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Articles and Their Chemical Composition Were Performed Rural Site Atmos. Chem. Phys., 16, 8831–8847, 2016 www.atmos-chem-phys.net/16/8831/2016/ doi:10.5194/acp-16-8831-2016 © Author(s) 2016. CC Attribution 3.0 License. Aerosol source apportionment from 1-year measurements at the CESAR tower in Cabauw, the Netherlands Patrick Schlag1,2, Astrid Kiendler-Scharr2, Marcus Johannes Blom3, Francesco Canonaco4, Jeroen Sebastiaan Henzing5, Marcel Moerman5, André Stephan Henry Prévôt4, and Rupert Holzinger1 1Institute for Marine and Atmospheric Research Utrecht (IMAU), Utrecht University, Utrecht, the Netherlands 2Institute for Energy and Climate Research (IEK-8): Troposphere, Forschungszentrum Jülich, Jülich, Germany 3Energy Research Centre of the Netherlands (ECN), Petten, the Netherlands 4Laboratory of Atmospheric Chemistry, Paul Scherrer Institute (PSI), Villigen, Switzerland 5Netherlands Organisation for Applied Scientific Research (TNO), Utrecht, the Netherlands Correspondence to: Patrick Schlag ([email protected]) Received: 10 November 2015 – Published in Atmos. Chem. Phys. Discuss.: 15 December 2015 Revised: 17 June 2016 – Accepted: 28 June 2016 – Published: 19 July 2016 Abstract. Intensive measurements of submicron aerosol mospheric aging processes for aerosol concentration at this particles and their chemical composition were performed rural site. Due to the large secondary fraction, the reduction with an Aerosol Chemical Speciation Monitor (ACSM) at of particulate mass at this rural site is challenging on a local the Cabauw Experimental Site for Atmospheric Research scale. (CESAR) in Cabauw, the Netherlands, sampling at 5 m height above ground. The campaign lasted nearly 1 year from July 2012 to June 2013 as part of the EU-FP7- ACTRIS project (Q-ACSM Network). Including equivalent 1 Introduction black carbon an average particulate mass concentration of 9.50 µg m−3 was obtained during the whole campaign with Atmospheric aerosols have large impacts on the climate di- dominant contributions from ammonium nitrate (45 %), or- rectly by scattering and absorbing shortwave radiation. Be- ganic aerosol (OA, 29 %), and ammonium sulfate (19 %). sides the resulting influence on the visibility (Ramanathan et There were 12 exceedances of the World Health Organiza- al., 2007; Romanou et al., 2007), this can have a cooling or −3 tion (WHO) PM2:5 daily mean limit (25 µg m / observed at heating effect on the atmosphere (IPCC, 2013). The indirect this rural site using PM1 instrumentation only. Ammonium effect refers to the impact of particles on cloud formation and nitrate and OA represented the largest contributors to total their properties. particulate matter during periods of exceedance. In addition, particles can adversely impact human health Source apportionment of OA was performed season-wise by, e.g., increasing the probability of cardiopulmonary by positive matrix factorization (PMF) using the multilin- and lung cancer mortality (Pope et al., 2002). The World ear engine 2 (ME-2) controlled via the source finder (SoFi). Health Organization (WHO) recently estimated that, glob- Primary organic aerosols were attributed mainly to traffic ally, 3.7 million deaths were attributable to ambient air pol- (8–16 % contribution to total OA, averaged season-wise) lution in both cities and rural areas in 2012 (EU, 2008). This and biomass burning (0–23 %). Secondary organic aerosols mortality is reported to be due to exposure to small particu- (SOAs, 61–84 %) dominated the organic fraction during the late matter (PM10/, which can cause cardiovascular and res- whole campaign, particularly on days with high mass load- piratory disease and cancers. Particles with smaller diame- ings. A SOA factor which is attributed to humic-like sub- ters such as PM2:5 or PM1 are reported to have enhanced stances (HULIS) was identified as a highly oxidized back- toxicological effects since they can deposit more deeply in ground aerosol in Cabauw. This shows the importance of at- the respiratory system and remain suspended for longer pe- riods of time (Pope and Dockery, 2006). Therefore, a num- Published by Copernicus Publications on behalf of the European Geosciences Union. 8832 P. Schlag et al.: Aerosol source apportionment from 1-year measurements ber of institutions established several air quality standards for olution. Due to the high amount of maintenance from skilled different particle sizes to limit aerosol mass. The WHO air and trained personnel needed for continuous operating mea- quality guideline (global update 2005, WHO, 2006) defines surement, campaigns using an AMS usually do not exceed 1 −3 a PM2:5 daily mean limit of 25 µg m and a PM2:5 annual or 2 months (Sun et al., 2012). Since the variation of aerosol mean limit of 10 µg m−3. The European Union Air Quality composition is very high depending on measurement site Directive 2008/50/EC provides only a target value of the an- and season (Jimenez et al., 2009), long-term measurements −3 nual mean limit of PM2:5 of 25 µg m (EU, 2008). (≥ 1 year) are clearly needed. At a European level, this effort Air quality and climate effects are not only dependent on is supported by the Aerosols, Clouds and Traces gases Re- the particle number concentration and size but also on their search InfraStructure network (ACTRIS) program that aims chemical composition. This information is not only relevant at pooling high-quality data from state-of-the-art instrumen- to investigate the nature and magnitude of each effect but also tation, such as the Aerodyne Aerosol Chemical Speciation for the identification and quantification of aerosol sources Monitor (ACSM). The quadrupole ACSM (Q-ACSM) is spe- and mitigation strategies for a potential reduction of aerosol cially designed for long-term continuous and real-time mea- mass concentrations. Major inorganic components of PM1 surements of mass concentrations and composition of NR- consist mainly of ammonium nitrate (NH4NO3/ and ammo- PM1 species (Ng et al., 2011b). nium sulfate ((NH4/2SO4/, formed in the presence of ammo- In this study, an ACSM was used to measure the submi- nia (NH3/, nitrogen oxides (NOx is NO plus NO2/, and sul- cron aerosol chemical composition from 11 July 2012 to fur dioxide (SO2/, respectively (Seinfeld and Pandis, 2006). 3 June 2013 at the CESAR tower in Cabauw, the Nether- Therefore, NH4NO3 and (NH4/2SO4 are strongly attributed lands, as part of the EU-FP7-ACTRIS project. A collocated to anthropogenic sources (Finlayson-Pitts and Pitts, 2000). multi-angle absorption photometer (MAAP, Thermo Scien- Since inorganic aerosols are formed by gaseous precursors tific Model 5012) provided equivalent black carbon (eBC) in the atmosphere, the condensed products are considered as data. Organic aerosol data were further analyzed by positive secondary aerosols, while primary aerosols like black carbon matrix factorization using the multilinear engine 2 (ME-2) (BC) are emitted directly. (Paatero, 1999) via the source finder (SoFi, Canonaco et al., In contrast, organic aerosols (OAs), which can also be of 2013). This data set shows the long-term variability of parti- primary (POA) or secondary (SOA) origin, consist of up to cle composition and is used for source apportionment of at- hundreds of thousands of different molecules (Goldstein and mospheric aerosols at this northwestern European rural site, Galbally, 2007), where SOA contributes on average 70 % to with the focus on periods where air quality standards were organic aerosol mass (Hallquist et al., 2009). SOA is formed violated. Information about aerosol composition and their by gas-to-particle conversion of atmospherically oxidized sources especially during pollution events can be further used semi- and low-volatile organic compounds (VOCs). Guen- to establish strategies for the reduction of particulate matter. ther et al. (1995) estimated a global VOC budget in the order of 1150 Tg carbon per year. Biogenic VOCs (BVOCs) con- tribute approximately 90 % of total VOC, including isoprene 2 Methodology (50 % of total BVOCs), monoterpenes (15 %), and sesquiter- 2.1 Site description: CESAR penes (3 %) (Guenther et al., 2012). In turn, 10 % of emitted VOCs are of anthropogenic origin, including, e.g., alkanes, The CESAR tower is 220 m high and managed and operated alkenes, benzene, and toluene. by the Royal Netherlands Meteorological Institute (KNMI, The investigation of the aerosol composition is critical for the Netherlands). It is located in a rural site (51.970◦ N, the development of climate models, since the composition 4.926◦ E) near Cabauw, the Netherlands, about 20 km south- influences important particle properties. However, its deter- west of the city of Utrecht and about 45 km southeast of the mination is still challenging, especially in case of OAs, which Dutch North Sea coast. The site conditions are typical for contribute significantly to atmospheric particulate matter northwestern Europe. They can either be maritime or conti- (Jimenez et al., 2009). In fact, the lack of knowledge on nental, depending on the wind direction. The surface eleva- particle composition is a key contribution to the large un- tion changes in the surrounding area are, at most, a few me- certainty for the determination of the total anthropogenic ra- ters over 20 km. The tower ground is approximately 0.7 m be- diative forcing (IPCC, 2013). low sea level; the diurnal variation of the temperature is rel- The development of online aerosol mass spectrometric atively stable (Vermeulen et al., 2011). The direct surround- techniques during the last decades enhanced the possibilities ings of the tower have a relatively low population density. to investigate aerosol chemical composition in real time (De- The nearby region is used mainly by agriculture, with a mix- Carlo et al., 2006; Jayne et al., 2000; Jimenez et al., 2003). ture of intensively and extensively managed grassland. These The Aerosol Mass Spectrometer (AMS, Aerodyne Research are used also for keeping animals like cattle and sheep beside Inc., Billerica, MA, USA) is a powerful instrument to quanti- nearby chicken farms. tatively measure the chemical composition of the nonrefrac- tory fraction of PM1 (NR-PM1/ with high time and mass res- Atmos.
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