Dataset Information

Large contribution of fossil-derived components to aqueous secondary organic aerosols in China.

ABSTRACT: Incomplete understanding of the sources of secondary organic aerosol (SOA) leads to large uncertainty in both air quality management and in climate change assessment. Chemical reactions occurring in the atmospheric aqueous phase represent an important source of SOA mass, yet, the effects of anthropogenic emissions on the aqueous SOA (aqSOA) are not well constrained. Here we use compound-specific dual-carbon isotopic fingerprints (δ¹³C and Δ¹⁴C) of dominant aqSOA molecules, such as oxalic acid, to track the precursor sources and formation mechanisms of aqSOA. Substantial stable carbon isotope fractionation of aqSOA molecules provides robust evidence for extensive aqueous-phase processing. Contrary to the paradigm that these aqSOA compounds are largely biogenic, radiocarbon-based source apportionments show that fossil precursors produced over one-half of the aqSOA molecules. Large fractions of fossil-derived aqSOA contribute substantially to the total water-soluble organic aerosol load and hence impact projections of both air quality and anthropogenic radiative forcing. Our findings reveal the importance of fossil emissions for aqSOA with effects on climate and air quality.

SUBMITTER: Xu B

PROVIDER: S-EPMC9433442 | biostudies-literature | 2022 Aug

REPOSITORIES: biostudies-literature

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Large contribution of fossil-derived components to aqueous secondary organic aerosols in China.

Xu Buqing B Zhang Gan G Gustafsson Örjan Ö Kawamura Kimitaka K Li Jun J Andersson August A Bikkina Srinivas S Kunwar Bhagawati B Pokhrel Ambarish A Zhong Guangcai G Zhao Shizhen S Li Jing J Huang Chen C Cheng Zhineng Z Zhu Sanyuan S Peng Pingan P Sheng Guoying G

Nature communications 20220831 1

Incomplete understanding of the sources of secondary organic aerosol (SOA) leads to large uncertainty in both air quality management and in climate change assessment. Chemical reactions occurring in the atmospheric aqueous phase represent an important source of SOA mass, yet, the effects of anthropogenic emissions on the aqueous SOA (aqSOA) are not well constrained. Here we use compound-specific dual-carbon isotopic fingerprints (δ<sup>13</sup>C and Δ<sup>14</sup>C) of dominant aqSOA molecules, ...[more]

PMID: 36045131

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Project description:To eliminate the spread of a novel coronavirus breaking out in the end of 2019 (COVID-19), the Chinese government has implemented a nationwide lockdown policy after the Chinese lunar New Year of 2020, resulting in a sharp reduction in air pollutant emissions. To investigate the impact of the lockdown on aerosol chemistry, the number fraction, size distribution and formation process of oxalic acid (C2) containing particles and its precursors were studied using a single particle aerosol mass spectrometer (SPAMS) at the urban site of Liaocheng in the North China Plain (NCP). Our results showed that five air pollutants (i.e., PM2.5, PM10, SO2, NO2, and CO) decreased by 30.0-59.8% during the lockdown compared to those before the lockdown, while O3 increased by 63.9% during the lockdown mainly due to the inefficient titration effect of O3 via NO reduction. The increased O3 concentration can boost the atmospheric oxidizing capacity and further enhance the formation of secondary organic aerosols, thereby significantly enhancing the C2 particles and its precursors as observed during the lockdown. Before the lockdown, C2 particles were significantly originated from biomass burning emissions and their subsequent aqueous-phase oxidation. The hourly variation patterns and correlation analysis before the lockdown suggested that relative humidity (RH) and aerosol liquid water content (ALWC) played a key role in the formation of C2 particles and the increased aerosol acidity can promote the conversion of precursors such as glyoxal (Gly) and methyglyoxal (mGly) into C2 particles in the aqueous phase. RH and ALWC decreased sharply but O3 concentration and solar radiation increased remarkably during the lockdown, the O3-dominated photochemical pathways played an important role in the formation of C2 particles in which aerosol acidity was ineffective. Our study indicated that air pollution treatment sponges on a joint-control and balanced strategy for controlling numerous pollutants.

Dataset Information

Large contribution of fossil-derived components to aqueous secondary organic aerosols in China.

Publications

Large contribution of fossil-derived components to aqueous secondary organic aerosols in China.

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