Origin of the water-soluble organic nitrogen in the maritime aerosol
Introduction
Investigations of organic nitrogen species in the ambient aerosols have been conducted at many areas around the world including urban, suburban, rural, and remote sites (e.g., Cornell et al., 2001, Zhang et al., 2002, Mace et al., 2003a, Mace et al., 2003b, Mace et al., 2003c, Nakamura et al., 2006, Calderón et al., 2007, Duan et al., 2009, Lin et al., 2010, Shi et al., 2010, González Benítez et al., 2010, Violaki and Mihalopoulos, 2010, Miyazaki et al., 2011, Miyazaki et al., 2014, Matsumoto et al., 2014). Many of these previous studies have reported that about 10–60% of the water-soluble nitrogen in the aerosol is of an organic form.
The water-soluble organic nitrogen (WSON) has been recognized to account for a significant fraction of particulate nitrogen, but its sources have not yet been sufficiently clarified. Various potential sources including both primary and secondary processes have been suggested in previous studies. Higher concentrations of the particulate WSON in the air masses affected by anthropogenic activities have been often reported (Shi et al., 2010, Violaki and Mihalopoulos, 2010, Matsumoto et al., 2014, Violaki et al., 2015), indicating significant influences of anthropogenic activities on the particulate WSON. The contribution of soil dust (Nakamura et al., 2006, Lesworth et al., 2010), biomass burning (Mace et al., 2003a, Zamora et al., 2011), and terrestrial vegetation (Miyazaki et al., 2014, Matsumoto et al., 2014) to the particulate WSON has also been reported in previous studies. On the other hand, marine biota has been suggested as a source of the particulate WSON in the remote marine atmosphere (Violaki et al., 2015, Altieri et al., 2016).
Our previous report demonstrated that the particulate WSON in the urban and forested atmospheres is derived from a similar production process with the particulate NH4+; that is, a reaction of its basic precursor gases with particulate or gaseous acidic species, such as H2SO4 and HNO3 (Matsumoto et al., 2014), which would be supported by the facts that basic amine compounds have been detected both in the particulate and gaseous phases (Ge et al., 2011 and references therein), and that the WSON was also detected in the gas phase and a large portion of the gaseous WSON was basic (Matsumoto and Yamato, 2017). The acid-catalyzed accretion reaction in the acid particulate phase has also been considered to be a potential production process for the particulate WSON (Wang et al., 2010, Miyazaki et al., 2014). This reaction has been suggested as a secondary production process of particulate organic species, especially high-molecular-weight organics, in many recent studies (e.g., Jang et al., 2002, Surratt et al., 2007).
For discussing the source of the WSON in the atmosphere, the correlation analysis with species of known source has been used in many previous studies as an effective tool (Cape et al., 2011). In this paper, we discuss the production process for the particulate WSON in the maritime atmosphere by the measurements of the WSON and the associated species in the aerosols and the correlation analysis between them.
Section snippets
Sample collection
Air sampling was conducted at the coastal site on Rishiri Island near the northern tip of Japan, of which the location is shown in Fig. 1. The sampling site was surrounded by scrub and away from the coastal line at a distance of about 800 m. There is a small residential area with a population of about 500 and a small fishing port about 1 km from the site. Other town areas on the island are also small and farther away from the site. The total population on the island is only about 4800. The
Measurements of the WSON in the aerosols
Measurements of the nitrogen species in the aerosols are summarized in Table 1. The WSON accounted for about 13% of the WSTN in the fine particles and particulate matter (fine + coarse particles). Similar ratios have been reported in our previous studies at urban and forested sites; about 16% and 13%, respectively, in the particulate matter (Matsumoto et al., 2014), and other previous studies; for instance, 9% in the particulate matter collected over the remote tropical Atlantic Ocean (Violaki
Summary
Measurements of the WSON and the associated species in the aerosols were conducted at the coastal site on Rishiri Island near the northern tip of Japan to clarify the production process for the particulate WSON in the maritime atmosphere.
The mean concentration of the WSON in the particulate matter (fine + coarse particles) was 0.077 μg m−3, which was within the previous measurements from the remote or rural clean sites. About 90% of the particulate WSON was detected in the fine-mode range
Acknowledgment
The authors gratefully acknowledge the NOAA Air Resources Laboratory (ARL) for the provision of the HYSPLIT transport and dispersion model and/or READY website (http://www.ready.noaa.gov) used in this publication. This study was financially supported by JSPS KAKENHI (Grant Number 25281002) and the Sumitomo Foundation (Grant Number 083226), and partly supported by the GRENE Arctic Climate Change Research Project of the Ministry of Education, Culture, Sports, Science, and Technology of Japan.
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