作者
Zhenguo Liu,Baolin Wang,Chen Wang,Yuchun Sun,Chuanyong Zhu,Lei Sun,Na Yang,Guolan Fan,Xiaoyan Sun,Zhiyong Xia,Guang Pan,Changtong Zhu,Yichao Gai,Xiaoyu Wang,Yang Xiao,Guihuan Yan,Chongqing Xu
摘要
Volatile organic compounds (VOCs) undergo substantial photochemical losses during their transport from emission sources to receptor sites, resulting in serious implications for their source apportionment and ozone (O3) formation. Based on the continuous measurements of VOCs in suburban Jinan in August 2022, the effects of photochemical losses on VOC source contributions and O3 formation were evaluated in this study. The observed and initial concentrations of total VOCs (TVOC) were 12.0 ± 5.1 and 16.0 ± 7.4 ppbv, respectively. Throughout the observation period, alkenes had the most prominent photochemical losses (58.2%), followed by aromatic hydrocarbons (23.1%), accounting for 80.6% and 6.9% of the total losses, respectively. During high O3 episodes, the photochemical loss of VOCs was 6.9 times higher than that during the cleaning period. Alkene losses (exceeding 67.3%), specifically losses of isoprene, propylene, ethylene, and n-butene, dominated the total losses of VOCs during the O3 increase period. Eight sources of VOCs were identified by positive matrix factorization (PMF) based on the observed and initial concentration data (OC-PMF and IC-PMF, respectively). Concentrations of all emission sources in the OC-PMF were underestimated by 2.4%–57.1%. Moreover, the contribution of each emission source was over- or underestimated compared with that in case of the IC-PMF. The contributions of biogenic and motor vehicle exhaust emissions were underestimated by 5.3 and 2.8 percentage points, respectively, which was associated with substantial oxidation of the emitted high-reactive species. The contributions of coal/biomass burning and natural gas were overestimated by 2.4 and 3.9 percentage points, respectively, which were related to the emission of low-reactive species (acetylene, ethane, and propane). Based on our results, the photochemical losses of VOCs grossly affect their source apportionment and O3 formation. Thus, photochemical losses of VOCs must be thoroughly accounted to establish a precise scientific foundation for air-pollution control strategies.