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Characteristics and sources of environmentally persistent free radicals in PM2.5 in Dalian, Northeast China: correlation with polycyclic aromatic hydrocarbons

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Abstract

Environmentally persistent free radicals (EPFRs) are an emerging class of environmental hazardous contaminants that extensively, stably exist in airborne particulate matter and pose harmful effects on human health. However, there was little research about the sources of EPFRs in actual atmospheric conditions. This study reported the occurrence, characteristics, and sources of EPFRs and polycyclic aromatic hydrocarbons (PAHs) in PM2.5 collected in Dalian, China. The concentrations of PM2.5-bound EPFRs ranged from 1.13 × 1013 to 8.97 × 1015 spins/m3 (mean value: 1.14 × 1015 spins/m3). Carbon-centered radicals and carbon-centered radicals with adjacent oxygen atoms were detected. The concentration of ∑PAHs ranged from 1.09 to 76.24 ng/m3, and PAHs with high molecular weight (HMW) were predominant species in PM2.5. Correlation of EPFRs with SO2, NO2, O3, and 12 kinds of PAHs indicated that both fuel (coal and biomass) combustion and photoreaction in atmosphere influenced the concentrations of EPFR. The positive matrix factorization (PMF) model results have shown that the primary sources contributed most of the EPFRs and those of secondary sources had a little proportion. Coal combustion (52.4%) was the primary contributor of EPFRs, followed by traffic emission (22.6%), industrial sources (9.6%), and secondary sources (9.2%) during the heating period, whereas industrial emission (39.2%) was the primary contributor, followed by coal combustion (38.1%), vehicular exhaust (23.5%), and secondary sources (9.6%) during the non-heating period. The finding of the present study provides an important evidence for further study on the formation mechanism of EPFRs in actual atmospheric to control the air pollution.

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Fig. 1
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Source appointment of EPFRs by PMF during heating and non-heating period in Dalian

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Funding

This research was financially supported by the Petro China Innovation Foundation (2019D-5007–0502), the Fundamental Research Funds for the Central Universities (DUT21LAB102), the National Natural Scientific Foundation of China (22176025), and the Natural Science Foundation of Liaoning Province (2019-MS-057).

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Authors and Affiliations

  1. Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education), School of Environmental Science and Technology, Dalian University of Technology, Linggong Road 2, Dalian, 116023, China

    Zhansheng Li, Hongxia Zhao, Xintong Li & Tadiyose Girma Bekele

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  1. Zhansheng Li
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  2. Hongxia Zhao
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  3. Xintong Li
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  4. Tadiyose Girma Bekele
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Contributions

ZL: Conceptualization, data curation, formal analysis, investigation, methodology, software, validation, visualization, writing—original draft.

HZ: Funding acquisition, project administration, resources, supervision, writing—reviewing and editing.

XL: Methodology, writing—reviewing and editing, resources.

TGB: Software, writing—reviewing and editing, resources.

All the authors read and approved the final manuscript.

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Correspondence to Hongxia Zhao.

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Li, Z., Zhao, H., Li, X. et al. Characteristics and sources of environmentally persistent free radicals in PM2.5 in Dalian, Northeast China: correlation with polycyclic aromatic hydrocarbons. Environ Sci Pollut Res 29, 24612–24622 (2022). https://doi.org/10.1007/s11356-021-17688-9

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