Stanier Charles O, Pathak Ravi K, Pandis Spyros N
Chemical and Biochemical Engineering Dept., University of Iowa, Iowa City, Iowa 52242, USA.
Environ Sci Technol. 2007 Apr 15;41(8):2756-63. doi: 10.1021/es0519280.
The temperature-dependence of secondary organic aerosol (SOA) concentrations is measured using a temperature-controlled smog chamber. Aerosols are generated from reaction of alpha-pinene (14-150 ppb) and ozone at a constant temperature of 22 +/- 2 degrees C in the presence of the OH-scavenger 2-butanol. After the reactions are completed the chamber is heated or cooled in a range from 20 to 40 degrees C. SOA volume concentrations increase at temperatures below the initial formation temperature and decrease at elevated temperatures. The response to the temperature change as measured by percent mass change per degree ranged from -0.4 to -3.6% K(-1), for a total mass reduction of 5-60% upon heating from 22 to 35 degrees C. The reported range is due to two factors: (1) experimental uncertainty, arising mainly from uncertainty in evaporation and condensation behavior of particles lost to the chamber wall; (2) differences in the temperature response from experiment to experiment. Aerosol temperature sensitivity was also measured by tandem differential mobility analysis (TDMA) where similarly generated SOA were heated from 20 to 25 degrees C to 30-40 degrees C with residence times of 0.5-1.5 min, resulting in particle volume reductions of up to 20%. The TDMA experiments indicate that evaporation of the SOA particles in this system occurs with a potentially significant mass transfer limitation (e.g., accommodation coefficient <0.1).
使用温度控制烟雾箱测量二次有机气溶胶(SOA)浓度的温度依赖性。在2 - 丁醇作为OH清除剂存在的情况下,α-蒎烯(14 - 150 ppb)与臭氧在22±2℃的恒定温度下反应生成气溶胶。反应完成后,将烟雾箱在20至40℃范围内加热或冷却。SOA体积浓度在低于初始形成温度时增加,在升高温度时降低。以每度质量变化百分比衡量的对温度变化的响应范围为-0.4至-3.6% K⁻¹,从22℃加热到35℃时总质量减少5 - 60%。报告的范围归因于两个因素:(1)实验不确定性,主要源于损失到箱壁的颗粒蒸发和冷凝行为的不确定性;(2)不同实验之间温度响应的差异。还通过串联差分迁移率分析(TDMA)测量气溶胶温度敏感性,其中类似生成的SOA在0.5 - 1.5分钟的停留时间内从20℃加热到25℃再到30 - 40℃,导致颗粒体积减少高达20%。TDMA实验表明,该系统中SOA颗粒的蒸发存在潜在显著的传质限制(例如,适应系数<0.1)。