Methylglyoxal-Urea Brown Carbon Aerosol: A Loss Process for Urea

Zachary R. Schiffman, Kevin T. Jansen, Eleanor C. Browne and Margaret A. Tolbert*, 
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Abstract

Recent studies reveal that urea (CO(NH2)2) is often a significant component of tropospheric reactive nitrogen in both the gas- and the condensed-phases; however, little is known about urea sources and sinks. Although it is generally assumed that deposition is the major sink, aqueous reactions in aerosols and clouds may be possible but have yet to be considered. Here, we report a study of the aqueous reactions of urea with methylglyoxal as a function of pH using optical property measurements as a proxy for reaction. UV-vis absorption spectroscopy is used to monitor bulk-phase browning while cavity ringdown and photoacoustic spectroscopies are used to measure the aerosol optical properties. We observe the reaction of urea with methylglyoxal produces brown carbon at low and high pH, with little absorption at mid-pH ranges. The urea brown carbon products absorb well into the visible range, providing a greater overlap with the solar emission spectrum than previously studied brown carbon systems including that of methylglyoxal and ammonium. These experiments suggest that urea could be chemically transformed in aqueous aerosol with the products contributing to aerosol absorption.

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甲基乙二醛-尿素棕碳气溶胶:尿素的损耗过程
最近的研究表明,尿素(CO(NH2)2)通常是对流层气相和凝结相中活性氮的重要组成部分;然而,人们对尿素的来源和汇却知之甚少。虽然人们普遍认为沉积是主要的吸收汇,但气溶胶和云中的水反应也是可能的,但尚未得到考虑。在此,我们报告了一项关于尿素与甲基乙二醛的水反应随 pH 值变化的研究,该研究使用光学特性测量作为反应的替代指标。紫外-可见吸收光谱法用于监测块相褐变,而空腔环落法和光声光谱法则用于测量气溶胶的光学性质。我们观察到,尿素与甲基乙二醛的反应会在低 pH 值和高 pH 值范围内产生棕碳,而在中间 pH 值范围内几乎没有吸收。尿素棕碳产物在可见光范围内有很好的吸收,与之前研究的棕碳系统(包括甲基乙二醛和铵)相比,与太阳辐射光谱有更大的重叠。这些实验表明,尿素可以在水溶液气溶胶中发生化学变化,其产物有助于气溶胶吸收。
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