Wet depositional fluxes of fossil fuel-derived carbon in East Asia: Dynamics of Brown carbon.

ABSTRACT

Over the past 50 years, fossil fuel consumption has increased dramatically, rising approximately eight-fold since 1950 and doubling since 1980. This surge has led to increased emissions of brown carbon (BrC) into the atmosphere, which are subsequently deposited onto oceans and land through dry or wet deposition processes. However, the source-specific fluxes of atmospheric organic carbon (OC) and BrC into the ocean are not adequately represented in the global carbon cycle. For the first time, we calculated BrC concentration using the optical intensity of organic matter and determined the global wet depositional flux of fossil fuel-derived BrC. Using the ratio of humic-like substances to OC fluxes, we estimated the global wet deposition of fossil fuel-derived BrC to be 2.0 ± 0.6 Tg C yr-1. Of this amount, the flux into oceans (0.7 ± 0.2 Tg C yr-1) represents 1.6% of the production rate of refractory dissolved organic carbon (RDOC) in the ocean (43 Tg yr-1). Notably, an increase in the proportion of fossil fuel-derived BrC in atmospheric OC may change the composition of OC in precipitation, resulting in a more refractory composition, which deviates from previously established paradigms. Our findings indicate that the flux of fossil fuel-derived RDOC from the atmosphere into the ocean, which is inadequately represented in current global DOC cycling models, may play a significant role in oceanic carbon cycles. These findings necessitate reconsidering our understanding of oceanic carbon cycling and highlight the need to improve existing models to better account for these newly identified processes and their potential impacts on global carbon dynamics.