Using Si depletion in aerosol to identify the sources of crustal dust in two Chinese megacities

Depletion of Si in transported dust has been recognized for many years. It can be used to distinguish between transported and local dust in cities, although it rarely has been. Here we use the variations of the Si/Al ratio in 15 months of continuous PM_2.5 samples at Beijing (northern China) and Chongqing (southwestern China) to reveal the seasonal patterns of their dust sources. For both cities, peaks of concentration for Si and Al in PM_2.5 corresponded with minima of Si/Al, and could often be linked to pulsed air flow from deserts to the northwest. With significant depletion (up to 80%) and homogeneous distribution at urban and rural sites, Si/Al showed a clear seasonal evolution, which decreased from spring to summer, increased from fall to winter, and collapsed during Chinese Spring Festival, indicating the dominance of transported dust, local fugitive dust and firework influence, respectively. The low ratios implied that desert dust is a common source during spring at Chongqing, whereas its presence during cold season at Beijing was also more frequent than expected. Failing to recognize the depletion of Si may lead to an overestimate of desert dust by 15%–65% when using the average abundance of Al in crust (6%–8%), as in previous studies. The difference in Si/Al ratio between local and transported dust implies that >60% of the dust at Beijing came from outside the city during the springs of 2004–2006. This result can help resolve the contradictory findings on this topic that have been presented earlier.