1 |
Stable Isotopes of Sulphur and Oxygen in Forested Catchments: Insight from New Techniques into Sulphur Cycling and Dissolved Organic Matter AlterationHumphries, Stefan January 2003 (has links)
Dissolved organic matter (DOM) is present in all forested catchments and can be important in binding metals, absorbing UV, and the transport of nutrients (C, N, S, P). DOM is extremely heterogeneous in time and space, making it difficult to characterize. New techniques have been developed to determine δ34S and δ18O in DOM. These techniques have been applied to samples from Harp and Plastic Lake catchments (45??23'N, 79?? 08'W, 45??11'N, 78?? 50'W) in order to obtain information about sources and sinks of DOM within forested catchments on the Canadian Shield. In conjunction with sulphate and DOC concentrations, this new data provides valuable insight into sulphur cycling and DOM alteration within these catchments. Data generated for δ34S-DOM and δ18O-DOM appears to be the first data reported in the literature for DOM.
The inorganic (δ34S-SO42-) and organic S (δ34S-DOM) differs by environment in both catchments. The range of δ34S-SO42- is between 3. 3‰ and 10. 3‰, and the range of δ34S-DOM is from 3. 4‰ to 8. 7‰. Sulphate in the Harp Lake catchment in most samples is subject to some sort of cycling within the watershed, since δ34S-SO42- differs from precipitation. In the Harp Lake catchment, upland δ34S-SO42- is influenced by historical precipitation. The δ34S-DOM is derived from leaching and microbial activity of DOM from organic horizons in the soil. The δ34S-SO42- and δ34S-DOM of wetland streams is extremely variable, controlled by hydrology. The δ34S-SO42- provides information on oxidation-reduction dynamics in the wetland, and δ34S-DOM provides information about sources of DOS in the wetland. The δ34S-SO42- and δ34S-DOM are possibly related in Harp Lake. Mineralization of DOS as evidenced by δ34S-DOM and DOS concentrations could be a small input of SO42- into Harp Lake.
It is possible δ18O-DOM could be an indicator of DOM alteration. The range of δ18O-DOM is between 8. 2‰ and 14. 4‰. The δ18O-DOM in the Harp Lake catchment is highly correlated with relative molecular weight, which has been shown to decrease with increasing alteration. Wetland streams show the largest range in δ18O-DOM, while uplands, groundwater, and Harp Lake are the least varied. The highest δ18O-DOM values are from sources of DOM such as leaf leachates (representative of forest floor litter) and wetlands. The most depleted samples are from groundwater and Harp Lake which typically contain highly altered DOM.
The δ34S-DOM and δ18O-DOM can provide valuable information on sources of DOM and DOM alteration within the catchment. The δ18O-DOM could also allow the separation of autochthonous and allochthonous DOM in lakes.
|
2 |
Stable Isotopes of Sulphur and Oxygen in Forested Catchments: Insight from New Techniques into Sulphur Cycling and Dissolved Organic Matter AlterationHumphries, Stefan January 2003 (has links)
Dissolved organic matter (DOM) is present in all forested catchments and can be important in binding metals, absorbing UV, and the transport of nutrients (C, N, S, P). DOM is extremely heterogeneous in time and space, making it difficult to characterize. New techniques have been developed to determine δ34S and δ18O in DOM. These techniques have been applied to samples from Harp and Plastic Lake catchments (45º23'N, 79º 08'W, 45º11'N, 78º 50'W) in order to obtain information about sources and sinks of DOM within forested catchments on the Canadian Shield. In conjunction with sulphate and DOC concentrations, this new data provides valuable insight into sulphur cycling and DOM alteration within these catchments. Data generated for δ34S-DOM and δ18O-DOM appears to be the first data reported in the literature for DOM.
The inorganic (δ34S-SO42-) and organic S (δ34S-DOM) differs by environment in both catchments. The range of δ34S-SO42- is between 3. 3‰ and 10. 3‰, and the range of δ34S-DOM is from 3. 4‰ to 8. 7‰. Sulphate in the Harp Lake catchment in most samples is subject to some sort of cycling within the watershed, since δ34S-SO42- differs from precipitation. In the Harp Lake catchment, upland δ34S-SO42- is influenced by historical precipitation. The δ34S-DOM is derived from leaching and microbial activity of DOM from organic horizons in the soil. The δ34S-SO42- and δ34S-DOM of wetland streams is extremely variable, controlled by hydrology. The δ34S-SO42- provides information on oxidation-reduction dynamics in the wetland, and δ34S-DOM provides information about sources of DOS in the wetland. The δ34S-SO42- and δ34S-DOM are possibly related in Harp Lake. Mineralization of DOS as evidenced by δ34S-DOM and DOS concentrations could be a small input of SO42- into Harp Lake.
It is possible δ18O-DOM could be an indicator of DOM alteration. The range of δ18O-DOM is between 8. 2‰ and 14. 4‰. The δ18O-DOM in the Harp Lake catchment is highly correlated with relative molecular weight, which has been shown to decrease with increasing alteration. Wetland streams show the largest range in δ18O-DOM, while uplands, groundwater, and Harp Lake are the least varied. The highest δ18O-DOM values are from sources of DOM such as leaf leachates (representative of forest floor litter) and wetlands. The most depleted samples are from groundwater and Harp Lake which typically contain highly altered DOM.
The δ34S-DOM and δ18O-DOM can provide valuable information on sources of DOM and DOM alteration within the catchment. The δ18O-DOM could also allow the separation of autochthonous and allochthonous DOM in lakes.
|
3 |
Sulphur transformation during pyrolysis of an Australian ligniteYani, Setyawati January 2009 (has links)
Australia has the largest economical lignite resources in the world. However, the utilisation of lignite is faced with a number of technical, economical and environmental problems due to its high moisture content and some of the deposits containing high sulphur and high inorganic matter. During pyrolysis, the first step of any thermochemical conversion processes of coal, some of the sulphur in lignite evolves as sulphur-bearing volatiles while others are retained in the solid phase of the lignite char. The present research aims to study the sulphur transformation during pyrolysis of Australian lignite. The specific objectives of this research include a study on the transformation of pyrite, sulphate and organic sulphur during lignite pyrolysis as well as an investigation of the effect of inorganic matter on the sulphur transformation during lignite pyrolysis. To help the interpretation of sulphur transformation, the lignite samples were characterised using a combination of analytical techniques, i.e. X-ray diffraction (XRD), X-ray fluorescent (XRF), ion chromatography (IC), Scanning electron microscope equipped with an energy-dispersive X-ray spectroscopy (SEM-EDS), Fourier transform infra red (FTIR), solid state 13C nuclear magnetic resonance (NMR) and petrographic analysis. Pyrolysis was carried out in a thermogravimetric analyser (TGA) and fixed bed reactor. The lignites and their chars were analysed for sulphur forms using a carbon sulphur (CS) analyser. To study the volatiles released during pyrolysis, experiments were also performed using a TGA coupled to a mass spectrometer (TGA-MS). Eleven (11) Australian lignite samples, denoted as L1 to L11, respectively, from the same lignite deposit but with different sulphur and inorganic matter concentrations were employed in this study. They are categorised as of low quality since they contain high Executive Summary Sulphur Transformation during Pyrolysis of an Australian Lignite v moisture, very high ash, low fixed carbon and thus they have low calorific value, except for L1. The lignites contain considerable amount of total sulphur, except for L1. Mineralogy of the lignites showed that the lignites contain extremely high sodium and chlorine. FTIR and solid state 13C NMR spectroscopy confirmed that oxygenated functional structures are significantly present in the lignites.
|
4 |
Traitement de composés soufrés organiques récalcitrants par biofiltration : optimisation des conditions opératoires pour une application industrielle / Treatment of recalcitrant organic sulphur compounds by biofiltration : optimization of operating conditions for an industrial application.Legrand, Paul 30 September 2011 (has links)
Les émissions odorantes constituent un enjeu environnemental dont l'importance n'a cessé de croître dans les zones urbaines et industrielles. Les émissions anthropogéniques de composés soufrés contribuent à une concentration locale excédant fortement le seuil de perception. Afin de satisfaire des contraintes règlementaires de plus en plus strictes, les procédés biologiques dont la biofiltration sont une alternative intéressante car respectueuse de l'environnement et de moindre coût. Les seuils de perception des composés soufrés, très bas (µg. m-3), obligent à atteindre des efficacités d'abattement particulièrement élevées, le résiduel de concentration pouvant être à l'origine d'un impact notable sur les populations riveraines. L'étude a donc consisté à améliorer les performances des biofiltres concernant l'élimination des composés soufrés i) en ajustant certains paramètres opératoires clefs tels que le sens de circulation de l'effluent gazeux, le pH et l'ensemencement du matériau support, ii) en considérant le dimensionnement des biofiltres mis en œuvre (unités pilotes de laboratoire et semi-industrielles) et iii) la complexité du gaz à traiter (mono-polluant et mélange de composés à traiter). / Odorous emissions are a serious concern whose importance became higher in urban and industrial areas. Anthropogenic emissions of sulphur compounds lead to local concentration that exceeds strongly the odour threshold of human nose. In order to fulfil legal requirements that have become stricter in recent years, biological processes and biofiltration more accurately are an interesting alternative as biofilters provide an expanding variety of opportunities for economical and environmentally friendly solutions for many waste gas emissions. The odour thresholds of sulphur compounds are very low (µg.m3 air) and then require that biofilters provide high removal efficiency as the residual concentration can induce an odorous impact on neighbourhood populations.Hence, the study consisted in improving biofilters performances concerning sulphur compounds treatment i) by upgrading important operating parameters such as air flow distribution, pH and inoculation of packing material, ii) by considering biofilters design (laboratory and semi-industrial pilot units) and iii) the gaseous effluent complexity (only one pollutant and mixture of different compounds).
|
Page generated in 0.0552 seconds