4.7 Article

Source profiles of molecular structure and light absorption of PM2.5 brown carbon from residential coal combustion emission in Northwestern China

期刊

ENVIRONMENTAL POLLUTION
卷 299, 期 -, 页码 -

出版社

ELSEVIER SCI LTD
DOI: 10.1016/j.envpol.2022.118866

关键词

brown carbon; Optical properties; Molecular compositions; Residential coal combustion

资金

  1. Natural Science Foundation of China, China [42007193, 41877383, 21661132005]
  2. SKLLQG, Chinese Academy of Sciences, China [SKLLQG 2028]
  3. Youth Talents Lifting Project of Science and Technology Association in Shaanxi Provinces Universities and Colleges, China [20190703]

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This study used Fourier transform-ion cyclotron resonance mass spectrometry and Fourier transform infrared spectroscopy to analyze the molecular compounds and structures of brown carbon (BrC) emissions from residential coal combustion. The results showed that BrC emissions from anthracite coal had greater light-absorbing capacity compared to emissions from bituminous coal. Additionally, the incomplete combustion of bituminous coal in traditional stoves resulted in higher BrC emissions. The study also found that BrC emissions from traditional stoves contained higher levels of sulfur-containing organics, while BrC emissions from improved stoves had more aliphatic groups.
Residential coal combustion is a prominent source of brown carbon (BrC) aerosols, but knowledge of their molecular structures and optical absorption were limited, which have notable used in ambient BrC source identification and radiative forcing calculation. In this study, the Fourier transform-ion cyclotron resonance mass spectrometry combined with partial least squares regression analysis as well as Fourier transform infrared spectroscopy analysis were used to insight the molecular compounds and structures of BrC from anthracite and bituminous coal combustions between traditional and improved stoves. The absorption angstrom ngstro center dot m exponents (AAE) and mass absorption efficiency (MAE) values for the BrC emitted from the combinations of bituminous were both 1.2-2.5 times lower than those of anthracite, interpreting that the BrC from the anthracite emissions had greater light-absorbing capacity. In contrast, the emission factor of light absorption (EFAbs) at 365 nm for the bituminous coal combusted in the traditional stove was the highest among all the tested scenarios, which revealed that the incomplete combustion of bituminous coal could emit more BrC. It was noted that primary BrC emitted from the coal combustion with traditional stoves contains higher aromaticity groups of C-C and C=O and higher S containing organics, whereas more aliphatic groups were found in BrC using the improved stoves. N-containing (CHON and CHONS) compounds were dominated in the total molecular formula of BrC, whereas the sum of CHON and CHO groups had high double-bond equivalent (DBE) values contributed 53.5%-87.1% to the total BrC absorption. Moreover, for CHOS, the lowest of estimated molecular absorption, DBE, and DBE/C should attribute to the non-chromophoric or weak absorptive S-containing compounds. This study supplied an effective evaluation method to compare BrC emissions and their absorption for coal combustion on regional scale.

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