adjustments. Further, the emission reduction was even higher when the target for adjusting engine parameters was to exclusively reduce either particulates or NO(x). In addition to particulate mass, different indicators of particulate emissions were also compared. These indicators included filter smoke number (FSN), total particle number, total particle surface area, and geometric mean diameter of the emitted particle size distribution. As a result of this comparison, a linear correlation between FSN and total particulate surface area at low FSN region was found.

Study of Miller timing on exhaust emissions of a hydrotreated vegetable oil (HVO)-fueled diesel engine.

The effect of intake valve closure (IVC) timing by utilizing Miller cycle and start of injection (SOI) on particulate matter (PM), particle number and nitrogen oxide (NOx) emissions was studied with a hydrotreated vegetable oil (HVO)-fueled nonroad diesel engine. HVO-fueled engine emissions, including aldehyde and polyaromatic hydrocarbon (PAH) emissions, were also compared with those emitted with fossil EN590 diesel fuel. At the engine standard settings, particle number and NOx emissions decreased at all the studied load points (50%, 75%, and 100%) when the fuel was changed from EN590 to HVO. Adjusting IVC timing enabled a substantial decrease in NOx emission and combined with SOI timing adjustment somewhat smaller decrease in both NOx and particle emissions at IVC -50 and -70 degrees CA points. The HVO fuel decreased PAH emissions mainly due to the absence of aromatics. Aldehyde emissions were lower with the HVO fuel with medium (50%) load. At higher loads (75% and 100%), aldehyde emissions were slightly higher with the HVO fuel. However, the aldehyde emission levels were quite low, so no clear conclusions on the effect of fuel can be made. Overall, the study indicates that paraffinic HVO fuels are suitable for emission reduction with valve and injection timing adjustment and thus provide possibilities for engine manufacturers to meet the strictening emission limits.

Elemental analysis of single ambient aerosol particles using laser-induced breakdown spectroscopy.

Analysing the composition of aerosol particles is essential when studying their health effects, sources and atmospheric impacts. In many environments the relevant particles occur in very low concentrations, meaning that their analysis requires efficient single particle techniques. Here we introduce a novel method to analyse the elemental composition of single aerosol particles sampled directly from the aerosol phase using size amplification aided aerosol charging (SAAC), linear electrodynamic quadrupole (LEQ) and laser-induced breakdown spectroscopy. We present results of the charging and focusing efficiencies of the SAAC and of the LEQ, and a proof-of-concept of the analysis method. The proof-of-concept test series was conducted with particle diameters down to 300 nm, sampled directly from the aerosol phase. The method shows unprecedented performance for spectroscopic submicron particle analysis from arbitrarily low concentrations and has exceptional potential for a portable analysis platform for various applications in the field of aerosol research.

Effect of fuel injection pressure on a heavy-duty diesel engine nonvolatile particle emission.

The effects of the fuel injection pressure on a heavy-duty diesel engine exhaust particle emissions were studied. Nonvolatile particle size distributions and gaseous emissions were measured at steady-state engine conditions while the fuel injection pressure was changed. An increase in the injection pressure resulted in an increase in the nonvolatile nucleation mode (core) emission at medium and at high loads. At low loads, the core was not detected. Simultaneously, a decrease in soot mode number concentration and size and an increase in the soot mode distribution width were detected at all loads. Interestingly, the emission of the core was independent of the soot mode concentration at load conditions below 50%. Depending on engine load conditions, growth of the geometric mean diameter of the core mode was also detected with increasing injection pressure. The core mode emission and also the size of the mode increased with increasing NOx emission while the soot mode size and emission decreased simultaneously.

Effects of driving conditions on secondary aerosol formation from a GDI vehicle using an oxidation flow reactor.

A comprehensive study on the effects of photochemical aging on exhaust emissions from a vehicle equipped with a gasoline direct injection engine when operated over seven different driving cycles was assessed using an oxidation flow reactor. Both primary emissions and secondary aerosol production were measured over the Federal Test Procedure (FTP), LA92, New European Driving Cycle (NEDC), US06, and the Highway Fuel Economy Test (HWFET), as well as over two real-world cycles developed by the California Department of Transportation (Caltrans) mimicking typical highway driving conditions. We showed that the emissions of primary particles were largely depended on cold-start conditions and acceleration events. Secondary organic aerosol (SOA) formation also exhibited strong dependence on the cold-start cycles and correlated well with SOA precursor emissions (i.e., non-methane hydrocarbons, NMHC) during both cold-start and hot-start cycles (correlation coefficients 0.95-0.99), with overall emissions of ∼68-94 mg SOA per g NMHC. SOA formation significantly dropped during the hot-running phases of the cycles, with simultaneous increases in nitrate and ammonium formation as a result of the higher nitrogen oxide (NOx) and ammonia emissions. Our findings suggest that more SOA will be produced during congested, slow speed, and braking events in highways.

Can real-world diesel exhaust particle size distribution be reproduced in the laboratory? A critical review.

Real-world particulate emission measurements usually include a fresh nanoparticle mode called the nucleation mode. The formation of the nucleation mode during mixing, dilution, and cooling of diesel exhaust is discussed based on existing experimental and modeling data. The further evolution of the nucleation mode and the local dilution ratio within the vehicle exhaust is reviewed. The nucleation mode forms at low dilution ratios (< or = 10) and is fully formed at the dilution ratio of approximately 100. The findings of the studies comparing real-world and dynamometer measurements are reviewed. A qualitative agreement of nucleation mode formation is generally observed. The geometric mean diameter of the nucleation mode, measured on-road, is well reproduced in the laboratory. However, the number concentration of the nucleation mode is too low in the laboratory (by a factor of 2-10). Nevertheless, the trends are reproduced, including those caused by differences in vehicle speed and engine load, engine and aftertreatment technology, as well as fuel and lubricant composition.

Particulate emissions of a modern diesel passenger car under laboratory and real-world transient driving conditions.

Exhaust emissions from diesel vehicles are significant sources of air pollution. In this study, particle number emissions and size distributions of a modern Euro 5b -compliant diesel passenger car exhaust were measured under the NEDC and US06 standard cycles as well as during different transient driving cycles. The measurements were conducted on a chassis dynamometer; in addition, the transient cycles were repeated on-road by a chase method. Since the diesel particulate filter (DPF) removed practically all particles from the engine exhaust, it was by-passed during most of the measurements in order to determine effects of lubricant on the engine-out exhaust aerosol. Driving conditions and lubricant properties strongly affected exhaust emissions, especially the number emissions and volatility properties of particles. During acceleration and steady speeds particle emissions consisted of non-volatile soot particles mainly larger than ∼50 nm independently of the lubricant used. Instead, during engine motoring particle number size distribution was bimodal with the modes peaking at 10-20 nm and 100 nm. Thermal treatment indicated that the larger mode consisted of non-volatile particles, whereas the nanoparticles had a non-volatile core with volatile material condensed on the surfaces; approximately, 59-64% of the emitted nanoparticles evaporated. Since during engine braking the engine was not fueled, the origin of these particles is lubricant oil. The particle number emission factors over the different cycles varied from 1.0 × 1014 to 1.3 × 1015 #/km, and engine motoring related particle emissions contributed 12-65% of the total particle emissions. The results from the laboratory and on-road transient tests agreed well. According to authors' knowledge, high particle formation during engine braking under real-world driving conditions has not been reported from diesel passenger cars.