In-Canopy Chemistry, Emissions, Deposition, and Surface Reactivity Compete to Drive Bidirectional Forest-Atmosphere Exchange of VOC Oxidation Products

In-Canopy Chemistry, Emissions, Deposition, and Surface Reactivity Compete to Drive Bidirectional Forest-Atmosphere Exchange of VOC Oxidation Products
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树冠内化学、排放、沉积和表面反应性相互竞争,推动 VOC 氧化产物的双向森林-大气交换

DOI:
10.1021/acsestair.3c00074
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发表时间:
2024
期刊:
ACS ES&T Air
影响因子:
--
通讯作者:
Farmer, Delphine K.
Farmer, Delphine K.
中科院分区:
--
文献类型:
--
作者:
Link, Michael F.;Pothier, Matson A.;Vermeuel, Michael P.;Riches, Mj;Millet, Dylan B.;Farmer, Delphine K.

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干沉积是森林生态系统中含氧挥发性有机化合物(OVOC)的重要汇。在2021年夏天,我们测量了来自科罗拉多黄松林的异戊二烯和3-甲基-3-丁烯-2-醇(MBO)氧化产物的浓度梯度和交换速度,作为通量封闭研究(FluCS)的一部分。MBO氧化产物在森林中表现出双向交换。MBO氧化产物的垂直梯度揭示了冠层内化学生产作为白天的来源,而从城市流出的前范围内的空气输送创建增强沉积期。我们在干旱、稀疏的松树林中观察到的沉积速度与以前在温带、密集的混交林表明,生态系统类型可能会影响沉积速率的方式目前没有捕捉到的地球观测系统化学。我们表明,以前推断的增加OVOC溶解度阈值叶铜不太可能解释所观察到的快速沉积速率,而是表明,过氧化物/环氧化物可被阔叶植物反应性吸收,而有机硝酸盐可被松针反应性吸收。我们指出,需要了解反应性OVOC吸收的作用及其对双向生态系统-大气交换的潜在影响。
Dry deposition is an important sink of oxygenated volatile organic compounds (OVOCs) in forest ecosystems. In the summer of 2021, we measured concentration gradients and exchange velocities of oxidation products of isoprene and 3-methyl-3-buten-2-ol (MBO) from a Colorado Ponderosa pine forest as part of the Flux Closure Study (FluCS). MBO oxidation products exhibited bidirectional exchange over the forest. Vertical gradients of MBO oxidation products reveal in-canopy chemical production as a daytime source, whereas air transported from the urban outflow of the front range creates periods of enhanced deposition. Differences between our observed deposition velocities over the arid, sparse pine forest and those from a previous study over a temperate, dense mixed forest suggest that ecosystem type may impact deposition rates in ways not currently captured by GEOS-Chem. We show that a previously inferred increased OVOC solubility threshold on leaf cuticles is not likely to explain the observed rapid rates of deposition but instead suggest that peroxides/epoxides could undergo reactive uptake to broadleaf vegetation while organic nitrates could undergo reactive uptake to pine needles. We point to the need to understand the role of reactive OVOC uptake and its potential implications for bidirectional ecosystem-atmosphere exchange.
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