Characteristics and evolution of brown carbon in western United States wildfires

被引:32
|
作者
Zeng, Linghan [1 ]
Dibb, Jack [2 ]
Scheuer, Eric [2 ]
Katich, Joseph M. [3 ,4 ]
Schwarz, Joshua P. [4 ]
Bourgeois, Ilann [3 ,4 ]
Peischl, Jeff [3 ,4 ]
Ryerson, Tom [3 ,4 ,9 ]
Warneke, Carsten [4 ]
Perring, Anne E. [5 ]
Diskin, Glenn S. [6 ]
DiGangi, Joshua P. [6 ]
Nowak, John B. [6 ]
Moore, Richard H. [6 ]
Wiggins, Elizabeth B. [6 ]
Pagonis, Demetrios [3 ,7 ,10 ]
Guo, Hongyu [3 ,7 ]
Campuzano-Jost, Pedro [3 ,7 ]
Jimenez, Jose L. [3 ,7 ]
Xu, Lu [3 ,4 ,8 ]
Weber, Rodney J. [1 ]
机构
[1] Georgia Inst Technol, Sch Earth & Atmospher Sci, Atlanta, GA 30332 USA
[2] Univ New Hampshire, Coll Engn & Phys Sci, Durham, NH 03824 USA
[3] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO USA
[4] NOAA, Chem Sci Lab, Boulder, CO USA
[5] Colgate Univ, Dept Chem, Hamilton, NY 13346 USA
[6] NASA, Langley Res Ctr, Hampton, VA 23665 USA
[7] Univ Colorado, Dept Chem, Boulder, CO 80309 USA
[8] CALTECH, Div Geol & Planetary Sci, Pasadena, CA 91125 USA
[9] Sci Aviat, Boulder, CO USA
[10] Weber State Univ, Dept Chem & Biochem, Ogden, UT 84408 USA
基金
美国国家航空航天局;
关键词
BIOMASS-BURNING AEROSOL; ABSORPTION ANGSTROM EXPONENT; HUMIC-LIKE SUBSTANCES; LIGHT-ABSORPTION; OPTICAL-PROPERTIES; ORGANIC AEROSOL; BLACK CARBON; AIR-QUALITY; COMPREHENSIVE CHARACTERIZATION; MOLECULAR CHARACTERIZATION;
D O I
10.5194/acp-22-8009-2022
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Brown carbon (BrC) associated with aerosol particles in western United States wildfires was measured between July and August 2019 aboard the NASA DC-8 research aircraft during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) study. Two BrC measurement methods are investigated, highly spectrally resolved light absorption in solvent (water and methanol) extracts of particles collected on filters and in situ bulk aerosol particle light absorption measured at three wavelengths (405, 532 and 664 nm) with a photoacoustic spectrometer (PAS). A light-absorption closure analysis for wavelengths between 300 and 700 nm was performed. The combined light absorption of particle pure black carbon material, including enhancements due to internally mixed materials, plus soluble BrC and a Mie-predicted factor for conversion of soluble BrC to aerosol particle BrC, was compared to absorption spectra from a power law fit to the three PAS wavelengths. For the various parameters used, at a wavelength of roughly 400 nm they agreed, at lower wavelengths the individual component-predicted particle light absorption significantly exceeded the PAS and at higher wavelengths the PAS absorption was consistently higher but more variable. Limitations with extrapolation of PAS data to wavelengths below 405 nm and missing BrC species of low solubility that more strongly absorb at higher wavelengths may account for the differences. Based on measurements closest to fires, the emission ratio of PAS-measured BrC at 405 nm relative to carbon monoxide (CO) was on average 0.13 Mm(-1) ppbv(-1); emission ratios for soluble BrC are also provided. As the smoke moved away from the burning regions, the evolution over time of BrC was observed to be highly complex; BrC enhancement, depletion or constant levels with age were all observed in the first 8 h after emission in different plumes. Within 8 h following emissions, 4-nitrocatechol, a well-characterized BrC chromophore commonly found in smoke particles, was largely depleted relative to the bulk BrC. In a descending plume where temperature increased by 15 K, 4-nitrocatechol dropped, possibly due to temperature-driven evaporation, but bulk BrC remained largely unchanged. Evidence was found for reactions with ozone, or related species, as a pathway for secondary formation of BrC under both low and high oxides of nitrogen (NOx) conditions, while BrC was also observed to be bleached in regions of higher ozone and low NOx, consistent with complex behaviors of BrC observed in laboratory studies. Although the evolution of smoke in the first hours following emission is highly variable, a limited number of measurements of more aged smoke (15 to 30 h) indicate a net loss of BrC. It is yet to be determined how the near-field BrC evolution in smoke affects the characteristics of smoke over longer timescales and spatial scales, where its environmental impacts are likely to be greater.
引用
收藏
页码:8009 / 8036
页数:28
相关论文
共 50 条
  • [1] Examination of brown carbon absorption from wildfires in the western US during the WE-CAN study
    Sullivan, Amy P.
    Pokhrel, Rudra P.
    Shen, Yingjie
    Murphy, Shane M.
    Toohey, Darin W.
    Campos, Teresa
    Lindaas, Jakob
    Fischer, Emily, V
    Collett, Jeffrey L., Jr.
    ATMOSPHERIC CHEMISTRY AND PHYSICS, 2022, 22 (20) : 13389 - 13406
  • [2] Wildfires and wood stoves: Woodsmoke toxicity and chemical characterization study in the north-western United States
    Hadley, Odelle
    Cutler, Anthony
    Schumaker, Ruth
    Bond, Robin
    ATMOSPHERIC ENVIRONMENT, 2021, 253 (253)
  • [3] Observationally constrained representation of brown carbon emissions from wildfires in a chemical transport model
    Neyestani, Soroush E.
    Saleh, Rawad
    ENVIRONMENTAL SCIENCE-ATMOSPHERES, 2022, 2 (02): : 192 - 201
  • [4] Light Absorption by Brown Carbon in the Southeastern United States is pH-dependent
    Phillips, Sabrina M.
    Bellcross, Aleia D.
    Smith, Geoffrey D.
    ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2017, 51 (12) : 6782 - 6790
  • [5] Spatial and Temporal Variability of Brown Carbon in the United States: Implications for Direct Radiative Effects
    June, Nicole A.
    Wang, Xuan
    Chen, L. -W. Antony
    Chow, Judith C.
    Watson, John G.
    Wang, Xiaoliang
    Henderson, Barron H.
    Zheng, Yiqi
    Mao, Jingqiu
    GEOPHYSICAL RESEARCH LETTERS, 2020, 47 (23)
  • [6] Long-term brown carbon spectral characteristics in a Mediterranean city (Athens)
    Liakakou, E.
    Kaskaoutis, D. G.
    Grivas, G.
    Stavroulas, I
    Tsagkaraki, M.
    Paraskevopoulou, D.
    Bougiatioti, A.
    Dumka, U. C.
    Gerasopoulos, E.
    Mihalopoulos, N.
    SCIENCE OF THE TOTAL ENVIRONMENT, 2020, 708
  • [7] Diel cycle impacts on the chemical and light absorption properties of organic carbon aerosol from wildfires in the western United States
    Sumlin, Benjamin
    Fortner, Edward
    Lambe, Andrew
    Shetty, Nishit J.
    Daube, Conner
    Liu, Pai
    Majluf, Francesca
    Herndon, Scott
    Chakrabarty, Rajan K.
    ATMOSPHERIC CHEMISTRY AND PHYSICS, 2021, 21 (15) : 11843 - 11856
  • [8] Evolution of brown carbon in wildfire plumes
    Forrister, Haviland
    Liu, Jiumeng
    Scheuer, Eric
    Dibb, Jack
    Ziemba, Luke
    Thornhill, Kenneth L.
    Anderson, Bruce
    Diskin, Glenn
    Perring, Anne E.
    Schwarz, Joshua P.
    Campuzano-Jost, Pedro
    Day, Douglas A.
    Palm, Brett B.
    Jimenez, Jose L.
    Nenes, Athanasios
    Weber, Rodney J.
    GEOPHYSICAL RESEARCH LETTERS, 2015, 42 (11) : 4623 - 4630
  • [9] Biomass burning dominates brown carbon absorption in the rural southeastern United States
    Washenfelder, R. A.
    Attwood, A. R.
    Brock, C. A.
    Guo, H.
    Xu, L.
    Weber, R. J.
    Ng, N. L.
    Allen, H. M.
    Ayres, B. R.
    Baumann, K.
    Cohen, R. C.
    Draper, D. C.
    Duffey, K. C.
    Edgerton, E.
    Fry, J. L.
    Hu, W. W.
    Jimenez, J. L.
    Palm, B. B.
    Romer, P.
    Stone, E. A.
    Wooldridge, P. J.
    Brown, S. S.
    GEOPHYSICAL RESEARCH LETTERS, 2015, 42 (02) : 653 - 664
  • [10] Photochemical evolution of the molecular composition of dissolved organic carbon and dissolved brown carbon from wood smoldering
    Zhao, Ranran
    Zhao, Weixiong
    Dai, Yong
    Zhou, Jiacheng
    Xu, Xuezhe
    Wang, Feng
    Zhang, Qixing
    Zhang, Yongming
    Zhang, Weijun
    ENVIRONMENT INTERNATIONAL, 2024, 186