Secondary aerosol formation and oxidation capacity in photooxidation in the presence of Al2O3 seed particles and SO2

被引:15
作者
Chu, Biwu [1 ]
Liu, Tengyu [2 ]
Zhang, Xiao [3 ,4 ]
Liu, Yongchun [1 ]
Ma, Qingxin [1 ]
Ma, Jinzhu [1 ]
He, Hong [1 ]
Wang, Xinming [2 ]
Li, Junhua [3 ]
Hao, Jiming [3 ]
机构
[1] Chinese Acad Sci, Res Ctr Ecoenvironm Sci, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100085, Peoples R China
[2] Chinese Acad Sci, Guangzhou Inst Geochem, State Key Lab Organ Geochem, Guangzhou 510640, Guangdong, Peoples R China
[3] Tsinghua Univ, Sch Environm, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100084, Peoples R China
[4] Nanjing Univ Informat Sci & Technol, Nanjing 210044, Jiangsu, Peoples R China
基金
中国国家自然科学基金;
关键词
secondary aerosol; oxidation capacity; synergetic promoting effect; Al2O3 seed particles; sensitivity; ORGANIC AEROSOL; ALPHA-PINENE; CARBONACEOUS AEROSOLS; MINERAL DUST; NOX; OZONOLYSIS; PM2.5; SULFATE; HYGROSCOPICITY; CYCLOALKENES;
D O I
10.1007/s11426-015-5456-0
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
To investigate the sensitivity of secondary aerosol formation and oxidation capacity to NO (x) in homogeneous and heterogeneous reactions, a series of irradiated toluene/NO (x) /air and alpha-pinene/NO (x) /air experiments were conducted in smog chambers in the absence or presence of Al2O3 seed particles. Various concentrations of NO (x) and volatile organic compounds (VOCs) were designed to simulate secondary aerosol formation under different scenarios for NO (x) . Under "VOC-limited" conditions, the increasing NO (x) 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 NO (x) due to a decreased oxidation capacity of the photooxidation system. Secondary organic aerosol (SOA) formation also decreased with the presence of high concentration of NO (x) , because organoperoxy radicals (RO2) react with NO (x) instead of with peroxy radicals (RO2 or HO2), resulting in the formation of volatile organic products. The increasing concentration of NO (x) enhanced the formation of sulfate, nitrate and SOA under "NO (x) -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 NO (x) on secondary aerosol formation in heterogeneous reactions was observed in the photooxidation. This synergetic effect strengthened the positive relationship between NO (x) and secondary aerosol formation under "NO (x) -limited" conditions but weakened or even overturned the negative relationship between NO (x) and secondary aerosol formation under "VOC-limited" conditions. Sensitivity of secondary aerosol formation to NO (x) 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 NO (x) was further investigated under "winter-like" and NH3-rich conditions. No obvious difference for the sensitivity of secondary aerosol formation except nitrate to NO (x) was observed.
引用
收藏
页码:1426 / 1434
页数:9
相关论文
共 50 条
  • [21] Heterogeneous oxidation mechanism of SO2 on γ-Al2O3 (110) catalyst by H2O2: A first-principle study
    Li, Hai-long
    Dong, Fa-qin
    Bian, Liang
    Huo, Ting -ting
    He, Xiao-chun
    Zheng, Fei
    Lv, Zhen-zhen
    Jiang, Lu-man
    Li, Bowen
    COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS, 2021, 611
  • [22] NO2-initiated multiphase oxidation of SO2 by O2 on CaCO3 particles
    Yu, Ting
    Zhao, Defeng
    Song, Xiaojuan
    Zhu, Tong
    ATMOSPHERIC CHEMISTRY AND PHYSICS, 2018, 18 (09) : 6679 - 6689
  • [23] Oxalate-Promoted SO2 Uptake and Oxidation on Iron Minerals: Implications for Secondary Sulfate Aerosol Formation
    Chen, Ziyue
    Li, Hao
    Shang, Huan
    Liu, Xupeng
    Guo, Furong
    Liu, Xiufan
    Yu, Linghao
    Zhou, Biao
    Liu, Xiao
    Shi, Yanbiao
    Zhang, Lizhi
    Ai, Zhihui
    ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2023, 57 (36) : 13559 - 13568
  • [24] Multiphase oxidation of SO2 by NO2 on CaCO3 particles
    Zhao, Defeng
    Song, Xiaojuan
    Zhu, Tong
    Zhang, Zefeng
    Liu, Yingjun
    Shang, Jing
    ATMOSPHERIC CHEMISTRY AND PHYSICS, 2018, 18 (04) : 2481 - 2493
  • [25] NH3 Weakens the Enhancing Effect of SO2 on Biogenic Secondary Organic Aerosol Formation
    Du, Lin
    Xu, Li
    Li, Kun
    George, Christian
    Ge, Maofa
    ENVIRONMENTAL SCIENCE & TECHNOLOGY LETTERS, 2023, 10 (02) : 145 - 151
  • [26] The effect of water on the heterogeneous reactions of SO2 and NH3 on the surfaces of α-Fe2O3 and γ-Al2O3
    Yang, Weiwei
    Ma, Qingxin
    Liu, Yongchun
    Ma, Jinzhu
    Chu, Biwu
    He, Hong
    ENVIRONMENTAL SCIENCE-NANO, 2019, 6 (09) : 2749 - 2758
  • [27] Relative Humidity Changes the Role of SO2 in Biogenic Secondary Organic Aerosol Formation
    Xu, Li
    Tsona, Narcisse T.
    Du, Lin
    JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 2021, 12 (30) : 7365 - 7372
  • [28] Effect of SO2 on the activity of Ag/γ-Al2O3 catalysts for NOx reduction in lean conditions
    Park, PW
    Boyer, CL
    APPLIED CATALYSIS B-ENVIRONMENTAL, 2005, 59 (1-2) : 27 - 34
  • [29] Effects of SO2 on optical properties of secondary organic aerosol generated from photooxidation of toluene under different relative humidity conditions
    Zhang, Wenyu
    Wang, Weigang
    Li, Junling
    Peng, Chao
    Li, Kun
    Zhou, Li
    Shi, Bo
    Chen, Yan
    Liu, Mingyuan
    Ge, Maofa
    ATMOSPHERIC CHEMISTRY AND PHYSICS, 2020, 20 (07) : 4477 - 4492
  • [30] Simulation of heterogeneous photooxidation of SO2 and NOx in the presence of Gobi Desert dust particles under ambient sunlight
    Yu, Zechen
    Jang, Myoseon
    ATMOSPHERIC CHEMISTRY AND PHYSICS, 2018, 18 (19) : 14609 - 14622