Exploring source footprint of Organophosphate esters in the Bohai Sea, China: Insight from temporal and spatial variabilities in the atmosphere from June 2014 to May 2019

Rong Sun; Xiaoping Wang; Chongguo Tian; Zheng Zong; Wenwen Ma; Shizhen Zhao; Yan Wang; Jianhui Tang; Song Cui; Jun Li; Gan Zhang

doi:10.1016/j.envint.2021.107044

Exploring source footprint of Organophosphate esters in the Bohai Sea, China: Insight from temporal and spatial variabilities in the atmosphere from June 2014 to May 2019

Environ Int. 2022 Jan 15:159:107044. doi: 10.1016/j.envint.2021.107044. Epub 2021 Dec 13.

Authors

Rong Sun¹, Xiaoping Wang², Chongguo Tian³, Zheng Zong⁴, Wenwen Ma⁵, Shizhen Zhao⁶, Yan Wang⁷, Jianhui Tang⁴, Song Cui⁸, Jun Li⁹, Gan Zhang⁶

Affiliations

¹ State Key Laboratory of Organic Geochemistry and Guangdong Province Key Laboratory of Environmental Protection and Resources Utilization, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China; CAS Key Laboratory of Coastal Environmental Processes and Ecological Remediation, Yantai Institute of Coastal Zone Research, Chinese Academy of Sciences, Shandong Key Laboratory of Coastal Environmental Processes, YICCAS, Yantai 264003, China; CAS Center for Excellence in Deep Earth Science, Guangzhou 510640, China; Guangdong-Hong Kong-Macao Joint Laboratory for Environmental Pollution and Control, Guangzhou Institute of Geochemistry, Chinese Academy of Science, Guangzhou 510640, China; University of Chinese Academy of Sciences, Beijing 100049, China.
² Ludong University, Yantai 264025, China.
³ CAS Key Laboratory of Coastal Environmental Processes and Ecological Remediation, Yantai Institute of Coastal Zone Research, Chinese Academy of Sciences, Shandong Key Laboratory of Coastal Environmental Processes, YICCAS, Yantai 264003, China; Center for Ocean Mega-Science, Chinese Academy of Sciences, Qingdao 266071, China. Electronic address: cgtian@yic.ac.cn.
⁴ CAS Key Laboratory of Coastal Environmental Processes and Ecological Remediation, Yantai Institute of Coastal Zone Research, Chinese Academy of Sciences, Shandong Key Laboratory of Coastal Environmental Processes, YICCAS, Yantai 264003, China; Center for Ocean Mega-Science, Chinese Academy of Sciences, Qingdao 266071, China.
⁵ CAS Key Laboratory of Coastal Environmental Processes and Ecological Remediation, Yantai Institute of Coastal Zone Research, Chinese Academy of Sciences, Shandong Key Laboratory of Coastal Environmental Processes, YICCAS, Yantai 264003, China.
⁶ State Key Laboratory of Organic Geochemistry and Guangdong Province Key Laboratory of Environmental Protection and Resources Utilization, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China; CAS Center for Excellence in Deep Earth Science, Guangzhou 510640, China; Guangdong-Hong Kong-Macao Joint Laboratory for Environmental Pollution and Control, Guangzhou Institute of Geochemistry, Chinese Academy of Science, Guangzhou 510640, China.
⁷ Key Laboratory of Industrial Ecology and Environmental Engineering (MOE), School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China.
⁸ International Joint Research Center for Persistent Toxic Substances (IJRC-PTS), School of Water Conservancy and Civil Engineering, Northeast Agricultural University, Harbin 150030, China.
⁹ State Key Laboratory of Organic Geochemistry and Guangdong Province Key Laboratory of Environmental Protection and Resources Utilization, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China; CAS Center for Excellence in Deep Earth Science, Guangzhou 510640, China; Guangdong-Hong Kong-Macao Joint Laboratory for Environmental Pollution and Control, Guangzhou Institute of Geochemistry, Chinese Academy of Science, Guangzhou 510640, China. Electronic address: junli@gig.ac.cn.

PMID: 34915353
DOI: 10.1016/j.envint.2021.107044

Abstract

Organophosphate esters (OPEs) are still produced and used in large quantities in the world-wide, and the environmental burden and behavior have generated widespread concern, especially in some large-scale waterbodies. This study conducted a comprehensive assessment on the temporal and spatial variabilities and budget of OPEs to trace the source for the Bohai Sea (BS), based on a 5-year seasonal monitoring campaign (June 2014 to May 2019) of 12 atmospheric sites around the BS and our previous studies. The average concentration of Σ₁₀OPEs in atmosphere during the sampling period was 7.65 ± 6.42 ng m^-3, and chlorinated OPEs were the major compounds. The Seasonal-Trend decomposition procedure based on Loess (STL) analyzed that during the 5-year sampling period, the atmospheric concentrations of Σ₁₀OPEs had a slightly increasing trend with a rate of + 0.092 ng m^-3 yr^-1, and the seasonal concentrations had a distinct seasonal distribution. The highest concentration of Σ₁₀OPEs was observed at the sampling site of Dalian, followed by Tianjin, Yantai, and Beihuangcheng. The estimation of the fugacity ratios and air-water gas exchange fluxes established that the concentration levels of two major components of chlorinated OPEs (tris-(2-chloroethyl) phosphate (TCEP) and tris-(1-chloro-2-propyl) phosphate (TCPP)) in the atmosphere were dominated by their volatilization from BS's seawater (1.24 ± 0.46 t yr^-1 for TCEP and 5.15 ± 2.15 t yr^-1 for TCPP), with 73% deriving from the coastal seawater. The budget assessment suggested that the volatile fluxes of TCEP and TCPP accounted for 8% and 29% of their storages (15.6 ± 5.32 t for TCEP and 17.6 ± 6.70 t for TCPP) in the BS seawater, which were mainly contributed by continental river input (20% for TCEP and 42% for TCPP). The efforts indicated that river inputs of TCEP and TCPP needed to be paid more attention for the improvement of environmental quality of the BS.

Keywords: Air-water gas exchange; Bohai Sea; Organophosphate esters; Source trace; Spatial and temporal variation.

Publication types

Research Support, Non-U.S. Gov't

MeSH terms

Atmosphere
China
Environmental Monitoring / methods
Esters
Flame Retardants* / analysis
Organophosphates

Substances

Esters
Flame Retardants
Organophosphates