Brunel University Institute for the Environment PhD Theses
Abstract
This thesis was submitted for the degree of Doctor of Philosophy and awarded by Brunel University, 04/02/2008.The leachability of cadmium, cobalt, copper, lead, nickel and zinc metals and their oxides, sulfides and carbonates by water, 0.5 mol dm-3 CH3COOH, 0.1 mol dm -3 HCl/NaCI (1: 1 mixture) and 2 mol dm -3 HNO3 is reported. The concentrations of the leached heavy metals are compared with the trigger levels set by World Health Organisation (WHO). Three leaching solutions (nitric, sulfuric and hydrochloric acids) were used to extract copper, zinc, cobalt, nickel, iron and lead from spent catalysts prior to the application of separation technologies. Leaching experiments were conducted using both traditional methods and a microwave-assisted extraction technique. Data are provided on the effects of leaching temperature, leaching time, solid to liquid ratio and acid concentration on the extraction of different metals. The use of 2 mol dm-3 sulfuric acid at 50°C for 60 minutes and at a solid/liquid (S/L) ratio of 1: 25 achieved more than 90% extraction for all the metals studied. A comparison of the results from traditional and microwave extraction techniques demonstrates that microwave heating reduced the time required to obtain maximum metal extraction. The kinetics for the traditional extraction procedure showed that diffusion was the ratecontrolling process, but it was not possible to conclusively establish the rate controlling process for the microwave leaching. The feasibility of using an electrodialysis process to separate metal ions, such as copper from zinc, was examined. A laboratory-scale three compartments membrane system was designed, constructed, used and optimised for the separation process. The separation of copper from zinc in the electrodialysis process exploited the greater stability of the Cu-EDTA complex compared with the Zn-EDTA complex. It was observed that Zn 2+ ions migrated through the cation-exchange membrane from central compartment to catholyte and, simultaneously, the negative Cu-EDTA complex transferred to the analyte compartment crossing the anion exchange membrane. The technique was successfully used to separate mixtures of Cu: Cd and Zn: Ni. The technique could not, however, be used for the separation of Zn from Cd. An adsorption process was used to prepare copper, iron, nickel and zinc oxides catalysts on y-A1203 as support. The materials prepared were used in a fixed bed reactor to assess the catalytic oxidation of volatile organic compounds (methane and ethane) in air. Cu/y- A1203 was found to be the most promising catalyst for the complete oxidation of methane and ethane at temperatures of 575°C and 525°C, respectively. Increasing the calcination temperature in the drying and pre-treatment of the catalysts resulted in a decrease in the catalytic activity