[1] The existence of gas-phase ammonia (NH 3 ) in the atmosphere and its interaction with other trace chemical species could have a substantial impact on tropospheric chemistry and global climate change. China is a large agricultural country with an enormous animal population, tremendous nitrogen fertilizer consumption and, consequently, a large emission of NH 3 . Despite the importance of NH 3 in the global nitrogen (N) cycle, considerable inaccuracies and uncertainty exist regarding its emission in China. In this study, a comprehensive NH 3 emission inventory was compiled for China on a 1 km  1 km grid, which is suitable for input to atmospheric models. We attempted to estimate NH 3 emissions accurately by taking into consideration as many native experiment results as possible and parameterizing the emission factors (EFs) by the ambient temperature, soil acidity and other factors. The total NH 3 emission in China was approximately 9.8 Tg in 2006. The emission sources considered included livestock excreta (5.3 Tg), fertilizer application (3.2 Tg), agricultural soil (0.2 Tg), nitrogen-fixing plants (0.05 Tg), crop residue compost (0.3 Tg), biomass burning (0.1 Tg), urine from rural populations (0.2 Tg), chemical industry (0.2 Tg), waste disposal (0.1 Tg) and traffic (0.1 Tg). The regions with the highest emission rates are located in Central and Southwest China. Seasonally, the peak ammonia emissions occur in spring and summer.

Ammonia (NH 3 ) can interact in the atmosphere with other trace chemical species, which can lead to detrimental environmental consequences, such as the formation of fine particulates and ultimately global climate change. China is a major agricultural country, and livestock numbers and nitrogen fertilizer use have increased drastically since 1978, following the rapid economic and industrial development experienced by the country. In this study, comprehensive NH 3 emissions inventories were compiled for China for 1980-2012. In a previous study, we parameterized emissions factors (EFs) considering ambient temperature, soil acidity, and the method and rate of fertilizer application. In this study, we refined these EFs by adding the effects of wind speed and new data from field experiments of NH 3 flux in cropland in northern China. We found that total NH 3 emissions in China increased from 5.9 to 11.1 Tg from 1980 to 1996, and then decreased to 9.7 Tg in 2012. The two major contributors were livestock manure and synthetic fertilizer application, which contributed 80-90 % of the total emissions. Emissions from livestock manure rose from 2.86 Tg (1980) to 6.16 Tg (2005, and then decreased to 5.0 Tg (2012); beef cattle were the largest source followed by laying hens and pigs. The remarkable downward trend in livestock emissions that occurred in 2007 was attributed to a decrease in the numbers of various livestock animals, including beef cattle, goats, and sheep. Meanwhile, emissions from synthetic fertilizer ranged from 2.

In order to understand the aging and processing of organic aerosols (OA), an intensive field campaign (Campaign of Air Pollution at Typical Coastal Areas IN Eastern China, CAPTAIN) was conducted March–April at a receptor site (a Changdao island) in central eastern China. Multiple fast aerosol and gas measurement instruments were used during the campaign, including a high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) that was applied to measure mass concentrations and non-refractory chemical components of submicron particles (PM₁^nr). The average mass concentration of PM₁(PM₁^nr+black carbon) was 47 ± 36 μg m⁻³ during the campaign and showed distinct variation, depending on back trajectories and their overlap with source regions. Organic aerosol (OA) is the largest component of PM₁ (30%), followed by nitrate (28%), sulfate (19%), ammonium (15%), black carbon (6%), and chloride (3%). Four OA components were resolved by positive matrix factorization (PMF) of the high-resolution spectra, including low-volatility oxygenated organic aerosol (LV-OOA), semi-volatile oxygenated OA (SV-OOA), hydrocarbon-like OA (HOA) and a coal combustion OA (CCOA). The mass spectrum of CCOA had high abundance of fragments from polycyclic aromatic hydrocarbons (PAHs) (m/z 128, 152, 178, etc.). The average atomic ratio of oxygen to carbon in OA (O / C) at Changdao was 0.59, which is comparable to other field studies reported at locations downwind of large pollution sources, indicating the oxidized nature of most OA during the campaign. The evolution of OA elemental composition in the van Krevelen diagram (H / C vs. O / C) showed a slope of −0.63; however, the OA influenced by coal combustion exhibits a completely different evolution that appears dominated by physical mixing. The aging of organic aerosols vs. photochemical age was investigated. It was shown that OA / ΔCO, as well as LV-OOA / ΔCO and SV-OOA / ΔCO, positively correlated with photochemical age. LV-OOA accounted for 73% of the OA secondary formation (SOA) in the oldest plumes (photochemical age of 25 h). The k_OH at Changdao, by assuming SOA formation and aging as a first-order process proportional to OH, was calculated to be 5.2 × 10⁻¹² cm³ molec.⁻¹ s⁻¹, which is similar to those determined in recent studies of polluted air in other continents