Evaluation of anthropogenic emissions of carbon monoxide in East Asia derived from the observations of atmospheric radon-222 over the western North Pacific

摘要

We used the observed CO/222Rn 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 222Rn (ERN) events associated with the long-range transport of continental air masses. 222Rn 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 222Rn when forced with a constant and uniform flux density of 1.0 atom cm?2 s?1, 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/222Rn between the observation and the model. The anthropogenic emissions of CO for China, Japan, and Korea were estimated to be 203 Tg CO yr?1, 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.