摘要
With rapid economic growth in China, anthropogenic reactive nitrogen (Nr) emissions have more than doubled over the last two or three decades. Atmospheric Nr pollution is an environmental concern in China especially in megacities such as Beijing. In order to identify the impact of emission sources on atmospheric Nr pollution, we measured atmospheric Nr concentrations and their isotopic composition (δ15N) dynamics at three typical sites: landfill, pig farm and road traffic sites in Beijing from April 2010 to March 2011. Passive samplers were used for monitoring ammonia (NH3) and nitrogen dioxide (NO2), two major Nr species, while their δ15N values were measured by a diffusion method combined with mass spectrometer approach. The raw water pool of the landfill and fattening house of the pig farm were important NH3 sources with mean NH3 concentrations being 2,829 and 2,369 μg/m3, respectively, while the road traffic site was a minor NH3 source (10.6 μg/m3). NH3 concentrations at sites besides the landfill and roads were high in summer and low in winter due to the annual variation of temperature and the change of emission source intensity. In contrast, the NH3 concentrations inside the pig farm house were high in winter and low in summer, for the barn windows were open in summer and closed in winter. The mean NO2 concentrations were 89.8, 32.9 and 23.0 μg/m3 at the road traffic, the landfill and pig farm sites, respectively. Due to vehicle fuel combustion, NO2 concentration at the road traffic was the highest among the three sources, and the road traffic was a main NO2 emission source. PM10, pNH4* and pNO3- concentrations in particulate matter were higher in summer than in winter (except PM10 for the pig farm). The δ15NH3 values ranged from -19.14‰ to 7.82‰, with an average of-0.05‰ for the landfill site, and the lowest values were observed in June and July. The δ15NH3 values for the pig farm site ranged from -29.78‰ to-14.05‰ with an average of-24.51‰, and the 515NH3 values were more negative in summer than in the other seasons. The (515NO2 values were -9.63%o to 7.04‰ with an average of -3.72%0 for the road traffic site. The δ15NO2 values were more negative in summer than those in the other seasons. The different δ15N values for the various Nr species in different sources may serve as important indicators for identifying atmospheric Nr sources in megacities. The results may also provide the theoretical basis for research on the atmospheric N deposition and its sources.
With rapid economic growth in China, anthropogenic reactive nitrogen (Nr) emissions have more than doubled over the last two or three decades. Atmospheric Nr pollution is an environmental concern in China especially in megacities such as Beijing. In order to identify the impact of emission sources on atmospheric Nr pollution, we measured atmospheric Nr concentrations and their isotopic composition (δ15N) dynamics at three typical sites: landfill, pig farm and road traffic sites in Beijing from April 2010 to March 2011. Passive samplers were used for monitoring ammonia (NH3) and nitrogen dioxide (NO2), two major Nr species, while their δ15N values were measured by a diffusion method combined with mass spectrometer approach. The raw water pool of the landfill and fattening house of the pig farm were important NH3 sources with mean NH3 concentrations being 2,829 and 2,369 μg/m3, respectively, while the road traffic site was a minor NH3 source (10.6 μg/m3). NH3 concentrations at sites besides the landfill and roads were high in summer and low in winter due to the annual variation of temperature and the change of emission source intensity. In contrast, the NH3 concentrations inside the pig farm house were high in winter and low in summer, for the barn windows were open in summer and closed in winter. The mean NO2 concentrations were 89.8, 32.9 and 23.0 μg/m3 at the road traffic, the landfill and pig farm sites, respectively. Due to vehicle fuel combustion, NO2 concentration at the road traffic was the highest among the three sources, and the road traffic was a main NO2 emission source. PM10, pNH4* and pNO3- concentrations in particulate matter were higher in summer than in winter (except PM10 for the pig farm). The δ15NH3 values ranged from -19.14‰ to 7.82‰, with an average of-0.05‰ for the landfill site, and the lowest values were observed in June and July. The δ15NH3 values for the pig farm site ranged from -29.78‰ to-14.05‰ with an average of-24.51‰, and the 515NH3 values were more negative in summer than in the other seasons. The (515NO2 values were -9.63%o to 7.04‰ with an average of -3.72%0 for the road traffic site. The δ15NO2 values were more negative in summer than those in the other seasons. The different δ15N values for the various Nr species in different sources may serve as important indicators for identifying atmospheric Nr sources in megacities. The results may also provide the theoretical basis for research on the atmospheric N deposition and its sources.
基金
supported by the National Basic Research Program of China(2014CB954202)
the National Natural Science Foundation of China(40425007,41071151,31421092)
the Suzhou University Startup Foundation for Doctor(2015jb04)