| 1. |
- Aurell, Johanna, et al.
(författare)
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Effects of quench time profiles on PCDD/F formation in the postcombustion zone during municipal solid waste incineration
- 2009
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Ingår i: Environmental Engineering Science. - : Mary Ann Liebert. - 1092-8758 .- 1557-9018. ; 26:3, s. 541-550
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Tidskriftsartikel (refereegranskat)abstract
- Effects of postcombustion zone temperatures and flue gas residence times on monochlorinated to octachlorinated dibenzo-p-dioxins and -furans (PCDD/F) in a laboratory-scale reactor combusting municipal solid waste were investigated. Four different quench time profiles were investigated, falling from 400°C to 200°C, 300°C to 100°C, 450°C to 200°C and 460°C to 260°C, with corresponding residence times of 1.4 to 4.4sec, 1.4 to 5.4sec, 1.3 to 4.3sec, and 1.3 to 4.0sec, respectively. Flue gas samples were collected simultaneously at three fixed sampling points, with an additional sampling of flue gas entering the postcombustion zone (640°C). The quench time profiles resulted in different total PCDD/F yields, as well as differences in homologue profiles and congener patterns. Thus, the formation pathways seem to be dependent on sufficient residence time within a specific temperature region. Formation of PCDD/F was shown to be rapid and mainly located to the 640°C to 400°C temperature region, with non-detectable levels at 640°C and concentrations at 400°C that did not increase or decrease significantly downstream. Furthermore, a prolonged residence time at and above 450°C/ 460°C showed low yields even downstream the postcombustion zone compared to the 400°C to 200°C and 300°C to 100°C profiles. The 460°C to 260°C profile resulted in increased abundance at the last two sampling points of PCDD congeners known to correlate with 2,4,6-trichlorophenols, suggesting that chlorophenol condensation reactions were promoted by this quench time profile.
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| 2. |
- Aurell, Johanna, et al.
(författare)
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Effects of sulfur on PCDD/F formation under stable and transient combustion conditions during MSW incineration
- 2009
-
Ingår i: Chemosphere. - : Elsevier. - 0045-6535 .- 1879-1298. ; 76:6, s. 767-773
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Tidskriftsartikel (refereegranskat)abstract
- SO2 levels in the flue gas from a laboratory-scale fluidized bed reactor combusting artificial municipal solid waste (MSW) were varied (resulting in four different SO2:HCl ratios 0, 0.2, 0.7 and 2.7 (by mass)) to study the effects of sulfur on the formation of polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs) and polychlorinated dibenzothiophenes (PCDTs). Sampling was performed simultaneously at three fixed points in the post-combustion zone with temperatures of 400, 300 and 200 °C, under normal combustion conditions and both during and after transient combustion conditions. The findings indicate that sulfur has a greater inhibitory effect on PCDF formation than on PCDD formation and that the PCDD/PCDF ratio in the flue gas depends on both the SO2:HCl ratio in the flue gas and memory effects arising from transient combustion conditions. The results also indicate that the relative importance of different pathways shifts in the post-combustion zone; condensation products increasing with reductions in temperature and increases in residence time. However, these changes appear to depend on the SO2:HCl ratio in the flue gas and combustion conditions. Sulfur seems to inhibit the chlorination of PCDFs. A tendency for increased SO2 levels in the flue gas to increase levels of PCDTs was also detected, but the increases were much less significant than the reductions in PCDF levels.
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| 3. |
- Aurell, Johanna, et al.
(författare)
-
Effects of transient combustion conditions on the formation of polychlorinated dibenzo-p-dioxins, dibenzofurans, and benzenes, and polycyclic aromatic hydrocarbons during municipal solid waste incineration
- 2009
-
Ingår i: Environmental Engineering Science. - : Mary Ann Liebert. - 1092-8758 .- 1557-9018. ; 26:3, s. 509-520
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Tidskriftsartikel (refereegranskat)abstract
- This study investigated the effects of transient combustion conditions on formation of polychlorinated dibenzo-p-dioxins (PCDD) and polychlorinated dibenzofurans (PCDF) along the postcombustion zone. Polychlorinated benzenes (PCBz) and polycyclic aromatic hydrocarbons (PAH) were also studied. The study was conducted in a laboratory fluidized-bed reactor fed with an artificial municipal solid waste (MSW) under controllable but realistic combustion conditions. PCDD/Fs, PCBz, and PAHs were monitored under normal, transient, and posttransient combustion conditions and simultaneously sampled at three different sampling points/temperatures (400°C, 300°C, and 200°C). Substantially higher PCDD/F, PCBz, and PAH concentrations were found during transient combustion than during normal combustion. Elevated concentrations were found to decrease with time. PCDD/F concentrations were similar at all points during normal and transient combustion conditions, but were found in higher concentrations at 200°C than 400°C under the posttransient combustion periods. Higher concentrations of the sum PAH and PCBz were also found at 200°C than 400°C in the posttransient combustion periods. Transient combustion conditions induced changes in both PCDD/F homologue profile and PCDD/F congener patterns compared to normal combustion. PCDD/PCDF ratios indicated an increase of the de novo synthesis during transient combustion conditions. Although, the PCDD/F congeners found to be most strongly affected by the transient combustion conditions indicated different reactions pathways active for formation of PCDF and PCDD, de novo synthesis and precursors, respectively. The most strongly affected PCDD/F congeners of transient combustion were identified and are presented.
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| 4. |
- Aurell, Johanna, et al.
(författare)
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Effects of varying combustion conditions on PCDD/F emissions and formation during MSW incineration
- 2009
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Ingår i: Chemosphere. - : Elsevier. - 0045-6535 .- 1879-1298. ; 75:5, s. 667-673
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Tidskriftsartikel (refereegranskat)abstract
- Process, combustion and fuel parameters were varied to elucidate factors that substantially affect the formation and emissions of polychlorinated dibenzo-p-dioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs) arising from municipal solid waste (MSW) incineration. The combustion conditions were varied by changing the: freeboard temperatures; quench time in the post-combustion zone; fuel load; chlorine and copper levels in the fuel; and the water, sulfur dioxide, carbon monoxide and oxygen levels in the combustion gases. The study was performed using a 5 kW laboratory-scale fluidized-bed reactor and PCDD/Fs were sampled at a point at 300 °C in the post-combustion zone. The results showed that increasing the SO2 level (from 0 to 130 ppm) substantially reduced the PCDD/F emissions, by up to 60%. In contrast, increasing the CO levels (due to transient combustion conditions), raising the Cl level (from 0.7% to 1.7%) and reducing the freeboard temperature (from 800 °C to 660 °C) all substantially increased the emission levels (more than 3-fold). Changes in PCDD/F profiles associated with increases in Cl, SO2 or CO levels and increasing the freeboard temperature (from 800 °C to 950 °C) indicate that the PCDFs were mainly formed by chlorination. In addition, increasing the Cl level increased the chlorination activity in the formation of PCDDs. Increasing the SO2 level appeared to be less effective in reducing the amount of PCDDs formed via the precursor pathway. While increased CO levels induced PCDD formation via the precursor pathway, although this was found to depend on the O2 level in the flue gas.
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| 5. |
- Aurell, Johanna, 1972-
(författare)
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Effects of Varying Combustion Conditions on PCDD/F Formation
- 2008
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Polychlorinated dibenzo-p-dioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs) are by-products emitted from combustion sources such as municipal solid waste (MSW) incineration plants. These organic compounds are recognized as toxic, bioaccumulative and persistent in the environment. PCDD/Fs are removed from flue gases before released from MSW incineration. However, the PCDD/Fs are not destroyed but retained in the residues, thus in the environment. Understanding the pathways that lead to their formation is important in order to develop ways to suppress their formation and prevent their release into the environment. Suppressing the formation can also allow less expensive air pollution control system to be used, and/or the costs of thermally treating the residues to be reduced. The main objective of the studies underlying this thesis was to elucidate process, combustion and fuel parameters that substantially affect the emission levels and formation of PCDD/Fs in flue gases from MSW incineration. The experiments were conducted under controllable, realistic combustion conditions using a laboratory-scale reactor combusting artificial MSW. The parameter found to most strongly reduce the PCDD/F emissions, was prolonging the flue gas residence time at a relatively high temperature (460°C). Increasing the sulfur dioxide (SO2) to hydrogen chloride (HCl) ratio to 1.6 in the flue gas was also found to reduce the PCDF levels, but not the PCDD levels. Fluctuations in the combustion process (carbon monoxide peaks), high chlorine levels in the waste (1.7%) and low temperatures in the secondary combustion zone (660°C) all tended to increase the emission levels. The PCDD/PCDF ratio in the flue gas was found to depend on the chlorine level in the waste, fluctuations in the combustion process and the SO2:HCl ratio in the flue gas. The formation pathways were found to be affected by the quench time profiles in the post-combustion zone, fluctuations in the combustion process and addition of sulfur. In addition, increased levels of chlorine in the waste increased the chlorination degrees of both PCDDs and PCDFs. A tendency for increased SO2 levels in the flue gas to increase levels of polychlorinated dibenzothiophenes (sulfur analogues of PCDFs) was also detected, however the increases were much less significant than the reduction in PCDF levels.
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| 6. |
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| 7. |
- Avakian, Maureen D., et al.
(författare)
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The origin, fate, and health effects of combustion by-products : A research framework
- 2002
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Ingår i: Journal of Environmental Health Perspectives. - : National Institute of Environmental Health Sciences. - 0091-6765 .- 1552-9924. ; 110:11, s. 1155-1162
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Tidskriftsartikel (refereegranskat)abstract
- Incomplete combustion processes can emit organic pollutants, metals, and fine particles. Combustion by-products represent global human and environmental health challenges that are relevant not only in heavily industrialized nations, but also in developing nations where up to 90% of rural households rely on unprocessed biomass fuels for cooking, warmth, and light. These issues were addressed at the Seventh International Congress on Combustion BY-Products, which convened 4-6 June 2001 in Research Triangle Park, North Carolina. This congress included a diverse group of multidisciplinary researchers and practitioners who discussed recent developments and future goals in the control of combustion by-products and their effects of exposure on human and ecologic health. Participants recommended that interdisciplinary, coordinated research efforts should be focused to capitalize on the important potential synergisms between efforts to reduce the adverse human health effects linked to exposures to combustion by-products and broader efforts to reduce greenhouse gas emissions and save energy through efficiency. In this article we summarize the principal findings and recommendations for research focus and direction.
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| 8. |
- Broz, J, et al.
(författare)
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The effect of oils on PAH, PCDD, PCDF, and PCB emissions from a spark engine fueled with leaded gasoline
- 2000
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Ingår i: Chemosphere. ; 41:12, s. 1905-11
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Tidskriftsartikel (refereegranskat)abstract
- The effect of synthetic and mineral oils on the formation of polyaromatic hydrocarbons (PAHs), polychlorinated dibenzo-p-dioxins (PCDDs), dibenzofurans (PCDFs), and biphenyls (PCBs) in emissions from a spark ignition engine was studied on a Skoda Favorit engine fueled with leaded gasoline. The test cycle simulated urban traffic conditions on a chassis dynamometer, in accordance with the ECC 83.00 test. The data for selected PAHs as well as PCDDs, PCDFs, and PCBs congener profiles are presented. PCDD/Fs emissions for an unused oil and the oil after 10000-km operation varied from 300 to 2000 fmol/m3, PCBs emissions from 75 to 178 pmol/m3, and PAHs emissions from 150 to 420 g/m3. The content of PCBs in oils varied from 2 to 920 mg/kg.
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| 9. |
- Börjeson, L, et al.
(författare)
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Characterization of automotive shredder residues from two shredding facilities with different refining processes in Sweden
- 2000
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Ingår i: Waste Management & Research. - : Wiley. - 0734-242X .- 1399-3070. ; 18:4, s. 358-66
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Tidskriftsartikel (refereegranskat)abstract
- Strict legislation imposing producer responsibility on car manufacturers, introduced in 1998 in Sweden, has prompted a search for new alternatives for recycling organic materials In end-of-life vehicles (ELVs), i.e. the automotive shredder residue (ASR). The recovery of materials from ELVs must increase from the present 70 to 75%, to 95% by 2015. The aim of this study was to characterize material other than ferrous components, i.e. the (automotive) shredder residue [(A)SR] and the non-ferrous (NF), material in order to investigate its suitability for energy recovery. The results show that the good heat value of the material gives it potential, but high levels of metals and chlorinated compounds may cause problems. Levels of elements, metals and polychlorinated dibenzodioxins/furans (PCDD/F), polychlorinated biphenyls (PCB) and polychlorinated benzenes (PCBz) in the ASR were also analysed, and the results are described and discussed.
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| 10. |
- Cieplik, M.K., et al.
(författare)
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Formation of dioxins from combustion micropollutants over MSWI fly ash.
- 2006
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Ingår i: Environmental Science and Technology. - 0013-936X. ; 40:4, s. 1263-9
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Tidskriftsartikel (refereegranskat)abstract
- Formation of polychlorinated dibenzofurans and dibenzo-p-dioxins (PCDD/Fs) from a model mixture of products of incomplete combustion (PICs) representative of municipal solid waste incineration (MSWI) flue gases, over a fixed bed of MSWI fly ash has been investigated. For comparison, a single model compound (chlorobenzene) was also briefly studied. A newly developed lab-scale system enabled the application of (very) low and stable concentrations of organic substances--of 10(-6) M or less-to approach realistic conditions. Samples taken at several time intervals allowed the observation of changes in rates and patterns due to depletion of the carbon in fly ash. The model flue gas continuously produced PCDDs and PCDFs after the de novo reaction had ceased to occur. Dioxin output levels are comparable to those of "old" MSW incinerators. Replacing the PIC trace constituent phenol by its fully 13C-labeled analogue led to, e.g., PCDD with one labeled ring as prominent product, meaning that the formation is about first order in phenol, contrary to earlier assumptions. The meaning of the results for the formation of dioxins in the MSWI boiler is discussed.
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| 11. |
- Cieplik, Mariusz K, et al.
(författare)
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On Dioxin Formation in Iron Ore Sintering
- 2003
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Ingår i: Environmental Science & Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 37:15, s. 3323-31
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Tidskriftsartikel (refereegranskat)abstract
- Iron ore sintering is an important source of "dioxins", polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs). This paper reports on attempts to identify materials, conditions, and mechanisms responsible for PCDD/F formation (i) by investigating salient properties of ores (viz., with respect to oxidation, condensation, and chlorination of model organics) and (ii) by mimicking the industrial process on a microscale with real-life materials. Principles of Design of Experiments (DOE) are employed. The reactivities of iron ores differ greatly. Limonite/goethite "soft" ore is a very active oxidation catalyst (e.g., for benzene and phenol), a property that may be useful in cleaning up crude sintering process offgases, whereas hematite/magnetite "hard" ore is not. The latter, however strongly promotes condensation of phenol to dibenzofuran. A newly built lab-microscale sintering facility could satisfactorily imitate the large-scale process, in part or as a whole. Results obtained with realistic feed mixtures point at dioxin formation in the sinter bed at levels significant enough to explain a major part of the outputs observed in the real-life process. With ~8 ppm (wt) of chloride added as NaCl, the PCDD/F output doubled, but with the same proportion of chlorine administered as C2Cl4, the dioxin output was over 2 orders of magnitude larger. The use of process reverts, etc. containing chlorinated organics should therefore be avoided. PCDD/F congener patterns are also reported and compared with those observed in practice.
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| 12. |
- Duong Phan, Ngoc Chau, et al.
(författare)
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Accurate sampling of PCDD/F in high temperature flue-gas using cooled sampling probes
- 2012
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Ingår i: Chemosphere. - : Elsevier. - 0045-6535 .- 1879-1298. ; 88:7, s. 832-836
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Tidskriftsartikel (refereegranskat)abstract
- In a laboratory-scale combustion reactor, flue-gas samples were collected at two temperatures in the post-combustion zone, 700 °C and 400 °C, using two different water-cooled sampling probes. The probes were the cooled probe described in the European Standard method EN-1948:1, referred to as the original probe, and a modified probe that contained a salt/ice mixture to assist the cooling, referred to as the sub-zero probe. To determine the efficiency of the cooling probes, internal temperature measurements were recorded at 5 cm intervals inside the probes. Flue-gas samples were analyzed for polychlorinated dibenzo-p-dioxin and dibenzofurans (PCDD/Fs). Samples collected at 700 °C using the original cooling probe showed higher concentrations of PCDD/Fs compared to samples collected using the sub-zero probe. No significant differences were observed between samples collected at 400 °C. The results indicated that artifact formation of PCDD/Fs readily occurs during flue-gas sampling at high temperatures if the cooling within the probe is insufficient, as found for the original probe at 700 °C. It was also shown that this problem could be alleviated by using probes with an enhanced cooling capacity, such as the sub-zero probe.Although this may not affect samples collected for regulatory purposes in exit gases, it is of great importance for research conducted in the high-temperature region of the post-combustion zone.
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| 13. |
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| 14. |
- Hedman, Björn, 1957-
(författare)
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Dioxin emissions from small-scale combustion of bio-fuel and household waste
- 2005
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Denna avhandling behandlar rökgasutsläpp av persistenta organiska föroreningar, framförallt dioxiner, vid förbränning av fasta biobränslen och torrt hushållsavfall i relativt små anläggningar (5-600 kW) utan avancerad rökgasreningsteknik.Samförbränning av avfall och biobränsle i effektiva mindre biobränslepannor testades som en alternativ strategi till den vanligen förekommande storskaliga hanteringen och förbränningen fast hushållsavfall. Medan storskalig förbränning av avfall ger investeringsmässiga fördelar med rökgasreningsteknik etc. kan små lokala anläggningar ha transportmässiga fördelar och möjligheter till utnyttjande av lokala biobränsletillgångar. Källsorterat, torrt, brännbart hushållsavfall insamlades från hushåll i glesbygd och samförbrändes i brikettform med energigräset rörflen i 150-600 kW biobränslepannor. Endast undantagsvis understeg dioxinemissionerna gällande gränsvärden för avfallsförbränning och nivåerna av väteklorid i rökgas översteg gränsvärdena flerfaldigt. Det bedömdes att någon form av extra rökgasrening är nödvändig för att säkerställa nivågränserna. Dioxiner hittades också i det eldade avfallet, framförallt i textilfraktionen. Dioxinmängderna i rökgaserna var oftast lägre än i det ingående bränslet.Intermittent pelletseldning gav oväntat höga utsläpp av dioxiner med en emissionsfaktor på 28 ng(WHO-TEQ)/kg. Vedeldning i en modern miljömärkt villapanna gav betydligt lägre utsläpp av dioxiner än eldning i en gammal kombipanna och eldning med full lufttillförsel, som kan jämföras med användning av ackumulatortank, resulterade i upp till 90% minskning av utsläpp av dioxiner jämfört med eldning med reducerat lufttillskott (’pyreldning’). Eldning av plastavfall i en vedpanna gav höga utsläpp av dioxiner.Okontrollerad förbränning av trädgårdsavfall och hushålls avfall i tunna eller som öppen eld ’bakgårdsbränning’, gav stora variationer i utsläppsnivåer som bara delvis kunde kopplas till avfallsinnehåll. Resultaten visar att denna typ av förbränning kan vara en betydande källa till dioxiner i miljön, och ett emissionsfaktorintervall på 4-72 ng (WHO-TEQ)/kg föreslås för bedömningar av utsläpp från backgårdsbränning av avfall med låga eller måttliga klorhalter.En sammanfattande slutsats av alla försök är att dioxin utsläpp beror på komplicerade samband mellan bränsleinnehåll och förbränningsbetingelser. Bränslen med mycket höga klorhalter av ger oftast högre utsläpp av dioxiner än bränslen med låga klorhalter medan små skillnader döljs av variationer i förbränningsbetingelser.
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| 15. |
- Hedman, Björn, et al.
(författare)
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Emission of PCDD/F, PCB, and HCB from combustion of firewood and pellets in residential stoves and boilers
- 2006
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Ingår i: Environmental Science and Technology. - Washington : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 40:16, s. 4968-4975
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Tidskriftsartikel (refereegranskat)abstract
- To assess potential emissions of polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), polychlorinated biphenyls (PCBs), and hexachlorobenzene (HCB) from residential combustion of biofuels, experiments were performed in which various types of pellets and firewood were combusted in four types of stoves and boilers, with both full and reduced rates of air supply. Intermittent combustion of wood pellets resulted in emissions of 11 ng-(WHO-TEQ)/kg combusted fuel (dry weight). A modern, environmentally certified boiler yielded somewhat lower emissions of PCCD/F and PCB than a wood stove. Both gave <0.1 ng(WHO-TEQ)/m3n (1.3-6.5 ng(WHO-TEQ)/kg) and considerably lower emissions than an old boiler (7.0-13 ng(WHO-TEQ)/kg). No positive effect on emissions could be observed in full air combustion (simulating the use of a heat storage tank) compared to combustion with reduced air. Two of the wood combustion experiments included paper and plastic waste fuels. Chlorine-containing plastic waste gave rise to high emissions: ca. 310 ng(WHO-TEQ)/ kg over the whole combustion cycle. The homologue profiles of PCDD/Fs show characteristic differences between ashes and flue gas from combustions with different levels of air supply. These differences do not, however, seem to have any correlation to the relative amount of toxic congeners.
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| 16. |
- Hedman, Björn, et al.
(författare)
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Emissions from small-scale energy production using co-combustion of biofuel and the dry fraction of household waste
- 2005
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Ingår i: Waste Management. - New York, N.Y. : Pergamon. - 0956-053X .- 1879-2456. ; 25:3, s. 311-321
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Tidskriftsartikel (refereegranskat)abstract
- In sparsely populated rural areas, recycling of household waste might not always be the most environmentally advantageous solution due to the total amount of transport involved. In this study, an alternative approach to recycling has been tested using efficient small-scale biofuel boilers for co-combustion of biofuel and high-energy waste. The dry combustible fraction of source-sorted household waste was mixed with the energy crop reed canary-grass (Phalaris Arundinacea L.), and combusted in both a 5-kW pilot scale reactor and a biofuel boiler with 140–180 kW output capacity, in the form of pellets and briquettes, respectively. The chlorine content of the waste fraction was 0.2%, most of which originated from plastics. The HCl emissions exceeded levels stipulated in new EU-directives, but levels of equal magnitude were also generated from combustion of the pure biofuel. Addition of waste to the biofuel did not give any apparent increase in emissions of organic compounds. Dioxin levels were close to stipulated limits. With further refinement of combustion equipment, small-scale co-combustion systems have the potential to comply with emission regulations.
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| 17. |
- Hedman, Björn, et al.
(författare)
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Emissions of polychlorinated dibenzodioxins and dibenzofurans and polychlorinated biphenyls from uncontrolled burning of garden and domestic waste (backyard burning)
- 2005
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Ingår i: Environmental Science and Technology. - Washington : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 39:22, s. 8790-8796
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Tidskriftsartikel (refereegranskat)abstract
- To assess emissions of dioxins (chlorinated dibenzodioxins and dibenzofurans) and PCB from uncontrolled domestic combustion of waste ("backyard burning"),test combustions in barrels and open fires were monitored. The waste fuels used were garden waste, paper, paper and plastic packaging, refuse-derived fuel (RDF), PVC, and electronic scrap. Combustions including PVC and electronic scrap emitted several orders of magnitude more dioxins than the other waste fuels. Emissions from the other fuels had considerable variations, but the levels were difficult to relate to waste composition. Emission factors of PCDD/F and PCB from the backyard burning ranged from 2.2 to 13 000 ng (WHO-TEQ)/kg. The levels found in ash usually were less than 5% of the total. For assessment of total emissions of dioxins and PCB from backyard burning of low and moderately contaminated wastes, an emission factor range of 4-72 ng (WHO-TEQ)/kg is suggested. These figures imply that combusting waste in the backyard could contribute substantially to total emissions, even if the amounts of fuel involved are equivalent to just a few tenths of a percent of the amounts combusted in municipal waste incinerators.
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| 18. |
- Hedman, Björn, et al.
(författare)
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PCDD/F in source-sorted waste fractions and emissions from their co-combustion with reed canary-grass
- 2007
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Ingår i: Waste Management. - Oxford : Pergamon Press. - 0956-053X .- 1879-2456. ; 27:11, s. 1580-1592
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Tidskriftsartikel (refereegranskat)abstract
- The dry combustible fraction of source-sorted household waste, including material that would otherwise be recycled, was mixed with the energy crop reed canary-grass (Phalaris arundinacea L.), and combusted as briquettes in 150 and 600 kW biofuel-boilers without advanced cleaning systems. The source-sorted waste was further sorted and characterized according to its material and chemical contents. The bulk of the waste’s chlorine content came from the non-package plastic fraction, whereas 90–95% of ∑PCDD/F (74–90% of WHO-TEQ) originated from the textile fraction. The sources of the dioxins in the waste fractions are discussed. The balance of dioxin levels was negative, i.e., the amounts of dioxins output in the flue gas were lower than those input in the fuel, except when there were operational disturbances in the combustion. In one of the combustion trials the total levels of dioxins in the flue-gas and ashes were also lower than the input levels. The use of additional cleaning equipment will be needed to ensure that emissions of dioxins and hydrochloric acid will be below legal limits.
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| 19. |
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| 20. |
- Jansson, Stina, et al.
(författare)
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Formation and chlorination of polychlorinated naphthalenes (PCNs) in the post-combustion zone during MSW combustion
- 2008
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Ingår i: Chemosphere. - : Elsevier BV. - 0045-6535 .- 1879-1298. ; 72:8, s. 1138-1144
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Tidskriftsartikel (refereegranskat)abstract
- Non- to octa-chlorinated naphthalenes (PCNs) were analyzed in flue gas samples collected simultaneously at three different temperatures (450 °C, 300 °C and 200 °C, respectively) in the post-combustion zone during waste combustion experiments using a laboratory-scale fluidized-bed reactor. PCN homologue profiles in all samples were dominated by the lower chlorinated homologues (mono- to triCN), with successive reductions in abundance with each additional degree of chlorination. The isomer distribution patterns reflected ortho-directionality behavior of the first chlorine substituent, and the β-positions, i.e. the 2,3,6,7-substitution sites, seemed to be favored for chlorination. Injection of naphthalene into the post-combustion zone resulted in increased PCN levels at 200 °C, demonstrating the occurrence of chlorination reactions in the post-combustion zone. However, the increases were restricted to the least-chlorinated homologue (monoCN), probably because there was insufficient residence time for further chlorination. In addition, an episode of poor combustion (manifested by high CO levels) was accompanied by extensive formation of 1,8-diCN, 1,2,3- and 1,2,8-triCN; congeners with substitution patterns that are not thermodynamically favorable. These are believed to be products of PAH breakdown reactions and/or chlorophenol condensation. Overall, PCN formation is likely to occur via more than one pathway, including chlorination of naphthalene that is already present, de novo synthesis from PAHs and, possibly, chlorophenol condensation.
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| 21. |
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| 22. |
- Jansson, Stina, et al.
(författare)
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Multivariate Relationships between Molecular Descriptors and Isomer Distribution Patterns of PCDD/Fs Formed during MSW Combustion
- 2009
-
Ingår i: Environmental Science & Technology. - : American Chemical Society. - 0013-936X .- 1520-5851. ; 43:18, s. 7032-8
-
Tidskriftsartikel (refereegranskat)abstract
- The isomer distribution patterns of mono- to hepta-chlorinated dibenzo-p-dioxins (PC1−7DD) and dibenzofurans (PC1−7DF) in postcombustion zone flue gas during incineration of an artificial municipal solid waste in a laboratory-scale fluidized-bed reactor were evaluated. Bidirectional orthogonal projections to latent structures (O2PLS) was used to correlate a set of physicochemical properties and chlorine substitution descriptors with the objective to identify parameters correlated with postcombustion zone PCDD and PCDF formation. The most influential variable for the distribution of PCDD congeners was chlorine substitution in positions 1 and 3 (Cl1 + 3), and overall the chlorine substitution descriptors exerted a larger impact on PCDDs than on PCDFs. For the PCDF, chlorination of the 9-position was the most influential X-variable. Distinct clustering was observed and was most pronounced for PCDFs, dividing most of the homologues into two or three subgroups of congeners. These subgroups seemed to correspond to the probability of formation by chlorophenol condensation. The sterically crowded dibenzofuran bay-sites (1- and 9-positions) were found to negatively influence PCDF formation, with chlorination of the 9-position having the greatest impact. Since PCDD/F toxicity is related to the lateral positions, elucidating the factors governing chlorination may be of great importance for detoxification of incineration byproducts.
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| 23. |
- Jansson, Stina, et al.
(författare)
-
Post-combustion formation of PCDD, PCDF, PCBz, and PCPh in a laboratory-scale reactor : Influence of dibenzo-p-dioxin injection
- 2009
-
Ingår i: Chemosphere. - : Elsevier. - 0045-6535 .- 1879-1298. ; 76:6, s. 818-25
-
Tidskriftsartikel (refereegranskat)abstract
- Formation of polychlorinated dibenzo-p-dioxins (PCDD), dibenzofurans (PCDF), benzenes (PCBz), and phenols (PCPh) was studied during combustion of an artificial municipal solid waste (MSW) in a laboratory-scale fluidized-bed reactor with simultaneous collection of flue gas samples at three different temperatures in the post-combustion zone (450 degrees C, 300 degrees C, and 200 degrees C). PCDF, PCBz, and PCPh were predominantly formed at or above the first sampling point (450 degrees C) with a dominance of the lower chlorinated homologues. PCDDs, on the other hand, were dominated by the intermediately chlorinated homologues with concentrations peaking at 300 degrees C. The dominating PCPh congeners clearly displayed the ortho-para directionality, which is indicative of electrophilic aromatic substitution, as did the PCBz isomer distribution patterns to some extent. Comparison of the observed PCBz isomer distribution patterns to prior work may indicate coupling of aliphatic species in chlorobenzene formation. The PCDDs seemed to be largely influenced by chlorophenol condensation reactions and to some extent chlorination reactions, while the PCDFs displayed a chlorination-oriented pattern for the mono- to tri-chlorinated homologues and a PCPh condensation pattern for the higher chlorinated homologues. Injection of non-chlorinated dibenzo-p-dioxin at 650 degrees C resulted in increased formation of Tri-HxCDD and a decrease in the dibenzofuran levels. The affected PCDD and PCDF congeners were not products expected to form from chlorine substitution, but instead are well known chlorophenol condensation products.
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| 24. |
- Jansson, Stina, 1975-
(författare)
-
Thermal formation and chlorination of dioxins and dioxin-like compounds
- 2008
-
Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- This thesis contributes to an increased understanding of the formation of dioxins and dioxin-like compounds in combustion processes. Although emissions to air from waste incineration facilities have been greatly reduced by the use of efficient air pollution control measures, the resulting residues (ashes and filters) are highly toxic and are classified as hazardous waste. The main objective of the work underlying this thesis was to elucidate the formation and chlorination pathways of dioxins and dioxin-like compounds in waste combustion flue gases in the temperature range 640-200°C in a representative, well-controlled laboratory-scale reactor using artificial municipal solid waste. This could contribute to the reduction of harmful emissions to air and also reduce the toxicity of waste incineration residues, thus reducing or even eliminating the need for costly and potentially hazardous after-treatment. A comparison of four different quenching profiles showed that the formation of polychlorinated dibenzo-p-dioxins (PCDD) and dibenzofurans (PCDF) was rapid and mainly occurred in the 640-400°C temperature region, with high dependency on sufficient residence time within a specific temperature region. Prolonged residence time at high temperatures (450/460°C) reduced the PCDD yields, even at lower temperatures along the post-combustion zone. PCDD, PCDF and PCN (polychlorinated naphthalene) isomer distribution patterns indicated contributions from chlorophenol condensation as well as chlorination reactions for all three classes of compounds. The formation of PCDDs was largely influenced by chlorophenol condensation and to some extent by chlorination reactions. For the PCDFs, chlorine substitution adjacent to the oxygen bridges was unfavoured, as demonstrated by the notably lower abundance of 1,9-substituted congeners. This was supported by bidirectional orthogonal partial least squares (O2PLS) modelling. The variable with the greatest influence on the distribution of PCDD congeners was the relative free energy (RΔGf). The O2PLS models displayed distinct clusters, dividing most of the homologues into two or three sub-groups of congeners which seemed to correspond to the probability of origination from chlorophenol condensation. The effects of injection of aromatic structures into the flue gas differed for each class of compounds. Injection of naphthalene increased the formation of monochlorinated naphthalene but the remaining homologues appeared to be unaffected. This was probably due to insufficient residence time at temperatures necessary for further chlorination. Injected dibenzo-p-dioxin was decomposed, chlorinated and re-condensated into PCDDs and PCDFs, whereas injection of dibenzofuran and fluorene reduced the PCDD levels in the flue gas.
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| 25. |
- Liljelind, Per, et al.
(författare)
-
Method for Multiresidue Determination of Halogenated Aromatics and PAHs in Combustion-Related Samples
- 2003
-
Ingår i: Environmental Science & Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 37:16, s. 3680-6
-
Tidskriftsartikel (refereegranskat)abstract
- Flue gas and fly ash samples have a complex composition. Thus, thorough extraction and selective cleanup prior to analysis are essential. This paper presents an evaluated method for determining halogenated dibenzo-p-dioxins (PXDD), halogenated dibenzofurans (PXDF), chlorinated biphenyls (PCB), chlorobenzenes (CBz), -phenols (CPh), dibenzo-p-dioxins (DD), dibenzofurans (DF), and polycyclic aromatic hydrocarbons (PAH) in a single sample. Since these combustion byproducts are ubiquitous, harmful environmental contaminants it is very important to obtain reliable assessments of them: especially specific PCDD/F and PCB congeners with Ah-receptor mediated toxicity. The reported method for this purpose includes techniques such as solid-phase extraction, Soxhlet-Dean-Stark extraction, cleanup using open liquid chromatographic columns, and finally GC/MS analysis/determination with quantification by the isotope dilution technique. The validation results presented here show good reproducibility for PXDD/F and PCB and are satisfactory for CPh, CBz, and PAH. An extraction efficiency test revealed that a nonpolar solvent did not completely extract a few analytes, i.e., diCPh and fluorene, which appear to require a more polar extraction agent. To pinpoint and minimize the loss of analytes, specific studies on reductions of their amounts during sample concentration were performed, showing that traditional rotary evaporation and nitrogen blow-down produce equally good results as a novel technique.
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| 26. |
- Liljelind, Per, et al.
(författare)
-
Removal of dioxins and related aromatic hydrocarbons from flue gas streams by adsorption and catalytic destruction
- 2001
-
Ingår i: Chemosphere. ; 42:5-7, s. 615-23
-
Tidskriftsartikel (refereegranskat)abstract
- The dioxin removing capacity of the shell dedioxin system (SDDS – a Ti/V oxidative type catalyst) has been tested using the Umeå lab-scale incinerator over the temperature range 100–230°C and at space velocities of 8000 and 40,000 h−1. Other analogous organic compounds, such as PCBs, PAHs, chlorobenzenes and chlorophenols have also been investigated. Results show a high degree of dioxin removal already at 100°C (82%), which occurs mainly by adsorption. When the temperature is raised a transition towards destruction is seen and at 150°C, gas hour space velocity (GHSV) 8000 and at 230°C, GHSV 40,000 virtually all removal is by destruction. High PCDD/F destruction efficiencies are reported (>99.9%, based on I-TEQ); the other dioxin-related species and PAHs are also removed and destroyed to a significant extent. The SDDS has proved to be an effective means of destroying organic compounds in the gas phase, particularly dioxins, at temperatures as low as 150°C.
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| 27. |
- Lundin, Lisa, et al.
(författare)
-
Distribution of mono- to octa-chlorinated PCDD/F in fly ashes from a municipal solid waste incinerator
- 2004
-
Ingår i: Environmental Science and Technology. - Washington : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 42:4, s. 1245-1250
-
Tidskriftsartikel (refereegranskat)abstract
- We have estimated the concentration and distribution of the mono to octa-chlorinated congeners of polychlorinated dibenzo-p-dioxins (PCDD) and dibenzofurans (PCDF) in fly ashes at various sampling points in a large-scale municipal solid waste incinerator at Umeå, Sweden, as they cooled from 700 to 170 °C. Differences between the ashes were observed, the PCDD homologue profile was found to vary with temperature. The total amount of PCDD and PCDF increased as the temperature decreased in the postcombustion zone. The increase was due to both adsorption to the fly ash and formation of PCDD and PCDF. Mono- to trichlorinated PCDD predominated at high temperatures, whereas hepta- and octachlorinated PCDD predominated at temperatures below 400 °C. PCDF predominated over PCDD in the whole temperature range. However, the changes in homologue profile for PCDF were minor. The isomer distribution within the homologue groups was not changed as the temperature decreased in the postcombustion zone.
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| 28. |
- Lundin, Lisa, et al.
(författare)
-
Distribution of mono to octa-chlorinated PCDD/Fs in fly ash from a municipal solid-waste incinerator.
- 2008
-
Ingår i: Environmental Science & Technology. - 0013-936X. ; 42:4, s. 1245-50
-
Tidskriftsartikel (refereegranskat)abstract
- We have estimated the concentration and distribution of the mono to octa-chlorinated congeners of polychlorinated dibenzo-p-dioxins (PCDD) and dibenzofurans (PCDF) in fly ashes at various sampling points in a large-scale municipal solid waste incinerator at Umeå, Sweden, as they cooled from 700 to 170 degrees C. Differences between the ashes were observed, the PCDD homologue profile was found to vary with temperature. The total amount of PCDD and PCDF increased as the temperature decreased in the postcombustion zone. The increase was due to both adsorption to the fly ash and formation of PCDD and PCDF. Mono-to trichlorinated PCDD predominated at high temperatures, whereas hepta- and octachlorinated PCDD predominated at temperatures below 400 degrees C. PCDF predominated over PCDD in the whole temperature range. However,the changes in homologue profile for PCDFwere minor. The isomer distribution within the homologue groups was not changed asthetemperature decreased in the postcombustion zone.
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| 29. |
|
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| 30. |
- Lundin, Lisa, 1976-
(författare)
-
Formation and degradation of PCDD/F in waste incineration ashes
- 2007
-
Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- The disposal of combustible wastes by incineration is a controversial issue that is strongly debated by both scientists and environmental activists due to the resulting emissions of noxious compounds, including (inter alia) polychlorinated dibenzo-p-dioxins (PCDDs), dibenzofurans (PCDFs), heavy metals and acid gases like sulfur dioxide. Currently available air pollution control devices are capable of effectively cleaning flue gases, and PCDD/F emissions to air from modern municipal solid waste (MSW) incinerators are low. However, the PCDD and PCDF end up in ash fractions that, in Sweden, are usually deposited in landfills. The European Union has recently set a maximum permitted total concentration of 15 µg TEQ/kg for PCDD/F species in waste. Fly ash from municipal solid waste (MSW) incineration containing PCDD/Fs at concentrations above this limit will have to be remediated to avoid disposing of them in landfills; an expensive and environmentally unfriendly option. Therefore, effective, reliable and cost-effective methods for degrading PCDD/F in fly ash are required, and a better understanding of the behavior of PCDDs and PCDFs during thermal treatment will be needed to develop them. In the studies this thesis is based upon both the formation and degradation of PCDDs and PCDFs in ashes from MSW incineration were studied. The main findings of the investigations regarding PCCD/F formation were: - The concentrations of PCDD and PCDF in fly ash increased with reductions in the temperature in the post-combustion zone. - The homologue profile in the ash changed when the temperature in the post-combustion zone changed. - The final amounts of PCDD and PCDF present were affected by their rates of both formation and degradation, and the mechanisms involved differ between PCDDs and PCDFs. The main findings from the degradation studies were: - The chemical composition of ash has a major impact on the degradation potential of PCDD and PCDF. - The presence of oxygen during thermal treatment can enhance the degradation of PCDD and PCDF. - Thermal treatment is a viable option for degrading PCDD and PCDF in ashes from MSW. - Shifts in chlorination degree occur during thermal treatment. - Rapid heat transfer into the ash is a key factor for ensuring fast degradation of PCDD and PCDF. - Degradation of other chlorinated organic compounds, e.g. PCB and HCB, also occurs during thermal treatment of ash. - Reductions in levels of PCDD and PCDF were not solely due to their desorption to the gas phase. - Differences between the behavior of 2378-substituted congeners of PCDD and PCDF and the other congeners during thermal treatment were observed. - Differences in isomer patterns of both PCDD and PCDF were observed between the ash and gas phases after thermal treatment at both 300 and 500 oC. Overall, the results show that the formation and degradation mechanisms of PCDDs differ substantially from those of PCDFs. Thus these groups of compounds should be separately considered in attempts to identify ways to reduce their concentrations.
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| 31. |
- Lundin, Lisa, et al.
(författare)
-
The behavior of PCDD and PCDF during thermal treatment of waste incineration ash
- 2011
-
Ingår i: Chemosphere. - : Elsevier. - 0045-6535 .- 1879-1298. ; 84:3, s. 305-310
-
Tidskriftsartikel (refereegranskat)abstract
- The polychlorinated dibenzo-p-dioxin (PCDD) and polychlorinated dibenzofuran (PCDF) content of three fly ash samples with different elemental compositions from different municipal waste incinerators were analyzed before and after thermal treatment at 300°C or 500°C. Gas phase emissions during the treatments were also collected and analyzed. Substantial reductions in the total PCCD/F content of the ashes were observed after treatment at 500°C, seemingly due to degradation rather than dechlorination. Treatment at 300°C resulted in an increase in the PCDD/F content of the three ashes. Initial concentration of PCDD/F in the untreated ashes did not reflect the outcome of the treatment at the different temperatures. In addition, the composition of the ash was found to influence the rate of decomposition and formation of PCDD and PCDF during thermal treatment; the results showed that Cu, Fe, Ca and S play important roles in these processes.
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| 32. |
- Lundin, Lisa, et al.
(författare)
-
The effect of developing nations' municipal waste composition on PCDD/PCDF emissions from open burning
- 2013
-
Ingår i: Atmospheric Environment. - : Elsevier. - 1352-2310 .- 1873-2844. ; 79, s. 433-441
-
Tidskriftsartikel (refereegranskat)abstract
- Open burning tests of municipal waste from two countries, Mexico and China, showed composition-related differences in emissions of polychlorinated dibenzodioxins and dibenzofurans (PCDDs/PCDFs). Twenty-six burn tests were conducted, comparing results from two laboratory combustion facilities. Waste was shredded to isolate composition-specific effects from those due to random waste orientation. Emissions ranged from 5 to 780 ng toxic equivalent/kg carbon burned (ng TEQ (kg C-b)(-1)) with an average of 140 ng TEQ (kg C-b)(-1) (stdev = 170). The waste from Mexico (17 ng TEQ (kg C-b)(-1)) had a statistically lower average emission factor than waste from China (240 ng TEQ (kg C-b)(-1). This difference was attributed primarily to waste composition differences, although one time-integrated combustion quality measure, Delta CO/Delta CO2, showed statistical significance between laboratories. However, waste composition differences were far more determinant than which laboratory conducted the tests, illustrated using both statistical techniques and comparison of cross-over samples (wastes tested at both facilities). Comparison of emissions from previous waste combustion tests in Sweden and the U.S.A, showed emission factors within the range of those determined for Mexico and China waste. For laboratory-scale combustion, existing emission factors and test methodologies are generally applicable to both developed and developing countries.
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| 33. |
|
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| 34. |
- Lundin, Lisa, et al.
(författare)
-
Thermal degradation of PCDD/F in municipal solid waste ashes in sealed glass ampules
- 2005
-
Ingår i: Environmental Science and Technology. - Washington : American Chemical Society. - 0013-936X .- 1520-5851. ; 39:10, s. 3872-3877
-
Tidskriftsartikel (refereegranskat)abstract
- Due to their high concentrations of toxic organic compounds such as polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/F), metals, and water-soluble salts, fly ashes are classified as hazardous waste in the European Union and are required to be deposited in controlled landfills. We have shown here that the tetra- to octachlorinated PCDD/F in fly ash can be degraded by thermal treatment. The temperature needed for total degradation of PCDD/F depends on the composition of the fly ash. Its concentrations of unburned carbon and alkaline compounds were found to be important in this respect. Experimental design was used to investigate the effects of varying the temperature, residence time, and atmosphere on the degradation of PCDD/F in three different types of fly ash. The results showed that the three ashes clearly showed different degradation potentials for PCDD/F during thermal treatment. The concentrations of unburned carbon, alkaline species such as CaO and Na2O, and metals such as copper and iron strongly influenced the degradation of PCDD/F. However, the different combinations of pH and amounts of native PCDD/F, unburned carbon, metals (Cu, Fe, Sn and Na), and sulfur in the ashes made it difficult or even impossible to conclude that any single parameter was responsible for the degradation of PCDD/F in these thermal treatment experiments. The decreases observed in all of the experiments are due to dechlorination and/or destruction of PCDD/F: depending on the temperature and ash composition, either of these processes may be the more important.
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| 35. |
- Lundin, Lisa, et al.
(författare)
-
Thermal degradation of PCDD/F, PCB and HCB in municipal solid waste ash.
- 2007
-
Ingår i: Chemosphere. - Oxford : Pergamon Press. - 0045-6535 .- 1879-1298. ; 67:3, s. 474-481
-
Tidskriftsartikel (refereegranskat)abstract
- A thermal degradation procedure for reducing the concentrations of mono- to octa-chlorinated PCDD/Fs, PCBs and hexa-chlorobenzenes (HCB) in filter ash from incinerated municipal solid waste (MSW) is described. Thermal treatment of filter ash samples at 500 °C for 60 min in a closed system providing low oxygen conditions resulted in 97% and 99% reductions in the total and I-TEQ concentrations of PCDD/Fs, to 6.8 μg kg−1 ash and <0.05 μg I-TEQ kg−1 ash, respectively. Increasing the thermal treatment time to 480 min, at the same temperature, yielded 99% reductions in both total and I-TEQ concentrations of the mono- to octa-chlorinated PCDD/Fs. Similar effects were observed for HCB and PCBs. The data from this study indicate that PCDD/Fs and other toxic organic compounds in ash from incinerated MSW, can be effectively degraded by this procedure, which combines relatively low-temperatures, short treatment times, and low oxygen conditions.
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| 36. |
|
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| 37. |
- Lönnermark, Anders, 1968-, et al.
(författare)
-
Emissions from simulated deep-seated fires in domestic waste
- 2008
-
Ingår i: Chemosphere. - : Elsevier BV. - 0045-6535 .- 1879-1298. ; 70:4, s. 626-39
-
Tidskriftsartikel (refereegranskat)abstract
- The emissions from deep-seated fires in domestic waste have been investigated. The gas phase yields of PAH, PCDD/F, PCB, HCB, particles, and metals associated to the particulate matter were analysed during a series of simulated deep-seated fires. The method of extinguishment was varied and in cases where water was used for extinguishment, the runoff water was analysed for PAH, PCDD/F, PCB, hexachlorobenzene, and metals. In total six tests were performed. In four of the tests, samples of the fire residue were analysed for PCDD/F, PCBs, and chlorobenzenes.
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| 38. |
- Marklund, Stellan, 1949-, et al.
(författare)
-
Determination of PCDDs and PCDFs in incineration samples and pyrolytic products
- 2018
-
Ingår i: Chlorinated dioxins and dibenzofurans in perspective. - Boca Raton : CRC Press. - 9781351070645 - 9781315891545 ; , s. 79-92
-
Bokkapitel (refereegranskat)abstract
- The formation of polychlorinated dioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs) in municipal solid waste (MSW) incinerators is now well documented and not controversial. It is interesting to compare the PCDD and the PCDF emissions from MSW incinerators with other energy sources. The identification of lower chlorinated PCDFs like penta-CDFs in pyrolysis of hexachloroethane indicates dechlorination to be an important pathway for the formation of PCDDs and PCDFs. The environmental and human health impact of the emissions of PCDDs and PCDFs from MSW incinerators have been discussed in Umea as well as at other places in Sweden and in other countries. The laboratory pyrolysis of PVC and Saran clearly shows that PVC and other organochlorine polymers can be precursors to the PCDDs and PCDFs found in various incinerators. The chapter discusses some of the data collected so far for various types of incinerators or incineration models.
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| 39. |
|
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| 40. |
- Nygren, Martin, et al.
(författare)
-
Identification of 2,3,7,8-substituted polychlorinated dioxins and dibenzofurans in environmental and human samples
- 1986. - 1
-
Ingår i: Chlorinated dioxins and dibenzofurans in perspective. - Boca Raton : CRC Press. - 9781315891545 - 9781351070645 ; , s. 17-34
-
Bokkapitel (övrigt vetenskapligt/konstnärligt)abstract
- Polychlorinated dibenzo-p-dioxins (PCDDs) and dibenzofurans (PCDFs) are two series of tricyclic, almost planar aromatic compounds that exhibit very similar physical, chemical, and biological properties. The human exposure to PCDDs and PCDFs by milk consumption is not negligible. Detection levels in ecological and human samples should be orders of magnitude below the usual detection levels obtained in pesticide analyses. One objective of the study is to identify background levels of PCDDs and PCDFs in these samples, especially those of human origin. The spectrum of toxic effects is species dependent but for humans they include chloracne and porphyria cutane tarda and for other animals edema, thymic atrophy, teratogenicity, liver lesions and a slow wasting syndrome followed by death. It is evident that it is of particular importance to identify the ultimate source or sources of the toxic 2,3,7,8-substituted PCDDs and PCDFs found as background constituents in the environmental and human samples, especially the samples of mother's milk, which are of toxicological interest.
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| 41. |
- Phan, Duong Ngoc Chau, 1985-, et al.
(författare)
-
A link between fly ash chemistry and the thermal formation of PCDDs, PCDFs, PCBs, and PCNs during waste incineration
-
Annan publikation (övrigt vetenskapligt/konstnärligt)abstract
- The relationship between the properties of fly ash generated during waste incineration and the thermal formation of polychlorinated dibenzo-p-dioxins (PCDDs), dibenzofurans (PCDFs), biphenyls (PCBs), and naphthalenes (PCNs) was investigated using a laboratory incinerator and two artificial wastes that were designed to reflect regional differences in municipal solid waste composition. Flue gas and fly ash samples were collected isokinetically via a sampling port in the post-combustion zone at a flue gas temperature of 300 °C. The mineralogical properties, morphology and sub-surface composition, surface composition and elemental oxidation states of the fly ash samples were determined. The flue gas samples were analyzed for Mo-OCDDs, Mo-OCDFs, Tri-DCBs, and Di-OCNs. Orthogonal Projections to Latent Structures (OPLS) modeling was used to study the relationship between the properties of the fly ash and the post-combustion formation of polychlorinated aromatics. The presence of high levels of ash-forming elements (i.e. Na, Mg, Fe, Ti, etc…) in the waste reduced the S content of the flue gas and thereby promoted the production of Cl2 via the Deacon process. Because this process is vital for the formation of polyaromatic species, wastes with depleted levels of fly ash-building elements should be favored to minimize the release of toxic PCDDs, PCDFs, PCBs, and PCNs during incineration.
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| 42. |
- Phan, Duong Ngoc Chau, 1985-, et al.
(författare)
-
Effects of regional differences in waste composition on the thermal formation of polychlorinated aromatics during incineration
- 2013
-
Ingår i: Chemosphere. - : Elsevier. - 0045-6535 .- 1879-1298. ; 93:8, s. 1586-1592
-
Tidskriftsartikel (refereegranskat)abstract
- Two artificial wastes (A and B) whose contents reflect regional differences in municipal solid waste composition, were used to investigate the thermal formation of polychlorinated dibenzo-p-dioxins (PCDDs), dibenzofurans (PCDFs), biphenyls (PCBs), and naphthalenes (PCNs) during incineration. Flue gas samples were simultaneously collected at three ports in the post-combustion zone corresponding to flue gas temperatures of 400, 300, and 200 °C. The combustion of Waste B, which had a higher chlorine and metal content than Waste A, produced greater levels of highly-chlorinated homologues, as demonstrated by a higher degree of chlorination. The total concentrations of PCDDs, PCDFs, PCBs, and PCNs formed in the combustion of both wastes increased as temperature decreased along the convector. There were no significant differences in total concentrations between Waste A and Waste B combustion at specific temperatures, with exception of PCDFs at 400 °C. Orthogonal Projections to Latent Structures Discriminant Analysis (OPLS-DA) modeling, used to evaluate the data for all compound groups, suggest that during flue gas quenching at temperatures of 400 °C low-chlorinated homologues are preferentially formed in the presence of copper, which is known to be a very active catalyst for this process. At 300 and 200 °C, the formation of highly-chlorinated homologues is favored.
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| 43. |
- Phan, Duong Ngoc Chau, 1985-
(författare)
-
The relationship between fly ash chemistry and the thermal formation of polychlorinated pollutants during waste incineration
- 2013
-
Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- The thermal formation of polychlorinated dibenzo-p-dioxins (PCDDs), dibenzofurans (PCDFs), biphenyls (PCBs), and naphthalenes (PCNs) is a major problem in waste incineration. Ideally, rather than relying on air cleaning systems and treatment techniques, their formation should be minimized or, if possible eliminated. The work presented in this thesis was conducted to obtain a deeper understanding of the thermal formation of PCDDs, PCDFs, PCBs, and PCNs during incineration using a 5 kW laboratory scale incinerator and two artificial wastes that were designed to reflect regional differences in waste composition.The first part of the thesis focuses on the validation of a recently-developed flue-gas sampling probe with enhanced cooling capabilities. Artifact formation of PCDDs and PCDFs can occur during the sampling of hot flue gases if the cooling is insufficient. The new probe was successfully used to collect samples at 700 °C without biasing the measured POP levels. The thermal formation of PCDDs, PCDFs, PCBs, and PCNs in the post-combustion zone of the incinerator was then studied by collecting flue gas samples at 400 °C, 300 °C, and 200 °C during the incineration of the two artificial wastes. Highly chlorinated POPs were formed in larger quantities when burning the waste with the higher content of metals and chlorine, which suggests that high metal levels in the waste favor the chlorination of less chlorinated POPs or otherwise facilitate the formation of highly chlorinated polyaromatics, possibly via the condensation of highly chlorinated phenols. The concentrations of these pollutants and the abundance of highly chlorinated homologues increased as the flue gas cooled. Fly ash particles play an important role in thermal POP formation by providing essential elements (carbon, chlorine, etc.) and catalytic sites. The chemical and mineralogical properties of fly ash samples were studied by X-ray diffraction (XRD), Fourier Transform Infrared (FTIR), Scanning Electron Microscopy/Energy Dispersive X-ray (SEM/EDX), and X-ray photoelectron spectroscopy (XPS) to determine their impact on thermal POP formation. Orthogonal Partial Least Squares (OPLS) modeling was used to identify correlations between the observed POP distributions and the physicochemical data. This investigation provided new insights into the impact of fly ash chemistry on thermal POP formation.In addition, the POP isomer distribution patterns generated during waste combustion were examined. These patterns are used to “fingerprint” mechanisms of POP formation. It was found that wastes containing large quantities of metals and chlorine favored the formation of highly chlorinated homologues including the very toxic 2,3,7,8-congeners. The data suggest that reducing fly ash emissions might increase the SO2 content of the flue gas and thereby suppress the Deacon process and the formation of harmful highly chlorinated aromatic species.
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| 44. |
- Rahm, Sara, 1972-
(författare)
-
Hydrolysis and photolysis of brominated flame retardants and some traditional persistent organic pollutants : Reactivity as a tool in fate assessement of chemicals
- 2004
-
Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- An organic compound that remains in the environment for a long time is regarded as a persistent organic pollutant (POP). Still, persistency is not a well defined property with a firm definition. Instead it is a conceptual property of chemicals for which DDT and PCB are typical representatives. No organic chemicals in the environment are inert and are thus subjected to chemical transformation reactions in air, water, soil sediments and in biota. Environmental pollutants are distributed in the environment based on their physicochemical properties and their reactivity. While the former properties have been thoroughly studied and used in modelling of the fate of chemicals in the environment, the latter property – reactivity – has been investigated poorly. The far-reaching objective with the present thesis is to introduce the reactivity of chemicals into the concept of persistency. More specifically the aim is to develop methodologies for defining chemical reactivity by determination of disappearance reaction constants for hydrolysis and photolysis of actual or potential environmental contaminants. Other transformation reactions in the environment such as oxidations reductions and radical reactions are not included at this stage. In this thesis, hydrolysis include both substitution and elimination reactions. The developmental work is performed largely by comparing the reactivity of brominated flame retardants but also include several traditional contaminants for comparative reasons. A new method for determination of the rate of hydrolysis of chemicals is developed using methoxide in methanol and DMF, which is done by using hexachlorobenzene (HCB) as the test chemical. The method is applied to several other chemicals, particularly polybrominated diphenyl ethers (PBDEs) but also traditional POPs. Chemicals such as DDT,TBBPA 2,3-dibromopropyl ether react very fast and the perbrominated diphenyl ether (BDE-209) is shown to undergo nucleophilic aromatic substitution faster than HCB. Compounds that can undergo elimination are rapidly degraded while the rates of substitution reactions of aromatic chemicals depend on the degree of halogenation. A new method is used for studying photolytic reactions based on irradiation of UV light at environmentally relevant wavelengths and with the study compounds dissolved in methanol/water (4:1). Disappearance constants and quantum yields are determined for several traditional and potential environmental contaminants. Halogenated phenols are rapidly transformed under these conditions. Polybrominated aromatics are indicated to react faster than the corresponding chlorinated compounds. The two methods for studying reactivity of chemicals have the potential of being useful to predict the persistency of chemicals in the environment. Such predictions must however also include the compound’s susceptibility to oxidation, reduction and radical reactions in all major environmental compartments and knowledge of their physicochemical characteristics.
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| 45. |
- Redin, LA, et al.
(författare)
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Co-combustion of shredder residues and municipal solid waste in a Swedish municipal solid waste incinerator
- 2001
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Ingår i: WASTE MANAGEMENT & RESEARCH. - 0734-242X. ; 19:6, s. 518-25
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Tidskriftsartikel (refereegranskat)abstract
- Incinerating automotive shredder residue (ASR) in order to increase the recovery from end of life vehicles (ELVs) is an attractive option when recycling this material. In this study, incineration combined with energy recovery, was investigated. The incineration experiments, where 20% shredder residue (SR) was burnt with conventional municipal solid waste (MSW), were conducted in a full-scale MSW horizontal grate incinerator. Measurements were made before, during and after the incineration. The results showed some minor increases in the emission levels of raw gases sampled after an electrostatic filter, but almost no significant differences when sampled after a wet scrubber. An increased level of 'non-toxic' metals was detected within the bottom ash. It was concluded that refined SR, in small quantities, is suitable to add to MSW.
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| 46. |
- Söderström, Gunilla, et al.
(författare)
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Formation of PBCDD and PBCDF during flue gas cooling
- 2004
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Ingår i: Environmental Science and Technology. - Washington : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 38:3, s. 825-830
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Tidskriftsartikel (refereegranskat)abstract
- The presence of bromine and chlorine in combustion, particularly in waste combustion, results in the formation of PBCDD and PBCDF. Formation pathways of PCDD/F are not fully understood, although much is known about them, and they are currently being further investigated. PBCDD/F is likely to be formed in reactions similar to those leading to PCDD/F, but the processes involved have been less intensively studied. In this study a fuel with bromine and chlorine in equal molar amounts was combusted in a pilot-scale fluid bed reactor and the cooling flue gas was sampled at 800, 350, and 250 C. Analysis revealed that levels of PBCDD and PBCDF increased between all sampling ports. The chlorine/bromine ratio also increased with reductions in temperature and increases in residence time for both PBCDD and PBCDF. However, the formation of PBCDD and PBCDF seems to follow different routes with respect to the level and pattern of halogenation.
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| 47. |
- Söderström, Gunilla, 1964-
(författare)
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On the combustion and photolytic degradation products of some brominated flame retardants
- 2003
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Many modern products, especially electronic goods, are protected by brominated flame retardants (BFR). Some of the most common flame retardants are polybrominated diphenylethers (PBDE), tetrabromobisphenol-A (TBBP-A) and hexabromocyclododecane (HBCD). These compounds have been found in environmental samples and shown to have physiological effects on experimental animals. This thesis considers end-of-life aspects of brominated flame retardants. When spread in the environment, these compounds may be degraded into other forms. For example, if sludge contaminated with PBDE is used as an agricultural fertilizer, the PBDE could be degraded by sunlight to species of PBDE with lower degree of bromination and, to some extent, also form polybrominated dibenzofurans (PBDF). In addition, PBDF and polybrominated dibenzo-p-dioxins (PBDD) are formed during combustion of brominated flame retardants. When waste products with brominated flame retardants are co-combusted with household waste or other chlorinated fuel, polybrominated- chlorinated dibenzo-p-dioxins (PBCDD) and polybrominated- chlorinated dibenzofurans (PBCDF)will be formed. The bromin/chlorine composition of dioxins and furans is dependent on the bromine/chlorine ratio in the fuel, but the types of brominated flame retardants that are being combusted is less important. In the studies reported here, bromine levels higher than "normal" for household waste has been used. The results show that there is a pronounced increase in total dioxin levels in fluegas when when bromine is present, implying that waste containing brominated flame retardants should only be incinerated at combustion plants with effecient air pollution control devices.
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| 48. |
- Söderström, Gunilla, et al.
(författare)
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PBCDD and PBCDF from incineration of waste-containing brominated flame retardants
- 2002
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Ingår i: Environmental science & technology. - 0013-936X. ; 36:9, s. 1959-64
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Tidskriftsartikel (refereegranskat)abstract
- Brominated organic flame retardants comprise a large, heterogeneous group of compounds that are useful but also potentially damaging to the environment. In this investigation, three common brominated flame retardants were co-combusted with an artificial municipal solid waste in a pilot-scale fluidized bed incinerator. Combustion conditions ensured degradation of the flame retardants, but stable brominated organic compounds such as polybrominated dibenzo-p-dioxins and polybrominated dibenzofurans were formed in the cooling flue gases. The incineration of fuels that contain both chlorine and bromine leads to the formation of a complex mixture of polybrominated/ chlorinated dibenzo-p-dioxins and dibenzofurans. More bromination than chlorination was observed in these experiments, and the chlorination levels increased when bromine was added to the fuel. The most favored reactions led to the formation of dibromodichlorodibenzo-p-dioxin and dibromodichlorodibenzofuran. Theoretical calculations show that there is more Br[2] than Cl[2] in the flue gas when the two halogens are present at equimolar levels, because chlorine is mainly found in the form of HCl. This may explain the higher bromination level. BrCl is also present, which drives the chlorination observed when bromine is added.
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| 49. |
- Weidemann, Eva, et al.
(författare)
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14th congress of combustion by-products and their health effects-origin, fate, and health effects of combustion-related air pollutants in the coming era of bio-based energy sources
- 2016
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Ingår i: Environmental Science and Pollution Research. - : Springer Science and Business Media LLC. - 0944-1344 .- 1614-7499. ; 23:8, s. 8141-8159
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Tidskriftsartikel (refereegranskat)abstract
- The 14th International Congress on Combustion By-Products and Their Health Effects was held in UmeAyen, Sweden from June 14th to 17th, 2015. The Congress, mainly sponsored by the National Institute of Environmental Health Sciences Superfund Research Program and the Swedish Research Council for Environment, Agricultural Sciences and Spatial Planning, focused on the Origin, fate and health effects of combustion-related air pollutants in the coming era of bio-based energy sources. The international delegates included academic and government researchers, engineers, scientists, policymakers and representatives of industrial partners. The Congress provided a unique forum for the discussion of scientific advances in this research area since it addressed in combination the health-related issues and the environmental implications of combustion by-products. The scientific outcomes of the Congress included the consensus opinions that: (a) there is a correlation between human exposure to particulate matter and increased cardiac and respiratory morbidity and mortality; (b) because currently available data does not support the assessment of differences in health outcomes between biomass smoke and other particulates in outdoor air, the potential human health and environmental impacts of emerging air-pollution sources must be addressed. Assessment will require the development of new approaches to characterize combustion emissions through advanced sampling and analytical methods. The Congress also concluded the need for better and more sustainable e-waste management and improved policies, usage and disposal methods for materials containing flame retardants.
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| 50. |
- Weidemann, Eva, 1982-, et al.
(författare)
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In-filter PCDF and PCDD formation at low temperature during MSWI combustion
- 2014
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Ingår i: Chemosphere. - : Elsevier. - 0045-6535 .- 1879-1298. ; 102, s. 12-17
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Tidskriftsartikel (refereegranskat)abstract
- This case study investigated PCDF and PCDD emissions from a 65 MW waste-to-energy plant to identify why an air pollution control system remodeling to accommodate increased production resulted in increased TEQ concentrations. Pre- and post-filter gases were collected simultaneously in four sample sets with varying filter temperatures and with/without activated carbon injection. Samples were analyzed to determine total PCDF and PCDD concentrations, as well as homologue profiles, and concentrations of individual congeners (some remained co-eluted). The total post filter PCDD concentrations where found to increase while the concentrations of PCDF and 2,3,7,8-substituted congeners declined. An investigation of the individual congener concentrations revealed that the increase of PCDD concentrations were due to a few congeners, suggesting a single formation route. The study also concludes that vital information about the formation could be obtained by not restricting the analysis to just the 2,3,7,8-substituted congeners.
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