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Articles, Acid Rain, and Eu- Ditions Atmos. Chem. Phys., 18, 167–184, 2018 https://doi.org/10.5194/acp-18-167-2018 © Author(s) 2018. This work is distributed under the Creative Commons Attribution 3.0 License. Role of ambient ammonia in particulate ammonium formation at a rural site in the North China Plain Zhaoyang Meng1, Xiaobin Xu1, Weili Lin2,a, Baozhu Ge3, Yulin Xie4,5, Bo Song4, Shihui Jia1,6, Rui Zhang7,8, Wei Peng1, Ying Wang1, Hongbing Cheng1, Wen Yang7, and Huarong Zhao1 1State Key Laboratory of Severe Weather & Key Laboratory for Atmospheric Chemistry of CMA, Chinese Academy of Meteorological Sciences, Beijing 100081, China 2CMA Meteorological Observation Centre, Beijing 100081, China 3State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China 4University of Science and Technology Beijing, Beijing 100083, China 5Baotou Steel Group Mining Research Institute, Baotou 014010, China 6South China University of Technology, Guangzhou 510641, China 7Chinese Research Academy of Environmental Sciences, Beijing 100012, China 8Beijing Municipal Research Institute of Environmental Protection, Beijing 100037, China anow at: College of Life and Environmental Sciences, Minzu University of China, Beijing 100081, China Correspondence: Zhaoyang Meng ([email protected]) Received: 26 February 2017 – Discussion started: 26 April 2017 Revised: 16 November 2017 – Accepted: 20 November 2017 – Published: 8 January 2018 2− Abstract. The real-time measurements of NH3 and trace namic equilibrium model ISORROPIA-II. Modelled SO , − 4 gases were conducted, in conjunction with semi-continuous NO , and NH3 values agree well with the measurements, 3 C measurements of water-soluble ions in PM2:5 at a rural site in while the modelled NH4 values largely underestimate the the North China Plain (NCP) from May to September 2013 measurements. Our observation and modelling results indi- in order to better understand chemical characteristics of am- cate that strong acids in aerosol are completely neutralised. monia and the impact of secondary ammonium aerosols on Additional NHC exists in aerosol, probably a result of the C 4 formation in the NCP. Extremely high NH3 and NH4 con- presence of a substantial amount of oxalic and other diacids. centrations were observed after a precipitation event within 7–10 days following urea application. Elevated NH3 levels C coincided with elevated NH4 , indicating that NH3 likely influenced particulate ammonium mass. For the sampling 1 Introduction C period, the average conversion = oxidation ratios for NH4 (NHR), SO2− (SOR), and NO− (NOR) were estimated to be Ammonia (NH3/ is a very important alkaline constituent 4 3 in the atmosphere, plays an important role in atmospheric 0.30, 0.64, and 0.24, respectively. The increased NH3 con- centrations, mainly from agricultural activities and regional chemistry and is closely related to ecosystems. NH3 has transport, coincided with the prevailing meteorological con- both direct and indirect impacts on critical environmental issues, including regional fine particles, acid rain, and eu- ditions. The high NH3 level with NHR of about 0.30 indi- trophication (Roelle and Aneja, 2002; Krupa, 2003; Reche cates that the emission of NH3 in the NCP is much higher et al., 2015). In addition, NH is a key species for neu- than needed for aerosol acid neutralisation, and NH3 plays an 3 important role in the formation of secondary aerosols as a key tralising H2SO4 and HNO3 in the atmosphere and forming neutraliser. The hourly data obtained were used to investigate (NH4/2SO4, NH4HSO4, and NH4NO3 (Erisman and Schaap, gas–aerosol partitioning characteristics using the thermody- 2004; Walker et al., 2004), which are major inorganic com- ponents of fine particulate matters and contribute to regional Published by Copernicus Publications on behalf of the European Geosciences Union. 168 Z. Meng et al.: Role of ambient ammonia in particulate ammonium formation haze (Ye et al., 2011; Meng et al., 2014; Wei et al., 2015). logical Observation and Experiment Station of the Chinese Global ammonia emission has more than doubled since pre- Academy of Meteorological Sciences. In Fig. 1, the location industrial times, mainly because of agricultural intensifica- of the site is shown on the NCP map with the NH3 emission tion (Galloway et al., 2003). The total ammonia emission in distribution for the year 2012 from the multi-resolution emis- China in 2006 was estimated to be 16.07 million tonnes (Mt) sion inventory of China (http://meicmodel.org/index.html). (Dong et al., 2010). Such high emission makes NH3 one of The measurement site chosen is situated for monitoring re- the key species related to atmospheric environmental prob- gional background concentrations of air pollutants in the lems. Some studies have indicated that reducing NH3 con- North China Plain and has good regional representativeness centrations could be an effective method for alleviating sec- (Lin et al., 2009). The site is approximately 110 km south- ondary inorganic PM2:5 pollution in China (Cao et al., 2009; west of Beijing, 130 km west of Tianjin, and 160 km north- Park et al., 2014; Wang et al., 2015; Xu et al., 2017). east of Shijiazhuang city in Hebei Province. The site is sur- As global food production requirements increase, agricul- rounded by farms, dense villages/towns, and the transporta- ture plays an increasingly important role in local, regional, tion network in the NCP. The main crops in the area sur- and global air quality (Walker et al., 2006). The North China rounding the site are wheat (winter and spring) and corn Plain (NCP) is a highly populated region with intensive agri- (summer and fall). The site is influenced by high NH3 emis- cultural production as well as heavy industry. The region has sions from fertiliser use and animal husbandry in the sur- been affected by severe haze and photochemical pollution in rounding area. Being in the warm temperate zone, the site recent years (Guo et al., 2010; Wang et al., 2010; Luo et al., has a typical temperate continental monsoon climate. Precip- 2013). Covering only 3.3 % of the national area, the NCP re- itation occurs mainly between May and August. gion provides 40 and 25 % of China’s wheat and corn produc- tion. To sustain such high agricultural productivity, chemical 2.2 Sampling and analysis fertilisers have been intensively applied. Less than 30 % ef- ficiency in N application causes approximately 40 % N loss Ambient NH3 was measured using an ammonia analyser − through various routes including the leaching of NO3 and (DLT-100, Los Gatos Research, USA), which utilises a emission of NH3,N2O, and N2 (Zhang et al., 2010). So far, unique laser absorption technology called off-axis integrated only a few limited studies have paid attention to the impacts cavity output spectroscopy. The analyser has a precision of of NH3 on air pollution in the NCP region. According to 0.2 ppb at a 100 s average and a maximum drift of 0.2 ppb some studies (Dong et al., 2010; Ianniello et al., 2010; Meng over 24 h. The response time of the analyser is less than 2 s et al., 2011, 2015; Shen et al., 2011), the high NH3 emis- (with an optional external N920 vacuum pump). During the sion intensities observed in the NCP have been caused by campaign, NH3 data were recorded at a 100 s average. In high fertiliser application rates and numerous intensive live- principle, the NH3 analyser does not need external calibra- stock farms. However, there were few simultaneous high- tion because the measured fractional absorption of light at an C time-resolution measurements of NH3 and NH4 in PM2:5 ammonia resonant wavelength is an absolute measurement that also investigated the role in fine particulate formation of the ammonia density in the cell (manual of economical in China. These studies are necessary to improve our under- ammonia analyser – benchtop model 908-0016, Los Gatos standing of ammonia pollution on regional air quality and of Research). However, we confirmed the good performance of the impact on formation of secondary ammonium aerosols in the NH3 analyser using a reference gas mixture NH3 = N2 the NCP. (Air Liquide, USA) traceable to the US National Institute for During May–September 2013, the intensive field measure- Standards and Technology (NIST). The reference gas of NH3 ments of NH3 and other trace gases, water-soluble ions in (25.92 ppm with an accuracy of ±2 %) was diluted to differ- PM2:5, and meteorological parameters took place at a rural ent concentrations using zero air and supplied to the analyser, site in the NCP. In this article, we report the results on NH3, and a sequence with five points of different NH3 concentra- trace gases and major water-soluble ions in PM2:5. We dis- tions (including zero and the concentrations ranging from 45 cuss temporal variations in and diurnal patterns of NH3 and to 180 ppb) were repeated for several times to check the per- C NH4 . We also show results from thermodynamic equilibrium formance of the analyser. simulations and compared them with observations. As shown in Fig. S1 in the Supplement, the analyser rapidly followed changes of the NH3 concentration, pro- duced stable response under stabilised NH3 concentrations, 2 Description of experiment and accurately repeated (within the uncertainty) the supplied NH3 concentrations. During the calibration, it took about 2.1 Measurement site 20 min for the instrument to show 90 % of the changes in the NH3 concentrations supplied through an aerosol filter The measurements were performed from May to September and a PTFE tubing (4.8 mm ID, about 3 m). However, these 2013 at Gucheng (39◦080 N, 115◦400 E, 15.2 m a.s.l.), a rural time delays also contained the balance time needed for the site in the NCP, which is an Integrated Ecological Meteoro- calibration system.
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