The impact of photochemical aging on secondary aerosol formation from a marine engine

doi:10.21203/rs.3.rs-4983538/v1

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The impact of photochemical aging on secondary aerosol formation from a marine engine

https://doi.org/10.21203/rs.3.rs-4983538/v1

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Ship traffic is known as one important contributor to air pollution. Recent regulations aimed at reducing sulfur oxide (SOx) pollution by limiting the fuel sulfur content (FSC) may also decrease fresh particulate matter (PM) emitted from ships. However, there is a knowledge gap regarding how the FSC affects secondary aerosol formation. Aerosol particle emissions from a research ship engine operated with either low sulfur heavy fuel oil (LS-HFO) (FSC=0.5%) or marine gas oil (MGO) (FSC=0.01%), were studied. The emissions were photochemically processed in the oxidation flow reactor “PEAR” to equivalent photochemical aging between 0-9 days in the atmosphere. It was found that FSC had no significant impact on secondary organic aerosol (SOA) formation after 3 days of aging, at 1.8±0.4g/kg and 1.5±0.4g/kg for MGO and LS-HFO, respectively. Furthermore, the composition and oxidative pathways remained similar regardless of FSC. However, as a result of the higher secondary SO4 formation and fresh aerosol emissions, LS-HFO had significantly higher total PM1 than MGO. Black carbon (BC) specifically was found to be 3 times higher for HFO than MGO. While the fuel with the lower sulfur content produces significantly less PM, the SOA formation remains similar regardless of FSC.

Earth and environmental sciences/Environmental sciences

Earth and environmental sciences/Environmental sciences/Environmental chemistry

Earth and environmental sciences/Environmental sciences/Environmental impact

Earth and environmental sciences/Climate sciences/Atmospheric science/Atmospheric chemistry

Ship emissions

maneuvering conditions MGO

HFO

emission factors

SOA

Secondary aerosol

OFR

Sulfur content

Atmospheric oxidation of ship engine exhaust, reveals significant impact of new regulations but highlights secondary organic aerosols as key pollutant.

International trade is dominated by the shipping industry, accounting for approximately 80% by volume¹ and is expected to triple from 2019 to 2050². Currently, international shipping is responsible for about 3% of global anthropogenic greenhouse gas emissions^{2, 3} approximately 9% SO_x, 17% NO_x, 4% PM2.5 and 4% non-methane volatile organic compounds (NMVOCs) of global anthropogenic emissions.^4–6

Up to 7% of global premature mortalities are attributable to air pollution.^7–10 As 70% of marine traffic occurs within 400 km from the coastline, ship emissions are relevant for public health.¹¹ Air pollution from shipping prior 2020 was estimated to attribute above 400 thousand premature deaths per year globally.¹² In 2020 the International maritime organisation (IMO) introduced global regulations limiting the maximum fuel sulfur content (FSC) from 3.5 to 0.5w%. These regulations aimed to directly reduce SO_x emissions from shipping by 77%,¹³ but indirectly also lower emissions of PM by the implied ban of most heavy fuel oils (HFO).¹⁴ These new regulations are expected to reduce premature deaths due to air pollution from ships by about 30%.¹² Furthermore, in 2015 sulfur emission control areas (SECA) were defined, including the North Sea, Baltic Sea, and North American coastal waters, with a maximum allowed FSC of 0.1%. From July 2024, HFO defined as fuels with a kinematic viscosity greater than 180 mm s^-1 at 50°C and a density larger than 900 kg m^-3 at 15°C are banned in Arctic waters.¹⁵

Introducing lower global FSC limit led to an increase in the use of marine gas oil (MGO), low-sulfur HFO (LS-HFO) and hybrid fuels with boiling ranges and impurities between MGO and LS-HFO. The boiling fraction of MGO, being a diesel-like fuel, has an intrinsically lower FSC than LS-HFO and is available with FSC ≤ 0.1%. Nevertheless, MGO has a significantly higher FSC than diesel used for road traffic, which has FSC < 0.001%.¹⁶

Beyond SO_x, substantial amounts of PM, BC, NO_x and NMVOCs are emitted at high levels from marine diesel engines, which are not equipped with exhaust aftertreatment technology, such as diesel oxidation catalysts (DOC) which reduces NMHC emissions. NMVOCs participate in oxidative gas-to-particle conversion, forming secondary organic aerosol (SOA). Observational studies have found that the highest contributor to SOA formation in coastal urban areas is shipping emissions with about 38%.¹⁷ The highest emission factors for hydrocarbons, black carbon (BC) and particulate mass (PM) were found during the lowest engine loads, such as near shore maneuvering conditions.^{16, 18, 19} Potential SOA precursors such as light poly aromatic hydrocarbons (PAHs) and other IVOCs have been reported from different fuel types with heavier fuels containing more PAHs than lighter diesel fuels²⁰. Furthermore, a significant increase in PAH and oxy-PAH was observed during low engine load.²¹

SOA from IVOCs, such as naphthalene representative for combustion-derived IVOC, have been shown to have adverse effect on human health.²² Even with a change from HFO to LS-HFO or MGO it has been predicted that shipping will remain a significant source of anthropogenic aerosol.²³ A recent study explored the impact of aging on HFO emissions at 65% engine load. The ship was equipped with a sulphur scrubber and a DOC as exhaust aftertreatment, and showed no significant SOA formation.²⁴ Therefore, in order to explore the SOA formation potential for other engine conditions and better understand the impacts of new IMO regulations on SOA formation, our study investigates the impacts of aging on low sulphur fuels such as LS-HFO and MGO fuel at low engine load.

SOA formation from LS-HFO and MGO photooxidation

Figure 1 illustrates the chemical composition of aerosols for both LS-HFO and MGO. At 0 days of equivalent photochemical aging the fresh aerosol has an OM/PM of 0.47 for LS-HFO and 0.34 for MGO, respectively. The MGO thus contains relatively less organic and more soot, however the total aerosol emitted is much lower for MGO than for LS-HFO. The LS-HFO emissions of POA were more than 5 times higher than those of the MGO, while BC emissions were approximately 3 times higher in LS-HFO than in MGO. Other non-refractory PM components including SO4 and NO3 were negligible for the total PM.

The fresh particles have a geometric mean diameter of 75 ± 6 nm for MGO and 94 ± 3 nm for LS-HFO (supplementary table S12), which is comparable to fresh particles emitted from HFO published by Karjalainen et al. 2022.²⁴ The most notable change from previous studies is that there is no SO4 contribution to the fresh aerosol emissions due to the fuel used in this study LS-HFO(FSC = 0.5%) in comparison to Karjalainen et al 2022 with an FSC of 1.9%. HFO with a FSC of 0.12% has previously been found to emit 2.57 ± 0.41g/kg total PM at 25% engine load,¹⁹ this is a lower FSC content than in the LS-HFO of this study, but the emissions factors are nevertheless similar.

Ozonolysis had the lowest impact on the aerosol in the PEAR in terms of chemical composition, particle size and PM. The total aerosol mass per kg fuel consumed for LS-HFO is consistently from fresh to 9 days of equivalent photochemical age more than twice that of MGO. As the emissions were photochemically processed in the PEAR, also the aerosol composition changed. At 1.5 days the aerosol composition is dominated by organics with an OM/PM of 0.60 for LS-HFO and 0.69 for MGO. BC is comparatively not affected by photochemical aging and the total BC mass remains constant at 1.1 ± 0.2g/kg for LS-HFO and 0.4 ± 0.1g/kg for MGO for all oxidation experiments. The increase in total mass can be attributed to SO4 and particularly SOA formation (Fig. 1). The SOA emission factor for both MGO and LS-HFO is similar and reaches a maximum of 1.5 ± 0.4 g/kg LS-HFO and 1.8 ± 0.4 g/kg MGO after 3.3 and 4.7 days of equivalent photochemical aging respectively, though smaller aging steps would be required to determine the specific maximum. However, the majority of SOA is formed within the first 1.5 days of equivalent photochemical aging. Some results from recent studies have suggested the majority of secondary aerosol (SA) from shipping is even formed within the first 3 hours after emission.³⁴ While photochemical aging increases SOA formation equally for the two fuels, SO4 aerosol formation is greatly enhanced in the LS-HFO emissions due to the higher FSC and thus emission of SO₂ compared to MGO.

Figure 1 shows that photochemical aging beyond 4.7 days does not yield additional SOA formation, and a further increase in total aerosol results from SO4 formation. After 9 days of equivalent photochemical aging, the LS-HFO aerosol is in a SO4 dominated state where OM/PM decreased to 0.23. For MGO, however, the aerosol remains organic-dominated with OM/PM > 0.5. This is further highlighted by the organic aerosol enhancement ratio, which indicates the 5-fold increase in organics for the MGO, whereas LS-HFO only increases 2-fold compared to POA. Therefore, the low FSC in the MGO significantly decreases the total aerosol mass concentration as secondary SO4 aerosol mass is reduced. But a change from LS-HFO to MGO does not significantly reduce SOA formation, resulting in an organic dominated aerosol.

Elemental composition and oxidation pathway

While more than 4.7 days of equivalent photochemical aging does not increase OA mass for either MGO or LS-HFO, the composition of the OA changes significantly. Initial photochemical aging from 0 to 4.7 days increases both f43 (the fraction of 43 m/z of total mass spectrum, mostly $\:{C}_{2}{H}_{3}{O}^{+}$) and f44 (the fraction of 44 m/z mostly $\:C{O}_{2}^{+}$) fraction, consistent with the increase in OA mass (Fig. 2A-B).^{35, 36} However, an equivalent age higher than 4.7 days results in a decrease of f43 and an increase of f44, similar to observations from EURO2 diesel vehicles .³⁷ This coincides with the plateau in SOA formation that was observed, suggesting a change in the oxidative pathway. This observation is valid for both MGO and LS-HFO. All aged aerosols fall within the triangular space, representing the occurrence of ambient aerosol .³⁵

The similarity between MGO and LS-HFO is further supported by the elemental ratios depicted as a Van Krevelen diagram (Fig. 2C-D).^{36, 38} The main difference in the elemental composition was found in the fresh aerosol, with the H/C ratio of ($\:1.79\pm\:0.05)$ for MGO and ($\:1.67\pm\:0.03$) for LS-HFO aerosol, resulting in a slope from fresh aerosol to 3 days of equivalent photochemical aging of -0.97±0.08 (r²=0.97) and − 0.89±0.04 (r² = 0.98) for MGO and LS-HFO, respectively. This result suggests that the initial photochemical aging from fresh to maximum SOA formation is equivalent to carboxylic acid formation with no fragmentation or carbonyl and hydroxyl addition on different carbons.³⁶ Further after just 3–4 days of photochemical aging there is no significant difference in the elemental ratios between two fuels. The slope of both MGO and LS-HFO after 3 days of age is -0.54±0.02 (r² = 0.99). Photochemical aging beyond the maximum SOA formation point thus suggests carboxylic acid formation with fragmentation. This is fitting with decrease in f43 but continued increase in f44 suggesting acid formation.³⁶ The fragmentation effectively results in a lower SOA yield which leads to a net zero mass change in SOA at higher photochemical age. Based on KinSim simulation the difference in oxidation is not a result of the difference in RO2 fate as HO2-RO2 reactions accounted for the > 50% of lost RO2 and HO accounting for > 25% at all ages for both fuels (supplementary table S8-9).

Implementing a global FSC limit to the current SECA level could incentivize the use of cleaner shipping fuels instead of residual fuel oils, potentially lowering emissions of total PM, BC, POA and sulphate. However, this may not impact the SOA mass formed after atmospheric aging. As both POA and BC are reduced, the fresh PM at emission point is significantly reduced by changing from current global FSC regulations to SECA compliant FSC fuels. The use of MGO over LS-HFO in harbor areas would thus decrease PM.

The majority of SOA was formed after only 1.5 days of equivalent photochemical aging while maximum SOA formation was reached at 3.3 days of equivalent photochemical age. Thus, SOA will presumably form close to the emission point, i.e. harbors and nearby populated areas, considering the emission scenario of low engine load. Since most of the population is located along coastlines, shipping emissions could have large public health effects. Notably the SOA levels would not be expected to decrease in these areas with a change from LS-HFO to MGO. Secondary sulfate formation proceeded much slower but continued to increase in mass during photochemical aging to the maximum of almost 9 days of equivalent photochemical age. The reduction in sulfate aerosol associated with changing from LS-HFO to MGO would thus have an environmental and air quality impact further from the emission point than the OA.

Regarding the composition of SOA, a high similarity was found for H/C, O/C, f43 and f44 for the LS-HFO and MGO. This suggests that the precursor for the SOA is similar between the two fuels, which are likely alkylated aromatic mono- to tricyclic structures.³⁹ Reducing aromatic VOC emissions would improve air quality and lessen the health burden associated with ship emissions during harbour maneuvers .

A four-stroke single-cylinder research diesel engine (80kW nominal power) was operated on either MGO (FSC = 0.01 S w%) or LS-HFO (FSC = 0.5 S w%) at low engine load (20kW, 25% of nominal power), representing docking maneuvers. Raw exhaust emissions were connected to diluters via heated tubing (constant at 350°C), see Fig. 3. A series configuration of a porous tube diluter and an ejector diluter was employed to achieve a dilution ratio of 1:250. The dilution ratio was determined by measuring the CO₂ concentrations in the raw exhaust, the diluted exhaust, and the dilution air. The dilution ratio was regulated by automatically adjusting the flow rate of the porous tube diluter, while maintaining a constant flow rate for the ejector diluter.

The diluted (1:250) exhaust sample passed through the oxidation flow reactor “Photochemical Emission Aging flow tube Reactor” (PEAR), which was operated at a flow rate of 100 lpm. ²⁵ At these flow conditions, the mean residence time in the PEAR is 70 s. At the entrance to the PEAR 10ppm of ozone was added in addition to water vapor keeping the relative humidity (RH) at approximately 50%. The photochemical aging was controlled through UV-lamp(254nm) intensity, water vapour supply for 50% relative humidity and constant ozone (10ppm) addition in order to obtain atmospheric aging equivalent to 0 to 9 days (supplementary table S7). The photochemical age was determined with d9-butanol decay measured by a Proton-transfer-reaction mass spectrometry (PTR-MS) based on the principle of the “photochemical clock”.²⁶ The Kinsim^27–31 model was used to verify the atmospheric relevancy by simulating the chemistry within the PEAR, by determining the RO2 fate to remove speculations on non-tropospheric chemistry occurring in the OFR. (supplementary table S7-9)

An additional ejector diluter was added after the PEAR for a further 10-fold dilution before online instruments, resulting in a total dilution ratio of 1:2500 for aerosol instruments presented here. Aerosol phase measurement were done with High-Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS)³² for obtaining the chemical composition of the non-refractory aerosol, aethalometer for BC and a scanning mobility particle sizer (SMPS) for particle number concentration and size distribution. SMPS data was treated with the AIM V. 10.3.1.0 software.

Optically defined black carbon (BC), “equivalent black carbon" (eBC), was quantified by the Aethalometer (AE33-7, Aerosol Magee Scientific), which measures light attenuation through a filter tape at 7 wavelengths (UV–IR, 370–950 nm). Using different corrections, such as multiple-scattering correction and loading compensation, attenuation coefficients were converted to absorption coefficients, and further to black carbon concentrations. A mass absorption coefficient (MAC) was used to quantify light absorption as a mass concentration. Absorption at 880 nm is generally assumed to be only caused by BC. Thus, the equivalent black carbon mass concentrations ($\:eBC$) was calculated (Eq. 1)

$$\:eBC=\frac{A\bullet\:\left(\frac{\varDelta\:ATN}{100}\right)}{{F}_{meas}\bullet\:\left(1-\zeta\:\right)\bullet\:\left(1-k\bullet\:AT{N}_{t}\right)*\varDelta\:t\bullet\:C\bullet\:MAC}\:,\:(eq.1)$$

where $\:A$ is the surface area of the filter spot, $\:\varDelta\:ATN$ the change of attenuation at 880nm during a time interval $\:\varDelta\:t$, $\:{F}_{meas}$ the measured flow rate, $\:\zeta\:$ the leakage factor (default value 0.01), $\:k$ the real-time loading compensation parameter³ $\:AT{N}_{t}$ the attenuation at time $\:t$ for 880nm, $\:C$ the multiple-scattering coefficient (here $\:C$ = 2.80 based on reference absorption measurement by PAX-870 during the campaign), and $\:MAC$ the mass absorption coefficient (here $\:MAC\left(880\:nm\right)$ = 5.47 m²/g, based on reference refractory black carbon (rBC) measurement by LII 300 and elemental carbon (EC) measurement by DRI 2015 during the campaign).

AMS data was treated in Tof-AMS Analysis Toolkit 1.65 (squirrel), and HR analysis was performed with ToF-AMS HR Analysis 1.25 (PIKA). Elemental analysis was performed by the Aiken method (aiken et al. 2007) The AMS was equipped to handle particles with an aerodynamic diameter between 42nm and 645nm. With small aerosol diameters, (supplementary table S12), falling outside the size range of the AMS.

Moreover, to the best of our knowledge no information is available on the density of aged aerosol emissions from ships but aging of aerosol emissions from solid fuel combustion demonstrate a particle size dependent increases in effective density with differences between fuels.³³ Therefor the mass of the aerosol is determined by the SMPS, with an assumed density of 1,5+-0,2 g/cm3. Composition of the aerosol is then calculated based on AMS and aethalometer as in Eq. 2.

$$\:{EF}_{x}=\left({EF}_{SMPS}-{EF}_{eBC}\right)\text{*}\frac{Con{c}_{x}}{Con{c}_{ams}},\:\:\:(eq.2)$$

Where $\:{EF}_{X}$ is the emission factor of an aerosol group, $\:Con{c}_{x}$ is the concentration of the aerosol group measured by the AMS, $\:{Conc}_{AMS}$ is the total concentration of aerosols measured by the AMS. $\:E{F}_{SMPS}$ is the emission factor determined by the SMPS and $\:E{F}_{eBC}$ is the emission factor of eBC determined by aethalometer. Primary organic aerosol (POA) was determined as the organic fraction with no photochemical aging. The SOA fraction was calculated by subtracting the POA from the total OA mass at a given simulated ageeq.3. Organic enhancement factor was calculated as the fractional increase of organics, see supplement equation Eq. 4.

$$\:SO{A}_{x}=O{M}_{x}-POA,\:\:\:\:\:(eq.3)$$

$$\:Or{g}_{enh,x}=\frac{O{M}_{x}}{POA},\:\:\:\:\:(eq.4)$$

Where POA is the total organic mass at 0 days of atmospheric aging and OMx is the total organic mass at X days of atmospheric aging.

Supporting Information

Additional experimental details, methods, fuel composition, model input & output and supporting tables (Supplement.docx)

Conflicts of interest

There are no conflicts to declare.

Author Contribution

A.P. wrote the main manuscript and prepared all figures.T.K., Z.F. and M.I. wrote parts of the methods segments in the main manuscript.U.E. prepared supplementary table 1-2.Data acquisition was conducted by A.P., T.K., Z.F., M.I., U.E. and H.C.All authors contributed to data analysis and interpretation.Supervision and funding by T.H.,H.C., O.S., Y.R., B.B. and R.Z.All authors revised the manuscript.Critical revision by T.H., H.C. T.K., Z.F., Y.R. and O.S.

Acknowledgement

We Thank the Helmholtz international Laboratory aeroHEALTH (InterLabs-0005; https://aerohealth.eu) and the ULTRHAS Horizon Europe project (agreement 955390) for supporting this work.

Data Availability

The datasets associated with the current study are available from the corresponding authors [[email protected] or [email protected]] on reasonable request.

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The impact of photochemical aging on secondary aerosol formation from a marine engine

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Abstract

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Introduction

Results and discussion

SOA formation from LS-HFO and MGO photooxidation

Elemental composition and oxidation pathway

Discussion

Methods

Declarations

Supporting Information

Conflicts of interest

Author Contribution

Acknowledgement

Data Availability

References

Additional Declarations

Supplementary Files

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