Environment Research Institute, Shandong University, Binhai Road 72, Qingdao, 266237, China.
Environment Research Institute, Shandong University, Binhai Road 72, Qingdao, 266237, China.
J Environ Sci (China). 2020 Jun;92:151-162. doi: 10.1016/j.jes.2020.02.011. Epub 2020 Feb 25.
Methylglyoxal (CHCOCHO, MG), which is one of the most abundant α-dicarbonyl compounds in the atmosphere, has been reported as a major source of secondary organic aerosol (SOA). In this work, the reaction of MG with hydroxyl radicals was studied in a 500 L smog chamber at (293 ± 3) K, atmospheric pressure, (18 ± 2)% relative humidity, and under different NOx and SO. Particle size distribution was measured by using a scanning mobility particle sizer (SMPS) and the results showed that the addition of SO can promote SOA formation, while different NOx concentrations have different influences on SOA production. High NOx suppressed the SOA formation, whereas the particle mass concentration, particle number concentration and particle geometric mean diameter increased with the increasing NOx concentration at low NOx concentration in the presence of SO. In addition, the products of the OH-initiated oxidation of MG and the functional groups of the particle phase in the MG/OH/SO and MG/OH/NOx/SO reaction systems were detected by gas chromatography mass spectrometry (GC-MS) and attenuated total reflection fourier transformed infrared spectroscopy (ATR-FTIR) analysis. Two products, glyoxylic acid and oxalic acid, were detected by GC-MS. The mechanism of the reaction of MG and OH radicals that follows two main pathways, H atom abstraction and hydration, is proposed. Evidence is provided for the formation of organic nitrates and organic sulfate in particle phase from IR spectra. Incorporation of NOx and SO influence suggested that SOA formation from anthropogenic hydrocarbons may be more efficient in polluted environment.
甲基乙二醛(CHCOCHO,MG)是大气中含量最丰富的α-二羰基化合物之一,已被报道为二次有机气溶胶(SOA)的主要来源。在这项工作中,在(293±3)K、大气压力、(18±2)%相对湿度和不同 NOx 和 SO 的条件下,在 500L 烟雾箱中研究了 MG 与羟基自由基的反应。使用扫描迁移率颗粒 sizer(SMPS)测量了粒径分布,结果表明 SO 的添加可以促进 SOA 的形成,而不同的 NOx 浓度对 SOA 的产生有不同的影响。高 NOx 抑制了 SOA 的形成,而在 SO 存在下,NOx 浓度较低时,颗粒质量浓度、颗粒数浓度和颗粒几何平均直径随 NOx 浓度的增加而增加。此外,通过气相色谱质谱(GC-MS)和衰减全反射傅里叶变换红外光谱(ATR-FTIR)分析检测了 MG/OH/SO 和 MG/OH/NOx/SO 反应体系中 OH 引发氧化 MG 的产物和颗粒相中的官能团。通过 GC-MS 检测到两种产物,即乙醛酸和草酸。提出了 MG 和 OH 自由基遵循两条主要途径(H 原子夺取和水合)反应的机制。IR 谱为颗粒相中有机硝酸盐和有机硫酸盐的形成提供了证据。NOx 和 SO 掺入的影响表明,在污染环境中,人为源碳氢化合物形成的 SOA 可能更有效。