Kuwata Mikinori, Liu Yingjun, McKinney Karena, Martin Scot T
School of Engineering and Applied Sciences & Department of Earth and Planetary Sciences, Harvard University, Cambridge, Massachusetts 02138, USA.
Phys Chem Chem Phys. 2015 Feb 28;17(8):5670-8. doi: 10.1039/c4cp04942j.
The production of secondary organic material (SOM) by the reactive uptake of isoprene photooxidation products was investigated using partially to wholly neutralized sulfuric acid particles. The experiments were performed at a relative humidity (RH) of <5% and a temperature of 20 °C. The extent X of neutralization was adjusted from that of sulfuric acid (X = 0) to that of ammonium sulfate (X = 1). Significant SOM production was observed only for X < 0.7. The threshold of 0.7 corresponded to the transition point of the sulfate particles from aqueous to solid for <5% RH. The phase transition of inorganic sulfate therefore regulated the particle-phase reactions that produce isoprene SOM, at least for the investigated conditions. For aqueous particles, a decreasing extent of neutralization was associated with increasing production of SOM, including increased production of oligomers and organosulfates. These results can underpin treatments of phase-dependent SOM production within chemical transport models, thereby improving the accuracy of simulations of biogenic-anthropogenic interactions in the atmosphere and the associated impacts of aerosol particles on climate and air quality.
利用部分中和至完全中和的硫酸颗粒,研究了异戊二烯光氧化产物的反应性摄取产生二次有机物质(SOM)的情况。实验在相对湿度(RH)<5%和温度20°C的条件下进行。中和程度X从硫酸的中和程度(X = 0)调整到硫酸铵的中和程度(X = 1)。仅在X < 0.7时观察到显著的SOM生成。0.7的阈值对应于相对湿度<5%时硫酸盐颗粒从水相转变为固相的转变点。因此,无机硫酸盐的相变至少在所研究的条件下调节了产生异戊二烯SOM的颗粒相反应。对于水相颗粒,中和程度的降低与SOM产量的增加相关,包括低聚物和有机硫酸盐产量的增加。这些结果可为化学传输模型中依赖相的SOM生成处理提供依据,从而提高对大气中生物源 - 人为相互作用以及气溶胶颗粒对气候和空气质量相关影响的模拟准确性。