| 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
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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)
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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
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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. |
- 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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| 8. |
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| 9. |
- 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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| 10. |
- 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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