德国Melpitz近10年PM1气溶胶化学成分、碳质气溶胶及其来源变化趋势

IF 3.7 2区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Atmospheric Environment Pub Date : 2025-04-01 Epub Date: 2025-01-30 DOI:10.1016/j.atmosenv.2025.121075
Samira Atabakhsh , Laurent Poulain , Alessandro Bigi , Martine Collaud Coen , Mira Pöhlker , Hartmut Herrmann
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引用次数: 0

摘要

亚微米颗粒(PM1)在空气质量、气候和人类健康中发挥着至关重要的作用。长期监测对于确定由自然或人为排放和过程引起的大气成分变化至关重要。本研究提供了10年的连续测量(2012年9月至8月)。2022)在德国的TROPOS Melpitz研究站,这是一个中欧农村背景站点,受其位于东欧和西欧之间的位置影响。利用气溶胶化学形态监测仪(ACSM)和多角度吸收光度计(MAAP),以及有机气溶胶(OA)源分配的rolling positive matrix factorization (PMF)模型,我们分析了近十年PM1的趋势、化学成分和源贡献。结果表明,PM1呈显著负趋势(- 4.59% y - 1),秋季和冬季下降明显。东部气团表现出明显的改善(- 28% y - 1),可能反映了区域缓解政策。OA占总PM1的44%,呈负- 2.05% y - 1趋势,由3个主要OA (POA)来源-类烃OA (HOA)、生物质燃烧OA (BBOA)和燃煤OA (CCOA)和2个氧化OA (OOA)因子(少氧化OA和多氧化OA、LO-OOA和MO-OOA)组成。HOA(占总OA的7%)保持相对稳定,在东部气团作用下略有下降(y - 0.25%)。相比之下,BBOA(占OA的10%)和CCOA(占OA的12%)在住宅供暖和能源生产的推动下表现出强烈的季节性。值得注意的是,夏季BBOA增加了+ 0.48% y - 1,可能是由于木屑颗粒加热,休闲和/或野火的增加,而CCOA在西部气团中显示出温和的增加(+0.27% y - 1)。OOA因子,LO-OOA和MO-OOA(分别占OA的31%和40%),反映了与大气形成途径相关的不同季节模式。两者均呈现东部气团下降趋势(- 1.52% y - 1和- 1.09% y - 1),表明生物源排放和/或人为前体的变化。最后,eBC(PM1)在强源依赖性下y - 1下降了- 1.3%。与城市地区相比,PM质量浓度和人为OA的总体下降似乎有限,强调城市以外的政治缓解效果可能较低。总体而言,这些发现强调了监测PM1组成和来源的长期变化的重要性,这对于了解气溶胶物理特性、改进气候模型和公共健康以及评估不同环境下减缓工作对空气质量和气候的影响至关重要。迫切需要对类似的方法进行进一步的研究,以便更好地了解气溶胶化学成分的地理变化并评估其潜在影响。
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Trends of PM1 aerosol chemical composition, carbonaceous aerosol, and source over the last 10 years at Melpitz (Germany)
Submicron particles (PM1) play a critical role in air quality, climate, and human health. Long-term monitoring is essential to identify changes in atmospheric composition driven by natural or anthropogenic emissions and processes. This study presents ten years of continuous measurements (Sept. 2012–Aug. 2022) at the TROPOS Melpitz research station in Germany, a Central European rural background site influenced by its location between Eastern and Western Europe. Using an aerosol chemical speciation monitor (ACSM) and a multi-angle absorption photometer (MAAP), alongside a rolling positive matrix factorization (PMF) model for organic aerosol (OA) source apportionment, we analyzed PM1 trends, chemical composition, and source contributions over a decade. The results reveal a significant negative PM1 trend of −4.59% y−1, with pronounced decreases occurring in fall and winter. Eastern air masses showed marked improvements (−28% y−1), likely reflecting regional mitigation policies. OA, contributing 44% of total PM1, showed a negative trend of −2.05% y−1 and comprised three primary OA (POA) sources—hydrocarbon-like OA (HOA), biomass burning OA (BBOA), and coal combustion OA (CCOA)—and two oxygenated OA (OOA) factors (less-oxidized and more-oxidized OA, LO-OOA and MO-OOA). HOA (7% of total OA) remained relatively stable, with a minor decline (−0.25% y−1) under Eastern air masses. In contrast, BBOA (10% of OA) and CCOA (12% of OA) displayed strong seasonality, driven by residential heating and energy production. Notably, BBOA increased by +0.48 % y−1 during summer, likely due to the rise in wood pellet heating, recreative, and/or wildfires, while CCOA showed a modest increase (+0.27% y−1) in Western air masses. The OOA factors, LO-OOA and MO-OOA (31% and 40% of OA, respectively), reflected distinct seasonal patterns tied to atmospheric formation pathways. Both showed declining trends in Eastern air masses (−1.52% y−1 and −1.09% y−1), indicating changes in biogenic emissions and/or anthropogenic precursors. Finally, eBC(PM1) decreased by −1.3 % y−1 with strong source dependency. Compared to urban areas, the overall decrease of PM mass concentration and anthropogenic OA looks limited, emphasizing a potentially lower effect of political mitigation outside cities. Overall, the findings underscore the importance of monitoring long-term changes in PM1 composition and sources, which are crucial for understanding aerosol physical properties, refining climate models and public health, and evaluating the impacts of mitigation efforts on air quality and climate in different environments. Further studies on a similar approach are strongly needed to better understand the geographical variation of the aerosol chemical composition and evaluate their potential effect.
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来源期刊
Atmospheric Environment
Atmospheric Environment 环境科学-环境科学
CiteScore
9.40
自引率
8.00%
发文量
458
审稿时长
53 days
期刊介绍: Atmospheric Environment has an open access mirror journal Atmospheric Environment: X, sharing the same aims and scope, editorial team, submission system and rigorous peer review. Atmospheric Environment is the international journal for scientists in different disciplines related to atmospheric composition and its impacts. The journal publishes scientific articles with atmospheric relevance of emissions and depositions of gaseous and particulate compounds, chemical processes and physical effects in the atmosphere, as well as impacts of the changing atmospheric composition on human health, air quality, climate change, and ecosystems.
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