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1.
Tipping E Lawlor AJ Lofts S Shotbolt L 《Environmental pollution (Barking, Essex : 1987)》2006,141(1):139-150
CHUM-AM was used to investigate the behaviours of atmospherically-deposited heavy metals (Ni, Cu, Zn, Cd and Pb) in three moorland sub-catchments in Cumbria UK. The principal processes controlling cationic metals are competitive partitioning to soil organic matter, chemical interactions in solution, and chemical weathering. Metal deposition histories were generated by combining measured data for the last 30 years with local lake sediment records. For Ni, Cu, Zn and Cd, default parameters for the interactions with organic matter provided reasonable agreement between simulated and observed present-day soil metal pools and average streamwater concentrations. However, for Pb, the soil binding affinity in the model had to be increased to match the observations. Simulations suggest that weakly-sorbing metals (Ni, Zn, Cd) will respond on timescales of decades to centuries to changes in metal inputs or acidification status. More strongly-sorbing metals (Cu, Pb) will respond over centuries to millennia. 相似文献
2.
Since the ban on the use of trichloroacetic acid (TCAA) as a herbicide in several countries, TCAA is still found ubiquitously in the environment. The presence of TCAA nowadays is suggested to originate mainly from the atmospheric degradation of tetrachloroethene. Our mass balance calculations indicate that this may be true for the presence of TCAA in the atmosphere. However, our mass balance calculations also provide tentative evidence for the formation of TCAA in soil. If our calculated production fluxes are realistic estimates, a very large source of TCAA in soil has been identified. 相似文献
3.
The study concerns the possible changes in the molecular characteristics of humic materials isolated from the same source as a function of time. A great deal of data has been reported concerning the contrast in molecular characteristics of humic substances isolated from different environments. This has primarily been an attempt to identify source-specific molecular characteristics. However, data presented in this paper suggests that humic substances isolated from a single catchment have significant changes in molecular characteristics over time. Two naturally occurring peat pools (X and Y) situated upon a small organic catchment on Great Dun Fell, Cumbria, UK were sampled monthly between November 1994 and November 1996. Dissolved organic matter (DOM) from the pool water samples was fractionated using macroporous nonionic resins (XAD8 and 4), and the humic, fulvic and hydrophilic acids were collected. These fractions were analysed for elemental composition (C, H and N), weight average molecular weight, functional group content and adsorption (340 nm) of a 1 g l(-1) solution measured in a 1-cm spectrophotometer cell. The molecular characteristics were compared to those of natural DOM described by Scott et al. (1998). Scott et al. reported that drought conditions and seasonal climatic changes could have appreciable effects upon molecular characteristics of natural DOM. Results showed that the atomic H/C ratio of the humic substances increased immediately after strong drought conditions experienced in the summer of 1995. This change was temporary with atomic H/C ratio decreasing gradually over the following months. A similar decrease was observed in the carboxyl group content of the isolated compounds. The data set suggested that atomic H/C ratio in the fulvic and hydrophilic fractions exhibited seasonal characteristics of higher ratios during the late summer/early autumn months. This was not observed in the humic fraction. Humic acids exhibited a seasonal pattern of higher weight average molecular weight during the summer months. These trends were explained in terms of summer production of DOM in the catchment soils, their sequestering in the soil due to limited soil water movement during the summer months and their relative ease of dissolution when rainfall and soil water movement increased during the late summer/early autumn period. The results were found to support seasonal and long-term patterns observed in natural DOM as reported by Scott et al. (1998). 相似文献
4.
E. Tipping J.J. Rothwell A.J. Lawlor 《Environmental pollution (Barking, Essex : 1987)》2010,158(5):1521-1529
Simulation modelling with CHUM-AM was carried out to investigate the accumulation and release of atmospherically-deposited heavy metals (Ni, Cu, Zn, Cd and Pb) in six moorland catchments, five with organic-rich soils, one with calcareous brown earths, in the Pennine chain of northern England. The model considers two soil layers and a third layer of weathering mineral matter, and operates on a yearly timestep, driven by deposition scenarios covering the period 1400-2010. The principal processes controlling heavy metals are competitive solid-solution partitioning of solutes, chemical interactions in solution, and chemical weathering. Agreement between observed and simulated soil metal pools and surface water concentrations for recent years was generally satisfactory, the results confirming that most contemporary soil metal is from atmospheric pollution. Metals in catchments with organic-rich soils show some mobility, especially under more acid conditions, but the calcareous mineral soils have retained nearly all anthropogenic metal inputs. Complexation by dissolved organic matter and co-transport accounts for up to 80% of the Cu in surface waters. 相似文献
5.
Canopy influence on trace metal atmospheric inputs on forest ecosystems: Speciation in throughfall 总被引:1,自引:0,他引:1
L. Gandois E. Tipping C. Dumat A. Probst 《Atmospheric environment (Oxford, England : 1994)》2010,44(6):824-833
Atmospheric inputs of selected Trace Metals (TM: Cd, Cu, Ni, Pb, Sb, Zn, as well as Al, Fe and Mn) were studied on six forested sites in France. In order to evaluate canopy interaction with atmospheric inputs, TM were measured in both Open Field Bulk Deposition (BD) and Throughfall (TF). Anthropogenic contribution to BD composition is high for Zn, Cd and Sb, reflecting actual TM emissions trends. Canopy greatly influences precipitation composition, through different processes, including assimilation and leaching by canopy, complexation as well as accumulation/dissolution of dry deposition. TM and Dissolved Organic Carbon (DOC) physical fractionation between colloidal and truly dissolved phases was performed with ultrafiltration. Al, Fe, Pb and Cu are found in the colloidal fraction whereas Cd, Ni, Zn and Sb are mostly in the truly dissolved fraction. Chemical speciation predicted with WHAM-VI shows that in throughfall, Al, Fe, Pb and Cu are almost entirely complexed by DOC, whereas Ni, Cd and Zn are present in average 30% in the free metal ion form. TM present in labile forms (Cd, Ni, Zn) interact with the canopy, are cycled in the ecosystem, and their concentration is either slightly increased or even decreased in throughfall. Sb, Pb and Cu concentration are increased through canopy, as a consequence of dry deposition accumulation. 相似文献
6.
Tipping E Poskitt JM Lawlor AJ Wadsworth RA Norris DA Hall JR 《Environmental pollution (Barking, Essex : 1987)》2011,159(12):3721-3729
The median total mercury concentration in 898 UK rural topsoils, sampled between 1998 and 2008, was 0.095 μg g−1. Approximate adjustment for unreactive metal produced an estimate of 0.052 μg g−1 for reactive Hg. The highest concentrations were in the north and west, where organic-rich soils with low bulk densities dominate, but the spatial pattern was quite different if soil Hg pools (mg m−2) were considered, the highest values being near to the industrial north of England and London. Possible toxic effects of Hg were best evaluated by comparison with soil Critical Limits expressed as ratios of Hg to soil organic matter, or soil solution Hg2+ concentrations, estimated by chemical speciation modelling. Only a few percent of the rural UK soils showed exceedance, and this also applied to rural soils from the whole of Europe. UK urban and industrial soils had higher Hg concentrations and more cases of exceedance. 相似文献
7.
Tipping E Thacker SA Wilson D Hall JR 《Environmental pollution (Barking, Essex : 1987)》2008,152(1):41-49
During the last 50 years nitrate concentrations in Buttermere and Wastwater (Cumbria, UK) have risen significantly, by 70 and 100%, respectively. By estimating contemporary nitrate fluxes in the lakes' catchments and in sub-catchments and comparing them with the fractional areas of different soil types, it is deduced that the surface water nitrate is derived almost entirely from organic-rich ranker soils that have a limited ability to retain atmospherically-deposited nitrogen. Little or no nitrate leaches from the other major soil type, a brown podzol, despite it having a lower C:N ratio (12.0 g g(-1)) than the ranker (17.0 g g(-1)), nor is there much contribution from the small areas of improved (chemically fertilised) grassland within the catchments. Although some nitrate leaching is occurring, total N losses are appreciably smaller than atmospheric inputs, so the catchment soils are currently accumulating between 3 and 4 g N m(-2) a(-1). 相似文献
8.
C D Vincent A J Lawlor E Tipping 《Environmental pollution (Barking, Essex : 1987)》2001,114(1):93-100
Measurements were made of the contents of Al, Mn, Fe, Cu, Zn, Cd and Pb in Scapania undulata in three streams (D2, D5, D11) in the English Lake District. The stream waters had average pH values of 5.35 (D2), 5.81 (D5) and 7.26 (D11), the main differences in other major chemical components being in Mg, Al, Ca and alkalinity. There was generally more metal accumulation in the older parts of the plants, but this was not significant in all cases. Extents of accumulation varied with stream pH and dissolved metal concentration. For Al, accumulation was greatest in streams D2 and D5. Mn accumulated most in D5 and Fe was without preference. Cu, Zn and Cd accumulated mostly in the plants in stream D11 and Pb accumulated more in D5 and D11. In terms of enrichment factors (amount of metal in the plants divided by stream water concentration) the sequence was Zn < Cd < Cu < Mn < Pb < Al < Fe. Laboratory experiments supported the findings of the field data, providing evidence that uptake increases with pH at constant total metal concentration. The results are interpreted qualitatively in terms of the chemical speciation of the metals in the stream water and competition between metal ions and protons at the plant-water interface. It is suggested that Al, Cu, Zn, Cd and Pb behave according to chemical complexation, whereas redox processes and/or colloidal interactions may be significant for Mn and Fe. 相似文献
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10.
Tipping E Bettney R Hurley MA Isgren F James JB Lawlor AJ Lofts S Rigg E Simon BM Smith EJ Woof C 《Environmental pollution (Barking, Essex : 1987)》2000,109(2):183-191
Long-term changes in stream water chemistry in the upper Duddon catchment (southwest Lake District, UK) were investigated. Ten streams were sampled and analysed weekly during 1998, and the results compared with data for the early 1970s and 1986. The waters exhibited a range of pH, average values for 1998 being 5.04-7.04. For all the streams, the average pH in 1998 was greater than that during 1971-73. Statistical analysis was carried out, using the 1970s data to estimate the magnitude of inter-annual variation, and taking discharge into account on the basis of antecedent rainfall. The results showed that for two of the streams the pH increase was significant at the 2.5% level, while for a further three it was significant at the 10% level. Comparison of the 1998 concentrations of nitrate and non-marine sulphate with data obtained for five streams in 1973-74 showed that average nitrate concentration had increased from 11 to 20 microeq dm(-3) while that of non-marine sulphate had decreased from 94 to 50 microeq dm(-3). For four of the streams, comparisons were also made between the 1998 data and those for 1986. In three cases, pH in 1998 was generally higher, and Al generally lower, than the values for 1986, but in the fourth case little difference was evident. The present results support observations for five nearby standing waters, strengthening the evidence for a general reversal of acidification in the southwest part of Lake District, due to a decline in the deposition of pollutant sulphur. 相似文献