Distinct Radiocarbon Ages Reveal Two Black Carbon Pools Preserved in Large River Estuarine Sediments.

Black carbon (BC), a group of environmentally concentrated organic pollutants, is widely distributed in marine sediments via riverine run-off and atmospheric deposition. The fate of BC transformation and cycling in marine sediments, however, has not been well studied. Here, we present radiocarbon measurements for sedimentary solid-phase BC (SBC) and porewater-dissolved BC (DBC) in surface sediments collected from the Yangtze and Yellow River estuaries and their adjacent coastal regions. Radiocarbon results revealed that two distinct BC pools in the sediments of the SBC had ancient radiocarbon ages (7110-15,850 years BP) that were 5370-14,935 years older than the 14C ages of porewater DBC. Using a radiocarbon mass balance model, we calculated that modern biomass-derived BC contributed 77-97% of the DBC pool and that fossil material-produced BC accounted for 61-87% of the SBC pools. This discrepancy between modern and dead BC contributions was associated with the BC budget after particulate BC (PBC) deposition; 38 ± 13% of the PBC was transferred to porewater as DBC and 62 ± 13% was sequestrated as SBC in sediments, serving as an important CO2 sink in marine sediments. We also provide evidence suggesting that DBC likely comprises some very fine particulate forms that are not completely dissolved as molecules. The nature and transformation mechanisms of DBC in natural aquatic systems need to be further studied.

Atmospheric Particles Are Major Sources of Aged Anthropogenic Organic Carbon in Marginal Seas.

Deposition of atmospheric particulates is a major pathway for transporting materials from land to the ocean, with important implications for climate and nutrient cycling in the ocean. Here, we report the results of year-round measurements of particulate organic carbon (POC) and black carbon (BC) in atmospheric aerosols collected on Tuoji Island in the coastal Bohai-Yellow Sea of China (2019-2020) and during a cruise in the western North Pacific. Aerosol POC contents ranged from 1.9 to 11.9%; isotope values ranged from -18.8 to -29.0‰ for δ13C and -150 to -892‰ for Δ14C, corresponding to 14C ages of 1,235 to 17,780 years before present (BP). Mass balance calculations indicated that fossil carbon contributed 19-66% of the POC, with highest values in winter. BC produced from fossil fuel combustion accounted for 18-54% of the POC. "Old" BC (mean 6,238 ± 740 yr BP) was the major contributor to POC, and the old ages of aerosol POC were consistent with the 14C ages of total OC preserved in surface sediments of the Bohai-Yellow Sea and East China Sea. We conclude that atmospheric deposition is an important source of aged OC sequestered in marginal sea sediments and thus represents an important sink for carbon dioxide from the atmosphere.

Sources and cycling of dissolved organic and inorganic carbon on the northern Qinghai-Tibetan Plateau: Radiocarbon results from Qinghai Lake.

Tibetan Plateau lakes are sensitive to climate variabilities and affect regional temperature, precipitation and ecosystems. In this study, we investigated the concentrations and carbon isotope (14C and 13C) compositions of dissolved organic and inorganic carbon (DOC and DIC) along with the concentrations of major lithologic ions (Na+, Mg2+, K+, Ca2+) and dissolved silicate (DSi) in a large lake, namely, Qinghai Lake, and its seven inflowing rivers on the northeastern Qinghai-Tibetan Plateau of China. Our results revealed large differences in concentrations and isotopic compositions between DOC and DIC, as well as differences in the concentrations of major ions between the rivers and lake. The chemical weathering of carbonate and silicates in the catchments played important roles in controlling the fates of major ions in the rivers. In Qinghai Lake, evaporation resulted in 40-290 times the accumulation of Na+, Mg2+, and K+ observed in the rivers, while biological uptake and precipitation reduced the concentrations of Ca2+ and DSi in the lake by 4-17 times compared with those in the rivers. In addition, the concentrations of DOC and DIC in the lake were 6-7 times those in the rivers. The carbon isotope (δ13C and Δ14C) signatures of DOC and DIC revealed that the rivers transport millennium-aged DOC (1254 ± 316 years) and DIC (1513 ± 857 years), as influenced largely by the chemical weathering of rocks and preaged soil carbon on the plateau. In contrast, in Qinghai Lake, the ages of DOC are significantly younger (684 ± 378 years) than the ages of riverine DOC, as regulated by newly biologically produced modern DOC. Moreover, the DIC ages in Qinghai Lake are all modern, indicating that exchange with atmospheric CO2 is the dominant process controlling the lake DIC. The accumulation and removal of riverine-aged DIC in Qinghai Lake, however, are not well understood, and the unbalanced radiocarbon in lake DIC remains a mystery that needs further study.

Succession of marine bacteria in response to Ulva prolifera-derived dissolved organic matter.

Increasing macroalgal blooms as a consequence of climate warming and coastal eutrophication have profound effects on the marine environment. The outbreaks of Ulva prolifera in the Yellow Sea of China occurring every summer since 2007 to present have formed the world's largest green tide. The green tide releases huge amounts of dissolved organic matter (DOM) to the seawater, causing an organic overload. However, how marine bacteria respond to this issue and the potential impact on the marine environment are still unclear. Here, we monitored the highly temporally resolved dynamics of marine bacterial community that occur in response to Ulva prolifera-derived DOM by performing a 168-h microcosm incubation experiment. DOM inputs significantly increased bacterial abundances within 6 h, decreased bacterial diversity and triggered clear community successions during the whole period of incubation. Vibrio of Gammaproteobacteria robustly and rapidly grew over short timescales (6-24 h), with its relative abundance accounting for up to 52.5% of active bacteria. From 24 to 48 h, some genera of Flavobacteriia grew rapidly, which was more conspicuous at a higher DOM concentration than at a lower concentration. The genus Donghicola of Alphaproteobacteria was predominant at later time points (>48 h). This bacterial community succession was accompanied by significant variations in the activity of 12 different extracellular enzymes, resulting in a rapid reduction of dissolved organic carbon by 74.5% within the first 36 h. In summary, our study demonstrates rapid successions of bacterial community and extracellular enzyme activity after DOM inputs, suggesting that the bacterial response to Ulva prolifera-derived organic matter may contribute to environmental restoration and may pose a health threat due to the bloom of potential pathogenic Vibrio.

Dissolved black carbon is not likely a significant refractory organic carbon pool in rivers and oceans.

Rivers are the major carriers of dissolved black carbon (DBC) from land to ocean; the sources of DBC during its continuous transformation and cycling in the ocean, however, are not well characterized. Here, we present new carbon isotope data for DBC in four large and two small mountainous rivers, the Yangtze and Yellow river estuaries, the East China Sea and the North Pacific Ocean. We found that the carbon isotope signatures of DBC are relatively homogeneous, and the DBC 14C ages in rivers are predominantly young and increase during continuous transport and cycling in the ocean. The results of charcoal leaching experiments indicate that DBC is released from charcoal and degraded by bacteria. Our study suggests that riverine DBC is labile and respired during transport and mixing into the ocean and that residual DBC is cycled and aged on the same time scales as bulk DOC in the ocean.