Secondary pollutant ozone (O3) formation in a particular area is often influenced by various factors. Source of emissions is one of the factors. In south east Texas, Houston-Galveston-Brazoria (HGB) is a marginal non-...Secondary pollutant ozone (O3) formation in a particular area is often influenced by various factors. Source of emissions is one of the factors. In south east Texas, Houston-Galveston-Brazoria (HGB) is a marginal non-attainment area for ozone (O3). A summer episode of May 28 to July 2, 2006 is simulated using Comprehensive Air Quality Model with extensions (CAMx). During this period O3 concentration in HGB often exceeds the National Ambient Air Quality Standards (NAAQS) 0.075 ppm of average 8 hour O3 concentration. HGB area has numerous point sources. Various studies found that some specific volatile organic compounds are very reactive in atmosphere. The objective of this study is to analyze the influence of volatile organic compounds present in point source emissions on the air quality of HGB area. For this purpose ozone sensitivity for HGB area is analyzed by the ratio of hydrogen peroxides (H2O2) to nitric acid (HNO3). HGB area is found NOx limited but reactive VOCs are found to be influential too. From (1-4 June, 2006) maximum O3 concentration was found on weekend, June 3. VOCs such as Acetaldehyde (ALD2), Formaldehyde (FORM) and Alkane (ETHA) showed good correlation with O3 concentrations on that day. In addition, Peroxyacetyl nitrate (PAN) formation was found correlated to higher ozone production. Criteria pollutant Sulfur dioxide (SO2) was found to influence the ALD2 and ETHA concentrations, and thus indirectly influenced O3 production.展开更多
We have quantified the impacts of anthropogenic emissions reductions caused by the Air Pollution Control Action Plan and changes in meteorological fields between 2013 and 2017 on the warm-season O3 concentration in Ch...We have quantified the impacts of anthropogenic emissions reductions caused by the Air Pollution Control Action Plan and changes in meteorological fields between 2013 and 2017 on the warm-season O3 concentration in China using a regional 3D chemical transport model. We found that the impact on daily maximum eight-hour (MDA8) O3 concentration by the meteorological variation that mostly increased O3 was greater than that from emission reduction, which decreased O3. Specifically, the control measures implemented since 2013 in China have reduced SO2, NOx, PM2.5, and VOC emissions by 33%, 25%, 30%, and 4% in 2017, while NH3 emissions have increased by 7%. The changes in anthropogenic emissions lowered MDA8 O3 by 0.4–3.7 ppb (0.8%–7.6%, varying by region and month), although MDA8 O3 was increased slightly in some urban areas (i.e. North China) at the beginning/end of warm seasons. Relative to 2013, the average 2 m temperature in 2017 shows increments in North, North-east, East, and South China (0.34℃–0.83℃) and decreases in Central China (0.24℃). The average solar radiation shows increments in North, North-east, and South China (7.0–9.7 w/m2) and decreases in Central, South-west, and North-west China (4.7–10.3 w/m2). The meteorological differences significantly change MDA8 O3 by -3.5–8.5 ppb (-8.2%–18.8%) with large temporal variations. The average MDA8 O3 was slightly increased in North, North-east, East, and South China. The response surface model suggests that the O3 formation regime transfers from NOx-saturated in April to NOx-limited in July on average in China.展开更多
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
文摘Secondary pollutant ozone (O3) formation in a particular area is often influenced by various factors. Source of emissions is one of the factors. In south east Texas, Houston-Galveston-Brazoria (HGB) is a marginal non-attainment area for ozone (O3). A summer episode of May 28 to July 2, 2006 is simulated using Comprehensive Air Quality Model with extensions (CAMx). During this period O3 concentration in HGB often exceeds the National Ambient Air Quality Standards (NAAQS) 0.075 ppm of average 8 hour O3 concentration. HGB area has numerous point sources. Various studies found that some specific volatile organic compounds are very reactive in atmosphere. The objective of this study is to analyze the influence of volatile organic compounds present in point source emissions on the air quality of HGB area. For this purpose ozone sensitivity for HGB area is analyzed by the ratio of hydrogen peroxides (H2O2) to nitric acid (HNO3). HGB area is found NOx limited but reactive VOCs are found to be influential too. From (1-4 June, 2006) maximum O3 concentration was found on weekend, June 3. VOCs such as Acetaldehyde (ALD2), Formaldehyde (FORM) and Alkane (ETHA) showed good correlation with O3 concentrations on that day. In addition, Peroxyacetyl nitrate (PAN) formation was found correlated to higher ozone production. Criteria pollutant Sulfur dioxide (SO2) was found to influence the ALD2 and ETHA concentrations, and thus indirectly influenced O3 production.
基金the National Key R&D Program of China(Nos.2018YFC0213805, 2017YFC0210006)National Natural Science Foundation of China(Grant Nos.21625701 ,51861135102)National Research Program for Key Issues in Air Pollution Control(Nos.DQGG0301 ,DQGG0305).This work was completed on the"Explorer 100"cluster system of Tsinghua National Laboratory for Information Science and Technology.
文摘We have quantified the impacts of anthropogenic emissions reductions caused by the Air Pollution Control Action Plan and changes in meteorological fields between 2013 and 2017 on the warm-season O3 concentration in China using a regional 3D chemical transport model. We found that the impact on daily maximum eight-hour (MDA8) O3 concentration by the meteorological variation that mostly increased O3 was greater than that from emission reduction, which decreased O3. Specifically, the control measures implemented since 2013 in China have reduced SO2, NOx, PM2.5, and VOC emissions by 33%, 25%, 30%, and 4% in 2017, while NH3 emissions have increased by 7%. The changes in anthropogenic emissions lowered MDA8 O3 by 0.4–3.7 ppb (0.8%–7.6%, varying by region and month), although MDA8 O3 was increased slightly in some urban areas (i.e. North China) at the beginning/end of warm seasons. Relative to 2013, the average 2 m temperature in 2017 shows increments in North, North-east, East, and South China (0.34℃–0.83℃) and decreases in Central China (0.24℃). The average solar radiation shows increments in North, North-east, and South China (7.0–9.7 w/m2) and decreases in Central, South-west, and North-west China (4.7–10.3 w/m2). The meteorological differences significantly change MDA8 O3 by -3.5–8.5 ppb (-8.2%–18.8%) with large temporal variations. The average MDA8 O3 was slightly increased in North, North-east, East, and South China. The response surface model suggests that the O3 formation regime transfers from NOx-saturated in April to NOx-limited in July on average in China.
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.
