Fischer E V, Jacob D J, Millet D B, Yantosca R M, Mao J
School of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts, USA.
Department of Soil, Water and Climate, University of Minnesota, St. Paul, Minnesota, USA.
Geophys Res Lett. 2012 Jan;39(1). doi: 10.1029/2011gl050086. Epub 2012 Jan 13.
Acetone is one of the most abundant carbonyl compounds in the atmosphere and it plays an important role in atmospheric chemistry. The role of the ocean in the global atmospheric acetone budget is highly uncertain, with past studies reaching opposite conclusions as to whether the ocean is a source or sink. Here we use a global 3-D chemical transport model (GEOS-Chem) simulation of atmospheric acetone to evaluate the role of air-sea exchange in the global budget. Inclusion of updated (slower) photolysis loss in the model means that a large net ocean source is not needed to explain observed acetone in marine air. We find that a simulation with a fixed seawater acetone concentration of 15 nM based on observations can reproduce the observed global patterns of atmospheric concentrations and air-sea fluxes. The Northern Hemisphere oceans are a net sink for acetone while the tropical oceans are a net source. On a global scale the ocean is in near-equilibrium with the atmosphere. Prescribing an ocean concentration of acetone as a boundary condition in the model assumes that ocean concentrations are controlled by internal production and loss, rather than by air-sea exchange. An implication is that the ocean plays a major role in controlling atmospheric acetone. This hypothesis needs to be tested by better quantification of oceanic acetone sources and sinks.
丙酮是大气中含量最为丰富的羰基化合物之一,在大气化学中发挥着重要作用。海洋在全球大气丙酮收支中的作用极不确定,过去的研究对于海洋是丙酮的源还是汇得出了相反的结论。在此,我们利用一个全球三维化学传输模型(GEOS-Chem)对大气丙酮进行模拟,以评估海气交换在全球收支中的作用。在模型中纳入更新后的(较慢的)光解损失意味着,无需大量的海洋净源来解释海洋空气中观测到的丙酮。我们发现,基于观测结果,固定海水丙酮浓度为15纳摩尔的模拟能够再现观测到的全球大气浓度和海气通量模式。北半球海洋是丙酮的净汇,而热带海洋是丙酮的净源。在全球尺度上,海洋与大气处于近乎平衡的状态。在模型中将丙酮的海洋浓度规定为边界条件,意味着假设海洋浓度由内部生成和损失控制,而非由海气交换控制。这意味着海洋在控制大气丙酮方面发挥着主要作用。这一假设需要通过对海洋丙酮源和汇进行更精确的量化来加以检验。