Accelerate ageing of refuse-derived-fuel (RDF) fly ashes

Sammanfattning: Ashes have properties that can be exploited in various applications, e.g. some ashes can be used in the construction of barriers in a landfill final top cover. A landfill top cover is a multilayer construction that protects the environment in several ways, for instance hindering gas emissions from the landfill body and water infiltration into the waste.Impervious natural materials like clay, synthetic materials like geomembranes or bentonite carpets, geosynthetic clay liners or combinations of such materials are commonly used in landfill top cover constructions. Since differential settlement may occur and the lifetimes of the synthetic materials are uncertain, it is advantageous to use thick mineral constructions. There is a great need for these materials, and substantial savings of resources can be made if alternative waste materials, like ashes, are used. Currently, ashes are either landfilled or used as construction materials. They are subject to weathering processes, including physical, chemical and mineralogical changes caused (inter alia) by fluctuations of temperature and humidity, atmospheric gases or acid rain. Ashes contain various potentially hazardous and non-hazardous chemical compounds. Therefore, precautions must be taken to avoid leaching of substances such as heavy metals into the surrounding environment. Mineral phases that are initially present and/or that form during the ageing are primarily responsible for the immobilization or leaching of diverse metals and salts. Newly formed mineral phases like clay minerals are of main interest, because of their very high cation exchange capacity, swelling and expansion properties.The conditions found in a landfill environment are likely to favour clay mineral formation. This thesis is based on studies on the effects of accelerated ageing on refuse-derived-fuel (RDF) fly ashes, in experiments under controlled laboratory conditions, intended to derive models to predict the stability of RDF fly ashes used in a landfill liner and the mineralogical changes that occur in them. A reduced factorial design was applied, followed by multivariate data analysis, to evaluate the effects of five factors - carbon dioxide (CO2) levels, temperature, relative air humidity (RH), time and the quality of added water - on mineral transformations within the ashes, and their acid neutralization capacity (ANC) and leaching behaviour.Minerals (ettringite and hydrocalumite) promoting the immobilization of hazardous compounds were found in both fresh ash and ash aged under atmospheric conditions, but these minerals disappeared upon carbonation. The main phases in ash at 20% and 100% CO2 were calcite, gypsum/anhydrite and vaterite. The abundance of gypsum and anhydrite was directly related to the temperature at which ashes were aged. The major mineral phases detected in ashes aged under 20% CO2, 65% RH and 30°C (corresponding to conditions generally found in a landfill cover) were calcite and gypsum/bassanite. The pH values of these ash specimens ranged from 7.2 to 7.6, indicating advanced carbonation. Ageing decreased pH values from 12.4 to 7.2, consequently affecting the leaching behaviour of most chemicals measured in the leachates. Levels of Ba, Ca, Cl, Cr, Cu, Pb, K and Na decreased over the study period while those of Mg, Zn and SO4 increased. No clay minerals were detected by XRD and SEM analysis in either fresh or aged ashes. However, geochemical modelling indicated that such minerals may precipitate. The modelling also indicated that clay minerals like saponite, vermiculite, chrysotile and hydrotalcite were likely to precipitate in most leachates from ash aged for 3, 10 and 22 months. Smectite, montmorillonite and illite may precipitate in leachates of ash aged for 31 months. The formation of smectite, montmorillonite and vermiculite would be advantageous due to their very high cation exchange capacities, which would favour the stabilization/immobilization of heavy metals in the mineral phases.