Fossil-driven secondary inorganic PM2.5 enhancement in the North China Plain: Evidence from carbon and nitrogen isotopes

Lim, Saehee; Yang, Xiaoyang; Lee, Meehye; Li, Gang; Gao, Yuanguan; Shang, Xiaona; Zhang, Kai; Czimczik, C. I.; Xu, Xiaomei; Bae, Min Suk; Moon, Kyungsun; Jeon, Kwonho

doi:10.1016/j.envpol.2020.115163

Cited by 25 publications

(32 citation statements)

References 87 publications

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“…Although agricultural emissions are the largest sources of NH 3 globally, 10 , 11 there is growing evidence that fossil fuel related and other sources may compete with agricultural sources in urban areas. 6 , 12 − 14 …”

Section: Introductionmentioning

confidence: 99%

“…Isotopic analysis has been applied in atmospheric chemistry studies, providing insight into atmospheric processes from emission to removal, with wide usage in studies of urban and background areas in East Asia. 6 , 18 , 34 − 39 Such studies have shown that fossil-fuel-related sources make a greater contribution to NH 3 levels than that estimated from emission inventories particularly in urban areas (e.g., Chang et al, 32 Pan et al, 18 , 40 , 41 and Zhang et al 42 ). In ambient samples, δ 15 N of NH 4 + was systematically higher than δ 15 N values of NH 3 due to isotope fractionation between gas- and particulate-phase, regardless of source types.…”

Section: Introductionmentioning

confidence: 99%

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Robust Evidence of ¹⁴C, ¹³C, and ¹⁵N Analyses Indicating Fossil Fuel Sources for Total Carbon and Ammonium in Fine Aerosols in Seoul Megacity

Lim

Hwang

Lee

et al. 2022

Environ. Sci. Technol.

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Carbon- and nitrogen-containing aerosols are ubiquitous in urban atmospheres and play important roles in air quality and climate change. We determined the 14 C fraction modern ( f M ) and δ 13 C of total carbon (TC) and δ 15 N of NH 4 + in the PM 2.5 collected in Seoul megacity during April 2018 to December 2019. The seasonal mean δ 13 C values were similar to −25.1‰ ± 2.0‰ in warm and −24.2‰ ± 0.82‰ in cold seasons. Mean δ 15 N values were higher in warm (16.4‰ ± 2.8‰) than in cold seasons (4.0‰ ± 6.1‰), highlighting the temperature effects on atmospheric NH 3 levels and phase-equilibrium isotopic exchange during the conversion of NH 3 to NH 4 + . While 37% ± 10% of TC was apportioned to fossil-fuel sources on the basis of f M values, δ 15 N indicated a higher contribution of emissions from vehicle exhausts and electricity generating units (power-plant NH 3 slip) to NH 3 : 60% ± 26% in warm season and 66% ± 22% in cold season, based on a Bayesian isotope-mixing model. The collective evidence of multiple isotope analysis reasonably supports the major contribution of fossil-fuel-combustion sources to NH 4 + , in conjunction with TC, and an increased contribution from vehicle emissions during the severe PM 2.5 pollution episodes. These findings demonstrate the efficacy of a multiple-isotope approach in providing better insight into the major sources of PM 2.5 in the urban atmosphere.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Robust Evidence of ¹⁴C, ¹³C, and ¹⁵N Analyses Indicating Fossil Fuel Sources for Total Carbon and Ammonium in Fine Aerosols in Seoul Megacity

Lim

Hwang

Lee

et al. 2022

Environ. Sci. Technol.

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“…It is also noteworthy that there are common chemical and meteorological characteristics in the occurrence of the PM2.5 haze pollution in northeast Asia, such as inorganic species-dominated chemical composition (Lim et al, in reviw;Lim et al, 2020;Shao et al, 2018;Wang et al, 2019a) and transboundary transport of haze aerosol depending on the synoptic atmospheric circulation (Quan et al, 2020;Shi et al, 2020;Zheng et al, 2019). Overall, approximately 40% of PM2.5 consists of NO3 -, SO4 2-, and NH4 + (secondary inorganic aerosol, "SIA") in both urban and background sites in China for the period of 2012-2013.…”

Section: Introductionmentioning

confidence: 99%

“…Overall, approximately 40% of PM2.5 consists of NO3 -, SO4 2-, and NH4 + (secondary inorganic aerosol, "SIA") in both urban and background sites in China for the period of 2012-2013. The contribution of SIA was further augmented up to 69% at urban Beijing and island sites (Changdao) in North China Plain ("NCP") during the 2016 spring (Lim et al, 2020). A large increase in SIA is particularly associated with efficient formation of NO3in cold months (most frequently in Dec. to Mar.…”

Section: Introductionmentioning

confidence: 99%

“…Recently, several studies have used Δ 17 O (NO3 -) measurements for quantifying NO3oxidation pathways Wang et al, 2019b) or  15 N (NO3 -) measurements for apportioning NOx emission sources (Chang et al, 2018;Kawashima, 2019;Li et al, 2019;Lim et al, 2020;Song et al, 2019;Zong et al, 2020) in China. However, to date, few field studies have coupled  15 N (NO3 -) and Δ 17 O (NO3 -) to investigate emission sources of NOx and NOx-to-NO3oxidation processes, e.g., a study in Japan (Nelson et al, 2018) and a study in west Virginia USA (Rose et al, 2019).…”

Section: Introductionmentioning

confidence: 99%

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Oxidation pathways and emission sources of atmospheric particulate nitrate in Seoul: based on δ15N and Δ 17O of PM2.5

Lim

Lee

Savarino

et al. 2021

Preprint

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Abstract. PM2.5 haze pollution driven by secondary inorganic NO3− has been a great concern in East Asia. It is, therefore, imperative to identify its sources and oxidation processes, for which nitrogen and oxygen stable isotopes are powerful tracers. Here, we determined the δ15N (NO3−) and Δ17O (NO3−) of PM2.5 in Seoul from 2018 to 2019, and estimated quantitatively the relative contribution of oxidation pathways for particulate NO3− and major NOx emission sources. In the range of PM2.5 mass concentration from 7.5 g m−3 (summer) to 139.0 g m−3 (winter), the mean δ15N was −0.7 ± 3.3 ‰ and 3.8 ± 3.7 ‰, and the mean Δ17O was 23.2 ± 2.2 ‰ and 27.7 ± 2.2 ‰ in the summer and winter, respectively. While OH oxidation was the dominant pathway for NO3− during the summer (87 %), nighttime formation via N2O5 and NO3 was more important (38 %) during the winter, when aerosol liquid water content (AWLC) and nitrogen oxidation ratio (NOR) were higher. Interestingly, the highest Δ17O was coupled with the lowest δ 15N and highest NOR in record-breaking winter PM2.5 episodes, revealing the critical role of photochemical oxidation process in severe winter haze development. For NOx sources, vehicle emissions were confirmed as a main contributor, followed by biomass combustion from various activities. The contribution from biogenic soil and coal combustion was slightly increased in summer and winter, respectively. Our results built on multiple-isotope approach provide the first explicit evidence for NO3− formation processes and major NOx emission sources in Seoul megacity and suggest an effective mitigation measure to improve PM2.5 pollution.

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Chemical characterization, source apportionment, and health risk assessment of PM2.5 in a typical industrial region in North China

Wang

Yan²,

Zhang

et al. 2022

Environ Sci Pollut Res

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Fossil-driven secondary inorganic PM2.5 enhancement in the North China Plain: Evidence from carbon and nitrogen isotopes

Cited by 25 publications

References 87 publications

Robust Evidence of ¹⁴C, ¹³C, and ¹⁵N Analyses Indicating Fossil Fuel Sources for Total Carbon and Ammonium in Fine Aerosols in Seoul Megacity

Robust Evidence of ¹⁴C, ¹³C, and ¹⁵N Analyses Indicating Fossil Fuel Sources for Total Carbon and Ammonium in Fine Aerosols in Seoul Megacity

Oxidation pathways and emission sources of atmospheric particulate nitrate in Seoul: based on δ<sup>15</sup>N and Δ <sup>17</sup>O of PM<sub>2.5</sub>

Chemical characterization, source apportionment, and health risk assessment of PM2.5 in a typical industrial region in North China

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Fossil-driven secondary inorganic PM2.5 enhancement in the North China Plain: Evidence from carbon and nitrogen isotopes

Cited by 25 publications

References 87 publications

Robust Evidence of 14C, 13C, and 15N Analyses Indicating Fossil Fuel Sources for Total Carbon and Ammonium in Fine Aerosols in Seoul Megacity

Robust Evidence of 14C, 13C, and 15N Analyses Indicating Fossil Fuel Sources for Total Carbon and Ammonium in Fine Aerosols in Seoul Megacity

Oxidation pathways and emission sources of atmospheric particulate nitrate in Seoul: based on δ&lt;sup&gt;15&lt;/sup&gt;N and Δ &lt;sup&gt;17&lt;/sup&gt;O of PM&lt;sub&gt;2.5&lt;/sub&gt;

Chemical characterization, source apportionment, and health risk assessment of PM2.5 in a typical industrial region in North China

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Robust Evidence of ¹⁴C, ¹³C, and ¹⁵N Analyses Indicating Fossil Fuel Sources for Total Carbon and Ammonium in Fine Aerosols in Seoul Megacity

Robust Evidence of ¹⁴C, ¹³C, and ¹⁵N Analyses Indicating Fossil Fuel Sources for Total Carbon and Ammonium in Fine Aerosols in Seoul Megacity

Oxidation pathways and emission sources of atmospheric particulate nitrate in Seoul: based on δ<sup>15</sup>N and Δ <sup>17</sup>O of PM<sub>2.5</sub>