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Investigating the yield of H<sub>2</sub>O and H<sub>2</sub> from methane oxidation in the stratosphere
oleh: F. Frank, P. Jöckel, S. Gromov, S. Gromov, M. Dameris
Format: | Article |
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Diterbitkan: | Copernicus Publications 2018-07-01 |
Deskripsi
<p>An important driver of climate change is stratospheric water vapor (SWV), which in turn is influenced by the oxidation of atmospheric methane (CH<sub>4</sub>). In order to parameterize the production of water vapor (H<sub>2</sub>O) from CH<sub>4</sub> oxidation, it is often assumed that the oxidation of one CH<sub>4</sub> molecule yields exactly two molecules of H<sub>2</sub>O. However, this assumption is based on an early study, which also gives evidence that this is not true at all altitudes. </p><p> In the current study, we re-evaluate this assumption with a comprehensive systematic analysis using a state-of-the-art chemistry–climate model (CCM), namely the ECHAM/MESSy Atmospheric Chemistry (EMAC) model, and present three approaches to investigate the yield of H<sub>2</sub>O and hydrogen gas (H<sub>2</sub>) from CH<sub>4</sub> oxidation. We thereby make use of the Module Efficiently Calculating the Chemistry of the Atmosphere (MECCA) in a box model and global model configuration. Furthermore, we use the kinetic chemistry tagging technique (MECCA-TAG) to investigate the chemical pathways between CH<sub>4</sub>, H<sub>2</sub>O and H<sub>2</sub>, by being able to distinguish hydrogen atoms produced by CH<sub>4</sub> from H<sub>2</sub> from other sources.</p><p>We apply three approaches, which all agree that assuming a yield of 2 overestimates the production of H<sub>2</sub>O in the lower stratosphere (calculated as 1.5–1.7). Additionally, transport and subsequent photochemical processing of longer-lived intermediates (mostly H<sub>2</sub>) raise the local yield values in the upper stratosphere and lower mesosphere above 2 (maximum  >  2.2). In the middle and upper mesosphere, the influence of loss and recycling of H<sub>2</sub>O increases, making it a crucial factor in the parameterization of the yield of H<sub>2</sub>O from CH<sub>4</sub> oxidation. An additional sensitivity study with the Chemistry As A Boxmodel Application (CAABA) shows a dependence of the yield on the hydroxyl radical (OH) abundance. No significant temperature dependence is found. We focus representatively on the tropical zone between 23° S and 23° N. It is found in the global approach that presented results are mostly valid for midlatitudes as well. During the polar night, the method is not applicable.</p><p>Our conclusions question the use of a constant yield of H<sub>2</sub>O from CH<sub>4</sub> oxidation in climate modeling and encourage to apply comprehensive parameterizations that follow the vertical profiles of the H<sub>2</sub>O yield derived here and take the chemical H<sub>2</sub>O loss into account.</p>