ACP Atmospheric Chemistry and Physics ACP 1680-7324 Copernicus GmbH Göttingen, Germany 10.5194/acp-12-12119-2012 Evaluation of anthropogenic emissions of carbon monoxide in East Asia derived from the observations of atmospheric radon-222 over the western North Pacific Wada A. 1 2 Matsueda H. 1 Murayama S. 3 Taguchi S. 3 Kamada A. 4 Nosaka M. 5 Tsuboi K. 1 Sawa Y. 1 Meteorological Research Institute, Tsukuba, Japan Meteorological College, Kashiwa, Japan National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba, Japan Osaka District Meteorological Observatory, Osaka, Japan Saga Local Meteorological Observatory, Saga, Japan 21 12 2012 12 24 12119 12132 This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited. This article is available from http://www.atmos-chem-phys.net/12/12119/2012/acp-12-12119-2012.html The full text article is available as a PDF file from http://www.atmos-chem-phys.net/12/12119/2012/acp-12-12119-2012.pdf

We used the observed CO/<sup>222</sup>Rn ratio in the Asian outflows at Minamitorishima (MNM), Yonagunijima (YON), and Ryori (RYO) in the western North Pacific from 2007 to 2011, together with a three-dimensional chemical transport model (STAG), in order to estimate anthropogenic emissions of CO in East Asia. The measurements captured high-frequency synoptic variations of enhanced <sup>222</sup>Rn (ERN) events associated with the long-range transport of continental air masses. <sup>222</sup>Rn and CO showed high correlation during the ERN events observed at MNM and YON in the winter and spring, but not at RYO. The STAG transport model reproduced well the concentrations of observed <sup>222</sup>Rn when forced with a constant and uniform flux density of 1.0 atom cm<sup>−2</sup> s<sup>−1</sup>, but underestimated the associated enhancement of synoptically variable CO caused by the underestimated flux values in the EDGAR ver. 4.1 emission database used in the model for East Asia. Better estimates for the East Asian emission were derived using a radon tracer method based on the difference in the enhancement ratio of CO/<sup>222</sup>Rn between the observation and the model. The anthropogenic emissions of CO for China, Japan, and Korea were estimated to be 203 Tg CO yr<sup>−1</sup>, 91% of which originated in China. When compared with other estimated emissions of CO, our estimated result showed consistency with those of the inverse method, whereas the emission database of EDGAR was about 45% smaller than our anthropogenic estimation for China.

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