Comment on acp-2022-556

Abstract

The methane chemical sink estimated by atmospheric chemistry models (bottom-up method) is significantly larger than estimates based on methyl-chloroform (MCF) inversions (top-down method). The difference is partly attributable to large uncertainties in hydroxyl radical (OH) concentrations simulated by the atmospheric chemistry models used to derive the bottom-up estimates. In this study, we propose a new approach based on OH precursor observations and a chemical box model. This approach improves the 3-dimensional distributions of tropospheric OH radicals obtained from atmospheric chemistry models and reconciles the bottom-up and top-down estimates of the methane sink due to chemical loss. By constraining the model simulated OH precursors with observations, the global tropospheric mean OH concentration ([OH]trop-M) is ~10×105 molec cm−3 (which is 2×105 molec cm−3 lower than the original model-simulated global [OH]trop-M) and agrees with that obtained by the top-down method based on MCF inversions. With the OH constrained by precursor observations, the methane chemical loss is 471–508 Tg yr−1 averaged from 2000 to 2009. The new adjusted estimate is more consistent with the top-down estimates in the recent global methane budget by the Global Carbon Project (GCP) (459–516 Tg yr−1) than the bottom-up estimates using the original model-simulated OH fields (577–612 Tg yr−1). The overestimation of global [OH]trop-M and methane chemical loss simulated by the atmospheric chemistry models is caused primarily by the models’ underestimation of carbon monoxide and total ozone column, and overestimation of nitrogen dioxide. Our results highlight that constraining the model simulated OH fields with available OH precursor observations can help improve the bottom-up estimated methane sink.