National Institute for Amazonian Research, Manaus, AM 69.060-000, Brazil.
Amazonas State University, Manaus, AM 69470000, Brazil.
Environ Sci Technol. 2022 Jul 19;56(14):9924-9935. doi: 10.1021/acs.est.2c01358. Epub 2022 Jul 8.
The Amazon rainforest suffers increasing pressure from anthropogenic activities. A key aspect not fully understood is how anthropogenic atmospheric emissions within the basin interact with biogenic emissions and impact the forest's atmosphere and biosphere. We combine a high-resolution atmospheric chemical transport model with an improved emissions inventory and in-situ measurements to investigate a surprisingly high concentration of ozone (O) and secondary organic aerosol (SOA) 150-200 km downwind of Manaus city in an otherwise pristine forested region. We show that atmospheric dynamics and photochemistry determine a gross production of secondary pollutants seen in the simulation. After sunrise, the erosion of the nocturnal boundary layer mixes natural forest emissions, rich in biogenic volatile organic compounds, with a lofted pollution layer transported overnight, rich in nitrogen oxides and formaldehyde. As a result, O and SOA concentrations greater than ∼47 ppbv and 1.8 μg m, respectively, were found, with maximum concentrations occurring at 2 pm LT, 150-200 km downwind of Manaus city. These high concentrations affect a large primary forested area of about 11,250 km. These oxidative areas are under a NO-limited regime so that changes in NO emissions from Manaus have a significant impact on O and SOA production.
亚马逊雨林正承受着越来越大的人为活动压力。其中一个尚未完全理解的关键方面是,流域内人为的大气排放如何与生物源排放相互作用,并影响森林的大气和生物圈。我们结合高分辨率大气化学输送模型、改进后的排放清单和现场测量数据,调查了在马瑙斯市下风方向 150-200 公里处的一片原本原始森林中,臭氧 (O) 和二次有机气溶胶 (SOA) 浓度高得惊人的现象。我们表明,大气动力学和光化学反应决定了模拟中二次污染物的总生成量。日出后,夜间边界层的侵蚀将富含生物挥发性有机化合物的天然森林排放物与夜间输送的抬升污染层混合,其中富含氮氧化物和甲醛。结果,在马瑙斯市下风方向 150-200 公里处,发现 O 和 SOA 浓度分别大于约 47 ppbv 和 1.8 μg m,最大浓度出现在当地时间下午 2 点。这些高浓度影响了约 11250 平方公里的大面积原始森林。这些氧化区处于氮限制状态,因此马瑙斯的 NO 排放变化对 O 和 SOA 的生成有重大影响。