Impact of marine and continental sources on aerosol characteristics using an on-board SPAMS over southeast sea, China
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The chemical composition of atmospheric aerosols was characterized using an on-board single particle aerosol mass spectrometer (SPAMS) over the Southeast China Sea. High-time-resolution observation of marine aerosols was carried out to clarify the source of aerosols and the interaction of marine and continental aerosols. Atmospheric aerosols were determined by the interaction of continental and marine sources over coastal area. Aerosols from continental sources flux into sea surfaces through deposition or diffusion, which results in the rapid decrease of continental aerosols. Five main subtypes of carbonaceous particles are identified as C_Al-Si, C_V-Ni, C_S, C_K, and C_secondary to clarify the impact of marine and continental sources on atmospheric aerosols. High fraction of C_Al-Si and C_secondary is present over XA (Xiamen anchorage), accounting for 23.8% and 18.6% of total carbonaceous particles. Contrarily, the relative percentage of C_S increases as the distance from land to sea increases. The influence of continental aerosols declines, while the contribution of marine aerosols increases as the distance from land to sea increases. Air masses in XA, LSA (land to sea area), SLA (sea to land area), and SA (sea area) were all from ocean during the observation period, resulting in low relative fraction of continental aerosols in SLA, SA, and LSA. High-time-resolution measurement is useful to understand aerosol source types and the impact of marine and continental sources on marine atmosphere aerosols.
KeywordsMarine aerosol Chemical compositions Size distribution On-board observation Single particle aerosol mass spectrometer (SPAMS)
Marine aerosols have a significant contribution to atmospheric aerosols, which affect the atmospheric radiative budget by dictating the cloud condensation nuclei (CCN) population. (Woods et al. 2010; Gkikas et al. 2016; Decesari et al. 2011). Large quantities of aerosols were inevitably emitted into the atmosphere with the rapid development of economic and energy consumption (Yao et al. 2009; Ohlstrom et al. 2000; Yang et al. 2010; Wang 2018). Consequently, marine atmosphere is significantly impacted by the continental pollutant emissions, especially in the coastal zone adjacent to urban or industrial areas (Fu et al. 2015; Yan et al. 2015; Masalaite et al. 2017). More and more continental aerosols flux into the upper ocean through air-sea exchange with the increase of aerosol pollution emissions, causing the change of nutrient supply, which affected marine primary productivity and marine ecological environment (Zhang et al. 2013; Murphy et al. 2009).
The Southeastern China Sea (SECS) is a marginal zone adjacent to the southeast China with a subtropical climate under the influence of Asian monsoon. As a transitional area, northeasterly wind is the dominant wind direction in cold seasons. Air masses mainly come from northern China during wintertime, which makes aerosols transport from continent to SECS easily (Yan et al. 2015; Zhang et al. 2012). In this area, complex mixed aerosols are formed by the interaction of marine aerosols and anthropogenic particles (Falkowska and Lewandowska 2004; Chalbot et al. 2013). Studies on marine aerosols have been carried out, such as aerosol chemical characteristics, size distribution, and air-sea deposition fluxes, in recent years. (Kim et al. 2009; Nakamura et al. 2006; Chen et al. 2010). However, offline sampling methods were conducted in previous studies. Sampling time for 24 h or even several days was required to accommodate the detection limits (Zhang et al. 2007). However, atmospheric aerosols change rapidly due to the oxidation or reaction occurred on particle surfaces. Long sampling interval of aerosol is difficult to estimate with the atmospheric process of marine aerosols, which makes it hard to clarify the aging process of aerosols and the interaction between different aerosols using offline sampling methods (Yan et al. 2016). Therefore, high-time-resolution observation is important to investigate the rapid change of aerosol properties in marine atmosphere.
Online aerosol mass spectrometry has been widely used in atmospheric aerosol observation, since it is available to provide size and chemical information of aerosols (Sullivan et al. 2007; Spencer et al. 2007). Recently, two types of aerosol mass spectrometers (such as aerosol time-of-flight mass spectrometer (ATOFMS) and quadrupole aerosol mass spectrometer (AMS)) were used in marine aerosol observation to characterize chemical compositions, sources, and size distribution of marine aerosols (Fu et al. 2015; Phinney et al. 2006; Hoomaert et al. 2003; Gaston et al. 2011; O’Dowd et al. 2004). Phinney used an on-board AMS to investigate characteristics of marine aerosols over the North Atlantic Ocean. AMS only detects the volatile and semi-volatile components (such as SO42−, NO3−, NH4+, Cl−, and organics) and provides the mass concentration of these species (Jimenez et al. 2003). It is useful to investigate the formation of secondary aerosols and classify the organic species. However, it is hard to clarify the aerosol sources due to the undetectable refractory species by AMS. While ATOFMS can provide particle size distribution and chemical compositions (such as heavy metals, elemental carbon, organic carbon, SO42−, NO3−, NH4+, K+, Na+, Mg+) (Gaston et al. 2011), which makes it possible to investigate mixed state and source of aerosols. But ATOFMS just provide the particle number count without the mass concentration. Recently, a newly developed single particle aerosol mass spectrometer (SPAMS) was proverbially used in urban atmospheric aerosol monitoring to investigate their sources and chemical compositions (Murphy et al. 2006; Li et al. 2014; Ma et al. 2016; Bi et al. 2011). However, rare studies of marine aerosols using SPAMS were present, especially with an on-board SPAMS observation. Single particle aerosol mass spectrometer provides particle size and chemical compositions of single particle. In this study, an on-board SPAMS was deployed on “Xiang Yang Hong 03” vessel to investigate aerosol chemical components and particle sources in different sea areas. This study aims to understand the rapid variation of atmospheric aerosol chemical compositions and the influence of continental and marine sources on marine atmospheric aerosols over the SECS. The backward trajectory results were also present to evaluate the pollutant sources during the observation period. It provides an insight into the interaction between marine aerosols and continental aerosols over the offshore marine atmosphere.
Experimental methods and data
The observation was directed by “Xiang Yang Hong 03” of Third Institute of Oceanography. On-board SPAMS monitoring system was deployed in the vessel, and the cruise covered the Southeast China Sea (N 20o54′26″-24o24′35″, E 117o15′55″-118o30′36″). The vessel tracks are given in Fig. S1. The SPAMS instrument was equipped to a stabilized platform and held on a mobile laboratory located on the front deck of the vessel. The stabilized platform can adjust the swing range when the vessel jolted to ensure the safety and steady run of the instrument. Note that there is a potential influence of the self-contamination from the vessel on the measurement. To minimize the impact of the sampling vessel emission, the sampling inlet connecting to the SPAMS was fixed in the foremast, which was about 20 m above the sea level (seen in Fig. S2). Pollution emissions from the vessel are located at the downwind of the sampling inlet, when the vessel is running. A continuous observation was carried out from 11 to 24 June 2016. In this study, a total of 347,590 particles were detected by SPAMS.
On-board SPAMS and data analysis
The method for aerosol detection and operation procedure for the on-board SPAMS is similar with other single particle mass spectrometer, which has been described in detail by Li et al. (2014). Sampling gases are dried with a Nafion dryer before entering into the SPAMS. A PM2.5 collector was deployed to remove particles larger than 2.5 μm. Fine particles were drawn into the vacuum system through a critical orifice, which were accelerated and focused to form a particle beam. Particle with special velocity then passed through two continuous diode Nd:YAG lasers (532 nm). The aerodynamic diameter of single particle was calculated based on the particle velocity. Individual particle was then ionized by an Nd:YAG laser (266 nm) to produce positive and negative fragment ions. The power density of ionization laser was kept at 1.55 × 108 w.cm−2. Fragment ions were detected by a bipolar time-of-flight mass spectrometer. Polystyrene latex spheres (PSL Nanosphere Size Standards, Duke Scientific Corp., Palo Alto) with different diameter of 0.2, 0.3, 0.5, 0.72, 1.0, and 2.0 μm were used to calibrate the particle size for SPAMS. PbNO3 particles with diameter of 0.35 μm generated by an aerosol generation and monitoring system (AGM-1500, MSP Corporation, USA) were used to clarify the mass spectrum.
In this study, the integration time employed for the analysis was 30 min. The particle size and mass spectra information were analyzed using YAADA software toolkit (http://www.yaada.org/) (Allen 2005). An adaptive resonance theory using neural network algorithm (ART-2a) was applied to cluster individual particles into separate groups based on the presence and intensity of ion peaks in single particle mass spectrum (Song et al. 1999), with a vigilance factor of 0.65, learning rate of 0.05, and a maximum of 20 iterations.
Identification of carbonaceous types
Carbonaceous material includes organic carbon (OC) and elemental carbon (EC). Fragment ions of CxHyOz+, CxHyOz−, CxHy+, and CxHy− were used to classify the organic carbon, and Cn− and Cn+ were used to classify the element carbon. Carbonaceous particles were extracted from the total particles firstly. The rules used to classify different carbonaceous subtypes are as follows: (1) particles with ions of Al+ (m/z 27), Si+ (m/z 28), and SiO2− (m/z − 60) were classified as C_Al-Si particles; (2) particles containing V+ (m/z 51), VO+ (m/z 67), and Ni+ (m/z 58) ions in the positive spectrum, element carbon chain ions, and fewer organic ions in the positive and negative spectrum were classified as C_V-Ni particles; (3) particles with ions of MSA− (m/z − 95), HSO4− (m/z − 97) in the negative spectrum, and Mg+ (m/z 24) in the positive spectrum were classified as C_S particles; (4) particles with clear ions of K+ (m/z 39) and organic species were classified as C_K particles; and (5) particles with abundant secondary ions (m/z − 80 [SO3]−, − 97 [HSO4]−, − 46 [NO2]−, − 62 [NO3]−, 18 [NH4]+) were classified as C_secondary particles. Carbonaceous particles other than the above types accounted only about 3% of total carbonaceous. Hence, these particles were not discussed in this study.
Meteorological parameter and back trajectory (BT) analysis
Wind speed and direction were monitored by the weather station equipped in the vessel during the cruise. Air mass backward trajectory analysis was calculated by HYSPLIT_4 model to clarify the effect of source regions on marine atmospheric aerosols. The meteorological data used for the computation of the trajectories was obtained from the GDAS archive maintained by the Aerological Research Laboratory (ARL) (available at http://ready.arl.noaa.gov/gdasl.php).
Results and discussion
Spatial distribution of aerosol chemical characteristics
Compared with aerosol chemical compositions over XA, a significant change of aerosol species fraction was present over LSA. The species of NO3− and SO42− decreased dramatically, accounting for only 2% and 15%. While the mean relative percentage of EC, OC, and Na+ increased to 36%, 16%, and 23%, respectively. Note that NO3− and SO42− were mainly from anthropogenic emission. The decrease of NO3− and SO42− containing particles meant that the impact of continental aerosols declined. As mentioned above, EC was mainly from vehicle or ship emission, high fraction of EC containing particles over LSA was contributed by the ship emission. This can be further demonstrated by the mass spectra of carbonaceous clusters and the spatial distribution of carbonaceous materials (seen in Fig. 4 and Fig. 5). Atmospheric aerosols were governed by marine sources over SA. Sodium, representing the sea salt particles (Udisti et al. 2012), was the only dominated species over SA, accounting for 57% of the total particles. Contrarily, the relative fraction of SO42−, NO3−, and EC was extremely low, accounting for 2%, 2%, and 9%, respectively. That means continental sources have few impacts on atmospheric aerosols over SA, since most of continental aerosols deposit during the transport process from land to sea. Generally, SO42− aerosols were from marine sources or anthropogenic sources (Yan et al. 2013). The relative percentage of SO42− was 25%, 15%, and 2% over XA, LSA, and SA, respectively, suggesting that the contribution of SO42− species decreased as the distance from land to sea increased. That means SO42− aerosols were mainly from anthropogenic emission in the observation area. Contrarily, high relative percentage of OC (31%) was present over SA, comparing with the value over LSA (16%) and XA (11%). Organic species was used to investigate the contribution of different emission sources, such as fossil combustion, biomass emission, and marine biogenic source (Yin et al. 2012). Since continental sources have few influence on marine atmospheric aerosols over SA, high relative fraction of OC indicated that OC was mainly derived from the marine biogenic source in this area.
High relative fraction of EC, OC, and Na+ containing particles, accounting for 25%, 37%, and 29% with low relative fraction of NO3− and SO42− (3% and 4%) was present over SLA. The average fraction of NH4+ and SO42− was about 2% and 4% over LSA, which was lower than the value (8% of NH4+ and 15% of SO42−) obtained over LSA. Compared with aerosol chemical compositions over LSA, higher contribution of marine aerosols was present over LSA, though SLA is closer to shore area. Generally, the impact of continental sources on atmospheric aerosols increased when the location was closed to the shore. However, the contribution of continental aerosols over SLA was lower than over LSA in this study. Note that observations over LSA and SLA were not performed simultaneously. Higher wind speed was present over SLA during the observation episode, which contributed to higher fraction of marine aerosols, as the production of marine aerosols from whitecaps was enhanced with the increase of wind speed (Norris et al. 2013).
Variation of particle number from land to sea
To further clarify the variation of continental and marine aerosols from land to sea, the average aerosol particle number of different species (OC, EC, NH4+, SO42−, NO3−, and Na+) varies with the linear distance from Xiamen is given in Fig. 2b. The particle number of OC, EC, SO42−, and NO3− decreased rapidly during the first 100 km. The particle number of NH4+, SO42−, and NO3− was low and showed few changes when the linear distance from Xiamen exceeded 150 km. As seen in Fig. 2b, the SO42− and NO3− particle number showed a dramatically drop in the first 50 km, varying from 96 to 22 and 82 to 6, respectively, as the linear distance increased from 0 to 50 km. Previous studies have shown that anthropogenic nitric acid can react with sea salt to form coarse particles of sodium nitrate (NaNO3), increasing the deposition velocity of particles in the coastal area. Moreover, surface reactions also occurred between sulfuric acid and sea salt to produce sodium sulfate (Aller et al. 2005). Abundant sea salt particles in the atmospheric during this sea area accelerated the deposition of SO42− and NO3−. As mentioned above, low particle numbers of SO42− and NO3− suggested a weak impact of continental sources on atmospheric aerosols in these sea areas, which was in accordance with the observation results obtained in Fig. 1. SO42−, NO3−, and NH4+ are considered to be secondary aerosol species (Wang et al. 2006). However, the variation of NH4+ was different from that of SO42− and NO3−. Low particle number count of NH4+ was present in this study.
Compared with the species of SO42− and NO3−, the variations of OC and EC were more complicated. The OC particle number count was lower than the particle number count of EC and SO42− in the linear distance range from 0 to 150 km, while the particle number count of OC exceeded the other species as the linear distance was over 150 km. As mentioned above, except the fossil combustion source, OC was also derived from marine biogenic source. Biogenic aerosols were primarily emitted into the atmosphere through bubble bursting and had an important contribution to marine aerosols (Després et al. 2012 and O’Dowd et al. 2004). Significant positive correlation between OC and Na+ was present during the observation over XA, LSA, and SA, suggesting that Na+ and OC may have the same sources from marine bubble bursting in these areas. This can be certified by the variations of OC and Na+ fraction in Fig. 1. The fraction of OC was lower than that of Na+ and displayed the same variation trend in SA, LSA, and XA. But the relative fraction of OC was higher than the fraction of Na+ in SLA and became the most dominant component in atmospheric aerosols.
Particle size distribution in different areas
Carbonaceous particle signature and variation characteristics
Mass spectra characteristics of carbonaceous types
The average spectra of C_V-Ni particles are shown in Fig. 4b, which were dominated by Cn+ and Cn− peaks in positive and negative spectra. An evident intense of V+ peak with weak peaks of VO+, Ni+, and Na+ was also present in positive spectrum. Note that V+ and Ni+ containing particles were regarded as a suitable tracer for ship emission. The presence of V+, VO+, and Ni+ in the C_V-Ni particles indicated that those particles were from ship emission. The lack of NO2−, NO3−, and SO42− fragment ions in C_V-Ni particles indicated that this type of C_V-Ni particles has not been aged in the atmosphere. NO2−, NO3−, and SO42− were considered to be the secondary species in atmospheric aerosols, and the uptake of these species on EC particles was often observed in aged aerosols (Zhang et al. 2007).
C_S was characterized by peaks associated with K+, Na+, Mg+, NaCl+, and oxygenated organics (CxHyOz) in positive spectrum, as seen in Fig. 4c. Strong peaks for methanesulfonic acid (MSA−) and HSO4− with weak peaks of CNO− and CHNO− were present in negative spectrum. MSA− was the oxidation product of dimethylsulfide (DMS) in the atmosphere (Zhang et al. 2015), which was an important marine biogenic gas oxidized by OH−, BrO−, and NO3− radicals by addition and abstraction reaction routs (Von Glasow and Crutzen 2004; Legrand and Pasteur 1998). Intense peaks of MSA− and HSO4− in C_S particles indicated that this type of particles was mainly from the secondary conversion of DMS, deriving from the marine biological activity.
C_K particles were characterized by a high intense peak of K+ with weak intense Na+ and Ca+ ion peaks in positive spectrum, seen in Fig. 4d. While high intense peaks of CN−, CNO−, CHNO−, and C2H3O2− with weak peaks of SO42−, O−, and OH− were observed in negative spectrum. Generally, K+ was identified as a suitable tracer for biomass burning particles (Spencer et al. 2007; Guazzotti et al. 2003.). However, biomass burning was not the only source of K particles. Previous study showed that particles from coal combustion or biological activity emission also contributed to the source of K particles (Wang et al. 2013; Ma et al. 2016). As seen in Fig. 4d, the presence of Na+ and Ca+ and the lack of carbonaceous species suggested that this type of C_K particles was influenced by the emission of marine biological activity. Studies have found that K containing particles can also be associated with marine sources by the bubble bursting (Yan et al. 2013).
C_secondary particles were dominated by intense CxHy+ and CxHyOz+ peaks with weak peak of Na+ in positive spectrum, as seen in Fig. 4e. While high ion peaks of NO2−, NO3−, and SO42−, C2H2+ with weak peaks of O−, OH−, CN−, CNO−, and SO32− were present in negative spectrum. SO42−, NO3−, and NH4+ were believed as derived mainly from secondary pollution particles produced by the transformation of their precursors of SO2, NO2, and NH3 (Wang et al. 2006). Generally, the heterogeneous reaction uptake of secondary species on the surfaces of primary aerosol particles was much easier than homogeneous reaction in the atmosphere (Yu and Turco 2011). Hence carbonaceous species often mixed with secondary sulfate and nitrate species. High percentage of C_secondary particles was observed over XA, as seen in Fig. 5. The contribution of this type of particles decreased rapidly with the increase of linear distance between the observation location and land. Relatively abundant gas precursors and high aerosol concentration with high value of RH were observed over XA, which was prone to the formation of secondary particles in this area (Foltescu et al. 1996). However, the aerosol number and gas precursors declined as the distance between observation location and continent increased, resulting in the decrease of secondary particles.
Variation characteristics of carbonaceous particles
Figure 5 shows the average fraction of different carbonaceous particle types, and the total carbonaceous particle number varies with the linear distance from Xiamen. The total carbonaceous particle number displayed a decreasing tendency as the linear distance from land to sea increased, suggesting that the carbonaceous aerosols were strongly influenced by the continental sources. However, note that the carbonaceous particle number increased as the linear distance increased from 300 to 350 km. Compared with the average fraction given in 300 km, the percentage of C_V-Ni type particles increased from 16.5 to 32.1%. As mentioned above, C_V-Ni particles were mainly from ship emission. Hence, the increase of carbonaceous particles was determined by the ship emission aerosols in this area.
As seen in Fig. 5, high fraction of C_Al-Si particles and C_secondary particles was observed over coastal area, accounting for 23.8% and 18.6%, individually. But the fraction of both type of particles decreased as the linear distance from land to sea increased. Contrarily, the relative percentage of C_S showed an increasing tendency as the linear distance from land to sea increased. Therefore, C_Al-Si and C_secondary particles were determined by the continental sources, while the C_S particles were strongly affected by marine sources, which were accord with the particle cluster analyses obtained in Fig. 4. However, the variation of C_V-Ni particles was more complex in this study. This type of particles was mainly from the primary ship emission. Hence, the type of C_V-Ni particles was concerned with the vessel activity in this area but not the distance from land.
Characteristics of particle sources in different sea areas
A high-time-resolution on-board single particle aerosol mass spectrometer (SPAMS) was deployed on “Xiang Yang Hong 03” vessel to measure size and chemical composition of single marine aerosol simultaneously over Southeastern China Sea to provide the impact of continental and marine sources on atmospheric aerosols over the coastal areas. The observation areas were divided into four main parts, Xiamen anchorage (XA), land to sea area (LSA), sea area (SA), and sea to land area (SLA). Sulfate, nitrate, Na+, and carbonaceous (including OC and EC) were the dominant aerosol species over XA, accounting for 25%, 21%, 19%, and 32%, representing the coastal urban area. LSA and SLA represented the interaction of continental and marine sources, as abundance of Na+, NO3−, SO42−, and OC were present in these areas. Atmospheric aerosols were governed by marine sources over SA with 57% of Na+ containing particles of the total particles. The particle number of OC, EC, SO42−, and NO3− decreased rapidly during the first 100 km from land to sea. The particle number of NH4+, SO42−, and NO3− containing particles was low and showed few changes when the linear distance from Xiamen exceeded 150 km.
Carbonaceous material, including organic carbon (OC) and elemental carbon (EC), was the major dominant aerosol components in this study, accounting for 31%, 52%, 40%, and 62% over XA, LSA, SA, and SLA, respectively. The source and variation of carbonaceous species in the observation areas were more complex than other aerosol species. Five major subtypes of carbonaceous particles were identified as C_Al-Si, C_V-Ni, C_S, C_K, and C_secondary based on the mass spectral similarity. High fraction of C_Al-Si particles and C_secondary particles was observed in coastal area, accounting for 23.8% and 18.6%. But the fraction of both types decreased, as the distance from land to sea increased. Contrarily, the relative percentage of C_S showed an increasing tendency, as the distance from land to sea increased. The variation of C_V-Ni containing particles was strongly influenced by the vessel activity in the observation areas.
In this study, six major classes were identified based on the mass spectra from SPAMS and clustered using ART-2a algorithm, including sea salt particles, secondary aerosols, K-rich particles, heavy metal particles, EC, and OC particles. The atmospheric aerosols were dominated by the interaction of continental and marine sources over XA. High fraction of secondary aerosols was observed over XA, while the value was extremely low in other sea areas. This was caused by air masses transport during the observation period, since most of the trajectories were from the ocean during the observation period.
The authors gratefully acknowledge Guangzhou Hexin Analytical Instrument Company Limited for the SPAMS data analysis and on-board observation technical assistance. The authors gratefully acknowledge NOAA Air Resources laboratory (ARL) for the provision of the HYSPLIT_4 transport model used in this publication.
This study is financially supported by Qingdao National Laboratory for marine science and technology (No. QNLM2016ORP0109), the Natural Science Foundation of Fujian Province, China (No. 2015J05024), the National Natural Science Foundation of China (No. 21106018 and No. 41305133), the Scientific Research Foundation of Third Institute of Oceanography, SOA. (No. 2014027), and the Special Fund for Marine Researches in the Public Interest (No. 2004DIB5J178).
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