To investigate the sensitivity of secondary aerosol formation and oxidation capacity to NOx in homogeneous and heterogeneous reactions, a series of irradiated toluene/NOx/air and ?-pinene/NOx/air experiments were cond...To investigate the sensitivity of secondary aerosol formation and oxidation capacity to NOx in homogeneous and heterogeneous reactions, a series of irradiated toluene/NOx/air and ?-pinene/NOx/air experiments were conducted in smog chambers in the absence or presence of Al2O3 seed particles. Various concentrations of NOx and volatile organic compounds(VOCs) were designed to simulate secondary aerosol formation under different scenarios for NOx. Under "VOC-limited" conditions, the increasing NOx concentration suppressed secondary aerosol formation, while the increasing toluene concentration not only contributed to the increase in secondary aerosol formation, but also led to the elevated oxidation degree for the organic aerosol. Sulfate formation was suppressed with the increasing NOx due to a decreased oxidation capacity of the photooxidation system. Secondary organic aerosol(SOA) formation also decreased with the presence of high concentration of NOx, because organo-peroxy radicals(RO2) react with NOx instead of with peroxy radicals(RO2 or HO2), resulting in the formation of volatile organic products. The increasing concentration of NOx enhanced the formation of sulfate, nitrate and SOA under "NOx-limited" conditions, in which the heterogeneous reactions played an important role. In the presence of Al2O3 seed particles, a synergetic promoting effect of mineral dust and NOx on secondary aerosol formation in heterogeneous reactions was observed in the photooxidation. This synergetic effect strengthened the positive relationship between NOx and secondary aerosol formation under "NOx-limited" conditions but weakened or even overturned the negative relationship between NOx and secondary aerosol formation under "VOC-limited" conditions. Sensitivity of secondary aerosol formation to NOx seemed different in homogeneous and heterogeneous reactions, and should be both taken into account in the sensitivity study. The sensitivity of secondary aerosol formation to NOx was further investigated under "winter-like" and NH3-rich conditions. No obvious difference for the sensitivity of secondary aerosol formation except nitrate to NOx was observed.展开更多
Seed particles Al2O3, Al2(SO4)3 and H2SO4 were selected to investigate their effects on secondary aerosol (SA) formation in toluene/NOx photooxidation under sulfur dioxide (SO2) and ammonia (NH3). Effect of se...Seed particles Al2O3, Al2(SO4)3 and H2SO4 were selected to investigate their effects on secondary aerosol (SA) formation in toluene/NOx photooxidation under sulfur dioxide (SO2) and ammonia (NH3). Effect of seed particles on SA formation was related to their acid-base properties and the presence of acid or alkaline gases. Under NH3-poor condition, SA formation increased with increasing SO2 concentration due to the acid-catalyzing effect of the oxidation products of SO2 (i.e. H2SO4), The enhancing effect of SO2 became unobvious under NH3-rieh condition, because NH3 would eliminate the acid-catalyzing effect by neutralizing the acid products. Acidic seeds H2SO4 accelerated SA formation under either SO2 or NH3 condition. Weak acidic Al2(SO4)3 seeds didn't affect obviously on SA formation. The inhibiting effect of amphoteric seeds Al2O3 on SA formation was related to the presence of SO2 / NH3 due to their acid-base property. Under NH3-poor condition, the inhibiting effect of Al2O3 on SA formation decreased with increasing concentration of SO2, while under NH3-rich condition, the inhibiting effect wasn't remarkable.展开更多
This paper is focused on the problem of the ability of seeding particles to follow the flow field. One of the most important factors influencing the resultant accuracy of the measurement is using the proper seeding pa...This paper is focused on the problem of the ability of seeding particles to follow the flow field. One of the most important factors influencing the resultant accuracy of the measurement is using the proper seeding particles for feeding the flow when measuring by PIV (Particle Image Velocimetry) method. The aim of the paper is to provide comprehensible instruction for choosing the proper type of seeding particles with regard to the flow characteristics and required measurement accuracy. The paper presents two methods with the help of which it is possible to determine the seeding particles' ability to follow the flow field. The first method is based on the direct calculation of the phase lag and amplitude ratio between the particle and the fluid. The calculation is based on solution of the BBO (Basset Boussinesq Oseen) equation for spherical particle. The other method results from the calculation of the particle time response, which defines the maximum frequency of disturbances, which are to be followed by the particle. In the conclusion, the method of choosing the seeding particles is proposed, depending on the required measurement accuracy.展开更多
An indoor chamber facility is described for investigation of atmospheric aerosol chemistry. Two sets of α-pinene ozonolysis experiments were conducted in the presence of dry ammonium sulfate seed particle: ozone limi...An indoor chamber facility is described for investigation of atmospheric aerosol chemistry. Two sets of α-pinene ozonolysis experiments were conducted in the presence of dry ammonium sulfate seed particle: ozone limited experiments and α-pinene limited experiments. The concentration of gas phase and particle phase species was monitored continuously by on-line instruments and recorded automatically by data sampling system. The evolution of size distribution was measured by a scanning mobility particle sizer ...展开更多
基金supported by the National Natural Science Foundation of China(21407158)the"Strategic Priority Research Program"of the Chinese Academy of Sciences(XDB05010300,XDB05040100,XDB05010200)
文摘To investigate the sensitivity of secondary aerosol formation and oxidation capacity to NOx in homogeneous and heterogeneous reactions, a series of irradiated toluene/NOx/air and ?-pinene/NOx/air experiments were conducted in smog chambers in the absence or presence of Al2O3 seed particles. Various concentrations of NOx and volatile organic compounds(VOCs) were designed to simulate secondary aerosol formation under different scenarios for NOx. Under "VOC-limited" conditions, the increasing NOx concentration suppressed secondary aerosol formation, while the increasing toluene concentration not only contributed to the increase in secondary aerosol formation, but also led to the elevated oxidation degree for the organic aerosol. Sulfate formation was suppressed with the increasing NOx due to a decreased oxidation capacity of the photooxidation system. Secondary organic aerosol(SOA) formation also decreased with the presence of high concentration of NOx, because organo-peroxy radicals(RO2) react with NOx instead of with peroxy radicals(RO2 or HO2), resulting in the formation of volatile organic products. The increasing concentration of NOx enhanced the formation of sulfate, nitrate and SOA under "NOx-limited" conditions, in which the heterogeneous reactions played an important role. In the presence of Al2O3 seed particles, a synergetic promoting effect of mineral dust and NOx on secondary aerosol formation in heterogeneous reactions was observed in the photooxidation. This synergetic effect strengthened the positive relationship between NOx and secondary aerosol formation under "NOx-limited" conditions but weakened or even overturned the negative relationship between NOx and secondary aerosol formation under "VOC-limited" conditions. Sensitivity of secondary aerosol formation to NOx seemed different in homogeneous and heterogeneous reactions, and should be both taken into account in the sensitivity study. The sensitivity of secondary aerosol formation to NOx was further investigated under "winter-like" and NH3-rich conditions. No obvious difference for the sensitivity of secondary aerosol formation except nitrate to NOx was observed.
基金This work was supported by Scientific Research Foundation for Returned Scholars from Ministry of Education of China (No. 2013S010), Six Talent Peaks Project in Jiangsu Province (No. R2015L12). This work was also supported by the "Strategic Priority Research Program" of the Chinese Academy of Sciences (Nos. XDB05010102 and XDB05030100) and National Natural Science Foundation of China (Grant No. 21407158).
文摘Seed particles Al2O3, Al2(SO4)3 and H2SO4 were selected to investigate their effects on secondary aerosol (SA) formation in toluene/NOx photooxidation under sulfur dioxide (SO2) and ammonia (NH3). Effect of seed particles on SA formation was related to their acid-base properties and the presence of acid or alkaline gases. Under NH3-poor condition, SA formation increased with increasing SO2 concentration due to the acid-catalyzing effect of the oxidation products of SO2 (i.e. H2SO4), The enhancing effect of SO2 became unobvious under NH3-rieh condition, because NH3 would eliminate the acid-catalyzing effect by neutralizing the acid products. Acidic seeds H2SO4 accelerated SA formation under either SO2 or NH3 condition. Weak acidic Al2(SO4)3 seeds didn't affect obviously on SA formation. The inhibiting effect of amphoteric seeds Al2O3 on SA formation was related to the presence of SO2 / NH3 due to their acid-base property. Under NH3-poor condition, the inhibiting effect of Al2O3 on SA formation decreased with increasing concentration of SO2, while under NH3-rich condition, the inhibiting effect wasn't remarkable.
文摘This paper is focused on the problem of the ability of seeding particles to follow the flow field. One of the most important factors influencing the resultant accuracy of the measurement is using the proper seeding particles for feeding the flow when measuring by PIV (Particle Image Velocimetry) method. The aim of the paper is to provide comprehensible instruction for choosing the proper type of seeding particles with regard to the flow characteristics and required measurement accuracy. The paper presents two methods with the help of which it is possible to determine the seeding particles' ability to follow the flow field. The first method is based on the direct calculation of the phase lag and amplitude ratio between the particle and the fluid. The calculation is based on solution of the BBO (Basset Boussinesq Oseen) equation for spherical particle. The other method results from the calculation of the particle time response, which defines the maximum frequency of disturbances, which are to be followed by the particle. In the conclusion, the method of choosing the seeding particles is proposed, depending on the required measurement accuracy.
基金the National Natural ScienceFundation of China (No. 20637001)
文摘An indoor chamber facility is described for investigation of atmospheric aerosol chemistry. Two sets of α-pinene ozonolysis experiments were conducted in the presence of dry ammonium sulfate seed particle: ozone limited experiments and α-pinene limited experiments. The concentration of gas phase and particle phase species was monitored continuously by on-line instruments and recorded automatically by data sampling system. The evolution of size distribution was measured by a scanning mobility particle sizer ...