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Particulate Mass and Nonvolatile Particle Number Emissions from Marine Engines Using Low-Sulfur Fuels, Natural Gas, or Scrubbers
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  • Kati Lehtoranta*
    Kati Lehtoranta
    VTT Technical Research Centre of Finland, P.O. Box 1000, FI-02044 VTT, Finland
    *E-mail: [email protected]; phone: +358 407236703.
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    Orcidhttp://orcid.org/0000-0001-9822-2565
  • Päivi Aakko-Saksa
    Päivi Aakko-Saksa
    VTT Technical Research Centre of Finland, P.O. Box 1000, FI-02044 VTT, Finland
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  • Timo Murtonen
    Timo Murtonen
    VTT Technical Research Centre of Finland, P.O. Box 1000, FI-02044 VTT, Finland
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  • Hannu Vesala
    Hannu Vesala
    VTT Technical Research Centre of Finland, P.O. Box 1000, FI-02044 VTT, Finland
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  • Leonidas Ntziachristos
    Leonidas Ntziachristos
    Tampere University of Technology, P.O. Box 692, FI-33101 Tampere, Finland
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  • Topi Rönkkö
    Topi Rönkkö
    Tampere University of Technology, P.O. Box 692, FI-33101 Tampere, Finland
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    Panu Karjalainen
    Tampere University of Technology, P.O. Box 692, FI-33101 Tampere, Finland
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  • Niina Kuittinen
    Niina Kuittinen
    Tampere University of Technology, P.O. Box 692, FI-33101 Tampere, Finland
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  • Hilkka Timonen
    Hilkka Timonen
    Finnish Meteorological Institute, P.O. Box 503, FI-00101 Helsinki, Finland
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Environmental Science & Technology

Cite this: Environ. Sci. Technol. 2019, 53, 6, 3315–3322
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https://doi.org/10.1021/acs.est.8b05555
Published February 19, 2019

Copyright © 2019 American Chemical Society. This publication is licensed under CC-BY.

Abstract

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In order to meet stringent fuel sulfur limits, ships are increasingly utilizing new fuels or, alternatively, scrubbers to reduce sulfur emissions from the combustion of sulfur-rich heavy fuel oil. The effects of these methods on particle emissions are important, because particle emissions from shipping traffic are known to have both climatic and health effects. In this study, the effects of lower sulfur level liquid fuels, natural gas (NG), and exhaust scrubbers on particulate mass (PM) and nonvolatile particle number (PN greater than 23 nm) emissions were studied by measurements in laboratory tests and in use. The fuel change to lower sulfur level fuels or to NG and the use of scrubbers significantly decreased the PM emissions. However, this was not directly linked with nonvolatile PN emission reduction, which should be taken into consideration when discussing the health effects of emitted particles. The lowest PM and PN emissions were measured when utilizing NG as fuel, indicating that the use of NG could be one way to comply with up-coming regulations for inland waterway vessels. Low PN levels were associated with low elemental carbon. However, a simultaneously observed methane slip should be taken into consideration when evaluating the climatic impacts of NG-fueled engines.

Copyright © 2019 American Chemical Society

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This article published February 28, 2019 with an error in the abstract artwork. The correct file published March 6, 2019.

Introduction

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Shipping is a very efficient way of transporting goods, and currently the majority of global trade volume is transported by sea. Although significant reductions in emissions of terrestrial vehicle engines have been achieved because of a series of environmental regulations and subsequent implementation of emission control techniques over the years, marine vessel emissions have not been thoroughly addressed. As a result, their relative contribution to air pollution has increased during recent years. (1)
Container ships, bulk carriers, and oil tankers, with slow-speed 2-stroke engines, consumed approximately 74% of all marine fuels in 2015, whereas ships having medium-speed 4-stroke engines (like most cruise ships) consumed approximately 23%. (2) However, compared to containers and cargo vessels, cruise ship routes are generally nearer to coastlines, and these ships may spend more time at anchor or berthing, which can have a significant effect on local air quality.
Around 15% of global anthropogenic NOx and 5–8% of global SOx emissions can be attributed to shipping operations. (3−5) In response, the International Maritime Organization (IMO) has introduced specific regulations to reduce shipping emissions of both pollutants. NOx limits have been set at a global level with Tier I and II standards, whereas lower limits are applicable to ships constructed after 2016 (Tier III) in NOx emission control areas (NECA). Tier III leads to an increase in the use of emission control devices, the most important of which is selective catalytic reduction (SCR). The SCR system utilizes a catalyst and externally fed ammonia to reduce NOx emissions. Catalysts in ship applications are usually vanadium-based, and an aqueous solution of urea is utilized as a source of ammonia (see, for example refs (6and7)).
In order to address SOx emissions, a global cap in fuel sulfur content (FSC) of marine fuels has been set at 0.5% m/m by 2020, compared to earlier permitted FSC levels of up to 3.5% m/m. In SOx emission control areas (SECA), the FSC is further limited to 0.1%. Higher sulfur levels are applicable only if an on-board sulfur scrubber is used. Different types of SOx scrubbers use fresh water (closed loop), seawater (open loop), a hybrid technology (either fresh or seawater), or dry removal agents. Alternatively, distillate fuels (ISO 8217), alcohols and biofuels, or gaseous fuels, primarily liquefied natural gas (LNG) with inherently low FSC, may be used for compliance with sulfur regulations. Of the distillate fuels, marine gas oil (MGO, free from residual fuel) is primarily used in marine engines with displacement less than 5 L per cylinder, whereas marine diesel oil (MDO, may have traces of residual fuel) is typically used in engines with greater than 5 L per cylinder. In addition, low sulfur residual marine fuel oils (also called hybrid fuels) may be utilized in ships operating in SECAs.
The IMO has not defined explicit emission limits for PM, despite its environmental and health implications. Shipping PM emissions are important especially in Asia, with China having 7 of the 10 largest ports in the world in terms of volume of transported goods. (8) Liu et al. (9) recently showed that during ship plume-influenced periods, shipping emissions contributed up to 20–30% of total PM2.5 within tens of kilometers of the coastal and riverside Shanghai regions. Chen et al. (10) estimated that the contribution of shipping emissions to ambient PM2.5 concentrations over the urban area of Qingdao could exceed 20%. Corbett et al. (5) estimated that on a global scale, shipping-related PM emissions are annually responsible for approximately 60 000 premature deaths related to cardiopulmonary and lung cancer diseases. Sofiev et al. (11) recently estimated that total premature mortality due to shipping is much higher, and that even low-sulfur marine fuels still account for approximately 250 000 deaths annually. SOx regulations also have an implicit impact on PM, because they lead to decreased particulate sulfate emissions. A recent study by Sofiev et al. (11) showed that low-sulfur fuels may provide pollution health benefits but with a climate trade-off, because the reduction in sulfate in PM decreases the climatic cooling effects of the exhaust aerosol. Although sulfate aerosol has a cooling effect, absorbent black carbon (BC) emissions warm the atmosphere and are not explicitly dependent on the FSC. (12) BC deposition on ice and subsequent albedo change is especially important in the Arctic area, which has recently experienced an increase in shipping activity. (13)
The existing evidence discussed above suggests that global shipping PM emissions have a clear effect on climate, air pollution, and public health. PM emission levels are also significantly influenced by regulations addressing other pollutants. The present study provides evidence on how different options enabling ships to operate within SECAs affect the PM emissions of marine engines. The options examined include lower sulfur level fuels (liquid and gaseous) as well as on-board scrubbers. Both the PM and nonvolatile PN emissions are studied in experiments conducted on board two different ships and in a marine engine laboratory.

Experimental Section

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Engines in Laboratory

Experiments with low-sulfur liquid fuels and natural gas were conducted in a marine engine laboratory. The first engine was a Wärtsilä Vasa 4R32, a four-cylinder medium-speed 4-stroke marine engine that was retrofitted to enable operation with natural gas in dual fuel (DF) mode. In this mode, a small quantity of liquid fuel is first injected to pilot combustion, which is then sustained by delivery of the main quantity of natural gas. The maximum power of this engine was 1400 kW. The engine was modified to run on natural gas in 2016, using state-of-the-art components of current commercial natural gas marine engines. The modification of the engine included, for example, installing gas admission valves on the cylinder heads and replacing the cylinder heads as well as the liners, pistons, camshaft, and turbocharger. In addition, the engine control system was updated and a pilot fuel line with a high-pressure pilot fuel pump was added. This engine was tested with the 40% and 85% loads that are considered representative of in-harbor maneuvering and open-seas operation, respectively. Emissions of PM and PN were also characterized from a second DF engine on the test bed. This was a 2017 production series Wärtsilä 20DF (medium speed, 4-stroke engine), which is of similar size to the 4R32 engine and delivers a maximum power output of 1000 kW.

Engines and Scrubbers on Board

Emission measurements were also made on board two ships during regular cruising conditions. A modern cruise ship equipped with SCR and a hybrid sulfur scrubber was first tested. The hybrid scrubber used closed loop scrubbing during harbor operation, whereas seawater scrubbing was used on the open sea. PM and PN emissions were measured from two main engines (E1 and E2) at constant engine loads of 40% and 75%. Both engines were medium-speed, 4-stroke, modern engines. For E1, the measurements were made upstream (engine outlet) and downstream of the scrubber. The E2 engine was equipped with the SCR placed upstream of the scrubber, so the measurement points were downstream of the scrubber and downstream of the SCR, before the scrubber. The second ship was a RoPax vessel (built for freight vehicle transport along with passenger accommodation) equipped with a diesel oxidation catalyst (DOC) and an open loop seawater-operating scrubber. PM and PN from one of its main engines (a medium-speed, 4-stroke engine, E3) were measured upstream of the scrubber (thus downstream of the DOC) and downstream of the scrubber. The ship operated normally, and the engine load varied during the cruise mainly in the range of 63–66% of maximum load. A schematic layout of all tested engines and related after-treatment is presented in the Supporting Information (Figure S1).

Fuels

Table 1 contains the main specifications of all liquid fuels used in the measurement campaigns. Two different liquid fuels (MDO and MGO) were used in the laboratory experiments with the Wärtsilä Vasa 4R32 engine when operated in liquid-fuel mode. The MDO had an FSC of 0.0822% and thus fulfilled the SECA requirements (limit 0.1% S), whereas the MGO was of even higher quality (on-road diesel quality, EN 590), with a very low sulfur level. High-quality MGO with a very low sulfur level is not widely utilized in ships today, but it was selected here based more on its role as a pilot in DF mode. In DF mode, the main fuel was compressed natural gas (CNG) and the pilot injection was with MGO according to the engine manufacturer’s instruction. The CNG had a high methane content (volumetric composition: 96.4% methane, 2.3% ethane, 0.35% propane, 0.15% other hydrocarbons, 0.57% nitrogen, and 0.21% carbon dioxide). In DF mode, the pilot fuel quantity was adjusted to 1.2% and 3.8% of the total fuel mass flow for 85% and 40% loads, respectively. LNG was used as the main fuel in the 20DF engine, because there was no natural gas distribution system available for that engine. The LNG used contained 90% methane and approximately 9% ethane. MGO was also used as pilot in this case, with an amount of approximately 2% of the total fuel mass flow for 75% engine load.
Table 1. Main Specifications of Liquid Fuels Used in the Measurement Campaigns
parameterunitMGO <0.001% SMDO <0.1% SHFO <0.7% SMGO <0.1% SHFO <2% S
use engine test bedcruise shipRoPax
engine 4R32 and 20DF4R32E1 and E2E2E3
density (15 °C)kg/m3836879873873984
viscosity (40 °C)mm2/s2.944.078863.87625
heating value, lowerMJ/kg42.842.240.842.040.5
flash point°C667814681109
sulfurmg/kg6.1822652078018600
ash% (m/m)<0.005<0.005<0.005<0.0050.165
carbon% (m/m)86.287.487.787.986.6
hydrogen% (m/m)13.912.511.512.810.7
nitrogenmg/kg40.63672490 5400
Nimg/kg<0.50<0.5012.4<0.5021.1
Vmg/kg<0.50<0.5017.2<0.50110
The cruise ship, equipped with a scrubber to meet SECA requirements, operated on heavy-fuel oil (HFO) with 0.65% sulfur content as a fuel (in all its engines). For comparison, the E2 engine was also operated on 0.10% FSC MGO for a period of 9 h with 40% load to conduct emission measurements. The RoPax ship operated on 1.9% FSC HFO.

Sampling and Analysis

Exhaust PM was sampled according to the ISO Standard 8178-1:2006, using an AVL Smart Sampler (or with a consistent in-house sampling system which was utilized in the case of the RoPax ship) that draws up and dilutes a sample of the exhaust flow. This is also the method specified for PM emissions sampling from inland waterway vessels in the EU, the only category of vessels for which PM regulations exist. According to this standard, PM is quantified as the mass of any material collected on a filter after diluting exhaust gas with clean, filtered air to a temperature greater than 42 °C and less than or equal to 52 °C, as measured at a point immediately upstream of the filter. The standard also defines a minimum dilution ratio of 4:1, but no maximum, before PM sampling is conducted. A schematic figure of the PM sampling system can be found in the Supporting Information (Figure S2). Smart Sampler and the in-house sampling system both had a flow-based control system for the dilution ratio. The correct filter temperature was achieved by heating the dilution air and placing the filter holders inside a heated cabinet. In the post scrubber measurements, a heated measurement probe and heated transfer line were utilized prior to the dilution tunnel.
Because the dilution ratio variation can result in significant changes in PM, (14,15) the dilution ratio was kept constant during the measurements, in addition to what the standard prescribed. We selected a DR of 10:1, which already significantly decreases the sensitivity of semivolatile material condensation while at the same time minimizing sampling duration. This is also in the same range as used for exhaust PM of on-road vehicles (16) and provides a common reference for comparing vehicle and vessel PM levels. Samples were collected on TX40HI20-WW filters (Ø 47 mm), with collection times ranging from 5 to 30 min. Measurements were repeated five times for each measurement point.
The concentrations of sulfate, organic carbon (OC), and elemental carbon (EC) were analyzed from the PM filter samples. Sulfate concentration was determined by electrophoresis from water and isopropanol mixture extracts. The OC/EC samples were collected on quartz filters, and the analysis was performed by the thermal-optical method. (17) Sunset Laboratories Inc.’s OC/EC analyzer mode 4L was used, and following ref (18), the EUSAAR2 temperature program was applied.
The PN measurement method used in this study originates from the Particle Measurement Programme (PMP) work and considers only nonvolatile particles with a diameter greater than 23 nm. This method is also mandated by the upcoming Stage V regulation for inland waterway vessels in 2020, which requires compliance with a nonvolatile PN limit. A Dekati Engine Exhaust Diluter (DEED) was used for PN sample conditioning in the current study. The system consists of two ejector diluters, providing a total dilution ratio of 100:1 in the case of NG fuel and 1000:1 in the case of diesel fuels, and an evaporation tube between the two dilution units (see Figure S1 in the Supporting Information). The temperature of the first ejector was ∼200 °C, and the temperature at the outlet of the DEED unit was below 35 °C. PN>23nm concentrations were determined with an Airmodus A23 Condensation Particle Counter (CPC). The DR setting in the case of nonvolatile PN sampling is much less critical than in the case of PM mass because of the elimination of condensation dynamics in the former case. The relatively high DR, which is recommended for road vehicles, was also adopted in this study to decrease coagulation dynamics and the corresponding PN concentration sensitivity to residence time before counting. (19) The DR setting would be even less relevant if nonvolatile PM rather than PN was to be characterized, as in the case of jet exhaust sampling, where DRs as low as 10 are being implemented. (20)
The concentrations of NOx (NO and NO2) in exhaust emissions were measured with a chemiluminescence detector (CLD), and carbon monoxide (CO) and carbon dioxide (CO2) were measured with a nondispersive infrared (NDIR) analyzer. Light hydrocarbon components were speciated with a gas chromatograph when natural gas was used as a fuel. A flame ionization detector (FID) was utilized in some of the tests to measure the total hydrocarbon (THC) content in the exhaust. Concentrations of sulfur dioxide (SO2) and water were measured with Fourier transform infrared spectroscopy (FTIR).

Results and Discussion

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PM and PN Emissions

Liquid Fuels

HFO was the fuel of choice for the majority of shipping operations before the global sulfur cap enforcement. In addition to high FSC, this fuel may contain large amounts of metals, such as V and Ni, and other ash components, compared to distillate fuels that contain practically no metals or ash (Table 1). Earlier experiments performed on the same Vasa 4R32 engine used in the current study demonstrated that marine engine PM emissions depend heavily on fuel quality. At 75% load, PM decreased from 850 mg/kWh, when using 2.5% FSC HFO, to 280 mg/kWh with 1% FSC HFO, (12) and down to 60 mg/kWh when using a light fuel oil (similar to MGO in the present study). (14)
The present results confirm previous evidence. Figure 1a presents PM emissions of the two laboratory engines fueled with NG, MDO, and MGO on the test bed. PM with MGO at 85% load was at a level similar to what has been measured previously at 75% load. (14) Earlier evidence using HFO has shown that sulfate and associated water comprise more than half of total PM. (12,21) With the lighter fuels used in the present study, sulfate accounted for only a minor fraction of total PM (Figure 1b); even in the case of MDO, the sulfate comprised only 4% of the total PM in the 85% load case. EC (18–19% of total PM) and OC (60–63% of PM) comprised the majority of PM for MDO and MGO. The “rest” PM fractions were calculated by subtracting the EC, OC, and sulfate amounts from the total PM. This rest fraction was not further specified in the present study, but typically it comprises water as well as fuel and lube-derived ash.

Figure 1

Figure 1. (a) PM and (c) nonvolatile PN>23nm emissions measured from 40% load mode and 85% load mode with the 4R32 DF engine utilizing MDO, MGO, and NG fuels and from 75% load with the 20DF engine utilizing MGO and LNG fuels (marked load 75% p). Error bars show the standard deviation of a minimum of five measurements. (b) PM composition of exhaust of the 4R32 DF engine fueled with MDO, MGO, and NG at 85% load.

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The particle emission results also show that the MGO produced 17–25% less PM than the MDO, but without any measurable effects on PN>23nm (see Figure 1c). Other studies (e.g., refs (21−24)) concluded that liquid fuel change has the potential to decrease particle emissions from ships, although they also concluded that such reductions are not only due to FSC reduction. Additionally, even if reduced sulfur content of the fuel efficiently reduced the PM emission, the BC emissions were not necessarily reduced. (12) Khan et al. (22) and Zetterdahl et al. (23) both compared emissions of HFO (higher S) to a lower sulfur level fuel. They both observed significant reductions in PM mass when changing to lower sulfur content fuel. Zetterdahl et al. observed 67% reduction in PM mass and smaller average particle size when changing to low sulfur level fuel, but the total particle number was found to be on similar levels for both fuels. In the present study, we also showed a PM decrease with fuel sulfur decrease, although no difference was found in the PN level.

Effect of Engine Load

Engine load was found to affect the work-specific PM emissions for the laboratory engine 4R32. PM emissions at low load (40%) were higher than when the load was increased, with all of the fuels used. Emission rates at low load were also more variable than at higher load, as indicated by the error bars in Figure 1a. In DF operation, the quantity of liquid fuel used per unit of energy was higher at low load (3.8% of main fuel) compared to high load (1.2% of main fuel), which may have contributed to the higher energy-specific PM emissions at low load. Marine engines are generally optimized for loads in the 75–90% range, which is the typical operation range for open-seas sailing. In ports, low loads are required for maneuvering and for berthing. Although in-port emissions make only a small contribution to the total emissions of any vessel, they are important for local air quality and associated health effects on populations in the vicinity of ports. (25) This means that any future regulation initiatives on PM emissions control from ships will require that emissions are also regulated at low-load operation.

Natural Gas

DF operation (with NG as main fuel) resulted in the lowest PM levels for both engines, at a level 63–69% lower than the MGO and 72–75% lower than the MDO. When shifting to DF operation, only traces of EC were observed and OC accounted for 83% of PM (Figure 1b). The impact of NG use was actually magnified when nonvolatile PN>23nm was considered, with PN levels 98–99% lower than when using liquid fuels (Figure 1c). Particles in this size range are often assumed to represent the soot mode that accounts for the major part of EC. The observed low PN>23nm for NG is consistent with the very low levels of EC measured for this particular fuel. The low soot emissions with NG also explain why changes in the load when in DF mode (85% load compared to 40% load with the 4R32 engine, Figure 1c) had practically no effect on the nonvolatile particle number, which is different from what is observed with liquid fuels.
Differences under DF mode are observed when comparing the retrofitted engine with the production-series engines; the latter were significantly lower in terms of both PM and PN>23nm emissions than the retrofitted engine. In addition to the impact of engine design, load level, and NG composition differences between the two engines, the lubricating oil might be a significant contributor to the observed differences, as observed in previous studies. (26−29) The two engines operated with lubricating oils of different specifications and, presumably, different consumption rates, although lubrication oil consumption was not measured in any of the engines. There were also differences in the pilot fuel amounts (i.e., 2% pilot fuel injection at 75% load of the production series engines compared to the 1.2% ratio used at 85% load of the retrofitted engine), but these do not provide an explanation for the observed lower PN>23nm emissions of the production engine.

PN>23nm Discussion

The level of PN>23nm emissions from marine engines is important in view of the upcoming EU regulations for inland waterway vessels. The Stage V regulation, applicable from 2020 on, has introduced the requirement of PN>23nm remaining below 1012 kWh–1 over a testing procedure involving several steady-state modes and weighing factors. Although we have not tested the complete range of conditions required by the regulation, the orders of magnitude of PN collected are indicative of the potential of different technology options.
PN>23nm emissions were well beyond the limit with all of the tested liquid fuels, almost 2 orders of magnitude or higher than the limit, with both engines tested. The retrofitted engine (with NG as the main fuel) produced 1.1 × 1012 kWh–1 and 1.0 × 1012 kWh–1 at 85% and 40% load, respectively, thus being within the range of regulatory requirements. The PN>23nm emissions of the production-series engine at 75% load with LNG was 1.3 × 1011 kWh–1, which was actually much lower than the limit (1012 kWh–1). These results indicate that the use of natural gas as a fuel for marine and inland waterway vessels could be one way to comply with upcoming regulations. The low nonvolatile PN>23nm level is also associated with low EC concentration (seen Figure 1). This strongly indicates that the regulation of PN>23nm may also be effective in controlling EC (and, correspondingly, BC) emissions of vessels and may thus contribute to decreasing the shipping impact on climate forcing. Figure 1c shows that light liquid fuel effects on PN>23nm were more marginal.
The observations related to fuel effects on PN>23nm emissions in this study refer to nonvolatile particles above 23 nm in size and could be different if smaller particles and/or semivolatile particles were included in the analysis. Anderson et al. (28) studied total particle emissions from an LNG-powered ship and also observed that LNG resulted in significantly lower PN numbers than when MGO was used. However, they also found that a significant fraction of particles were in the sub-23 nm size range. Alanen et al. (29) observed a remarkable amount of sub-23 nm nanoparticles with diameters down to only a few nanometers when using NG. Marine exhaust PN conclusions should therefore be observed carefully in relation to the particle population to which they refer.

Scrubbers on Board

The results of PM and PN>23nm measurements conducted on board the two different ships are presented in Figure 2. The PM level from the E3 engine (RoPax ship) during regular vessel operation with the engine load varying between 63% and 66% was the highest. In this case, the FSC of the HFO used was significantly higher than that of the HFO used on the cruise ship (engines E1 and E2). Operation of the scrubber was found to decrease the PM level by 21–45% in the high load cases (E1, E2, and E3, loads 63–66% and 75%) and 8–17% at low load (40%, E1 and E2). The PM composition analysis (Figure 2b) showed that the organic carbon was reduced by the scrubber. Interestingly, sulfate aerosol was at the same level both upstream and downstream of the scrubber, whereas EC seemed to be decreased by passage over the scrubber. The “rest” part of PM (consisting typically of sulfate-associated water and ash) was almost halved by the scrubber.

Figure 2

Figure 2. (a) PM and (c) nonvolatile PN>23nm emissions measured on board two different ships (i.e., engines E1 and E2 on a cruise ship and E3 on a RoPax). (b) PM composition from measurements made on engine E1 at 75% load. Note: In the case of engine E3, the HFO differed from the HFO utilized with engines E2 and E1 (see Table 1).

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The impact of the scrubber on PM emitted from the E1 and E2 engines was different, despite the fact that both engines were on the same ship and utilizing the same scrubber. One reason for this is that sampling from the E2 was conducted downstream of the SCR to which the engine was connected. First, the SCR by itself was most probably having a positive impact on PM emissions. The SCR system has been shown to have an impact on PM, for example, by decreasing the organic fraction. (6) The additional benefit that the scrubber can offer is therefore lower than the improvement it offers over engine-out PM emissions.
Even though PM clearly decreased over the scrubber, its effect on the nonvolatile PN was less clear. In the case of E1, the PM decrease was 41% in 75% load mode, whereas there was practically no change in the PN>23nm level. On the other hand, in the case of E2 and 75% load, the PM decrease was 21% and the PN>23nm decrease was observed to be 30%. However, bearing in mind that the standard deviation for PN measurements made in the laboratory (with MDO fuel) was ±15–18%, this PN decrease is considered to be minor.
Use of MGO in engine E2 led to lower PM and PN>23nm concentrations than were observed downstream of the scrubber with HFO fuel. However, this is only one example (one MGO fuel, one engine, and one load mode) and cannot be presented as a general conclusion.
Fridell and Salo (30) also studied the particle emissions from a marine engine equipped with a scrubber (open-loop wet scrubber using seawater). They found the total number of particles to be reduced by 92% in the scrubber, while the solid fraction was reduced by 48%. The PM was also significantly decreased; that is, about 75% of the total PM was captured by the scrubber. These are all higher reduction values than in the present study, and there might be several reasons for this, for example, differences in engines, fuels, and/or scrubbers. Moreover, one big difference is the particle measurement method. Fridell and Salo measured the PN with an engine exhaust particle sizer with a size range of 5.6–560 nm therefore also covering particles below 23 nm size, which were not measured in the present study. Several studies performed with liquid fuels report particle size distributions from marine engines suggesting that a share of nonvolatile PN resides below the 23 nm level. (28,31−33) In addition to the PN 23 nm limit, the results of Ntziachristos et al. (14,21) show that even when conducted following the ISO 8178 protocol, the dilution system can have a significant effect on the measured PM result. At minimum, the dilution ratio range allowed should be more strictly defined in order to obtain comparable results.
To the authors’ knowledge, the standard PM and nonvolatile PN measurement methods were utilized for the first time in the present study in studying ship emissions with different fuels and after-treatment systems. Furthermore, the dilution conditions were strictly controlled in order to make comparison of the results of different measurement campaigns possible both on board and in engine laboratories.

Gaseous Exhaust Emissions

Liquid Fuels and Natural Gas

With the laboratory engine (4R32), gaseous emissions were also studied (Table 2). Lower levels of NOx were measured with NG compared to MGO or MDO. This was most probably due to the homogeneous premixing of the gas with air and the lower combustion temperature of NG (in lean burn conditions). As expected, no SO2 was detected in the exhaust gas when utilizing either NG or MGO (<0.001% S). The assumption that all the sulfur in fuel and lubricating oil ends up in SO2 in the exhaust results in below 2 ppm in the MGO case and even less in the NG case. With the FTIR, it is possible to measure accurately only levels above 2 ppm.
Table 2. Gaseous Emissions Measured from the Marine Laboratory Engine 4R32a
fuelload (%)NOx (g/kWh)SO2 (g/kWh)CO2 (g/kWh)CO (g/kWh)THC (g/kWh)CH4 (g/kWh)C2H6 (g/kWh)C3H8 (g/kWh)
natural gas852.7bd420.01.7–5.60.240.05
 403.6bd484.33.8–13.80.620.05
MGO859.0bd582.20.30.4bdbdbd
 4010.1bd645.80.80.5bdbdbd
MDO8510.00.31611.10.40.3bdbdbd
 4011.20.35639.10.80.4bdbdbd
a

bd, below detection limit; −, no measurement. The detection limit for CH4 was 10 ppm, and for C2H6, C3H8, and SO2, the detection limit was 2 ppm.

Compared to diesel fuels the CO2 emission was lower with NG use, which is because NG is mainly composed of methane, with a higher hydrogen-to-carbon (H/C) ratio compared to diesel. The carbon monoxide and hydrocarbon emissions, on the other hand, were higher with the NG compared to diesel fuels. These results are in line with those of other studies. (28,34−36) CO and hydrocarbon emission levels were found to depend largely on engine load; higher levels were measured at lower loads of 40%.
Because natural gas is mainly composed of methane, one could expect to have some methane emissions if small quantities of gas escape from the combustion process. This was found to be true in the present study. In addition to methane, smaller quantities of ethane and propane were also found from the engine exhaust when running on natural gas (see Table 2). No methane, ethane, or propane were detected from the engine exhaust when running on MGO or MDO. However, the measured total hydrocarbon emission was 0.3–0.5 g/kWh when running on MGO and MDO, probably consisting only of longer chain hydrocarbon components.
Because methane is a greenhouse gas, its emissions should be minimized. The methane emission levels measured in the present study were relatively high, and it should be noted that these might not be typical values for the modern DF engines in production today. The measured methane levels were also higher than previously measured on board an LNG ship. (28) The difference between these two studies could be due to the different engine sizes. The engine on board was a 7600 kW engine with a larger cylinder and lower speed, meaning that there was more time for the combustion compared to the engine of the present study. In addition, the combustion chamber design was probably different, resulting in differences in the NG amounts escaping the cylinder. According to refs (37and38), methane emissions could be reduced, for example, by better fuel mixing conditions, by improvements in combustion chamber design, and by reducing crevices. One option could also be the use of oxidation catalysts, but further research is needed to solve the long-term performance of methane catalysts.
Natural gas is a flexible and cost-effective way to support the decarbonization of transport and to tackle air quality issues. The low levels of PM and PN measured in the present study also support the use of NG. However, as shown in the study, there is also a challenge with methane slip, which needs to be solved in order not to compromise the climate benefit gained from the CO2 decrease. If available, biogas would be one possible attractive fuel in future marine engines aiming to reduce greenhouse gas emissions by 50% by 2050, as presented recently by IMO.

Scrubbers on Board

The NOx levels were found to be significantly lower with the E2 engine than with the E1 engine of the same ship (or E3 in the other ship) (Table 3). The E2 engine was equipped with SCR, which explains this difference. The somewhat higher CO levels from the E2 engine could also be influenced by the SCR, because CO has been found to increase in SCR-equipped applications because of thermal decomposition of urea and/or partial oxidation of HC compounds over the catalyst. (39)
Table 3. Gaseous Emissions Measured on Board Downstream of Scrubbers and with MGO without a Scrubber
shipfuelengine and after-treatmentload (%)NOx (g/kWh)SO2 (g/kWh)CO2 (g/kWh)CO (g/kWh)
cruiseHFOE1 + scrubber7511.40.0336200.34
   4019.50.0196530.61
cruiseHFOE2 + SCR + scrubber751.20.0066270.56
   4050.0136500.94
cruiseMGOE2 + SCR404.30.3276471.44
RoPaxHFOE3 + scrubber63–66150.075440.16
The SO2 level measured from engine E2 with MGO fuel (fulfilling the SECA limitations with 780 ppm of S level) was 0.327 g/kWh at 40% engine load. In the same mode, the SO2 level measured downstream of the scrubber (HFO fuel) was remarkably lower, resulting in a level of 0.013 g/kWh (see Table 3). Furthermore, in the case of the E3 engine, a very low level of SO2 of 0.07 g/kWh was observed downstream of the scrubber when utilizing HFO with FSC of 1.9%. As a reference, FSC should be well below 0.02% in order to maintain the theoretical SO2 output below 0.07 g/kWh, meaning an SO2 level 2 orders of magnitude lower compared to the 1.9% S HFO fuel utilization (without any scrubber). The theoretical value is based on the assumption that all the sulfur from the fuel ends up as SO2 in the exhaust. These results confirm that the scrubber was working effectively in decreasing the SOx level, as intended. The lower PM levels measured with scrubbers in the present study also favor the utilization of scrubbers, but the effect of a scrubber on PN was not straightforward. With the growing trend in utilization of scrubbers, further studies are needed to clarify their effects on particle number and size, especially when discussing the health impacts of ship emissions.

Supporting Information

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.8b05555.

  • Schematic of the layout of all engines tested on the engine test bed and on board (Figure S1) and PM measurement system according to ISO8178:2006 and the “PMP” PN (nonvolatiles >23) measurement system (Figure S2) (PDF)

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Author Information

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  • Corresponding Author
  • Authors
    • Päivi Aakko-Saksa - VTT Technical Research Centre of Finland, P.O. Box 1000, FI-02044 VTT, Finland
    • Timo Murtonen - VTT Technical Research Centre of Finland, P.O. Box 1000, FI-02044 VTT, Finland
    • Hannu Vesala - VTT Technical Research Centre of Finland, P.O. Box 1000, FI-02044 VTT, Finland
    • Leonidas Ntziachristos - Tampere University of Technology, P.O. Box 692, FI-33101 Tampere, Finland
    • Topi Rönkkö - Tampere University of Technology, P.O. Box 692, FI-33101 Tampere, Finland
    • Panu Karjalainen - Tampere University of Technology, P.O. Box 692, FI-33101 Tampere, Finland
    • Niina Kuittinen - Tampere University of Technology, P.O. Box 692, FI-33101 Tampere, Finland
    • Hilkka Timonen - Finnish Meteorological Institute, P.O. Box 503, FI-00101 Helsinki, Finland
  • Notes
    The authors declare no competing financial interest.

Acknowledgments

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This study was part of several projects: HERE, SEA-EFFECTS BC, and INTENS, funded by Business Finland and several Finnish companies, and Hercules-2 with funding from the European Union’s Horizon 2020 research and innovation programme under Grant Agreement No. 634135.

References

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    Fuel (2016), 186 (), 456-465CODEN: FUELAC; ISSN:0016-2361. (Elsevier Ltd.)
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    Emissions were measured on-board a ship in the Baltic Sea, which is a sulfur emission control area (SECA), before and after the implementation of the strict fuel sulfur content (FSC) limit of 0.1 m/m% S on the 1st of Jan. 2015. Prior to Jan. 2015, the ship used a heavy fuel oil (HFO) but switched to a low-sulfur residual marine fuel oil (RMB30) after the implementation of the new FSC limit. The emitted particulate matter (PM) was measured in terms of mass, no., size distribution, volatility, elemental compn., content of orgs., black and elemental carbon, polycyclic arom. hydrocarbons (PAHs), microstructure and micro-compn., along with the gaseous emissions at different operating conditions. The fuel change reduced emissions of PM mass up to 67%. The no. of particles emitted remained unchanged and were dominated by nanoparticles. Furthermore, the fuel change resulted in an 80% redn. of SO2 emissions and decreased emissions of total volatile org. compds. (VOCs). The emissions of both monoarom. and lighter polyarom. hydrocarbon compds. increased with RMB30, while the heavy, PM-bound PAH species that belong to the carcinogenic PAH family were reduced. Emissions of BC remained similar between the two fuels. This study indicates that the use of low-sulfur residual marine fuel oil is a way to comply with the new FSC regulation and will reduce the anthropogenic load of SO2 emissions and secondary PM formed from SO2. Emissions of primary particles, however, remain unchanged and do not decrease as much as would be expected if distd. fuel was used. This applies both to the no. of particles emitted and some toxic components, such as heavy metals, PAHs or elemental carbon (EC). The micro-compn. analyses showed that the soot particles emitted from RMB30 combustion often do not have any trace of sulfur compared with particles from HFO combustion, which always have a sulfur content over 1%m/m. The soot sulfur content can impact aging and cloud condensation properties. This study is an in-depth comparison of the impact of these two fuels on the emissions of particles as well as their compn. and microstructure. To evaluate the impact of the use of low-sulfur residual marine fuel oils on emissions from ships, addnl. research is needed to investigate the varied fuel types and compns. as well as the wide range of engine conditions and properties.
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    The particle size distribution, volatility, and effective d. of particulate matter emitted from a homogeneous charge compression ignition (HCCI) engine fueled by port injected compressed natural gas were measured and compared to emissions emitted from the same engine during motoring and spark ignition for two compression ratios. The particle concn. and geometric mean diam. were greater at high compression ratio, and also, the total particulate mass was lower for spark ignition and homogeneous charge compression ignition than during motoring. Volatility tests showed that all operating conditions have less than 5% of the particulate matter remaining when denuding the sample at 100 °C. Effective d. measurements also show that the particles for each operating mode have a relatively const. d. with respect to particle size (approx. 850 kg/m3).
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    Atmospheric Measurement Techniques (2014), 7 (1), 149-161CODEN: AMTTC2; ISSN:1867-8548. (Copernicus Publications)
    Four measurement campaigns were performed in two different environments - inside the harbor areas in the city center of Helsinki, and along the narrow shipping channel near the city of Turku, Finland - using a mobile lab. van during winter and summer conditions in 2010-2011. The characteristics of gaseous (CO, CO2, SO2, NO, NO2, NOx) and particulate (no. and vol. size distributions as well as PM2.5) emissions for 11 ships regularly operating on the Baltic Sea were studied to det. the emission parameters. The highest particle concns. were 1.5×106 and 1.6×105 cm-3 in Helsinki and Turku, resp., and the particle no. size distributions had two modes. The dominating mode peaked at 20-30 nm, and the accumulation mode at 80-100 nm. The majority of the particle mass was volatile, since after heating the sample to 265 °C, the particle vol. of the studied ship decreased by around 70 %. The emission factors for NOx varied in the range of 25-100 g (kg fuel)-1, for SO2 in the range of 2.5-17.0 g (kg fuel)-1, for particle no. in the range of (0.32-2.26)×1016 # (kg fuel)-1, and for PM2.5 between 1.0-4.9 g (kg fuel)-1. The ships equipped with SCR (selective catalytic redn.) had the lowest NOx emissions, whereas the ships with DWI (direct water injection) and HAMs (humid air motors) had the lowest SO2 emissions but the highest particulate emissions. For all ships, the averaged fuel sulfur contents (FSCs) were less than 1% (by mass) but none of them was below 0.1% which will be the new EU directive starting 1 Jan. 2015 in the SOx emission control areas; this indicates that ships operating on the Baltic Sea will face large challenges.
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    Amanatidis, S.; Ntziachristos, L.; Karjalainen, P.; Saukko, E.; Simonen, P.; Kuittinen, N.; Aakko-Saksa, P.; Timonen, H.; Rönkkö, T.; Keskinen, J. Comparative Performance of a Thermal Denuder and a Catalytic Stripper in Sampling Laboratory and Marine Exhaust Aerosols. Aerosol Sci. Technol. 2018, 52 (4), 420– 432,  DOI: 10.1080/02786826.2017.1422236
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    Comparative performance of a thermal denuder and a catalytic stripper in sampling laboratory and marine exhaust aerosols
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    Aerosol Science and Technology (2018), 52 (4), 420-432CODEN: ASTYDQ; ISSN:0278-6826. (Taylor & Francis, Inc.)
    The performance of a thermal denuder (thermodenuder-TD) and a fresh catalytic stripper (CS) was assessed by sampling lab. aerosol, produced by different combinations of sulfuric acid, octacosane, and soot particles, and marine exhaust aerosol produced by a medium-speed marine engine using high sulfur fuels. The intention was to study the efficiency in sepg. non-volatile particles. No particles could be detected downstream of either device when challenged with neat octacosane particles at high concn. Both lab. and marine exhaust aerosol measurements showed that sub-23 nm semi-volatile particles are formed downstream of the thermodenuder when upstream sulfuric acid approached 100 ppbv. Charge measurements revealed that these are formed by re-nucleation rather than incomplete evapn. of upstream aerosol. Sufficient diln. to control upstream sulfates concn. and moderate TD operation temp. (250°C) are both required to eliminate their formation. Use of the CS following an evapn. tube seemed to eliminate the risk for particle re-nucleation, even at a ten-fold higher concn. of semi-volatiles than in case of the TD. Particles detected downstream of the CS due to incomplete evapn. of sulfuric acid and octacosane aerosol, did not exceed 0.01% of upstream concn. Despite the superior performance of CS in sepg. non-volatile particles, the TD may still be useful in cases where increased sensitivity over the traditional evapn. tube method is needed and where high sulfur exhaust concn. may fast deplete the catalytic stripper adsorption capacity. 2018 American Assocn. for Aerosol Research.
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    A comprehensive comparison of emissions from vehicles fueled with diesel or compressed natural gas (CNG) was developed from 25 reports on transit and school buses, refuse trucks, and passenger cars. Emissions of most compds. were highest for untreated exhaust gas and lowest for treated exhaust gas. CNG buses without after-treatment had the highest CO, hydrocarbon, non-methane hydrocarbon, volatile org. compd. (e.g., benzene, butadiene, ethylene, etc.), and carbonyl compd. (e.g., formaldehyde, acetaldehyde, acrolein) emissions. Diesel buses without after-treatment had the highest particulate matter and polycyclic arom. hydrocarbon emissions. Exhaust after-treatment reduced most emissions to similar concns. in diesel and CNG buses. NOx and CO2 emissions were similar for most vehicle types, fuels, and exhaust after-treatment with some exceptions. Diesel school buses had higher CO2 emissions than CNG buses. CNG transit buses and passenger cars equipped with 3-way catalysts had lower NOx emissions. Diesel buses equipped with traps had higher NO2 emissions. Fuel economy was best in diesel buses not equipped with exhaust after-treatment.
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    Liu, J.; Yang, F.; Wang, H.; Ouyang, M.; Hao, S. Effects of Pilot Fuel Quantity on the Emissions Characteristics of a CNG/diesel Dual Fuel Engine with Optimized Pilot Injection Timing. Appl. Energy 2013, 110, 201– 206,  DOI: 10.1016/j.apenergy.2013.03.024
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    Applied Energy (2013), 110 (), 201-206CODEN: APENDX; ISSN:0306-2619. (Elsevier Ltd.)
    For CNG/diesel dual fuel engines, the effects of pilot fuel quantity and injection timing are noticeable and significant. In this study, the emission characteristics of a CNG-diesel dual fuel engine with different pilot diesel fuel quantity and optimized pilot injection timing were investigated. The CO emission levels under dual fuel mode are considerably higher than that under normal diesel operation modes even at high load, which indicated that there exist some flame extinction regions. Dual fuel mode reduces NOx emissions by 30% averagely in comparison to diesel mode. That is because most of the fuel is burned under lean premixed conditions which result in lower local temp. The unburned HC emissions under dual-fuel mode are obviously higher than that of the normal diesel mode, esp. at low to medium loads. And around 90% of the THC emissions were unburned methane, which means the flame does not propagate throughout the charge. THC emissions reduce significantly with the increase of the pilot diesel quantity. Thanks to the premixed nature of the combustion mode and the methane mol. structure, the PM emission is reduced obviously under dual fueling condition. The PM emission is increased with the increase of the pilot fuel quantity.
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Cite this: Environ. Sci. Technol. 2019, 53, 6, 3315–3322
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Published February 19, 2019

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  • Abstract

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    Figure 1

    Figure 1. (a) PM and (c) nonvolatile PN>23nm emissions measured from 40% load mode and 85% load mode with the 4R32 DF engine utilizing MDO, MGO, and NG fuels and from 75% load with the 20DF engine utilizing MGO and LNG fuels (marked load 75% p). Error bars show the standard deviation of a minimum of five measurements. (b) PM composition of exhaust of the 4R32 DF engine fueled with MDO, MGO, and NG at 85% load.

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    Figure 2

    Figure 2. (a) PM and (c) nonvolatile PN>23nm emissions measured on board two different ships (i.e., engines E1 and E2 on a cruise ship and E3 on a RoPax). (b) PM composition from measurements made on engine E1 at 75% load. Note: In the case of engine E3, the HFO differed from the HFO utilized with engines E2 and E1 (see Table 1).

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  • References

    This article references 39 other publications.

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      Impact of maritime transport emissions on coastal air quality in Europe
      Viana, Mar; Hammingh, Pieter; Colette, Augustin; Querol, Xavier; Degraeuwe, Bart; de Vlieger, Ina; van Aardenne, John
      Atmospheric Environment (2014), 90 (), 96-105CODEN: AENVEQ; ISSN:1352-2310. (Elsevier Ltd.)
      A review. Shipping emissions are currently increasing and will most likely continue to do so in the future due to the increase of global-scale trade. Ship emissions have the potential to contribute to air quality degrdn. in coastal areas, in addn. to contributing to global air pollution. With the aim to quantify the impacts of shipping emissions on urban air quality in coastal areas in Europe, an in depth literature review was carried out focussing on particulate matter and gaseous pollutants but also reviewing the main chem. tracers of shipping emissions, the particle size distribution of ship-derived particulates and their contributions to population exposure and atm. deposition. Mitigation strategies were also addressed. In European coastal areas, shipping emissions contribute with 1-7% of ambient air PM10 levels, 1-14% of PM2.5, and at least 11% of PM1. Contributions from shipping to ambient NO2 levels range between 7 and 24%, with the highest values being recorded in the Netherlands and Denmark. Impacts from shipping emissions on SO2 concns. were reported for Sweden and Spain. Shipping emissions impact not only the levels and compn. of particulate and gaseous pollutants, but may also enhance new particle formation processes in urban areas.
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      Viana, M.; Hammingh, P.; Colette, A.; Querol, X.; Degraeuwe, B.; de Vlieger, I.; van Aardenne, J. Impact of Maritime Transport Emissions on Coastal Air Quality in Europe. Atmos. Environ. 2014, 90, 96– 105,  DOI: 10.1016/j.atmosenv.2014.03.046
      3
      Impact of maritime transport emissions on coastal air quality in Europe
      Viana, Mar; Hammingh, Pieter; Colette, Augustin; Querol, Xavier; Degraeuwe, Bart; de Vlieger, Ina; van Aardenne, John
      Atmospheric Environment (2014), 90 (), 96-105CODEN: AENVEQ; ISSN:1352-2310. (Elsevier Ltd.)
      A review. Shipping emissions are currently increasing and will most likely continue to do so in the future due to the increase of global-scale trade. Ship emissions have the potential to contribute to air quality degrdn. in coastal areas, in addn. to contributing to global air pollution. With the aim to quantify the impacts of shipping emissions on urban air quality in coastal areas in Europe, an in depth literature review was carried out focussing on particulate matter and gaseous pollutants but also reviewing the main chem. tracers of shipping emissions, the particle size distribution of ship-derived particulates and their contributions to population exposure and atm. deposition. Mitigation strategies were also addressed. In European coastal areas, shipping emissions contribute with 1-7% of ambient air PM10 levels, 1-14% of PM2.5, and at least 11% of PM1. Contributions from shipping to ambient NO2 levels range between 7 and 24%, with the highest values being recorded in the Netherlands and Denmark. Impacts from shipping emissions on SO2 concns. were reported for Sweden and Spain. Shipping emissions impact not only the levels and compn. of particulate and gaseous pollutants, but may also enhance new particle formation processes in urban areas.
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      Corbett, J. J.; Winebrake, J. J.; Green, E. H.; Kasibhatla, P.; Eyring, V.; Lauer, A. Mortality from Ship Emissions: A Global Assessment. Environ. Sci. Technol. 2007, 41 (24), 8512– 8518,  DOI: 10.1021/es071686z
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      Mortality from Ship Emissions: A Global Assessment
      Corbett, James J.; Winebrake, James J.; Green, Erin H.; Kasibhatla, Prasad; Eyring, Veronika; Lauer, Axel
      Environmental Science & Technology (2007), 41 (24), 8512-8518CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Epidemiol. studies consistently link ambient particulate matter (PM) concns. to neg. health impacts, including asthma, heart attack, hospital admission, and premature mortality. The authors modeled ambient PM concns. from ocean-going ships using 2 geo-spatial emissions inventories and 2 global aerosol models. Global and regional mortalities were estd. by applying ambient PM increases due to ship emissions to cardiopulmonary and lung cancer concn.-risk functions and population models. Results indicated shipping-related PM emissions are responsible for ∼60,000 cardiopulmonary and lung cancer deaths annually; most deaths occurred near coastlines in Europe and East and South Asia. Under current regulation and with the expected growth in shipping activity, the authors est. annual mortalities could increase by 40% by 2012.
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      Lehtoranta, K.; Vesala, H.; Koponen, P.; Korhonen, S. Selective Catalytic Reduction Operation with Heavy Fuel Oil: NO X NH 3 and Particle Emissions. Environ. Sci. Technol. 2015, 49 (7), 4735– 4741,  DOI: 10.1021/es506185x
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      Magnusson, M.; Fridell, E.; Ingelsten, H. H. The Influence of Sulfur Dioxide and Water on the Performance of a Marine SCR Catalyst. Appl. Catal., B 2012, 111–112, 20– 26,  DOI: 10.1016/j.apcatb.2011.09.010
      7
      The influence of sulfur dioxide and water on the performance of a marine SCR catalyst
      Magnusson, Mathias; Fridell, Erik; Ingelsten, Hanna H.
      Applied Catalysis, B: Environmental (2012), 111-112 (), 20-26CODEN: ACBEE3; ISSN:0926-3373. (Elsevier B.V.)
      This work assessed how S affects NOx redn. over a com. V-based urea selective catalytic redn. (SCR) catalyst for marine applications, particularly at low temps. and in conjunction with water. Adding SO2 in the absence of water promoted NOx redn. at 350°; adding water in the absence of SO2 decreased NOx redn. and inhibited N2O formation. The same trends were obsd. at transient temps., but no SO2 promotional effect was obsd. at temps. <230°. The long term effect of SO2 and water was assessed and NOx redn. remained stable, also after long-term SO2 exposure. NH3 desorption was examd. in temp.-programmed desorption expts. in the presence and absence of SO2. Generally, in the presence of water and SO2, the catalyst did not display any sign of deactivation at temps. >300° and fairly low space velocities (<12,200/h); however, at lower temps. (250°) and/or higher space velocities, catalytic performance for NOx redn. decreased over time.
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      Zhang, Y.; Yang, X.; Brown, R.; Yang, L.; Morawska, L.; Ristovski, Z.; Fu, Q.; Huang, C. Shipping Emissions and Their Impacts on Air Quality in China. Sci. Total Environ. 2017, 581–582, 186– 198,  DOI: 10.1016/j.scitotenv.2016.12.098
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      Shipping emissions and their impacts on air quality in China
      Zhang, Yan; Yang, Xin; Brown, Richard; Yang, Liping; Morawska, Lidia; Ristovski, Zoran; Fu, Qingyan; Huang, Cheng
      Science of the Total Environment (2017), 581-582 (), 186-198CODEN: STENDL; ISSN:0048-9697. (Elsevier B.V.)
      A review concerning the broad field of ship emissions in China and their atm. impacts is given, including ship engine emissions and control, ship emission factors and their measurements, development of ship emission inventories, shipping and port emissions of the main shipping areas, and quant. contribution of shipping emissions to local and regional air pollution. Topics covered include: introduction; overview of Chinese shipping and ports; ship emission factors and ship emission inventory (ship emission factors used, real-time measurement of in-ship emission, building ship emission inventory [vessel visa data, automatic identification system activity data]); overview of shipping and port emissions (Pearl River Delta [PRD], Yangtze River Delta [YRD], Bohai-Rim area and other regions); contribution of ship emission to local and regional air pollution (PRD, YRD, Bohai-Rim area and other regions); control of ship engine emissions (marine diesel oil and gas oil ship engines, heavy fuel oil engines, dual fuel engines); and summary.
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      Liu, Z.; Lu, X.; Feng, J.; Fan, Q.; Zhang, Y.; Yang, X. Influence of Ship Emissions on Urban Air Quality: A Comprehensive Study Using Highly Time-Resolved Online Measurements and Numerical Simulation in Shanghai. Environ. Sci. Technol. 2017, 51 (1), 202– 211,  DOI: 10.1021/acs.est.6b03834
      9
      Influence of Ship Emissions on Urban Air Quality: A Comprehensive Study Using Highly Time-Resolved Online Measurements and Numerical Simulation in Shanghai
      Liu, Zhanmin; Lu, Xiaohui; Feng, Junlan; Fan, Qianzhu; Zhang, Yan; Yang, Xin
      Environmental Science & Technology (2017), 51 (1), 202-211CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Shanghai, China, is an international shipping center. This work combined multi-year measurements and high resoln. air quality modeling results with hourly ship emission inventory to det. the effect of ship emissions on urban Shanghai. Aerosol time-of-flight mass spectrometer measurements were performed at an urban site from Apr. 2009 to Jan. 2013. During the sampling period, most of the half-hourly averaged no. fractions of primary ship-emitted particles were 1.0-10.0%; however, this no. fraction could be up to 50% for individual ship plume cases. Ship plume-affected periods usually occurred in spring and summer. Weather Research and Forecasting/Community Multiscale Air Quality model simulations in conjunction with the hourly ship emission inventory provided highly time-resolved concns. of ship-related air pollutants during a ship plume case. It showed ships could contribute 20-30% (2-7 μg/m3) of total PM2.5 within tens of kilometers of coastal and riverside Shanghai during ship plume-affected periods. Results showed ship emissions substantially contribute to air pollution in urban Shanghai. Ship emission control measures should be taken considering its neg. environment and human health effects.
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      Chen, D.; Wang, X.; Nelson, P.; Li, Y.; Zhao, N.; Zhao, Y.; Lang, J.; Zhou, Y.; Guo, X. Ship Emission Inventory and Its Impact on the PM2.5 Air Pollution in Qingdao Port, North China. Atmos. Environ. 2017, 166, 351– 361,  DOI: 10.1016/j.atmosenv.2017.07.021
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      Sofiev, M.; Winebrake, J. J.; Johansson, L.; Carr, E. W.; Prank, M.; Soares, J.; Vira, J.; Kouznetsov, R.; Jalkanen, J.-P.; Corbett, J. J. Cleaner Fuels for Ships Provide Public Health Benefits with Climate Tradeoffs. Nat. Commun. 2018, 9 (1), 406,  DOI: 10.1038/s41467-017-02774-9
      11
      Cleaner fuels for ships provide public health benefits with climate tradeoffs
      Sofiev Mikhail; Johansson Lasse; Prank Marje; Soares Joana; Vira Julius; Kouznetsov Rostislav; Jalkanen Jukka-Pekka; Winebrake James J; Carr Edward W; Corbett James J
      Nature communications (2018), 9 (1), 406 ISSN:.
      We evaluate public health and climate impacts of low-sulphur fuels in global shipping. Using high-resolution emissions inventories, integrated atmospheric models, and health risk functions, we assess ship-related PM2.5 pollution impacts in 2020 with and without the use of low-sulphur fuels. Cleaner marine fuels will reduce ship-related premature mortality and morbidity by 34 and 54%, respectively, representing a ~ 2.6% global reduction in PM2.5 cardiovascular and lung cancer deaths and a ~3.6% global reduction in childhood asthma. Despite these reductions, low-sulphur marine fuels will still account for ~250k deaths and ~6.4 M childhood asthma cases annually, and more stringent standards beyond 2020 may provide additional health benefits. Lower sulphur fuels also reduce radiative cooling from ship aerosols by ~80%, equating to a ~3% increase in current estimates of total anthropogenic forcing. Therefore, stronger international shipping policies may need to achieve climate and health targets by jointly reducing greenhouse gases and air pollution.
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    12. 12
      Aakko-Saksa, P.; Murtonen, T.; Vesala, H.; Koponen, P.; Nyyssönen, S.; Puustinen, H.; Lehtoranta, K.; Timonen, H.; Teinilä, K.; Karjalainen, P.; Black Carbon Measurements Using Different Marine Fuels. 28th CIMAC World Congress ; 2016; Paper 068.
      There is no corresponding record for this reference.
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      Winther, M.; Christensen, J.; Plejdrup, M.; Ravn, E.; Eriksson, O.; Kristensen, H. Emission Inventories for Ships in the Arctic Based on Satellite Sampled AIS Data. Atmos. Environ. 2014, 91, 1– 14,  DOI: 10.1016/j.atmosenv.2014.03.006
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    14. 14
      Ntziachristos, L.; Saukko, E.; Rönkkö, T.; Lehtoranta, K.; Timonen, H.; Hillamo, R.; Keskinen, J. Impact of Sampling Conditions and Procedure on Particulate Matter Emissions from a Marine Diesel Engine. 28th CIMAC World Congress ; 2016; Paper 165.
      There is no corresponding record for this reference.
    15. 15
      Ristimaki, J.; Hellen, G.; Lappi, M. Chemical and Physical Characterization of Exhaust Particulate Matter from a Marine Medium Speed Diesel Engine. 26th CIMAC World Congress ; 2010; Paper 73.
      There is no corresponding record for this reference.
    16. 16
      Giechaskiel, B.; Maricq, M.; Ntziachristos, L.; Dardiotis, C.; Wang, X.; Axmann, H.; Bergmann, A.; Schindler, W. Review of Motor Vehicle Particulate Emissions Sampling and Measurement: From Smoke and Filter Mass to Particle Number. J. Aerosol Sci. 2014, 67, 48– 86,  DOI: 10.1016/j.jaerosci.2013.09.003
      16
      Review of motor vehicle particulate emissions sampling and measurement: From smoke and filter mass to particle number
      Giechaskiel, Barouch; Maricq, Matti; Ntziachristos, Leonidas; Dardiotis, Christos; Wang, Xiaoliang; Axmann, Harald; Bergmann, Alexander; Schindler, Wolfgang
      Journal of Aerosol Science (2014), 67 (), 48-86CODEN: JALSB7; ISSN:0021-8502. (Elsevier Ltd.)
      A review. Particulate emissions from motor vehicles have received increased attention over the past two decades owing to assocns. obsd. between ambient particulate matter (PM) levels and health effects. This has led to numerous changes in emissions regulations worldwide, including more stringent stds., the broadening of these to include non-road engines, and the adoption of new metrics. These changes have created a demand for new instruments that are capable of real time measurement, enhanced sensitivity, and on-board vehicle operation. In response, researchers and instrument manufacturers have developed an array of new and improved instruments and sampling methods. It is generally recognized that the exhaust aerosol concn. measured depends on both the sampling technique and the instrument used. Hence, many of the new instruments are complementary and offer merits in measuring a variety of particulate emissions attributes. However, selecting the best instrument for each application is not a straightforward task; it requires on one hand a clear measurement objective and, on the other, an understanding of the characteristics of the instrument employed. This paper reviews how vehicle exhaust particulate emission measurements have evolved over the years. The focus is on current and newly evolving instrumentation, including gravimetric filter measurement, chem. anal. of filters, light extinction, scattering and absorption instruments, and instruments based on the elec. detection of exhaust aerosols. Correlations between the various instruments are examd. in the context of steadily more stringent exhaust emissions stds. The review concludes with a discussion of future instrument and sampling requirements for the changing nature of exhaust aerosols from current and future vehicles.
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      Birch, M. E.; Cary, R. A. Elemental Carbon-Based Method for Monitoring Occupational Exposures to Particulate Diesel Exhaust. Aerosol Sci. Technol. 1996, 25 (3), 221– 241,  DOI: 10.1080/02786829608965393
      17
      Elemental carbon-based method for monitoring occupational exposure to particulate diesel exhaust
      Birch, M. E.; Cary, R. A.
      Aerosol Science and Technology (1996), 25 (3), 221-241CODEN: ASTYDQ; ISSN:0278-6826. (Elsevier)
      Results of investigation of a thermal-optical technique for anal. of the carbonaceous fraction of particulate diesel exhaust are reported. With this technique, speciation of org. and elemental C is accomplished through temp. and atm. control, and by an optical feature that corrects for pyrolytically generated C (char) which is formed during the anal. of some materials. The thermal-optical method was selected because the instrument has desirable design features not present in other C analyzers. Although various C types are detd., elemental C is the superior marker of diesel particulate matter because elemental C constitutes a large fraction of the particulate mass, it can be quantified at low levels, and its only significant source in most workplaces is the diesel engine. Exposure-related issues and results of investigation of various sampling methods for particulate diesel exhaust are discussed.
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      Aakko-Saksa, P.; Koponen, P.; Aurela, M.; Vesala, H.; Piimäkorpi, P.; Murtonen, T.; Sippula, O.; Koponen, H.; Karjalainen, P.; Kuittinen, N. Considerations in Analysing Elemental Carbon from Marine Engine Exhaust Using Residual, Distillate and Biofuels. J. Aerosol Sci. 2018, 126, 191– 204,  DOI: 10.1016/j.jaerosci.2018.09.005
      18
      Considerations in analysing elemental carbon from marine engine exhaust using residual, distillate and biofuels
      Aakko-Saksa, Paivi; Koponen, Paivi; Aurela, Minna; Vesala, Hannu; Piimakorpi, Pekka; Murtonen, Timo; Sippula, Olli; Koponen, Hanna; Karjalainen, Panu; Kuittinen, Niina; Panteliadis, Pavlos; Ronkko, Topi; Timonen, Hilkka
      Journal of Aerosol Science (2018), 126 (), 191-204CODEN: JALSB7; ISSN:0021-8502. (Elsevier Ltd.)
      Elemental carbon (EC) concns. in the exhaust of a medium-speed marine engine was evaluated using thermal-optical anal. (TOA). Particulate matter (PM) samples were collected at 75% and 25% engine loads using residual and distillate fuels with sulfur contents of 2.5%, 0.5% and 0.1%, and a biofuel (30% of bio-component). The EC anal. of PM samples from a marine engine proved to be challenging. For example, transformations of structure of the sampled particles in the inert and the oxygen mode were obsd. for marine engine exhaust samples. The relationship between constituents present in the samples from the marine engine using different fuels, and phenomena obsd. in the thermograms are discussed. Temp. protocol selection and sample pre-treatment (extns. and drying) affected the reported EC mass. Modifications in the methodol. were suggested to increase the accuracy of the anal. Repeatability and reproducibility of the EC anal. was studied in the round-robin of three labs.
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      Isella, L.; Giechaskiel, B.; Drossinos, Y. Diesel-Exhaust Aerosol Dynamics from the Tailpipe to the Dilution Tunnel. J. Aerosol Sci. 2008, 39 (9), 737– 758,  DOI: 10.1016/j.jaerosci.2008.04.006
      19
      Diesel-exhaust aerosol dynamics from the tailpipe to the dilution tunnel
      Isella, L.; Giechaskiel, B.; Drossinos, Y.
      Journal of Aerosol Science (2008), 39 (9), 737-758CODEN: JALSB7; ISSN:0021-8502. (Elsevier Ltd.)
      We study, exptl. and theor., the dynamics of non-volatile particles emitted from a diesel EURO 3 light-duty vehicle along the transfer tube that conducts exhaust fumes from the tailpipe to the diln. tunnel. Particle agglomeration, diffusional and thermophoretic transport are modeled. For turbulent, but moderate, Reynolds nos. and under steady-state conditions we map the combustion-generated nanoparticle dynamics onto a one-dimensional dynamics of aerosol particles in an ageing chamber. The aggregate fractal dimension, detd. self-consistently by comparing mass distributions, varied from 2 to 2.3. The relative importance of aerosol processes is estd. by defining appropriate characteristic time scales. Agglomeration and convection by the bulk motion of the fluid are the dominant processes for inlet no. concns. of the order of 108 particles/cm3 and transfer-tube lengths of 6-9 m. Thermophoretic losses are calcd. to be non-negligible. For modern vehicles with particulate filters agglomeration is estd. to be negligible, whereas thermophoresis may be significant.
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    20. 20
      Brem, B. T.; Durdina, L.; Siegerist, F.; Beyerle, P.; Bruderer, K.; Rindlisbacher, T.; Rocci-Denis, S.; Andac, M. G.; Zelina, J.; Penanhoat, O. Effects of Fuel Aromatic Content on Nonvolatile Particulate Emissions of an In-Production Aircraft Gas Turbine. Environ. Sci. Technol. 2015, 49 (22), 13149– 13157,  DOI: 10.1021/acs.est.5b04167
      There is no corresponding record for this reference.
    21. 21
      Ntziachristos, L.; Saukko, E.; Lehtoranta, K.; Rönkkö, T.; Timonen, H.; Simonen, P.; Karjalainen, P.; Keskinen, J. Particle Emissions Characterization from a Medium-Speed Marine Diesel Engine with Two Fuels at Different Sampling Conditions. Fuel 2016, 186, 456– 465,  DOI: 10.1016/j.fuel.2016.08.091
      21
      Particle emissions characterization from a medium-speed marine diesel engine with two fuels at different sampling conditions
      Ntziachristos, L.; Saukko, E.; Lehtoranta, K.; Ronkko, T.; Timonen, H.; Simonen, P.; Karjalainen, P.; Keskinen, J.
      Fuel (2016), 186 (), 456-465CODEN: FUELAC; ISSN:0016-2361. (Elsevier Ltd.)
      Particle emission characteristics for a medium-speed four-stroke marine diesel engine were studied using a variety of sampling systems. Measurements were conducted at 25% and 75% load employing a heavy fuel oil (HFO) and a lighter marine distillate oil. The measurements, esp. with HFO, revealed that marine exhaust particles mostly consist of nanometer sized ash particles on which heavy volatile species condense during exhaust diln. and cooling. The soot mode no. concn. was low with both fuels tested, in particular when HFO was used. Total particle no. emissions ranged in the order of 5.2-6.9 × 1015 per kg of fuel and formed a monomodal size distribution when a porous tube diluter combined with an ageing chamber and operating at low diln. ratio was used for sampling. The levels and size distributions obtained in the lab using a porous tube diluter were similar to the ones reported in the literature studying ship plumes following atm. diln. Lab measurements with ejector-type diluters mostly led to bi-modal distributions that did not well resemble atm. size distributions. Moreover, the nucleation mode formed with the ejector diluters was variable in size and concn. When used with diln. air at ambient temp., ejector diluters were inappropriate for primary diln. due to clogging.
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    22. 22
      Khan, M. Y.; Giordano, M.; Gutierrez, J.; Welch, W. A.; Asa-Awuku, A.; Miller, J. W.; Cocker, D. R. Benefits of Two Mitigation Strategies for Container Vessels: Cleaner Engines and Cleaner Fuels. Environ. Sci. Technol. 2012, 46 (9), 5049– 5056,  DOI: 10.1021/es2043646
      There is no corresponding record for this reference.
    23. 23
      Zetterdahl, M.; Moldanová, J.; Pei, X.; Pathak, R. K.; Demirdjian, B. Impact of the 0.1% Fuel Sulfur Content Limit in SECA on Particle and Gaseous Emissions from Marine Vessels. Atmos. Environ. 2016, 145, 338– 345,  DOI: 10.1016/j.atmosenv.2016.09.022
      23
      Impact of the 0.1% fuel sulfur content limit in SECA on particle and gaseous emissions from marine vessels
      Zetterdahl, Maria; Moldanova, Jana; Pei, Xiangyu; Pathak, Ravi Kant; Demirdjian, Benjamin
      Atmospheric Environment (2016), 145 (), 338-345CODEN: AENVEQ; ISSN:1352-2310. (Elsevier Ltd.)
      Emissions were measured on-board a ship in the Baltic Sea, which is a sulfur emission control area (SECA), before and after the implementation of the strict fuel sulfur content (FSC) limit of 0.1 m/m% S on the 1st of Jan. 2015. Prior to Jan. 2015, the ship used a heavy fuel oil (HFO) but switched to a low-sulfur residual marine fuel oil (RMB30) after the implementation of the new FSC limit. The emitted particulate matter (PM) was measured in terms of mass, no., size distribution, volatility, elemental compn., content of orgs., black and elemental carbon, polycyclic arom. hydrocarbons (PAHs), microstructure and micro-compn., along with the gaseous emissions at different operating conditions. The fuel change reduced emissions of PM mass up to 67%. The no. of particles emitted remained unchanged and were dominated by nanoparticles. Furthermore, the fuel change resulted in an 80% redn. of SO2 emissions and decreased emissions of total volatile org. compds. (VOCs). The emissions of both monoarom. and lighter polyarom. hydrocarbon compds. increased with RMB30, while the heavy, PM-bound PAH species that belong to the carcinogenic PAH family were reduced. Emissions of BC remained similar between the two fuels. This study indicates that the use of low-sulfur residual marine fuel oil is a way to comply with the new FSC regulation and will reduce the anthropogenic load of SO2 emissions and secondary PM formed from SO2. Emissions of primary particles, however, remain unchanged and do not decrease as much as would be expected if distd. fuel was used. This applies both to the no. of particles emitted and some toxic components, such as heavy metals, PAHs or elemental carbon (EC). The micro-compn. analyses showed that the soot particles emitted from RMB30 combustion often do not have any trace of sulfur compared with particles from HFO combustion, which always have a sulfur content over 1%m/m. The soot sulfur content can impact aging and cloud condensation properties. This study is an in-depth comparison of the impact of these two fuels on the emissions of particles as well as their compn. and microstructure. To evaluate the impact of the use of low-sulfur residual marine fuel oils on emissions from ships, addnl. research is needed to investigate the varied fuel types and compns. as well as the wide range of engine conditions and properties.
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    24. 24
      Winnes, H.; Fridell, E. Emissions of NOX and Particles from Manoeuvring Ships. Transp. Res. Part D Transp. Environ. 2010, 15 (4), 204– 211,  DOI: 10.1016/j.trd.2010.02.003
      There is no corresponding record for this reference.
    25. 25
      Cooper, D. A. Exhaust Emissions from Ships at Berth. Atmos. Environ. 2003, 37 (27), 3817– 3830,  DOI: 10.1016/S1352-2310(03)00446-1
      There is no corresponding record for this reference.
    26. 26
      Jayaratne, E. R.; Meyer, N. K.; Ristovski, Z. D.; Morawska, L. Volatile Properties of Particles Emitted by Compressed Natural Gas and Diesel Buses during Steady-State and Transient Driving Modes. Environ. Sci. Technol. 2012, 46 (1), 196– 203,  DOI: 10.1021/es2026856
      There is no corresponding record for this reference.
    27. 27
      Bullock, D. S.; Olfert, J. S. Size, Volatility, and Effective Density of Particulate Emissions from a Homogeneous Charge Compression Ignition Engine Using Compressed Natural Gas. J. Aerosol Sci. 2014, 75, 1– 8,  DOI: 10.1016/j.jaerosci.2014.04.005
      27
      Size, volatility, and effective density of particulate emissions from a homogeneous charge compression ignition engine using compressed natural gas
      Bullock, Dallin S.; Olfert, Jason S.
      Journal of Aerosol Science (2014), 75 (), 1-8CODEN: JALSB7; ISSN:0021-8502. (Elsevier Ltd.)
      The particle size distribution, volatility, and effective d. of particulate matter emitted from a homogeneous charge compression ignition (HCCI) engine fueled by port injected compressed natural gas were measured and compared to emissions emitted from the same engine during motoring and spark ignition for two compression ratios. The particle concn. and geometric mean diam. were greater at high compression ratio, and also, the total particulate mass was lower for spark ignition and homogeneous charge compression ignition than during motoring. Volatility tests showed that all operating conditions have less than 5% of the particulate matter remaining when denuding the sample at 100 °C. Effective d. measurements also show that the particles for each operating mode have a relatively const. d. with respect to particle size (approx. 850 kg/m3).
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    28. 28
      Anderson, M.; Salo, K.; Fridell, E. Particle- and Gaseous Emissions from an LNG Powered Ship. Environ. Sci. Technol. 2015, 49 (20), 12568– 12575,  DOI: 10.1021/acs.est.5b02678
      There is no corresponding record for this reference.
    29. 29
      Alanen, J.; Saukko, E.; Lehtoranta, K.; Murtonen, T.; Timonen, H.; Hillamo, R.; Karjalainen, P.; Kuuluvainen, H.; Harra, J.; Keskinen, J. The Formation and Physical Properties of the Particle Emissions from a Natural Gas Engine. Fuel 2015, 162, 155– 161,  DOI: 10.1016/j.fuel.2015.09.003
      29
      The formation and physical properties of the particle emissions from a natural gas engine
      Alanen, Jenni; Saukko, Erkka; Lehtoranta, Kati; Murtonen, Timo; Timonen, Hilkka; Hillamo, Risto; Karjalainen, Panu; Kuuluvainen, Heino; Harra, Juha; Keskinen, Jorma; Ronkko, Topi
      Fuel (2015), 162 (), 155-161CODEN: FUELAC; ISSN:0016-2361. (Elsevier Ltd.)
      Natural gas engine particle emissions were studied using an old gasoline engine modified to run with natural gas. The tests were steady-state tests performed on two different low loads in an engine dynamometer. Exhaust particle no. concn., size distribution, volatility and elec. charge were measured. Exhaust particles were obsd. to have peak diams. below 10 nm. To get the full picture of particle emissions from natural gas engines, size range 1-5 nm is relevant and important to take into consideration. A particle size magnifier (PSM) was used in this engine application for measuring particles smaller than 3 nm and it proved to be a useful instrument when measuring natural gas engine exhaust particles. It is concluded that the detected particles probably originated from the engine cylinders or their vicinity and grew to detectable sizes in the sampling process because a small fraction of the particles were obsd. to carry elec. charge and the particles did not evap. totally at 265 °C.
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    30. 30
      Fridell, E.; Salo, K. Measurements of Abatement of Particles and Exhaust Gases in a Marine Gas Scrubber. Proc. Inst. Mech. Eng. Part M J. Eng. Marit. Environ. 2016, 230 (1), 154– 162,  DOI: 10.1177/1475090214543716
      There is no corresponding record for this reference.
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      Kasper, A.; Aufdenblatten, S.; Forss, A.; Mohr, M.; Burtscher, H. Particulate Emissions from a Low-Speed Marine Diesel Engine. Aerosol Sci. Technol. 2007, 41 (1), 24– 32,  DOI: 10.1080/02786820601055392
      31
      Particulate emissions from a low-speed marine diesel engine
      Kasper, A.; Aufdenblatten, S.; Forss, A.; Mohr, M.; Burtscher, H.
      Aerosol Science and Technology (2007), 41 (1), 24-32CODEN: ASTYDQ; ISSN:0278-6826. (Taylor & Francis, Inc.)
      The tail pipe emissions of particulate matter from a turbocharged common rail 2-stroke marine diesel engine (4RTX-3 from Wartsila) were investigated at various operating conditions and using 2 different fuels. Size distributions were measured with a SMPS (Scanning Mobility Particle Sizer). A thermodesorber (TD) was applied to remove volatile material. In addn., filter samples were taken for gravimetric and chem. anal. The mean diams. of the particles ranged 20-40 nm, which is considerably smaller than the diam. of particles known from 4-stroke diesel engines as used in cars. A TD operated at 400° evapd. the majority of the particles. The particle mass is dominated by volatile org. material, the fraction of which is significantly higher than for engines in cars. A high nucleation mode was found instead of a pronounced accumulation mode as known from 4-stroke diesel engines.
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    32. 32
      Pirjola, L.; Pajunoja, A.; Walden, J.; Jalkanen, J.-P.; Rönkkö, T.; Kousa, A.; Koskentalo, T. Mobile Measurements of Ship Emissions in Two Harbour Areas in Finland. Atmos. Meas. Tech. 2014, 7 (1), 149– 161,  DOI: 10.5194/amt-7-149-2014
      32
      Mobile measurements of ship emissions in two harbour areas in Finland
      Pirjola, L.; Pajunoja, A.; Walden, J.; Jalkanen, J.-P.; Ronkko, T.; Kousa, A.; Koskentalo, T.
      Atmospheric Measurement Techniques (2014), 7 (1), 149-161CODEN: AMTTC2; ISSN:1867-8548. (Copernicus Publications)
      Four measurement campaigns were performed in two different environments - inside the harbor areas in the city center of Helsinki, and along the narrow shipping channel near the city of Turku, Finland - using a mobile lab. van during winter and summer conditions in 2010-2011. The characteristics of gaseous (CO, CO2, SO2, NO, NO2, NOx) and particulate (no. and vol. size distributions as well as PM2.5) emissions for 11 ships regularly operating on the Baltic Sea were studied to det. the emission parameters. The highest particle concns. were 1.5×106 and 1.6×105 cm-3 in Helsinki and Turku, resp., and the particle no. size distributions had two modes. The dominating mode peaked at 20-30 nm, and the accumulation mode at 80-100 nm. The majority of the particle mass was volatile, since after heating the sample to 265 °C, the particle vol. of the studied ship decreased by around 70 %. The emission factors for NOx varied in the range of 25-100 g (kg fuel)-1, for SO2 in the range of 2.5-17.0 g (kg fuel)-1, for particle no. in the range of (0.32-2.26)×1016 # (kg fuel)-1, and for PM2.5 between 1.0-4.9 g (kg fuel)-1. The ships equipped with SCR (selective catalytic redn.) had the lowest NOx emissions, whereas the ships with DWI (direct water injection) and HAMs (humid air motors) had the lowest SO2 emissions but the highest particulate emissions. For all ships, the averaged fuel sulfur contents (FSCs) were less than 1% (by mass) but none of them was below 0.1% which will be the new EU directive starting 1 Jan. 2015 in the SOx emission control areas; this indicates that ships operating on the Baltic Sea will face large challenges.
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    33. 33
      Amanatidis, S.; Ntziachristos, L.; Karjalainen, P.; Saukko, E.; Simonen, P.; Kuittinen, N.; Aakko-Saksa, P.; Timonen, H.; Rönkkö, T.; Keskinen, J. Comparative Performance of a Thermal Denuder and a Catalytic Stripper in Sampling Laboratory and Marine Exhaust Aerosols. Aerosol Sci. Technol. 2018, 52 (4), 420– 432,  DOI: 10.1080/02786826.2017.1422236
      33
      Comparative performance of a thermal denuder and a catalytic stripper in sampling laboratory and marine exhaust aerosols
      Amanatidis, Stavros; Ntziachristos, Leonidas; Karjalainen, Panu; Saukko, Erkka; Simonen, Pauli; Kuittinen, Niina; Aakko-Saksa, Paivi; Timonen, Hilkka; Ronkko, Topi; Keskinen, Jorma
      Aerosol Science and Technology (2018), 52 (4), 420-432CODEN: ASTYDQ; ISSN:0278-6826. (Taylor & Francis, Inc.)
      The performance of a thermal denuder (thermodenuder-TD) and a fresh catalytic stripper (CS) was assessed by sampling lab. aerosol, produced by different combinations of sulfuric acid, octacosane, and soot particles, and marine exhaust aerosol produced by a medium-speed marine engine using high sulfur fuels. The intention was to study the efficiency in sepg. non-volatile particles. No particles could be detected downstream of either device when challenged with neat octacosane particles at high concn. Both lab. and marine exhaust aerosol measurements showed that sub-23 nm semi-volatile particles are formed downstream of the thermodenuder when upstream sulfuric acid approached 100 ppbv. Charge measurements revealed that these are formed by re-nucleation rather than incomplete evapn. of upstream aerosol. Sufficient diln. to control upstream sulfates concn. and moderate TD operation temp. (250°C) are both required to eliminate their formation. Use of the CS following an evapn. tube seemed to eliminate the risk for particle re-nucleation, even at a ten-fold higher concn. of semi-volatiles than in case of the TD. Particles detected downstream of the CS due to incomplete evapn. of sulfuric acid and octacosane aerosol, did not exceed 0.01% of upstream concn. Despite the superior performance of CS in sepg. non-volatile particles, the TD may still be useful in cases where increased sensitivity over the traditional evapn. tube method is needed and where high sulfur exhaust concn. may fast deplete the catalytic stripper adsorption capacity. 2018 American Assocn. for Aerosol Research.
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      Hesterberg, T. W.; Lapin, C. A.; Bunn, W. B. A Comparison of Emissions from Vehicles Fueled with Diesel or Compressed Natural Gas. Environ. Sci. Technol. 2008, 42 (17), 6437– 6445,  DOI: 10.1021/es071718i
      34
      A Comparison of Emissions from Vehicles Fueled with Diesel or Compressed Natural Gas
      Hesterberg, Thomas W.; Lapin, Charles A.; Bunn, William B.
      Environmental Science & Technology (2008), 42 (17), 6437-6445CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      A comprehensive comparison of emissions from vehicles fueled with diesel or compressed natural gas (CNG) was developed from 25 reports on transit and school buses, refuse trucks, and passenger cars. Emissions of most compds. were highest for untreated exhaust gas and lowest for treated exhaust gas. CNG buses without after-treatment had the highest CO, hydrocarbon, non-methane hydrocarbon, volatile org. compd. (e.g., benzene, butadiene, ethylene, etc.), and carbonyl compd. (e.g., formaldehyde, acetaldehyde, acrolein) emissions. Diesel buses without after-treatment had the highest particulate matter and polycyclic arom. hydrocarbon emissions. Exhaust after-treatment reduced most emissions to similar concns. in diesel and CNG buses. NOx and CO2 emissions were similar for most vehicle types, fuels, and exhaust after-treatment with some exceptions. Diesel school buses had higher CO2 emissions than CNG buses. CNG transit buses and passenger cars equipped with 3-way catalysts had lower NOx emissions. Diesel buses equipped with traps had higher NO2 emissions. Fuel economy was best in diesel buses not equipped with exhaust after-treatment.
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      https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD1cXovFSkt70%253D&md5=6482d8654ff06551e5f8f05204e189a4
    35. 35
      Liu, J.; Yang, F.; Wang, H.; Ouyang, M.; Hao, S. Effects of Pilot Fuel Quantity on the Emissions Characteristics of a CNG/diesel Dual Fuel Engine with Optimized Pilot Injection Timing. Appl. Energy 2013, 110, 201– 206,  DOI: 10.1016/j.apenergy.2013.03.024
      35
      Effects of pilot fuel quantity on the emissions characteristics of a CNG/diesel dual fuel engine with optimized pilot injection timing
      Liu, Jie; Yang, Fuyuan; Wang, Hewu; Ouyang, Minggao; Hao, Shougang
      Applied Energy (2013), 110 (), 201-206CODEN: APENDX; ISSN:0306-2619. (Elsevier Ltd.)
      For CNG/diesel dual fuel engines, the effects of pilot fuel quantity and injection timing are noticeable and significant. In this study, the emission characteristics of a CNG-diesel dual fuel engine with different pilot diesel fuel quantity and optimized pilot injection timing were investigated. The CO emission levels under dual fuel mode are considerably higher than that under normal diesel operation modes even at high load, which indicated that there exist some flame extinction regions. Dual fuel mode reduces NOx emissions by 30% averagely in comparison to diesel mode. That is because most of the fuel is burned under lean premixed conditions which result in lower local temp. The unburned HC emissions under dual-fuel mode are obviously higher than that of the normal diesel mode, esp. at low to medium loads. And around 90% of the THC emissions were unburned methane, which means the flame does not propagate throughout the charge. THC emissions reduce significantly with the increase of the pilot diesel quantity. Thanks to the premixed nature of the combustion mode and the methane mol. structure, the PM emission is reduced obviously under dual fueling condition. The PM emission is increased with the increase of the pilot fuel quantity.
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    36. 36
      Lehtoranta, K.; Murtonen, T.; Vesala, H.; Koponen, P.; Alanen, J.; Simonen, P.; Rönkkö, T.; Timonen, H.; Saarikoski, S.; Maunula, T. Natural Gas Engine Emission Reduction by Catalysts. Emiss. Control Sci. Technol. 2017, 3 (2), 142– 152,  DOI: 10.1007/s40825-016-0057-8
      36
      Natural Gas Engine Emission Reduction by Catalysts
      Lehtoranta, Kati; Murtonen, Timo; Vesala, Hannu; Koponen, Paivi; Alanen, Jenni; Simonen, Pauli; Ronkko, Topi; Timonen, Hilkka; Saarikoski, Sanna; Maunula, Teuvo; Kallinen, Kauko; Korhonen, Satu
      Emission Control Science and Technology (2017), 3 (2), 142-152CODEN: ECSTG9; ISSN:2199-3637. (Springer International Publishing AG)
      In order to meet stringent emission limits, after-treatment systems are increasingly utilized in natural gas engine applications. In this work, two catalyst systems were studied in order to clarify how the catalysts affect, e.g. hydrocarbons, NOx and particles present in natural gas engine exhaust. A passenger car engine modified to run with natural gas was used in a research facility with possibilities to modify the exhaust gas properties. High NOx redns. were obsd. when using selective catalytic redn., although a clear decrease in the NOx redn. was recorded at higher temps. The relatively fresh methane oxidn. catalyst was found to reach redns. greater than 50% when the exhaust temp. and the catalyst size were sufficient. Both the studied catalyst systems were found to have a significant effect on particulate emissions. The obsd. particle mass redn. was found to be due to a decrease in the amt. of orgs. passing over the catalyst. However, esp. at high exhaust temps., high nanoparticle concns. were obsd. downstream of the catalysts together with higher sulfate concns. in particles. This study contributes to understanding emissions from future natural gas engine applications with catalysts in use.
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    37. 37
      Järvi, A. Methane Slip Reduction in Wärtsilä Lean Burn Gas Engines. 26th CIMAC World Congress ; 2010; Paper 106.
      There is no corresponding record for this reference.
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      Hiltner, J.; Loetz, A.; Fiveland, S. Unburned Hydrocarbon Emissions from Lean Burn Natural Gas Engines - Sources and Solutions. 28th CIMAC World Congress ; 2016; Paper 032.
      There is no corresponding record for this reference.
    39. 39
      Lehtoranta, K.; Turunen, R.; Vesala, H.; Nyyssoenen, S.; Soikkeli, N.; Esselstroem, L. Testing SCR in High Sulphur Application. 27th CIMAC World Congress ; 2013; Paper 107.
      There is no corresponding record for this reference.

  • Supporting Information

    Supporting Information

    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.8b05555.

    • Schematic of the layout of all engines tested on the engine test bed and on board (Figure S1) and PM measurement system according to ISO8178:2006 and the “PMP” PN (nonvolatiles >23) measurement system (Figure S2) (PDF)


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