Department of Atmospheric Science, Yunnan University, Kunming, 650091, China.
Key Laboratory of Regional Climate-Environment for Temperate East Asia, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing, 100029, China; University of Chinese Academy of Sciences, Beijing, 100049, China.
Environ Pollut. 2022 Aug 1;306:119383. doi: 10.1016/j.envpol.2022.119383. Epub 2022 Apr 30.
Various precursor emissions and chemical mechanisms for secondary organic aerosol (SOA) formation were incorporated into a regional air quality model system (RAQMS) and applied to investigate the distribution, composition, and source contribution of SOA over east China in summer 2018. Model comparison against a variety of observations at a national scale demonstrated that the model was able to reasonably reproduce meteorological variables, O and PM concentrations, and the model simulated SOA concentration generally agreed with observations, with the overall NMB of 7.0% and R of 0.4 in 10 cities over east China. The simulated period-mean SOA concentrations of 4-15 μg m were mainly distributed over the North China Plain (NCP), the middle and lower reaches of the Yangtze River and Chongqing district. SOA dominated organic aerosol (OA) over China in summertime (90%). The percentage contributions to SOA from ASOA (SOA produced from anthropogenic volatile organic compounds (AVOC)), BSOA (SOA produced from biogenic volatile organic compounds (BVOC)), DSOA (SOA produced from aqueous uptake of glyoxal and methylglyoxal) and S/I-SOA (SOA produced from semi-volatile and intermediate volatile organic compounds) were estimated to be 48.3%, 28.6%, 14.3%, and 8.8% respectively, over east China in summertime. In terms of domain and period average, ASOA contributed most to SOA (59%) in north China, while BSOA contributed most to SOA (37.3%) in northeast China. The percentage contribution of DSOA to SOA reached 21.5% in southwest China. S/I-SOA accounted for approximately 10% of SOA in most areas of east China. This study reveals that while AVOC dominates SOA formation on average over east China, the SOA source contributions differ considerably in different regions of China. BVOC makes the same contribution to SOA formation as AVOC in northeast China and southwest China, where forest coverage and BVOC emission are higher and anthropogenic emissions are relatively low, highlighting the significant role of BVOC in summer SOA formation in China.
各种前体排放物和二次有机气溶胶(SOA)形成的化学机制被纳入区域空气质量模型系统(RAQMS)中,并应用于研究 2018 年夏季中国东部地区 SOA 的分布、组成和来源贡献。该模型与全国范围内的各种观测结果进行了比较,结果表明该模型能够合理地再现气象变量、O 和 PM 浓度,且模型模拟的 SOA 浓度与观测结果基本一致,在中国东部 10 个城市的总体 NMB 为 7.0%,R 为 0.4。模拟的夏季 SOA 浓度(4-15μg/m)主要分布在华北平原(NCP)、长江中下游和重庆地区。SOA 在夏季占中国有机气溶胶(OA)的主导地位(90%)。来自 ASOA(人为挥发性有机化合物(AVOC)产生的 SOA)、BSOA(生物源挥发性有机化合物(BVOC)产生的 SOA)、DSOA(乙二醛和甲基乙二醛水相吸收产生的 SOA)和 S/I-SOA(半挥发性和中间挥发性有机化合物产生的 SOA)对中国东部夏季 SOA 的贡献比例分别估计为 48.3%、28.6%、14.3%和 8.8%。从区域和时段平均来看,AVOC 对北方地区 SOA 的贡献最大(59%),而 BVOC 对东北地区 SOA 的贡献最大(37.3%)。DSOA 对 SOA 的贡献在西南地区达到 21.5%。S/I-SOA 在中国东部大部分地区占 SOA 的 10%左右。本研究表明,虽然 AVOC 平均在中国东部地区主导 SOA 的形成,但不同地区的 SOA 来源贡献差异很大。在中国东北和西南部,由于森林覆盖率和 BVOC 排放较高,人为排放相对较低,BVOC 对 SOA 形成的贡献与 AVOC 相同,这突出了 BVOC 在夏季中国 SOA 形成中的重要作用。