Future trends in transport and fate of diffuse contaminants in catchments,with special emphasis on stable isotope applications     

Jeffrey Turner  Hans‐Jrgen Albrechtsen  Mike Bonell  Jean‐Pierre Duguet  Bob Harris  Rainer Meckenstock  Kevin McGuire  Roger Moussa  Norman Peters  Hans H. Richnow  Barbara Sherwood‐Lollar  Stefan Uhlenbrook  Henny van Lanen 《水文研究》2006,20(1):205-213

A summary is provided of the first of a series of proposed Integrated Science Initiative workshops supported by the UNESCO International Hydrological Programme. The workshop brought together hydrologists, environmental chemists, microbiologists, stable isotope specialists and natural resource managers with the purpose of communicating new ideas on ways to assess microbial degradation processes and reactive transport at catchment scales. The focus was on diffuse contamination at catchment scales and the application of compound‐specific isotope analysis (CSIA) in the assessment of biological degradation processes of agrochemicals. Major outcomes were identifying the linkage between water residence time distribution and rates of contaminant degradation, identifying the need for better information on compound specific microbial degradation isotope fractionation factors and the potential of CSIA in identifying key degradative processes. In the natural resource management context, a framework was developed where CSIA techniques were identified as practically unique in their capacity to serve as distributed integrating indicators of process across a range of scales (micro to diffuse) of relevance to the problem of diffuse pollution assessment. Copyright © 2006 John Wiley & Sons, Ltd.  相似文献   

Extreme precipitation in WRF during the Newcastle East Coast Low of 2007     

James B. Gilmore  Jason P. Evans  Steven C. Sherwood  Marie Ekström  Fei Ji 《Theoretical and Applied Climatology》2016,125(3-4):809-827

In the context of regional downscaling, we study the representation of extreme precipitation in the Weather Research and Forecasting (WRF) model, focusing on a major event that occurred on the 8^th of June 2007 along the coast of eastern Australia (abbreviated “Newy”). This was one of the strongest extra-tropical low-pressure systems off eastern Australia in the last 30 years and was one of several storms comprising a test bed for the WRF ensemble that underpins the regional climate change projections for eastern Australia (New South Wales/Australian Capital Territory Regional Climate Modelling Project, NARCliM). Newy provides an informative case study for examining precipitation extremes as simulated by WRF set up for regional downscaling. Here, simulations from the NARCliM physics ensemble of Newy available at ～10 km grid spacing are used. Extremes and spatio-temporal characteristics are examined using land-based daily and hourly precipitation totals, with a particular focus on hourly accumulations. Of the different physics schemes assessed, the cumulus and the boundary layer schemes cause the largest differences. Although the Betts-Miller-Janjic cumulus scheme produces better rainfall totals over the entire storm, the Kain-Fritsch cumulus scheme promotes higher and more realistic hourly extreme precipitation totals. Analysis indicates the Kain-Fritsch runs are correlated with larger resolved grid-scale vertical moisture fluxes, which are produced through the influence of parameterized convection on the larger-scale circulation and the subsequent convergence and ascent of moisture. Results show that WRF qualitatively reproduces spatial precipitation patterns during the storm, albeit with some errors in timing. This case study indicates that whilst regional climate simulations of an extreme event such as Newy in WRF may be well represented at daily scales irrespective of the physics scheme used, the representation at hourly scales is likely to be physics scheme dependent.  相似文献   

The influence of carbon source on abiotic organic synthesis and carbon isotope fractionation under hydrothermal conditions   总被引：2，自引：0，他引：2  

Thomas M. McCollom  Barbara Sherwood Lollar  Jeffrey S. Seewald 《Geochimica et cosmochimica acta》2010,74(9):2717-155

A series of laboratory experiments were performed to investigate the relative contributions of CO and other single-carbon compounds to abiotic synthesis of organic compounds in hydrothermal environments. Experiments were conducted by heating aqueous solutions of CO, CO₂, HCOOH, or CH₄ at 250 °C under reducing conditions, and observing production of CH₄ and other hydrocarbons. Native Fe was included in the experiments as a source of H₂ through reaction with water and as a potential catalyst. Experiments with CO or HCOOH as the carbon source resulted in rapid generation of CH₄ and other hydrocarbons that closely resembled typical products of Fischer-Tropsch organic synthesis. In contrast, experiments using CO₂ or CH₄ as the carbon source yielded no detectable hydrocarbon products. Carbon isotope measurements of reaction products from the CO experiments indicate that the CH₄ and other hydrocarbons were substantially depleted in ¹³C, with CH₄ δ¹³C values 30 to 34‰ lighter than the initial CO. Most of the fractionation apparently occurs during attachment of CO to the catalyst surface and subsequent reduction to surface-bound methylene. The initial step in polymerization of these methylene units to form hydrocarbons involves a small, positive fractionation, so that ethane and ethene are slightly enriched in ¹³C relative to CH₄. However, subsequent addition of carbon molecules to the growing hydrocarbon chain proceeds with no net observable fractionation, so that the isotopic compositions of the C₃₊ light hydrocarbons are controlled by isotopic mass balance. This result is consistent with a previously proposed model for carbon isotopic patterns of light hydrocarbons in natural samples. The abundance and isotopic composition of light hydrocarbons produced with HCOOH as the carbon source were similar to those generated with CO, but the isotopic compositions of non-volatile hydrocarbons diverged, suggesting that the higher hydrocarbons were formed by different mechanisms in the CO and HCOOH experiments. The experiments indicate that CO, and possibly HCOOH, may be critical intermediates in the abiotic formation of organic compounds in geologic environments, and suggest that the low levels of these compounds present in most hydrothermal systems could represent a bottleneck restricting the extent of abiotic organic synthesis in some circumstances.  相似文献   

Carbon Isotope Fractionation of PCE and TCE During Dechlorination by Vitamin B12     

G.F. Slater  B. Sherwood Lollar  S. Lesage  S. Brown 《Ground Water Monitoring & Remediation》2003,23(4):59-67

Reductive dechlorination of perchloroethylene (PCE) and trichloroethylene (TCE) by vitamin B12 is an analogue of the microbial reductive dechlorination reaction and is presently being applied as a remediation technique. Stable carbon isotopic analysis, an effective and powerful tool for the investigation and monitoring of contaminant remediation, was used to characterize the isotopic effects of reductive dechlorination of PCE and TCE by vitamin B12 in laboratory microcosms. In laboratory experiments, 10 mg/L vitamin B12 degraded >90% of the initial 20 mg/L PCE with TCE, the primary product of PCE degradation, accounting for between 64% and 72% of the PCE degraded. In experiments with TCE, 147 mg/L vitamin B12 degraded >90% of the initial 20 mg/L TCE with cis -dichloroethene ( c DCE), the primary product of degradation accounting for between 30% and 35% of the TCE degraded. Degradation of both PCE and TCE exhibited first-order kinetics. Strong isotopic fractionation of the reactant PCE and of the reactant TCE was observed over the course of degradation. This fractionation could be described with a Rayleigh model using enrichment factors of −16.5%o and −15.8%o for PCE, and −17.2%o and −16.6%o for TCE. Fractionation was similar in all experiments, with a mean enrichment factor of −16.5%o ± 0.6%o. The occurrence of such large enrichment factors indicates that isotopic analysis can be used to monitor the dechlorination of PCE and TCE by vitamin B12 and remediation of ground water plumes. Evidence indicates that isotopic fractionation is taking place during complexation of the chlorinated ethenes to vitamin B12, as has been suggested for reductive dechlorination by zero valent iron. The differences between e values for this reaction and those observed for anaerobic biodegradation of the chlorinated ethenes suggest that there may be differences in the rate-determining step for these two processes.  相似文献   

The application of FAMM (Fluorescence Alteration of Multiple Macerals) analyses for evaluating rank of Paraná Basin coals, Brazil     

W. Kalkreuth  N. Sherwood  G. Cioccari  Z. Corrêa da Silva  M. Silva  N. Zhong  L. Zufa 《International Journal of Coal Geology》2004,57(3-4):167-185

Combining vitrinite reflectance (VR) and fluorescence alteration of multiple macerals (FAMM) analyses provide insights into the chemical nature of vitrinites (i.e., perhydrous vs. orthohydrous vs. subhydrous compositions) in Permian Gondwana coals of the Paraná Basin, Brazil. The FAMM-derived equivalent VR (EqVR) values and relationships with VR can be determined according to calibration curves based largely on Permian Gondwana coals of eastern Australia.The analytical results indicate that vitrinites in the Paraná Basin coals studied generally range from orthohydrous to perhydrous, with interpreted VR suppression ranging up to 0.2% absolute for the most perhydrous case. The EqVR values of the Santa Catarina coals, which range from about 0.85% to 0.95% differ from VR values by about 0.10–0.15% absolute, potentially having significant implications on coal utilization.The causes of vitrinite reflectance suppression in the Paraná Basin coals are as yet poorly understood, but are likely to be related to a combination of factors.  相似文献   

The relationship between magnetic field strength and reversal frequency: Preliminary palaeointensity results from the cretaceous quiet zone     

Graham J. Sherwood  John Shaw 《Studia Geophysica et Geodaetica》1991,35(4):325-333

Summary It has been predicted that the geomagnetic field strength will be at its highest during periods of low reversal frequency. Using basaltic lavas from Israel and India, which were erupted during the 35 Ma interval of normal polarity in the mid-Cretaceous (the Cretaceous Quiet Zone), we have obtained palaeointensity estimates. The mean virtual dipole moments from the two areas are about 75% of the present value. This suggests that there is no simple relationship between the time averaged strength of the dipole and the frequency of reversals.  相似文献   

Chloride loading in the South Fork of the Shenandoah River,Virginia, U.S.A.     

W. Cullen Sherwood 《Environmental Geology》1989,14(2):99-106

Loading trends and sources of CI^– in the South Fork of the Shenandoah River, Virginia were analyzed for the period 1929–1982. CI^– has increased from approximately 2 mg/L (2,776 tons/yr) to over 10 mg/L (14,256 tons/yr). Natural CI^– is estimated to be 1.01 mg/L (1,388 tons/yr) with precipitation providing 0.99 mg/L and rocks 0.02 mg/L. From 1929 to 1949 CI^– concentrations were relatively constant and independent of discharge, conforming to the Type II curve of Davis and Zobrist (1978), indicative of natural or relatively uncontaminated streams. Since 1952 CI^– concentrations increased exponentially as river discharge decreases conforming to the Type I curve of Davis and Zobrist for polluted streams. Since 1965 anthropogenic CI^– loading at 12,868 tons/yr has remained relatively constant. Four major sources contribute 92.2 percent (11,871 tons/yr) of the anthropogenic CI^–: (1) deicing salts—4,149 tons/yr, (2) domestic sewage—3,015 tons/yr, (3) livestock and poultry wastes—2,458 tons/yr, and (4) commercial fertilizers—2,249 tons/yr.  相似文献   

Field measurements of fairweather bottom boundary layer processes and sediment suspension on the Louisiana inner continental shelf   总被引：1，自引：0，他引：1  

L. D. Wright  C. R. Sherwood  R. W. Sternberg 《Marine Geology》1997,140(3-4):329-345

Field measurements of bottom boundary layer and sediment-transport processes were made on the Louisiana inner continental shelf in spring 1992 at a depth of 15.5 m, and in spring and summer 1993 at a depth of 20.5 m. Two different wave–current boundary layer/sediment-transport models were applied to the measured near-bed flows. In addition, the log-profile method was applied to estimate hydraulic roughness and bed stress. Consistent with the results of others, our measurements show that near-bed flows were very weak under non-storm conditions. Bed stresses were typically too low to resuspend bed sediments. However, the advection of high-turbidity layers or plumes past the instrumentation apparently caused a sustained period of high suspended sediment concentration throughout the log layer in spring 1993. In the absence of wave activity or high suspended sediment concentrations, boundary layer profiles showed the bed to have been hydraulically very smooth with cm. However, wave agitation, combined with increased suspended sediment concentration caused hydraulically rough conditions with cm.  相似文献   

Colloidally separated samples from Allende residues: Noble gases,carbon and an ESCA-study     

Ulrich Ott  Johann Kronenbitter  Jose Flores  Sherwood Chang 《Geochimica et cosmochimica acta》1984,48(2):267-280

A non-colloidal fraction separated by physical means from an $\text{HF}\text{HCl}$-resistant residue of the Allende carbonaceous meteorite exhibits a ratio of isotopically “normal” (Q-type) xenon to “anomalous” xenon (X-type) that is ~4 times larger than usually observed. Coincidentally this fraction contains carbon that is isotopically heavier by ~10%. than bulk Allende residue samples. ESCA analyses of companion colloidal separates show that the major portion of the S contained in our $\text{HF}\text{HCl}$-residues is elemental rather than a sulfide. They also confirm earlier observations that no elementally distinct surface coating is present, in accord with the absence of a surface-sited sulfur-bearing gas carrier, and that the oxygen content is increased after etching with nitric acid. For these separates noble gas data coupled with the ESCA data for nitrogen and the isotopic data for carbon point to the existence of heterogeneities among the noble gas-, carbon- and nitrogen-bearing phases and, thus, preservation of discrete components from the variety of source regions (or production mechanisms, or both) sampled by the Allende parent body. In sharp contrast to the success of physical and chemical methods in yielding samples in which one of the major noble gas components predominates to an extraordinary degree over the other, carbon isotopic compositions that have been inferred for the respective carrier phases in these same samples are strongly contradictory. Mass and isotope balance considerations lead us to conclude that a major fraction of the carbonaceous matter in Allende is noble-gas-poor, a result that could be confirmed by direct isolation of a sample, the carbon in which is dominated by this variety; and for that reason no simple relationship is discernable yet between observed isotopic compositions and either major noble gas component. Similar ambiguities may exist for nitrogen. The possible relationship between carbon-rich phases in ureilites and carbonaceous chondrites is considered.  相似文献   

World-wide increase in tropospheric methane, 1978–1983     

Donald R. Blake  F. Sherwood Rowland 《Journal of Atmospheric Chemistry》1986,4(1):43-62

Tropospheric concentrations of methane in remote locations have averaged a yearly world-wide increase of 0.018±0.002 parts per million by volume (ppmv) during the period from January 1978 to December 1983. The concentrations in the north temperate zone are always greater than those in the south temperate zone by 7±1% because the major methane sources are all predominantly located in the northern hemisphere. The average world-wide tropospheric concentration of methane in dry air was 1.625 ppmv at the end of 1983, measured against an NBS standard certified as 0.97 ppmv (but with an accuracy of only ±1%). The world-wide concentration increases are described by a linear equation with a standard deviation of 0.003 ppmv for ten different collection periods during 1978–1983. The precision of measurement of the methane concentration in the atmospheric samples and in the standard was measured to be ±0.4% for each. Repetitive measurements of an air sample collected in November 1977 have shown the same concentration for six years with a standard deviation for these data of ±0.003 ppmv.The causes for the steady increase in methane concentration in the troposphere cannot be fixed with certainty from present data. Contributing causes can include increases in the source strengths from cattle and rice fields. The atmospheric concentrations of CO, CH₄ and HO are all closely coupled with one another, and increased concentrations of CO and/or CH₄ should cause reduced concentrations of HO, which in turn should lengthen the atmospheric lifetimes of CO and CH₄.Among other physical and chemical effects, a increase of 0.18 ppmv per decade should contribute a greenhouse warming of about 0.04°C per decade. Other secondary contributions to the greenhouse effect from increases in CH₄ may arise from methane-induced increases in stratospheric H₂O, in tropospheric O₃, and in numerous other trace species whose concentration is controlled by reaction with HO radicals.An increased CH₄ source strength may result from the effect of increasing atmospheric temperatures on the known aqueous biological CH₄ sources, such as swamps, and may be an added consequence of the greenhouse effect.  相似文献