Dai Minhan

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Intercalibration studies of short-lived thorium-234 in the water column and marine particles

(Association for the Sciences of Limnology and Oceanography, 2012-09) Maiti, Kanchan ; Buesseler, Ken O. ; Pike, Steven M. ; Benitez-Nelson, Claudia R. ; Cai, Pinghe ; Chen, Weifang ; Cochran, Kirk ; Dai, Minhan ; Dehairs, Frank ; Gasser, Beat ; Kelly, Roger P. ; Masqué, Pere ; Miller, Lisa A. ; Miquel, Juan Carlos ; Moran, S. Bradley ; Morris, Paul J. ; Peine, Florian ; Planchon, Frederic ; Renfro, Alisha A. ; Rutgers van der Loeff, Michiel M. ; Santschi, Peter H. ; Turnewitsch, Robert ; Waples, James T. ; Xu, Chen

Intercomparision of 234Th measurements in both water and particulate samples was carried out between 15 laboratories worldwide, as a part of GEOTRACES inter-calibration program. Particulate samples from four different stations namely BATS (both shallow and deep) and shelf station (shallow) in Atlantic and SAFE (both shallow and deep) and Santa Barbara station (shallow) in Pacific were used in the effort. Particulate intercalibration results indicate good agreement between all the participating labs with data from all labs falling within the 95% confidence interval around the mean for most instances. Filter type experiments indicate no significant differences in 234Th activities between filter types and pore sizes (0.2-0.8 μm). The only exception are the quartz filters, which are associated with 10% to 20% higher 234Th activities attributed to sorption of dissolved 234Th. Flow rate experiments showed a trend of decreasing 234Th activities with increasing flow rates (2-9 L min-1) for > 51 μm size particles, indicating particle loss during the pumping process. No change in 234Th activities on small particles was observed with increasing flow-rates. 234Th intercalibration results from deep water samples at SAFe station indicate a variability of < 3% amongst labs while dissolved 234Th data from surface water at Santa Barbara Station show a less robust agreement, possibly due to the loss of 234Th from decay and large in-growth corrections as a result of long gap between sample collection and processing.
How significant is submarine groundwater discharge and its associated dissolved inorganic carbon in a river-dominated shelf system?

(Copernicus Publications on behalf of the European Geosciences Union, 2012-05-22) Liu, Q. ; Dai, Minhan ; Chen, W. ; Huh, C.-A. ; Wang, Guihua ; Li, Q. ; Charette, Matthew A.

In order to assess the role of submarine groundwater discharge (SGD) and its impact on the carbonate system on the northern South China Sea (NSCS) shelf, we measured seawater concentrations of four radium isotopes 223,224,226,228Ra along with carbonate system parameters in June–July, 2008. Complementary groundwater sampling was conducted in coastal areas in December 2008 and October 2010 to constrain the groundwater end-members. The distribution of Ra isotopes in the NSCS was largely controlled by the Pearl River plume and coastal upwelling. Long-lived Ra isotopes (228Ra and 226Ra) were enriched in the river plume but low in the offshore surface water and subsurface water/upwelling zone. In contrast, short-lived Ra isotopes (224Ra and 223Ra) were elevated in the subsurface water/upwelling zone as well as in the river plume but depleted in the offshore surface water. In order to quantify SGD, we adopted two independent mathematical approaches. Using a three end-member mixing model with total alkalinity (TAlk) and Ra isotopes, we derived a SGD flux into the NSCS shelf of 2.3–3.7 × 108 m3 day−1. Our second approach involved a simple mass balance of 228Ra and 226Ra and resulted in a first order but consistent SGD flux estimate of 2.2–3.7 × 108 m3 day−1. These fluxes were equivalent to 12–21 % of the Pearl River discharge, but the source of the SGD was mostly recirculated seawater. Despite the relatively small SGD volume flow compared to the river, the associated material fluxes were substantial given their elevated concentrations of dissolved inorganic solutes. In this case, dissolved inorganic carbon (DIC) flux through SGD was 153–347 × 109 mol yr−1, or ~23–53 % of the riverine DIC export flux. Our estimates of the groundwater-derived phosphate flux ranged 3–68 × 107 mol yr−1, which may be responsible for new production on the shelf up to 0.3–6.3 mmol C m−2 d−1. This rate of new production would at most consume 11 % of the DIC contribution delivered by SGD. Hence, SGD may play an important role in the carbon balance over the NSCS shelf.
A review of present techniques and methodological advances in analyzing Th-234 in aquatic systems

( 2005-10-10) Rutgers van der Loeff, Michiel M. ; Sarin, Manmohan M. ; Baskaran, Mark ; Benitez-Nelson, Claudia R. ; Buesseler, Ken O. ; Charette, Matthew A. ; Dai, Minhan ; Gustafsson, Orjan ; Masqué, Pere ; Morris, Paul J. ; Orlandini, Kent ; Rodriguez y Baena, Alessia ; Savoye, Nicolas ; Schmidt, Sabine ; Turnewitsch, Robert ; Voge, Ingrid ; Waples, James T.

The short-lived thorium isotope 234Th (half-life 24.1 days) has been used as a tracer for a variety of transport processes in aquatic systems. Its use as a tracer of oceanic export via sinking particles has stimulated a rapidly increasing number of studies that require analyses of 234Th in both marine and freshwater systems. The original 234Th method is labour intensive. Thus, there has been a quest for simpler techniques that require smaller sample volumes. Here, we review current methodologies in the collection and analysis of 234Th from the water column, discuss their individual strengths and weaknesses, and provide an outlook on possible further improvements and future challenges. Also included in this review are recommendations on calibration procedures and the production of standard reference materials as well as a flow chart designed to help researchers find the most appropriate 234Th analytical technique for a specific aquatic regime and known sampling constraints.
Plutonium in groundwater at the 100K-Area of the U.S. DOE Hanford Site

( 2004-01-27) Dai, Minhan ; Buesseler, Ken O. ; Pike, Steven M.

We examined the concentration, size distribution, redox state and isotopic composition of plutonium (Pu) in groundwater at the 100K-Area at the US Department of Energy’s (DOE) Hanford Site. Total concentrations of Pu isotopes were extremely low (10-4 to 10-6 pCi/kg, ≈ 104 to 106 atoms/kg), but measurable for the first time in the 100K-Area wells using mass spectrometric analyses that are much more sensitive than alpha spectroscopy methods used previously. Size fractionation data from two wells suggests that 7-29% of the Pu is associated with colloids, operationally defined here as particles between 1 kDa – 0.2 μm in size. These colloids were collected using a 1 kDa cross-flow ultrafiltration system developed specifically for groundwater actinide studies to include careful controls both in the field and during processing to ensure in-situ geochemical conditions are maintained and size separations can be well characterized. Pu in this colloidal fraction was exclusively in the more reduced Pu(III/IV) form, consistent with the higher affinity of Pu for particle surfaces in the lower oxidation states. While the overall concentrations of Pu were low, the Pu isotopic composition suggests at least two local sources of groundwater Pu, namely local Hanford reactor operations at the 100K-Area, and spent nuclear fuel from the N reactor, which was stored in concrete pools at this site. Differences between this site and the Savannah River Site (SRS) are noted, since groundwater Pu at the F-Area seepage basin at SRS has been found using these same 2 methods, to be characterized by much lower colloidal abundances and higher oxidation states. This difference is not directly attributable to groundwater redox potential or geochemical conditions, but rather the physical-chemical difference in Pu sources, which at SRS appear to be dominated downstream from the seepage basins by decay of 244Cm, resulting in more oxidized forms of 240Pu. There is no clear evidence for colloid facilitated transport of Pu in groundwater at this site, since downstream wells have both an order of magnitude lower concentrations of Pu, but also a lower fractional colloidal distribution.
An improvement in the small-volume technique for determining thorium-234 in seawater

( 2005-06-09) Cai, Pinghe ; Dai, Minhan ; Lv, Dongwei ; Chen, Weifang

The recently developed 2‐5 L small‐volume MnO2 coprecipitation method for determining 234Th in seawater has provided a new way to substantially increase, both temporally and spatially, the sampling resolution of 234Th and 234Th‐based particulate organic carbon export estimates in the upper ocean. In this study, we further optimize the technique by reducing reagent quantities and the use of an additional water bath heating step. This optimization allows the filtration of the MnO2 precipitate onto a 25‐mm diameter, 1.0 μm pore size QMA filter to be completed within < 30 minutes for unfiltered waters from the South China Sea. In addition, we have modified the MnO2 purification procedure to allow for alpha spetrometric measurements of 234Th recoveries. Results from recovery experiments suggest that reagent amounts can be reduced to 0.0375 mg KMnO4 and 0.1 mg MnCl2∙4H2O per liter of sample, while still maintaining high 234Th recovery. This study further confirms that the addition of a yield monitor is necessary for the application of this small‐volume method.
Sources and accumulation of organic carbon in the Pearl River Estuary surface sediment as indicated by elemental, stable carbon isotopic, and carbohydrate compositions

(Copernicus Publications on behalf of the European Geosciences Union, 2010-10-28) He, B. ; Dai, Minhan ; Huang, W. ; Liu, Q. ; Chen, H. ; Xu, Li

Organic matter in surface sediments from the upper reach of the Pearl River Estuary and Lingdingyang Bay, as well as the adjacent northern South China Sea shelf was characterized using a variety of techniques, including elemental (C and N) ratio, bulk stable organic carbon isotopic composition (δ13C), and carbohydrate composition analyses. Total organic carbon (TOC) content was 1.21±0.45% in the upper reach, down to 1.00±0.22% in Lingdingyang Bay and to 0.80±0.10% on the inner shelf and 0.58±0.06% on the outer shelf. δ13C values ranged from −25.1‰ to −21.3‰ in Lingdingyang Bay and the South China Sea shelf, with a trend of enrichment seawards. The spatial trend in C/N ratios mirrored that of δ13C, with a substantial decrease in C/N ratio offshore. Total carbohydrate yields ranged from 22.1 to 26.7 mg (100 mg OC)−1, and typically followed TOC concentrations in the estuarine and shelf sediments. Total neutral sugars, as detected by the nine major monosaccharides (lyxose, rhamnose, ribose, arabinose, fucose, xylose, galactose, mannose, and glucose), were between 4.0 and 18.6 mg (100 mg OC)−1 in the same sediments, suggesting that significant amounts of carbohydrates were not neutral aldoses. Using a two end-member mixing model based on δ13C values and C/N ratios, we estimated that the terrestrial organic carbon contribution to the surface sediment TOC was ca. 78±11% for Lingdingyang Bay, 34±4% for the inner shelf, and 5.5±1% for the outer shelf. The molecular composition of the carbohydrate in the surface sediments also suggested that the inner estuary was rich in terrestrially derived carbohydrates but that their contribution decreased offshore. A relatively high abundance of deoxyhexoses in the estuary and shelf indicated a considerable bacterial source of these carbohydrates, implying that sediment organic matter had undergone extensive degradation and/or transformation during transport. Sediment budget based on calculated regional accumulation rates showed that only ~50% of the influxes of terrestrial organic carbon were accumulated in the estuary. This relatively low accumulation efficiency of terrestrial organic matter as compared to the total suspended solids (accumulation efficiency ~73%) suggested significant degradation of the terrestrial organic carbon within the estuarine system after its discharge from the river. This study demonstrated that the combination of the bulk organic matter properties together with the isotopic composition and molecular-level carbohydrate compositions can be an efficient way to track down the source and fate of organic matter in highly dynamic estuarine and coastal systems. The predominance of terrestrially originated organic matter in the sediment and its generally low accumulation efficiency within the estuary is not surprising, and yet it may have important implications in light of the heavy anthropogenic discharges into the Pearl River Estuary during the past thirty years.
Cyclone-driven deep sea injection of freshwater and heat by hyperpycnal flow in the subtropics

(American Geophysical Union, 2010-11-04) Kao, Shuh-Ji ; Dai, Minhan ; Selvaraj, K. ; Zhai, W. ; Cai, Pinghe ; Chen, Shih-Nan ; Yang, J. Y. T. ; Liu, J. T. ; Liu, C. C. ; Syvitski, James P. M.

The western tropical Pacific gives birth to 23 tropical cyclones annually, bringing torrential rainfall to mountainous islands across Oceania resulting in a global sediment production hotspot, in which many rivers have great hyperpycnal potential. By using a temperature (T) and salinity (S) profiler, we observed anomalously warm, low salinity turbid water at 3000–3700 m depths in seas ∼180 km off southwestern Taiwan immediately after Typhoon Morakot in 2009. This 250m-thick bottom-hugging water occupies ∼2400 km2, and contains 0.15% freshwater, suggesting a remarkably high fraction (6–10%) of event rainfall from southwestern Taiwan. These characteristics indicate the turbid water originated from shallow coastal waters via hyperpycnal flow. Apparently, sediment produced from the land during tropical cyclones open an “express gate” to convey heat and freshwater vertically to the deep ocean basin subsequently warming the deep water from the bottom up.
Fukushima Daiichi–derived radionuclides in the ocean : transport, fate, and impacts

(Annual Reviews, 2016-06-30) Buesseler, Ken O. ; Dai, Minhan ; Aoyama, Michio ; Benitez-Nelson, Claudia R. ; Charmasson, Sabine ; Higley, Kathryn ; Maderich, Vladimir ; Masqué, Pere ; Morris, Paul J. ; Oughton, Deborah ; Smith, John N.

The events that followed the Tohoku earthquake and tsunami on March 11, 2011, included the loss of power and overheating at the Fukushima Daiichi nuclear power plants, which led to extensive releases of radioactive gases, volatiles, and liquids, particularly to the coastal ocean. The fate of these radionuclides depends in large part on their oceanic geochemistry, physical processes, and biological uptake. Whereas radioactivity on land can be resampled and its distribution mapped, releases to the marine environment are harder to characterize owing to variability in ocean currents and the general challenges of sampling at sea. Five years later, it is appropriate to review what happened in terms of the sources, transport, and fate of these radionuclides in the ocean. In addition to the oceanic behavior of these contaminants, this review considers the potential health effects and societal impacts.
A synthesis of global coastal ocean greenhouse gas fluxes

(American Geophysical Union, 2024-01-20) Resplandy, Laure ; Hogikyan, Allison ; Muller, Jens Daniel ; Najjar, Raymond G. ; Bange, Hermann W. ; Bianchi, Daniele ; Weber, Thomas ; Cai, Wei-Jun ; Doney, Scott C. ; Fennel, Katja ; Gehlen, Marion ; Hauck, Judith ; Lacroix, Fabrice ; Landschutzer, Peter ; Le Quere, Corinne ; Roobaert, Alizee ; Schwinger, Jorg ; Berthet, Sarah ; Bopp, Laurent ; Chau, Thi Tuyet Trang ; Dai, Minhan ; Gruber, Nicolas ; Ilyina, Tatiana ; Kock, Annette ; Manizza, Manfredi ; Lachkar, Zouhair ; Laruelle, Goulven G. ; Liao, Enhui ; Lima, Ivan D. ; Nissen, Cara ; Rodenbeck, Christian ; Seferian, Roland ; Toyama, Katsuya ; Tsujino, Hiroyuki ; Regnier, Pierre

The coastal ocean contributes to regulating atmospheric greenhouse gas concentrations by taking up carbon dioxide (CO2) and releasing nitrous oxide (N2O) and methane (CH4). In this second phase of the Regional Carbon Cycle Assessment and Processes (RECCAP2), we quantify global coastal ocean fluxes of CO2, N2O and CH4 using an ensemble of global gap-filled observation-based products and ocean biogeochemical models. The global coastal ocean is a net sink of CO2 in both observational products and models, but the magnitude of the median net global coastal uptake is ∼60% larger in models (−0.72 vs. −0.44 PgC year−1, 1998–2018, coastal ocean extending to 300 km offshore or 1,000 m isobath with area of 77 million km2). We attribute most of this model-product difference to the seasonality in sea surface CO2 partial pressure at mid- and high-latitudes, where models simulate stronger winter CO2 uptake. The coastal ocean CO2 sink has increased in the past decades but the available time-resolving observation-based products and models show large discrepancies in the magnitude of this increase. The global coastal ocean is a major source of N2O (+0.70 PgCO2-e year−1 in observational product and +0.54 PgCO2-e year−1 in model median) and CH4 (+0.21 PgCO2-e year−1 in observational product), which offsets a substantial proportion of the coastal CO2 uptake in the net radiative balance (30%–60% in CO2-equivalents), highlighting the importance of considering the three greenhouse gases when examining the influence of the coastal ocean on climate.

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