This work investigates mercury flux in soil amended by gypsum from flue gas desulphurization (FGD) units of coal-fired power plants. There are two phases of this research, including field and greenhouse studies. Previous studies indicate that FGD gypsum could increase corn yield, but may lead to more mercury uptake by corn. Recent studies have been carried out in greenhouses to investigate mercury transport in FGD gypsum treated soil. Major aspects include uptake of mercury by plants and emission of mercury into the atmosphere based on application rates of FGD gypsum. Additional aspects include rainfall, temperature, soil, and plants types. Higher FGD gypsum application rates generally led to higher mercury concentration in the soil, as well as, increased mercury emission into the atmosphere, and increased mercury levels in plants, especially roots and leaves. Soil properties and plant species also played important roles in mercury transport. In addition, it was also found that increased water and higher temperatures may contribute to mercury emission in the atmosphere. Some plants, such as tall fescue, were able to prevent mercury from atmospheric emission and infiltration within the soil. Mercury concentration in the stem of plants was found to be increased and then plateaued upon increasing FGD gypsum application. However, mercury in roots and leaves was generally increased upon increasing FGD gypsum application rates. Some mercury was likely absorbed by leaves of plants from mercury in the surrounding atmosphere.

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Flue gas desulphurisation (FGD) is a crucial method to minimise the SO2 emissions from industrial processes. The FGD system utilise an alkaline sorbent to remove SO2 from the flue gases. Calcium in form of limestone is a commonly used sorbent where gypsum is produced asa by-product. However, the limestone reactivity, along with impurities within the sorbent, can significantly influence the effectiveness of SO2 removal and the quality of the by-products. At Heidelberg materials Cement Sverige an intermediate product, raw meal (RM) 8, is used assorbent in the FGD and gypsum is used as setting retarder in the cement. The aim with this project is to examine if raw meal 7 or A-sten is a better sorbent than raw meal 8 with respect to consumption rate, gypsum quality and its effect on the cement properties, and economic viability. To accomplish this a theoretical study was performed along with data analysis. RM 7 and A-sten are both purer than RM 8 but the raw material cost for RM 7 is about 1.24 times the raw material cost for RM 8 and the production costs and transportation costs are greater for RM 7 than for RM 8. The raw material cost for A-sten is about 0.45 times the cost for RM 8 but is not produced on site. All sorbents contain magnesium which can react with sulphur and precipitate as epsomite or hexahydrite, which also acts as retarders, where epsomite retard the cement setting time significantly compared to gypsum. To calculate the consumption rate of raw meal and A-sten into the scrubber three different methods were used. The difference between the methods lies in the consideration of how the calcium and magnesium species in the sorbent react with sulphur, with all calcium and magnesium reacting with sulphur in method 1, method 2 take the mass fraction of sulphurcontaining species into consideration, and method 3 incorporating mole fractions of calcium and magnesium species as well as sulphur from the sorbent. The pH and SO2 emissions were analysed for two different time periods where the first analysed period shows a correlation between low pH and high SO2 emissions, while the latter analysed period lacks a clear pH-SO2 correlation. A correlation between a lower pH and a lower percentage of MgSO4⸱6H2O and MgSO4⸱7H2O in the slurry could be made. The calculated rawmeal flow rate for RM 8 is between 520 and 554 kg/h, depending on the method used. To achieve the same desulphurisation efficiency with RM 7 the flow was calculated to 499-538kg/h and 427-464 kg/h for A-sten. Given the comparable mass flow rates of RM 8 and RM 7 it is advisable to retain RM 8 as asorbent in the scrubber regardless of the higher magnesium content due the higher cost associated with RM 7. However, the epsomite content in the slurry should be considered when optimising sulphur in cement production. Using A-sten as sorbent would minimise the rawmaterial costs and result in purer gypsum slurry with a lower epsomite content. Operating with a purer sorbent can also enhance the efficiency of the FGD process, leading to lower SO2 emissions. The calculations in the report assume that calcium and magnesium in the different sorbents react similarly, further analysis of their reactivity is recommended for more accurate results. / Rökgasavsvavling är en avgörande metod för att minimera SO2-utsläppen från industriella processer. Rökgasavsvaling använder en alkalisk sorbent för att avlägsna SO2 från rökgaserna. Kalcium i form av kalksten är en vanligt förekommande sorbent där gips produceras som en biprodukt. Kalkstensreaktiviteten, tillsammans med föroreningar i sorbenten kan emellertid avsevärt påverka avsvavlingseffektiviteten och biproduktens kvalitet. På Heidelberg materials Cement Sverige används en mellanprodukt, råmjöl (RM) 8, somsorbent i avsvavlingsprocessen och gipset används som härdningshämmare i cementet. Syftet med detta projekt är att undersöka om råmjöl 7 eller A-sten är en bättre sorbent än råmjöl 8 med avseende på konsumtionshastighet, gipskvalitet och dess effekt på cementens egenskapersamt ekonomisk bärkraft. För att uppnå syftet genomfördes en teoretisk studie tillsammans med dataanalys. RM 7 och A-sten är båda renare än RM 8 men råvarukostnaden för RM 7 är cirka 1,24 gånger råvarukostnaden för RM8. Dessutom är produktions- och transportkostnaderna högre för RM7 än för RM 8. Råvarukostnaden för A-sten är cirka 0,45 gånger råvarukostnaden för RM 8, dock mals inte A-sten på plats. Alla sorbenter innehåller magnesium som kan reagera med svavel och fälla ut som epsomit eller hexahydrit, vilka också har en härdningshämmande effekt, där epsomit fördröjer cementens härdning signifikant jämfört med gips. För att beräkna konsumtionshastigheten för råmjöl och A-sten i skrubbern användes tre olika metoder. Skillnaden mellan metoderna är hur kalcium- och magnesiumarterna i sorbenten reagerar med svavel, där allt kalcium och magnesium reagerar med svavel i metod 1. Metod 2 tar hänsyn till massfraktionen av svavelhaltiga ämnen och metod 3 innehåller molfraktioner av kalcium- och magnesiumarter samt svavel från sorbenten. pH och SO2-utsläppen analyserades under två olika tidsperioder där den första perioden visar ett samband mellan lågt pH och höga SO2-utsläpp, medan den senare analyserade perioden saknar ett tydligt pH-SO2-samband. En korrelation mellan ett lägre pH och en lägre andel MgSO4⸱6H2O och MgSO4⸱7H2O i gipsslurryn skulle kunna göras. Det beräknade flödet av råmjöl för RM 8 är mellan 520 och 554 kg/h, beroende på vilken metod som används. För att uppnå samma avsvavlingseffektivitet med RM 7 måste flödet vara 499–538 kg/h och 427–464 kg/h för A-sten. Med tanke på de jämförbara massflödena för RM 8 och RM 7 är det lämpligt att behålla RM 8 som sorbent i skrubbern, trots den högre magnesiumhalten, på grund av de högre kostnaderna för RM 7. Epsomithalten i slurryn bör dock tas i beakting vid optimering av svavel i cementproduktionen. Att använda A-sten som sorbent skulle minimera råvarukostnaderna och resultera i en renare gipsslurry med lägre epsomithalt. Att använda med en renare sorbent kan också förbättra avsvavlingseffektiviteten, vilket leder till lägre SO2-utsläpp. Beräkningarna i rapporten förutsätter att kalcium och magnesium i de olika sorbenterna reagerar lika, ytterligare analys av deras reaktivitet rekommenderas för mer exakta resultat.

One of the most common ways to produce heat and electricity in Europe today is by the incineration of waste or combustion of coal. These materials can be very sulfurous and during combustion sulfur dioxide is produced. This is an environmental and health related toxic substance which is why power plants have strict regulations on removing it from the flue gas. Sulfur dioxide is removed from the flue gas by adding a limestone reagent. The sulfur dioxide reacts with the limestone and the synthetic product obtained is “Flue Gas Desulfurization gypsum”. This byproduct, from combustion, provides an environmentally friendly solution when used in building material such as plasterboards. The FGD gypsum that is being used in different types of building materials does not derive from waste incinerated power plants. We have more than 30 of these in Sweden and some of them get FGD gypsum as a byproduct. The purpose of this thesis was to find out whether a particular waste incineration plant in Sweden can reuse their gypsum waste instead of disposing it at landfill.

[pt] SO2 é conhecido com um grande contaminante ambiental e muitos países estabeleceram regras para o controle da sua emissão para a atmosfera. Como resultado a maioria das plantas fornecedoras de energia foram equipadas com instalações de dessulfurização de gases de combustão. Embora esta tecnologia seja bem sucedida no abate de SO2, ela gera uma grande quantidade de gesso FGD (flue gas desulfurization) como resíduo. Grandes esforços estão sendo feitos para aproveitar este resíduo (gesso FGD). No presente estudo o gesso FGD foi avaliado como aditivo retardador do tempo de pega substituindo o gesso natural na fabricação do cimento Portland (CP II E-32). Os resultados da caracterização físico-química e morfológica do gesso natural e de gesso FGD identificam um material de alta pureza, sulfato de cálcio di-hidratado para o gesso natural, e presença principalmente de bassanita (CaSO4.0,6H2O) e hannebachite (CaSO3.0,5H2O) com baixas concentrações de impurezas no gesso FGD. Baseado nos resultados, o gesso FGD é uma alternativa adequada para substituir o gesso natural. O tempo de pega mostrou cerca de uma hora de retardo em comparação com gesso natural e seu efeito sobre a resistência à compressão para as amostras de 3, 7 e 28 dias depende da composição das misturas, atingindo um valor máximo para a argamassa com 2,1 porcento de gesso FGD e 1,4 porcentode gesso natural. Também foi estimado o impacto ambiental do gesso FGD, examinando a liberação de seus constituintes inorgânicos seguindo a norma ABNT NBR 10004:2004 e classificando o resíduo como não perigoso e não inerte. / [en] The SO2 is well known as an important environmental contaminant and many countries have established rules to control its emission to the atmosphere and as result most of power supply plants were equipped with flue gas desulfurization systems. Although this technology is successful in the discharge of SO2, its generates a large amount of gypsum FGD (flue gas desulfurization) as a residue. Great efforts are being made to find destinations for this residue. In the present study, the FGD gypsum was evaluated as setting retarder to replace the natural gypsum in the production of Portland cement (CP II E-32). The results of physical-chemistry and morphological characterization of both products, natural and FGD gypsum showed a material of high purity, calcium sulfate dehydrate for natural gypsum, and the presence of bassanite (CaSO4.0,6H2O) and hannebachite (CaSO3.0,5H2O) with low concentrations of impurities for FGD gypsum. Based on the results, the FGD gypsum is a suitable alternative to replace natural gypsum. The setting time with FGD gypsum showed about 1 hour delay compared with natural gypsum and its effect on compressive strength, for samples of 3, 7 e 28 days, depend the composition of the mixtures, reaching the maximum value for the mixture of 1,4 weight percent natural gypsum and 2,1 weight percent FGD gypsum. The FGD gypsum environmental impact was evaluated by determining its potential in releasing inorganic constituents, following the standard ABNT NBR 10004:2004, and it was classified as a non-hazardous and non-inert.

The ever-increasing quantity of by-products generated from burning coal in the production of electricity has brought about the need for new areas of utilization. This study examined the use of FGD gypsum and fluidized bed combustion ash along with Class F fly ash in the production of low-energy, 100% by-product cement blends. The cement blends used the advantageous properties of the by-product materials to create cementing properties rather than energy intensive clinker used in ordinary portland cement. The FGD gypsum was converted to hemihydrate which rapidly hydrated to provide the cement with early strength gains, whilst the fluidized bed combustion ash reacted with the Class F fly ash to form pozzolanic cementitious phases which provided the longer-term compressive strength and possibly resistance to weathering. The rate of compressive strength gains and minimizing detrimental expansion were two properties of particular interest in the study. Chemical admixtures were used to improve the compressive strengths of the cement mortars and decrease their solubility.

Doctor of Philosophy / Department of Agronomy / Ganga M. Hettiarachchi / Constructed wetland treatment systems (CWTSs) are an alternative adaptation for flue-gas desulfurization (FGD) wastewater purification. A series of laboratory-based soil column studies mimicking a pilot-scale CWTS was carried out to evaluate the performance of the treatment system in detail. The main objectives of studies were to (1) understand the transport characteristics, retention capacity and transformation of selenium and other FGD constituents in the CWTS, (2) evaluate the effectiveness of soil treatments and influent flow rate on the performance of the CWTS, and (3) develop a mechanistic understanding of the CWTS performance through monitoring interrelationships of selenium (Se), arsenic (As), iron (Fe), and sulfur (S). Ferrihydrite (1% w/w), and labile organic carbon (OC) were used as soil treatments. Different influent flow rates, X (1.42 mL/hour), 2X, or 1/2X were used depending on the objectives of each study. Deoxygenated 1:1 mixture of FGD: raw water was the influent. It was delivered to the saturated columns with an upward flow. Effluent samples were collected continuously, and analyzed for constituents of concern. End of these experiments, soil from sectioned columns were used for total elemental analysis, sequential extraction procedure (SEP) for Se, and synchrotron-based X-ray spectroscopy analyses. Results indicated a complete Se retention by the columns. Boron, and fluorine partially retained whereas sodium, sulfur, and chlorine retention was weak, agreeing with field observations. Some of the initially-retained Se (~ 4 to 5%) was mobilized by changing redox conditions in the soil. Selenium fed with the wastewater accumulated in the bottom 1/3 (inlet) of the soil columns and was mainly sequestrated as stable forms revealed by SEP. Bulk-, and micro-XANES analyses suggested the retention mechanism of Se from the FGD wastewater was via the transformation of Se into reduced/stable forms [Se(IV), organic Se, and Se(0)]. Under wetland conditions, native soil As was mobilized by reductive dissolution of As associated minerals. However, the ferrihydrite amendment suppressed the native soil As mobility. Micro-XRF mapping integrated with As, and Fe-XANES suggested that the mechanism of native soil As retention was the sequestration of released As with newly precipitated secondary Fe minerals. A long-term study carried out with X, 1/2X flow rates, and OC source indicated enhanced S retention by the slow flow rate (1/2X), most likely due to the time dependency of biogenic S reduction. Further, bulk S-, As-, and Fe-XANES revealed that long submergence period and the slow flow rate increased the formation of reduced and/or biogenic S, realgar-like, and greigite-like species. These observations indicated that modified flow rates could have a significant impact on the long-term trace element (such as As) sequestration in the CWTS. Our studies provide useful information to improve the performance, and longevity of a full-scale CWTS for FGD wastewaters.

>Magister Scientiae - MSc / Over the past 5 years, South Africa has been experiencing a severe drought. This has caused industrial and agricultural processes, to compete for a limited supply of water. Since the economy relies mostly on agricultural activities, water consumption by industrial processes is taking its toll. One of these processes is the introduction of wet flue gas desulphurization (FGD) treatment at Eskom coal fired power stations. This dissertation explores the possibility of using membrane technology as a means of water recovery after the coal combustion flue gas has been treated with wet FGD. A lab-scale permeance testing system was specially built and modified to have complete thermal control of the environment inside the system. The permeance testing system produced a gas, similar to that of a wet FGD treated flue gas, which was then tested. A tubular lab-scale membrane module was designed and produced for the permeance testing system. The permeance figures of both Nitrogen gas and water vapour were determined for the membrane used in module production. These figures coincided with figures provided by the supplier, which warranted successful permeance testing. After success of the lab-scale testing, the data was used to design and develop a pilot-scale membrane module. This module was designed to meet pre-determined requirements as set forth by the project team. Producing lab-scale membrane modules helped identify and address possible problems in pilot-scale module design. This lead to the successful design and construction of a pilot-scale membrane module that could be used to recover the water that is needed to run the wet FGD process.

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