Aqueous Photolysis of Water-Soluble Brown Carbon from Simulated Prescribed and Wildfire Biomass Burning

Mingrui Sun, Chase K. Glenn, Omar El Hajj, Kruthika V. Kumar, Anita Anosike, Robert Penland, Mac A. Callaham Jr., E. Louise Loudermilk, Joseph J. O’Brien, Rawad Saleh and Geoffrey D. Smith*, 
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Abstract

This work, as part of the Georgia Wildland fire Simulation Experiment (G-WISE) campaign, explores the aqueous photolysis of water-soluble brown carbon (W-BrC) in biomass burning aerosols from the combustion of fuel beds collected from three distinct ecoregions in Georgia: Piedmont, Coastal Plain, and Blue Ridge. Burns were conducted under conditions representative of wildfires, which are common unplanned occurrences in Southeastern forests (low fuel moisture content), and prescribed fires, which are commonly used in forest management (higher fuel moisture content). Upon exposure to radiation from UV lamps equivalent to approximately 5 h in the atmosphere, the absorption spectra of all six samples exhibited up to 40% photobleaching in the UV range (280–400 nm) and as much as 30% photo-enhancement in the visible range (400–500 nm). Together, these two effects reduced the absorption Ångström exponent (AAE), a measure of the wavelength dependence of the spectrum, from 6.0–7.9 before photolysis to 5.0–5.7 after. Electrospray ionization ultrahigh-resolution mass spectrometry analysis shows the potential formation of oligomeric chromophores due to aqueous photolysis. This work provides insight into the impacts that aqueous photolysis has on W-BrC in biomass burning aerosols and its dependence on fuel bed composition and moisture content.

This work studies the effect of UV photolysis on the absorption spectra and chemical composition of the water-soluble fraction of biomass burning aerosol generated from simulated wildfire and prescribed burning of fuel beds from three different ecoregions.

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模拟预设和野火生物质燃烧产生的水溶性棕碳的水光解作用
作为佐治亚荒地火灾模拟实验(G-WISE)活动的一部分,这项研究探索了生物质燃烧气溶胶中水溶性棕碳(W-BrC)的水光解作用,这些气溶胶来自从佐治亚州三个不同生态区域收集的燃料床燃烧:皮德蒙特、沿海平原和蓝岭。燃烧是在代表野火和处方火的条件下进行的,野火是东南部森林中常见的意外情况(燃料含水量低),而处方火是森林管理中常用的情况(燃料含水量较高)。在大气中暴露于紫外线灯辐射约 5 小时后,所有六个样品的吸收光谱在紫外线范围(280-400 纳米)显示出高达 40% 的光漂白,在可见光范围(400-500 纳米)显示出高达 30% 的光增强。这两种效应共同作用,使吸收Ångström 指数(AAE)从光解前的 6.0-7.9 降至光解后的 5.0-5.7。电喷雾电离超高分辨率质谱分析表明,水性光解可能会形成低聚发色团。这项工作深入研究了水光解对生物质燃烧气溶胶中 W-BrC 的影响及其与燃料床成分和水分含量的关系。
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