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Despite extensive preventative efforts, the problem of controlling infections associated with biomedical materials persists. Bacteria tend to colonize on biocompatible materials and form biofilms; thus, novel biomaterials with antibacterial properties are of great interest. In this thesis, titanium dioxide (TiO2)-associated photocatalysis under ultraviolet (UV) irradiation was investigated as a strategy for developing bioactivity and antibacterial properties on biomaterials. Although much of the work was specifically directed towards dental materials, the results presented are applicable to a wide range of biomaterial applications. Most of the experimental work in the thesis was based on a resin-TiO2 nanocomposite that was prepared by adding 20 wt% TiO2 nanoparticles to a resin-based polymer material. Tests showed that the addition of the nanoparticles endowed the adhesive material with photocatalytic activity without affecting the functional bonding strength. Subsequent studies indicated a number of additional beneficial properties associated with the nanocomposite that appear promising for biomaterial applications. For example, irradiation with UV light induced bioactivity on the otherwise non-bioactive nanocomposite; this was indicated by hydroxyapatite formation on the surface following soaking in Dulbecco’s phosphate-buffered saline. Under UV irradiation, the resin-TiO2 nanocomposite provided effective antibacterial action against both planktonic and biofilm bacteria. UV irradiation of the nanocomposite also provided a prolonged antibacterial effect that continued after removal of the UV light source. UV treatment also reduced bacterial adhesion to the resin-TiO2 surface. The mechanisms involved in the antibacterial effects of TiO2 photocatalysis were studied by investigating the specific contributions of the photocatalytic reaction products (the reactive oxygen species) and their disinfection kinetics. Methods of improving the viability analysis of bacteria subjected to photocatalysis were also developed.

Irradiation with ultraviolet (UV) light is used for the disinfection of bacterial contaminants in the production of potable water, and in the treatment of selected wastewaters. However, efficacy of UV disinfection is limited by the combined effect of suspended solids concentration and UV absorbance. Limited published UV disinfection data are available that account for the combined effects of UV dose, suspended solids concentration and UV absorbance. This present lack of a rigorous quantitative understanding of the kinetics of UV disinfection limits process optimisation and wider application of UV treatment. The development and validation of an adequate model to describe UV disinfection kinetics presented in this thesis can therefore be justified by an increased confidence of reliability of design for UV disinfection. Using the published data of Nguyen (1999), four established model forms were assessed to account for the combined effect of suspended solids and/or soluble UV absorbing compounds, and UV dose on the efficacy of disinfection. The four model forms were: a log-linear form, Davey Linear-Arrhenius (DL-A), Square-Root (or Ratkowsky- Belehradek) and a general nth order Polynomial (nOP) form that was limited to a third order. Criteria for assessment of an adequate predictive model were established including: accuracy of predicted against observed values, percent variance accounted for (%V), and; appraisal of residuals. The DL-A model was shown to best fit the data for UV disinfection of Escherichia coli (ATCC 25922); followed by the nOP, log-linear and Square-Root forms. However, the DL-A form must be used in conjunction with a first-order chemical reaction equation, and was shown to predict poorly at high experimental values of UV dose (> 40,000 μWs cm-2). The DL-A model was not amenable to extrapolation beyond the observed UV dose range. To overcome the shortcomings of the Davey Linear-Arrhenius model synthesis of two new, non-linear model forms was undertaken. The two models were a modified exponentially damped polynomial (EDPm) and a form based on the Weibull probability distribution. The EDPm model has three terms: a rate coefficient (k), a damping coefficient (λ), and; a breakpoint dose ([dose]B). The rate coefficient governs the initial rate of disinfection prior to the onset of tailing, whilst the breakpoint is the UV dose that indicates the onset of tailing. The damping coefficient controls curvature in the survivor curve. The Weibull model has just two terms: a dimensionless scale parameter (β0), and; a shape parameter (β1). The scale parameter represents the level of disinfection in the tail of the survivor curve (as log10 N/N0), whilst the shape parameter governs the degree of curvature of the survivor data. Each model was assessed against the independent and published UV disinfection data of Nelson (2000) for treatment of faecal coliforms in a range of waste stabilisation pond effluents. Both models were found to be well suited to account for tailing in these UV disinfection data. Overall, the EDPm model gave a better fit to the data than the Weibull model form. To rigorously validate the suitability of the new EDPm and Weibull models a series of experimental trials were designed and carried out in a small-scale pilot UV disinfection unit. These trials included data determined specifically at low values of UV dose (<10,000 μWs cm-2) to fill the gap in the experimental data of Nguyen (1999). The experimental trials were carried out using a commercially available, UV disinfection unit (LC5TM from Ultraviolet Technology of Australasia Pty Ltd). Purified water contaminated with Escherichia coli (ATCC 25922) with a range of feed water flow rates (1 to 4 L min-1) was used. E. coli was selected because it is found in sewage, or water contaminated with faecal material, and is used as an indicator for the presence of enteric pathogens. E. coli should not be present in potable water. The hydrodynamics of water flow within the disinfection unit were established using digital video photography of dye trace studies with Methylene Blue. Nominal UV dose (2,700 to 44,200 μWs cm-2) was controlled by manipulating the flow rate of feed water through the UV disinfection unit (i.e. residence time), or by varying the exposed length of the control volume of the disinfection unit. The transmittance of the feed water (at 254 nm) was adjusted by the addition of either a soluble UV absorbing agent (International RoastTM instant coffee powder; 0.001 to 0.07 g L-1), or by addition of suspended matter as diatomaceous earth (Celite 503TM; 0.1 to 0.7 g L-1, with a median particle size of 23 μm). The absorbing agent (instant coffee), when in a comparable concentration, was found to produce a greater reduction in water transmission than the suspended material (Celite 503TM). It therefore contributed to a greater reduction in the initial rate of disinfection. Neither agent was found to produce a systematic reduction in the observed efficacy of disinfection however. Experimental results highlight that in the absence of soluble absorbing agents, or suspended solids, the initial rate of disinfection is higher when fewer viable bacteria are initially present. Both the new EDPm and Weibull forms gave a good fit to the experimental data. The EDPm better fitted the data on the basis of residual sum-of-squares (0.03 to 2.13 for EDPm cf. 0.16 to 4.37 for the Weibull form). These models are both of a form suitable for practical use in modelling UV disinfection data. Results of this research highlight the impact of water quality, as influenced by the combined effect of UV dose, suspended solids concentration and UV absorbance, on small-scale UV disinfection for potable water production. Importantly, results show that the concentration of soluble UV absorbing agents and suspended solids are not in themselves sufficient criteria on which to base assessment of efficacy of UV disinfection / http://proxy.library.adelaide.edu.au/login?url= http://library.adelaide.edu.au/cgi-bin/Pwebrecon.cgi?BBID=1342403 / Thesis (M.Eng.Sc.) - University of Adelaide, School of Chemical Engineering, 2008

Irradiation with ultraviolet (UV) light is used for the disinfection of bacterial contaminants in the production of potable water, and in the treatment of selected wastewaters. However, efficacy of UV disinfection is limited by the combined effect of suspended solids concentration and UV absorbance. Limited published UV disinfection data are available that account for the combined effects of UV dose, suspended solids concentration and UV absorbance. This present lack of a rigorous quantitative understanding of the kinetics of UV disinfection limits process optimisation and wider application of UV treatment. The development and validation of an adequate model to describe UV disinfection kinetics presented in this thesis can therefore be justified by an increased confidence of reliability of design for UV disinfection. Using the published data of Nguyen (1999), four established model forms were assessed to account for the combined effect of suspended solids and/or soluble UV absorbing compounds, and UV dose on the efficacy of disinfection. The four model forms were: a log-linear form, Davey Linear-Arrhenius (DL-A), Square-Root (or Ratkowsky- Belehradek) and a general nth order Polynomial (nOP) form that was limited to a third order. Criteria for assessment of an adequate predictive model were established including: accuracy of predicted against observed values, percent variance accounted for (%V), and; appraisal of residuals. The DL-A model was shown to best fit the data for UV disinfection of Escherichia coli (ATCC 25922); followed by the nOP, log-linear and Square-Root forms. However, the DL-A form must be used in conjunction with a first-order chemical reaction equation, and was shown to predict poorly at high experimental values of UV dose (> 40,000 μWs cm-2). The DL-A model was not amenable to extrapolation beyond the observed UV dose range. To overcome the shortcomings of the Davey Linear-Arrhenius model synthesis of two new, non-linear model forms was undertaken. The two models were a modified exponentially damped polynomial (EDPm) and a form based on the Weibull probability distribution. The EDPm model has three terms: a rate coefficient (k), a damping coefficient (λ), and; a breakpoint dose ([dose]B). The rate coefficient governs the initial rate of disinfection prior to the onset of tailing, whilst the breakpoint is the UV dose that indicates the onset of tailing. The damping coefficient controls curvature in the survivor curve. The Weibull model has just two terms: a dimensionless scale parameter (β0), and; a shape parameter (β1). The scale parameter represents the level of disinfection in the tail of the survivor curve (as log10 N/N0), whilst the shape parameter governs the degree of curvature of the survivor data. Each model was assessed against the independent and published UV disinfection data of Nelson (2000) for treatment of faecal coliforms in a range of waste stabilisation pond effluents. Both models were found to be well suited to account for tailing in these UV disinfection data. Overall, the EDPm model gave a better fit to the data than the Weibull model form. To rigorously validate the suitability of the new EDPm and Weibull models a series of experimental trials were designed and carried out in a small-scale pilot UV disinfection unit. These trials included data determined specifically at low values of UV dose (<10,000 μWs cm-2) to fill the gap in the experimental data of Nguyen (1999). The experimental trials were carried out using a commercially available, UV disinfection unit (LC5TM from Ultraviolet Technology of Australasia Pty Ltd). Purified water contaminated with Escherichia coli (ATCC 25922) with a range of feed water flow rates (1 to 4 L min-1) was used. E. coli was selected because it is found in sewage, or water contaminated with faecal material, and is used as an indicator for the presence of enteric pathogens. E. coli should not be present in potable water. The hydrodynamics of water flow within the disinfection unit were established using digital video photography of dye trace studies with Methylene Blue. Nominal UV dose (2,700 to 44,200 μWs cm-2) was controlled by manipulating the flow rate of feed water through the UV disinfection unit (i.e. residence time), or by varying the exposed length of the control volume of the disinfection unit. The transmittance of the feed water (at 254 nm) was adjusted by the addition of either a soluble UV absorbing agent (International RoastTM instant coffee powder; 0.001 to 0.07 g L-1), or by addition of suspended matter as diatomaceous earth (Celite 503TM; 0.1 to 0.7 g L-1, with a median particle size of 23 μm). The absorbing agent (instant coffee), when in a comparable concentration, was found to produce a greater reduction in water transmission than the suspended material (Celite 503TM). It therefore contributed to a greater reduction in the initial rate of disinfection. Neither agent was found to produce a systematic reduction in the observed efficacy of disinfection however. Experimental results highlight that in the absence of soluble absorbing agents, or suspended solids, the initial rate of disinfection is higher when fewer viable bacteria are initially present. Both the new EDPm and Weibull forms gave a good fit to the experimental data. The EDPm better fitted the data on the basis of residual sum-of-squares (0.03 to 2.13 for EDPm cf. 0.16 to 4.37 for the Weibull form). These models are both of a form suitable for practical use in modelling UV disinfection data. Results of this research highlight the impact of water quality, as influenced by the combined effect of UV dose, suspended solids concentration and UV absorbance, on small-scale UV disinfection for potable water production. Importantly, results show that the concentration of soluble UV absorbing agents and suspended solids are not in themselves sufficient criteria on which to base assessment of efficacy of UV disinfection / http://proxy.library.adelaide.edu.au/login?url= http://library.adelaide.edu.au/cgi-bin/Pwebrecon.cgi?BBID=1342403 / Thesis (M.Eng.Sc.) - University of Adelaide, School of Chemical Engineering, 2008

Irradiation with ultraviolet (UV) light is used for the disinfection of bacterial contaminants in the production of potable water, and in the treatment of selected wastewaters. However, efficacy of UV disinfection is limited by the combined effect of suspended solids concentration and UV absorbance. Limited published UV disinfection data are available that account for the combined effects of UV dose, suspended solids concentration and UV absorbance. This present lack of a rigorous quantitative understanding of the kinetics of UV disinfection limits process optimisation and wider application of UV treatment. The development and validation of an adequate model to describe UV disinfection kinetics presented in this thesis can therefore be justified by an increased confidence of reliability of design for UV disinfection. Using the published data of Nguyen (1999), four established model forms were assessed to account for the combined effect of suspended solids and/or soluble UV absorbing compounds, and UV dose on the efficacy of disinfection. The four model forms were: a log-linear form, Davey Linear-Arrhenius (DL-A), Square-Root (or Ratkowsky- Belehradek) and a general nth order Polynomial (nOP) form that was limited to a third order. Criteria for assessment of an adequate predictive model were established including: accuracy of predicted against observed values, percent variance accounted for (%V), and; appraisal of residuals. The DL-A model was shown to best fit the data for UV disinfection of Escherichia coli (ATCC 25922); followed by the nOP, log-linear and Square-Root forms. However, the DL-A form must be used in conjunction with a first-order chemical reaction equation, and was shown to predict poorly at high experimental values of UV dose (> 40,000 μWs cm-2). The DL-A model was not amenable to extrapolation beyond the observed UV dose range. To overcome the shortcomings of the Davey Linear-Arrhenius model synthesis of two new, non-linear model forms was undertaken. The two models were a modified exponentially damped polynomial (EDPm) and a form based on the Weibull probability distribution. The EDPm model has three terms: a rate coefficient (k), a damping coefficient (λ), and; a breakpoint dose ([dose]B). The rate coefficient governs the initial rate of disinfection prior to the onset of tailing, whilst the breakpoint is the UV dose that indicates the onset of tailing. The damping coefficient controls curvature in the survivor curve. The Weibull model has just two terms: a dimensionless scale parameter (β0), and; a shape parameter (β1). The scale parameter represents the level of disinfection in the tail of the survivor curve (as log10 N/N0), whilst the shape parameter governs the degree of curvature of the survivor data. Each model was assessed against the independent and published UV disinfection data of Nelson (2000) for treatment of faecal coliforms in a range of waste stabilisation pond effluents. Both models were found to be well suited to account for tailing in these UV disinfection data. Overall, the EDPm model gave a better fit to the data than the Weibull model form. To rigorously validate the suitability of the new EDPm and Weibull models a series of experimental trials were designed and carried out in a small-scale pilot UV disinfection unit. These trials included data determined specifically at low values of UV dose (<10,000 μWs cm-2) to fill the gap in the experimental data of Nguyen (1999). The experimental trials were carried out using a commercially available, UV disinfection unit (LC5TM from Ultraviolet Technology of Australasia Pty Ltd). Purified water contaminated with Escherichia coli (ATCC 25922) with a range of feed water flow rates (1 to 4 L min-1) was used. E. coli was selected because it is found in sewage, or water contaminated with faecal material, and is used as an indicator for the presence of enteric pathogens. E. coli should not be present in potable water. The hydrodynamics of water flow within the disinfection unit were established using digital video photography of dye trace studies with Methylene Blue. Nominal UV dose (2,700 to 44,200 μWs cm-2) was controlled by manipulating the flow rate of feed water through the UV disinfection unit (i.e. residence time), or by varying the exposed length of the control volume of the disinfection unit. The transmittance of the feed water (at 254 nm) was adjusted by the addition of either a soluble UV absorbing agent (International RoastTM instant coffee powder; 0.001 to 0.07 g L-1), or by addition of suspended matter as diatomaceous earth (Celite 503TM; 0.1 to 0.7 g L-1, with a median particle size of 23 μm). The absorbing agent (instant coffee), when in a comparable concentration, was found to produce a greater reduction in water transmission than the suspended material (Celite 503TM). It therefore contributed to a greater reduction in the initial rate of disinfection. Neither agent was found to produce a systematic reduction in the observed efficacy of disinfection however. Experimental results highlight that in the absence of soluble absorbing agents, or suspended solids, the initial rate of disinfection is higher when fewer viable bacteria are initially present. Both the new EDPm and Weibull forms gave a good fit to the experimental data. The EDPm better fitted the data on the basis of residual sum-of-squares (0.03 to 2.13 for EDPm cf. 0.16 to 4.37 for the Weibull form). These models are both of a form suitable for practical use in modelling UV disinfection data. Results of this research highlight the impact of water quality, as influenced by the combined effect of UV dose, suspended solids concentration and UV absorbance, on small-scale UV disinfection for potable water production. Importantly, results show that the concentration of soluble UV absorbing agents and suspended solids are not in themselves sufficient criteria on which to base assessment of efficacy of UV disinfection / http://proxy.library.adelaide.edu.au/login?url= http://library.adelaide.edu.au/cgi-bin/Pwebrecon.cgi?BBID=1342403 / Thesis (M.Eng.Sc.) - University of Adelaide, School of Chemical Engineering, 2008