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1.
Distribution and inventories of 90Sr, 137Cs, 241Am and Pu isotopes in sediments of the Northwest Pacific Ocean 总被引:1,自引:0,他引:1
《Marine Geology》2005,216(4):249-263
Bottom sediments collected in the Northwest (NW) Pacific Ocean in 1997 were analysed for 90Sr, 137Cs, 239,240Pu and 241Am contents to determine their distribution patterns, inventories and sources. Enhanced inventories of 239,240Pu and 241Am were observed in the latitudinal belts of 10–20°N and 30–40°N, which correspond to major areas of local (tropospheric) and global (stratospheric) fallout (with a contribution from local fallout), respectively. The sediment inventory of 239,240Pu near the Bikini Atoll exceeded its overlying water inventory, however, in the mid-latitudes, more than 70% of 239,240Pu still remains in the water column. 241Am inventories in sediments exceeded that of the water column for the entire NW Pacific Ocean. Higher 137Cs and 90Sr sediment inventories in the latitudinal belt of 30–40°N are due to global fallout, and they account for about 10% and less than 5% of the water column inventories, respectively. The observed activity ratios of 137Cs/90Sr, 238Pu/239,240Pu and 241Am/239,240Pu in sediment were at some stations higher than the global fallout ratios due to contributions from local fallout and due to specific processes in the water column. Two end-member mixing model based on the 240Pu/239Pu atom ratios observed in global and local fallout yielded ∼60% contribution of the local fallout in the bottom sediments near the Bikini Atoll. The upward decrease in the 240Pu/239Pu atom ratios in the sediment column indicates a decrease in the contribution of local fallout to the Pu inventory with time. 241Am and 241Pu dating of sediment layers was utilized to explain a hiatus in sediment accumulation in the deep seafloor. 相似文献
2.
《Estuarine, Coastal and Shelf Science》1987,25(2):169-174
A study was made of the 239Pu, 240Pu, 238Pu and 137Cs concentrations in tidal marsh sediments of the Savannah River estuary. Tidal marshes are identified as special locations for plutonium deposition because of the high biological productivity and relative stability of sediments as compared to channel sediments. The 239,240Pu deposition averaged 3·2 mCi km−2, which is higher than land-based fallout values of about 2 mCi km−2. The 239,240Pu to 137Cs ratio was about three times higher than fallout deposition estimates, indicating a more rapid desorption of 137Cs from sediment in the saline waters of the area. 相似文献
3.
Surface intertidal sediments from 35 sites in the Irish Sea have been analysed for their 238Pu and 239,240Pu activities, together with an intensive study of plutonium in sediments of the Esk Estuary (NW England). The range of plutonium activities for the whole survey were 0·14–4118 and 1·3–16 026 Bq kg−1 for 238Pu and 239,240Pu, respectively. The levels of Pu activity, derived from the Sellafield nuclear fuel reprocessing effluents, in sediments are controlled by lithological factors and the influence of transport and post-depositional processes. Grain size distribution is particularly important, the major part of plutonium activity being in the mud fraction of all sediments.The data suggest that over the Irish Sea coastline, dynamic mixing of sediment grains by reworking and resuspension and/or by dispersion in tidal currents are important in determining plutonium distributions. The exponential decrease in sediment plutonium activities away from the Sellafield source is attributed to the progressive mixing with older contaminated and uncontaminated sediments. 相似文献
4.
The distribution and inventory of artificial radionuclides,239,240Pu and137Cs were determined in the East China and the Yellow Seas in 1987. Almost all of239,240Pu and 50 to 80% of137Cs in the continental shelf area are retained in the sediment column.239,240Pu sediment inventory in the sea area is larger than the fallout input and tends to increase southwardly. This excess239,240Pu and the lateral distribution are attributable to the supply of239,240Pu by the Yangtze River discharge. On the contrary,137Cs sediment inventory shows a decrease to the south, and the fact can be accounted for by the southward dispersion of fine silt particles discharged from the Yellow River. Total137Cs inventory is smaller than the estimated fallout input, and the fact seems to indicate dispersion of137Cs out of the shelf region. Vertical profiles of239,240Pu and137Cs contents in sediments differ from that of natural210Pb, implying the effect of varied accumulation rates of the artificial radionuclides over the sediment particle mixing by benthic organisms. Apparent maximum sediment particle mixing coefficient (D
B
) calculated from the excess210Pb profiles in stations located between the inner and outer shelves ranged from 1.4 to 8.3 cm2y–1. ThisD
B
value is higher than that in the Okinawa Trough (1.0 cm2y–1), but lower than previously estimatedD
B
value (26 cm2y–1) in the outer shelf mud. 相似文献
5.
Concentrations and inventories of137Cs and239,240Pu were determined in sea waters and sediments columns from the western North Pacific from 1980 to 1986.The239,240Pu/137Cs activity ratio in the water column shows a tendency to increase from the surface (10–3) to bottom waters (10–1), but the ratio in sediment is within a rather narrow range (10–2 to 10–1), indicating more effective removal of plutonium from the water column than137Cs. In regions south of 40N, the radionuclide inventories in the water column significantly exceed the estimated global fallout (stratospheric fallout due to the atmospheric nuclear explosion), especially in the case of239,240Pu. These excess inventories imply that local or close-in fallout derived from nuclear explosions in the equatorial North Pacific are well-preserved and retained in the regions, despite about 20 years since the atmospheric nuclear explosion moratorium. Data suggesting lateral transport of137Cs in surface water from north of 40N to southern regions is shown. Some data on90Sr contents are also shown. 相似文献
6.
《Deep Sea Research Part I: Oceanographic Research Papers》2007,54(8):1289-1310
Arctic sea ice can incorporate sediment and associated chemical species during its formation in shallow shelf environments and can also intercept atmospherically transported material during transit. Release of this material in ice ablation areas (e.g. the Fram Strait) enhances fluxes of both sediments and associated species in such areas. We have used a suite of natural (7Be, 210Pb) and anthropogenic (137Cs, 239Pu, 240Pu) radionuclides in sea ice, sea-ice sediments (SIS), sediment trap material and bottom sediments from the Fram Strait to estimate transit times of sea ice from source to ablation areas, calculate radionuclide fluxes to the Fram Strait and investigate the role of sea-ice entrained sediments in sedimentation processes. Sea ice intercepts and transports the atmospherically supplied radionuclides 7Be and 210Pb, which are carried in the ice and are scavenged by any entrained SIS. All of the 7Be and most of the excess 210Pb measured in SIS collected in the Fram Strait are added to the ice during transit through the Arctic Ocean, and we use these radionuclides as chronometers to calculate ice transit times for individual ice floes. Transit times estimated from the 210Pb inventories in two ice cores are 1–3 years. Values estimated from the 7Be/210Pbexcess activity ratio of SIS are about 3–5 years. Finally, equilibrium values of the activity ratio of 210Pb to its granddaughter 210Po in the ice cores indicate transit times of at least 2 years. These transit times are consistent with back-trajectory analyses of the ice floes. The latter, as well as the clay-mineral assemblage of the SIS (low smectite and high illite content), suggest that the sampled sea-ice floes originated from the eastern Siberian Arctic shelf seas such as the eastern Laptev Sea and the East Siberian Sea. This result is in agreement with the relatively low activities of 239,240Pu and 137Cs and the 240Pu/239Pu atom ratios (∼0.18, equivalent to that in global fallout) in SIS, indicating that prior global atmospheric fallout, rather than nuclear fuel reprocessing facilities, forms the main source of these anthropogenic radionuclides reaching the western Fram Strait at the time of sampling (1999). Transport of radionuclides by sea ice through the Arctic Ocean, either associated with entrained SIS or dissolved in the ice, accounts for a significant flux in ablation areas such as the Fram Strait, up to several times larger than the current atmospheric flux in the area. Calculated fluxes derived from sea-ice melting compare well to fluxes obtained from sediment traps deployed in the Fram Strait and are consistent with inventories in bottom sediments. 240Pu/239Pu atomic ratios lower than 0.18 in bottom sediments from the Fram Strait provide evidence that plutonium from a source other than atmospheric fallout has reached the area. Most likely sources of this Pu include tropospheric fallout from atomic weapons testing of the former Soviet Union prior to 1963 and Pu released from nuclear reprocessing facilities, intercepted and transported by sea ice to the ablation areas. Future work is envisaged to more thoroughly understand the actual mechanisms by which radionuclides are incorporated in sea ice, focusing on the quantification of the efficiency of scavenging by SIS and the effect of melting and refreezing processes over the course of several years during transit. 相似文献
7.
《Marine Chemistry》2001,73(2):125-152
We report here bioturbation and sediment accumulation rates determined from replicate sediment cores at four different sampling sites on the Palos Verdes shelf, Southern California, using bomb fallout and natural radionuclides (137Cs, 239,240Pu, 210Pb, 234Th, and 14C), along with supporting measurements of organic carbon (OC), porosity and granulometry. Present-day particle reworking, on time scales of several months, is restricted to the upper 3 cm, with rates ranging from 13 to 200 cm2/year, as deduced from 234Thxs profiles. There is little evidence that particle reworking reached depths significantly greater than 5 cm. Post-1963 (or post-1971) sediment accumulation rates ranged from 0.7 to 1.4 g/cm2/year (equivalent to 1.1–1.8 cm/year for surficial sediments), as calculated from Pu and Cs isotope profiles, with little change over time or distance from the outfall. Lateral transport of older sediment and multiple sediment sources on the Palos Verdes shelf is suggested from radiocarbon measurements on foraminifera and bulk sedimentary organic matter at two sampling sites, which showed variable, old and refractory sources of OC. Pre-1953 sediments accumulated at rates that were at least 0.4 g/cm2/year (≥0.3 cm/year), based on 210Pbxs dating. Given the abundance of sediment sources to the Palos Verdes shelf, the high sedimentation rates, and shallow particle mixed layers, contaminant-enriched layers should continue to move deeper into the sediments. 相似文献
8.
Sang-Han Lee Pavel P. Povinec Janine Gastaud Beniamino Oregioni Laurent Coppola Catherine Jeandel 《Journal of Oceanography》2009,65(3):397-406
Anthropogenic 90Sr, 239,240Pu and 241Am were used as tracers of water mass circulation in the Crozet Basin of the South Indian Ocean, represented by three main
water fronts—Agulhas (AF), Subtropical (STF) and Subantarctic (SAF). Higher 90Sr concentrations observed north of 43°S were due to the influence of AF and STF, which are associated with the south branch
of the Subtropical gyre, which acts as a reservoir of radionuclides transported from the North to the South Indian Ocean.
On the other hand, the region south of 43°S has been influenced by SAF, bringing to the Crozet Basin Antarctic waters with
lower radionuclide concentrations. The 238Pu/239,240Pu activity ratios observed in water and zooplankton samples indicated that, even 35 years after the injection of 238Pu to the Indian Ocean from the burn-up of the SNAP-9A satellite, the increased levels of 238Pu in surface water and zooplankton are still well visible. The radionuclide concentrations in seawater and their availability
to zooplankton are responsible for the observed 210Po, 239,240Pu and 241Am levels in zooplankton. 相似文献
9.
Lee W. Cooper J. M. Kelley L. A. Bond K. A. Orlandini J. M. Grebmeier 《Marine Chemistry》2000,69(3-4)
We report here thermal ionization mass spectrometry measurements of 239Pu, 240Pu, 241Pu, 242Pu, and 237Np isolated from oceanic, estuarine, and riverine sediments from the Arctic Ocean Basin. 238Pu/239+240Pu activity ratios are also reported for alpha spectrometric analyses undertaken on a subset of these samples. Our results indicate that the Pu in sediments on the Alaskan shelf and slope, as well as that in the deep basins (Amerasian and Eurasian) of the Arctic Ocean, has its origin in stratospheric and tropospheric fallout. Sediments from the Ob and Yenisei Rivers show isotopic Pu signatures that are distinctly different from those of northern-hemisphere stratospheric fallout and indicate the presence of weapons-grade Pu originating from nuclear fuel reprocessing wastes generated at Russian facilities within these river catchments. Consequently, sediments of the Eurasian Arctic Ocean, particularly those in the Barents and Kara Seas, probably contain a mixture of Pu from stratospheric fallout, tropospheric fallout, and fuel-reprocessing wastes of riverine origin. In particular, the 241Pu/239Pu ratios observed in these sediments are inconsistent with significant contributions of Pu to the arctic sediments studied from western European reprocessing facilities, principally Sellafield in the UK. Several other potential sources of Pu to arctic sediments can also be excluded as significant based upon the transuranic isotope ratios presented. 相似文献
10.
11.
D. Knapinska-Skiba R. Bojanowski Z. Radecki G. E. Millward 《Estuarine, Coastal and Shelf Science》2001,53(6):779
The activity concentrations of dissolved137Cs have been determined in the water column and137Cs and134Cs in the sediments and the sediment porewaters of the southern Baltic Sea. The mean activity concentration of dissolved137Cs in the Gdansk Deep declined from 109 Bq m−3in June 1986 to 61 Bq m−3in 1999. In sediments, the activity concentrations of137Cs (33-231 Bq kg−1) were highest in muds and the activity concentrations of134Cs were about 6% of the total Cs activity. The Chernobyl contribution to137Cs activity was between 43% and 77%. The porewater activity concentrations of137Cs in muddy sediments were in the range 71 to 3900 Bq m−3and were higher than those in the overlying seawater. The diffusive flux of dissolved137Cs from the muddy sediments was estimated in the range 5 to 480 Bq m−2year−1. The flux of137Cs from sediment porewaters of the southern Baltic Sea was about 45% of the total, including fluxes of137Cs from wet and dry atmospheric deposition and the fluvial inputs. The results were used to elucidate the rate of recovery of the sediments and the waters of the southern Baltic from Chernobyl-derived137Cs. 相似文献
12.
Masashi Kusakabe Naohiko Inatomi Hyoe Takata Takahito Ikenoue 《Journal of Oceanography》2017,73(5):529-545
Radioactivity has been monitored in seafloor sediments off Fukushima and nearby prefectures regularly. During the initial monitoring period (May–September 2011), 137Cs concentrations in the surface sediments (0–3 cm) generally increased to 8–580 Bq/kg. Subsequently, concentrations decreased at variable rates. In the latest data, from February 2016, concentrations were still higher at 0.8–141 Bq/kg than the pre-accident level. The geometric mean concentration declined steadily from 47 Bq/kg in September 2011 to 13 Bq/kg in February 2016. The 137Cs abundance (Bq/m2) in the surface sediment at each station decreased similarly. The rate of decrease of surface abundance varied spatially by almost one order of magnitude, ranging from 1.1 × 10?4 to 1.7 × 10?3/day, equivalent to halving times of 16–1.1 years, respectively. The rate of decrease was related to the median sediment grain size at each station. In addition, bottom-water dynamics, through the redistribution of bottom sediments, may have caused spatial variability in the rate of decrease, whereas vertical profiles of 137Cs concentrations in the sediment suggest that vertical migration of 137Cs was not a major mechanism reducing the surface 137Cs concentration. From September 2011 to February 2016, the overall halving time of 137Cs in the surface sediment in the monitoring area, excluding the area inside a 30-km radius from the Fukushima Dai-ichi Nuclear Power Plant, was 2.3 years. Thus, 76% of the originally deposited 137Cs (46 × 1012 Bq) in the surface sediment was transported out of the area during that period. 相似文献
13.
《Estuarine, Coastal and Shelf Science》1987,25(4):413-434
The distribution of 239,240Pu between dissolved and particulate forms has been measured in four estuaries on the north-east coast of the United States (Connecticut River, Delaware Bay, Chesapeake Bay, and Mullica River). The data cover the whole salinity range from freshwater input to shelf waters at 35‰ and includes one profile from a nearly anoxic basin in the Chesapeake Bay.In the organic-rich Mullica River estuary, large-scale removal of riverine dissolved 239,240Pu occurs at low salinities due to salt-induced coagulation, a mechanism analogous to that for iron and humic acids. Within the 0 to 25–30‰ zone in the other three estuaries, the activity of dissolved 239,240Pu increases almost conservatively. The activities of particulate 239,240Pu are highest in the more turbid waters of low salinity regime (0–15‰), but become increasingly insignificant with respect to dissolved 239,240Pu as salinities increase. At higher salinities corresponding to shelf water, there is a sharp increase in dissolved 239,240Pu activity. The dissolved 239,240Pu activity within each estuary appears to be inversely related to the flushing time of water. For example, Chesapeake Bay has a 6–12 month flushing time and has much lower dissolved 239,240Pu activities than does the Connecticut River Estuary which has a flushing time of a few days. This and other data from the shelf waters are interpreted as indicating that the sharp decrease in dissolved 239,240Pu activities between shelf and estuarine waters is driven by removal within the estuaries themselves rather than on the shelf.Dissolved 239,240Pu activities are lower in the nearly-anoxic bottom waters of Chesapeake Bay indicating enhanced removal by redox transformation of Pu [i.e., Pu(V) to Pu(IV)]. 相似文献
14.
本文对东海及毗邻海域中239+240Pu比活度、240Pu/239Pu原子比值和239+240Pu累积通量或沉积通量数据进行整理,首次从大气沉降、海水中、生物体中、沉积物捕获器中以及沉积物中的239+240Pu 5个方面阐述了东海及毗邻海域中239+240Pu的地球化学行为。研究结果表明,全球大气沉降和太平洋核试验场输入的239+240Pu是东海海水和沉积物中239+240Pu的两个主要来源;在长江径流、浙闽沿岸流、台湾暖流、黑潮与上升流等水团的混合作用以及清除作用的影响下,东海近岸海水中239+240Pu浓度在时间上呈现被清除而减少的趋势,相应近岸浅水区沉积物中239+240Pu的埋藏深度高于远岸深水海域。在黑潮入侵和上升流的作用下,冲绳海槽区尤其是台湾岛东北部,沉积物中的239+240Pu比活度与沉积通量显著增大。同时,利用东海表层沉积物中239+240Pu比活度和240Pu/239Pu原子比值的相关关系证实了台湾东北部黑潮底层分支流的存在,并指示出台湾暖流与黑潮底层分支流可能交汇的海域位置。 相似文献
15.
Contents of90Sr,137Cs and60Co in surface sediments were investigated in and around Urazoko Bay, Fukui Prefecture, where a nuclear power plant has been operating since 1969 and the waste effluent has been released into the sea. The main source of90Sr and137Cs was recognized to be radioactive fallout, whereas60Co was considered to originate from the nuclear power plant. Using the137Cs concentration as an indicator of sorption capacity of the sediment, the behaviour of60Co was investigated. No seasonal variation was observed in the distribution pattern of60Co/137Cs ratio and the retention of the heavy initial discharge in 1969 was considered to dominate the radionuclide level in the sediment. Correlation of60Co/137Cs ratio in the sediment and the distance from the discharge outlet was expressed by a simple exponential function of the distance. It was suggested that the contamination is spreading out gradually to the outer region of Urazoko Bay. 相似文献
16.
北太平洋西部和印度洋东部及其邻近海域表层水体中137Cs的分布 总被引:1,自引:0,他引:1
对北太平洋西部海域、苏禄海及印尼海、中国南海、印度洋东部海域、孟加拉湾及安达曼海等表层水体中放射性核素137Cs的活度进行了测定。结果表明,上述海域表层水体中137Cs活度显示了较大的变化范围,最低值出现在南极附近的南大洋(1.1Bqm-3),较高的活度值则出现在北太平洋西部海域及中国南海(3Bqm-3)。在所研究水域范围内,137Cs活度的纬度分布特征并没有完全有效地反映出137Cs的全球理论大气沉降趋势及其纬度效应。综合本研究及Miyake等人(1988)的测定结果,我们计算出137Cs自表层海水中的析出速率在苏禄海及印尼海约为0.016/a,在孟加拉湾及安达曼海约为0.033/a,在中国南海约为0.029/a,这一结果明显低于西北太平洋日本沿海表层水体中137Cs的析出速率。这可能是因为在这些海域,横向及纵向的水体混合过程相对都较慢,而且颗粒物对137Cs的吸附析出过程也比较弱所致。 相似文献
17.
Hideyuki Kawamura Toshimichi Ito Takuya Kobayashi Shigeyoshi Otosaka Naoki Hirose Orihiko Togawa 《Journal of Oceanography》2010,66(5):649-662
A numerical experiment is carried out to reproduce distribution of concentration of 90Sr and 137Cs, estimate their total amount and verify their source in the Japan Sea. Model results are in good agreement with observational
findings in the Japan Sea expeditions between 1997 and 2002 by the Japan Atomic Energy Agency. Vertical profiles of the concentration
of 90Sr and 137Cs show exponential decreases with depth from the sea surface to the sea bottom. From the model and observational results,
it is suggested that the concentration of 90Sr and 137Cs in the surface layer is approximately in the range of 1.0–1.5 Bq/m3 and 2.0–2.5 Bq/m3, respectively. On the other hand, it is found that the concentration in the intermediate and deep layer
is higher than that observed in the northwestern Pacific Ocean, suggesting active winter convection in the Japan Sea. The
total amount of 90Sr and 137Cs in the seawater is evaluated to be 1.34 × 1015 Bq and 2.02 × 1015 Bq, respectively, in the numerical experiment, which demonstrates an estimation by observational data obtained in the Japan
Sea expeditions. The total amount of 90Sr and 137Cs changed during the second half of 20th century corresponding to deposition at the sea surface with the maximums of 4.86
× 1015 Bq for 90Sr and 7.33 × 1015 Bq for 137Cs, respectively, in the mid-1960s. The numerical experiment suggests that the main source of 90Sr and 137Cs has been global fallout, although there have been some potential sources in the Japan Sea. 相似文献
18.
19.
Peter H. Santschi Scott Nixon Michael Pilson Carlton Hunt 《Estuarine, Coastal and Shelf Science》1984,19(4):427-449
The accumulation of sediments, trace metals and hydrocarbons has been estimated from the analysis of the sediment from six coring sites in Narragansett Bay. Radionuclides (234Thxs, 210Pbxs, 239,240Pu) with known input functions and trace metals (Cu, Pb) were used. We estimate that 6·9 × 104 tons of sediments, 51–90 tons of Pb, 72–100 tons of Cu and 400–1000 tons of total hydrocarbons accumulate annually under present conditions in the bay. This represents 64–117% (Pb), 89–123% (Cu) and 23–58% (hydrocarbons), respectively, of present day inputs to the bay. Furthermore, close to 100% of the particle-reactive radionuclides 210Pb and 239,240Pu accumulate in the bay. Present day inputs to the bay were calculated independently as 77–80 tons Pb and 81 tons of Cu. Sewage effluents were the dominant source of Cu, whereas atmospheric deposition and urban runoff were most important for Pb. Dredging activities by the U.S. Army Corps of Engineers between 1946 and 1971 removed more sediments from the bay than would have accumulated during the same time in the undredged areas of the bay. Copper smelting and coal mining on the shores of the upper bay during 1866–1880 left an imprint in the sediments which is still evident. Model derived accumulation rates of Pb, Cu and coal during that time were 3–4 times present-day inputs. 相似文献
20.
To investigate the factors controlling lead (Pb) concentration and identify the sources of Pb in Yellow Sea sediments along the Korean coast, the concentration of Pb and Pb isotopes in 87 surface and 6 core sediment samples were analyzed. The 1 M HCl leached Pb concentrations had a similar geographic distribution to those of fine-grained sediments, while the distribution of residual Pb concentrations resembled that of coarse-grained sediments. Leached Pb was presumed to be associated with manganese (Mn) oxide and iron (Fe) oxy/hydroxide, while residual Pb was associated with potassium (K)-feldspar, based on good linear relationships between the leached Pb and the Fe/Mn concentrations, and the residual Pb and K concentrations. Based on a ratio–ratio plot with three isotopes (207Pb/206Pb and 208Pb/206Pb) and the geographic location of each sediment, sediments were categorized into two groups of samples as group1 and group2. Group 1 sediments, which were distributed in Gyeonggi Bay and offshore (north of 36.5°N), were determined to be a mixture of anthropogenic and natural Pb originating from the Han River, based on a 208Pb/206Pb against a Cs/Pbleached mixing plot of core and surface sediments. Group 2 sediments, which were distributed in the south of 36.5°N, also showed a two endmembers mixing relationship between materials from the Geum River and offshore materials, which had very different Pb concentrations and isotope ratios. Based on the isotopes and their concentrations in core and surface sediments, this mixing relationship was interpreted as materials from two geographically different origins being mixed, rather than anthropogenic or natural mixing of materials with the same origin. Therefore, the relative percentage of materials supplied from the Geum River was calculated using a two endmembers mixing model and estimated to be as much as about 50% at 35°N. The spatial distribution of materials derived from the Geum River represented that of fine-grained sediments originating from the Geum River. It was concluded that Pb isotopes in sediments could be used as a tracer in studies of the origin of fine-grained sediments along the Korean Yellow Sea coast. 相似文献