Major rivers play important roles in transporting large amounts of terrestrial organic matter from land to the ocean each year, and the organic matter carried by rivers contains a significant fraction of black carbon (BC). A recent study estimated that 0.027 Gt of BC is transported in the dissolved phase by rivers each year, which accounts for ~10% of the global flux of dissolved organic carbon. The relative sources of this large amount of riverine dissolved black carbon (DBC) from biomass burning (young, modern 14C) and fossil fuel (old, 14C free) combustion are not known. We present radiocarbon measurements of BC in both dissolved and particulate phases transported by the Changjiang and Huanghe Rivers, the two largest rivers in China, during 2015. We show that two, distinct BC pools (young and old) were carried by the rivers. The DBC pool was much younger than the particulate BC (PBC) pool. Mass balance calculations indicate that most (78–85%) of the DBC in the Changjiang and Huanghe Rivers was derived from biomass burning, and only 15–22% was from fossil fuel combustion. In contrast, PBC from biomass burning and fossil fuel combustion were approximately equal in these two rivers. Export of PBC and DBC by the rivers are decoupled, and fluxes of PBC were 4.1 and 6.7 times higher than DBC in the Changjiang and Huanghe Rivers, respectively. The 14C age differences of the two BC pools suggest that BC derived from biomass burning and fossil fuel combustion are mobilized in different phases and on different time scales in these rivers.

The Changjiang (Yangtze River) and Huanghe (Yellow River) are the two largest rivers in China, and they transport large amounts of terrestrial carbon to the coastal waters of the East China Sea and the Bohai Sea. The sources and cycling of riverine carbon in these two large river estuaries, however, have not been well studied. In this article, we present the results of dual isotope (D 14 C and d 13 C) measurements of dissolved inorganic carbon (DIC) collected in the low reaches of the Changjiang and Huanghe and their estuaries during two cruises in 2014. Our results indicate that both the Changjiang and Huanghe carry very high concentrations of DIC ranging from 1384 lmol kg 21 to 1732 lmol kg 21 and 2711 lmol kg 21 to 4120 lmol kg 21 , respectively, and DIC levels varied with flow rates during high and low discharge periods. The cycling of DIC exhibited conservative behavior in both the Changjiang and Huanghe estuaries, suggesting DIC levels were controlled mainly by physical mixing processes.D 14 C-DIC values indicate that the Changjiang and Huanghe transport aged DIC (1060-1380 yr old). Both D 14 C-DIC and d 13 C-DIC values also showed conservative mixing in the two estuaries. Using a dual carbon isotopic model, we calculated that atmospheric CO 2 consumed mainly by silicate weathering was a major source, contributing 65.2 6 9.0% and 73.4 6 3.0% of DIC in the Changjiang and Huanghe, and 96.9-97.7% (by air-sea exchange) of DIC in the coastal waters of the East China Sea (ECS) and Bohai Sea, respectively. Our results indicate that carbonate dissolution was an important (12.3-17.4%) but not major process controlling the high DIC levels in both rivers, as suggested previously. Compared with the large Amazon River, respiration of riverine organic matter (OM) played a less important role, contributing only 15.4-17.2% of DIC in the two Asian rivers. Flux calculations indicate that the Changjiang and Huanghe discharged 1.46 3 10 13 g and 6.28 3 10 11 g DIC into the ECS and Bohai Sea in 2014, which were 9 and 17 times higher than the DOC fluxes in the two rivers. These large fluxes of riverine DIC, especially of aged DIC, could have significant impacts on primary production and carbon cycling in the ECS and Bohai Sea.

No abstract

We present results from a 1-year study of radiocarbon and stable carbon isotope measurement of dissolved organic carbon (DOC) of wet precipitation samples collected in the Shandong province of China. A total of 32 rainfall and 4 snow samples were collected from two coastal cities (Qingdao and Yantai) and one inland site (Taian) during 2014. Concentrations of DOC in the rainwater and snow samples varied widely from 28 to 616 μM. In general, rainwater originating from marine sources had relatively low DOC concentrations compared with continentally generated precipitation. Values of δ 13 C-DOC and Δ 14 C-DOC in the snow and rainwater ranged from −19.0 to −29.4‰ and −23 to −494 ‰, with corresponding radiocarbon ages of 125 to 5410 years before present. The dominant DOC in the wet precipitation had a relatively old 14 C age (average 2841 years) and a depleted 13 C value (average −24.4‰), indicating the mixing of contemporary organic carbon with 14 Cdepleted fossil fuel-derived soluble organic carbon in the atmosphere. Using a dual isotopic two-endmember model, we calculate that 7 % to 52 % of DOC in the snow and rainfall originated from fossil fuels. It is estimated that the flux of DOC in continental rainfall of China is 23×10 12 g C yr −1 and of this, 7.1×10 12 g C yr −1 could be fossil-fuel OC. On a global scale, the DOC flux in rainfall is estimated to be 357 Tg C yr −1 , and 110 Tg C yr −1 could be fossil fuel-derived. Our study demonstrates that wet precipitation is an important removal process for old fossil fuel carbon from the atmosphere. This removal mechanism could play an important role in the carbon cycle, especially for the anthropogenically derived fraction, and it should be taken into consideration in global carbon cycle models.