Simultaneous disinfection and microcontaminants elimination of urban wastewater secondary effluent by solar advanced oxidation sequential treatment at pilot scale.

The effect of different times of Fe:Ethylenediamine-N, N'-disuccinic acid (EDDS) dosing and H2O2 as well as different Fe:EDDS concentrations in the sequential treatment sunlight/H2O2 followed by sunlight/H2O2/Fe:EDDS at circumneutral pH was investigated for the first time focusing both in contaminants of emerging concern (CECs) and bacteria removal in urban wastewater treatment plant effluents. Process efficiency was evaluated in terms of (i) degradation of five CECs (namely caffeine, carbamazepine, diclofenac, sulfamethoxazole and trimethoprim) at the initial concentration of 100 µgL-1 each and (ii) bacteria inactivation (Escherichia coli (E. coli) and Salmonella spp). The effect of H2O2, Fe and EDDS concentration and Fe:EDDS dosing time was evaluated. 60% removal of the sum of total CECs and pathogens inactivation below the detection limit (DL) were observed by the sequential treatment with Fe:EDDS additions at 60 min and 45 min in simulated urban wastewater effluent. Sequential treatment was validated in actual urban wastewater effluent, being able to remove 60% of the target CECs and inactivate bacteria below the DL. Increasing EDDS concentration negatively affected Salmonella spp inactivation. Sequential treatment based on 120 min of sunlight/H2O2 (50 mg L-1) and subsequent SPF with Fe:EDDS (0.1:0.1 mM) was chosen as best operation conditions for full scale treatment in urban wastewater treatment plants.

Sunlight advanced oxidation processes vs ozonation for wastewater disinfection and safe reclamation.

Solar processes (sunlight/H2O2, solar photo-Fenton with EDDS at neutral pH) were compared to a consolidated technology (ozonation) in the inactivation of target bacteria (E. coli, Salmonella spp. and Enterococcus spp.) under realistic conditions (real secondary treated urban wastewater (WW), pilot scale reactors, natural sunlight) to evaluate their possible industrial application. The highest bacteria inactivation rate (all the target pathogens were inactivated below the detection limit (DL) (100 CFU/100 mL) within 45 min treatment) was observed for ozonation (83 mgO3/L h). Similar inactivation behavior for all bacteria was observed for sunlight/H2O2 (50 mg/L) and solar photo-Fenton (SPF) with EDDS (1:1 molar ratio, 0.1 mM of Fe and 50 mg/L of H2O2). Although the DL was not reached, faster inactivation kinetics (0.007, 0.013 and 0.002 1/min for E. coli, Salmonella spp. and Enterococcus spp., respectively) and lower bacterial concentration after a 180 min treatment were observed for sunlight/H2O2 process compared to SPF (0.005, 0.01 1/min and no inactivation, respectively), Enterococcus spp. being the higher resistance microorganism. The negative effect of carbonates on disinfection performance was also evaluated. Quantitative microbial risk assessment for the ingestion of lettuce irrigated with untreated and treated WW was estimated. Disinfection by ozonation and sunlight/H2O2 processes were found to drastically decrease the associated microbiological risk (the mean risk of illness decreased from 0.10 (untreated) to 1.35 × 10-4 (treated) for E. coli and from 0.03 to 2.21 × 10-6 for Salmonella).

Simultaneous removal of contaminants of emerging concern and pathogens from urban wastewater by homogeneous solar driven advanced oxidation processes.

Simultaneous removal of contaminants of emerging concern and bacteria inactivation in simulated municipal wastewater effluent (SMWW) through solar advanced oxidation processes, namely sunlight/H2O2 and solar photo-Fenton with Ethylenediamine-N,N'-disuccinic acid (EDDS) at neutral pH was investigated. Process efficiency was evaluated in terms of (i) degradation of five contaminants of emerging concern (CECs, namely caffeine, carbamazepine, diclofenac, sulfamethoxazole and trimethoprim) at the initial concentration of 100 µgL-1 each and (ii) bacteria inactivation (E. coli, S. enteritidis and E. faecalis), at the initial concentration of 103 CFU mL-1 each. Solar photo-Fenton process was first investigated at lab scale in a solar simulator to evaluate the effect of iron concentration (0.1 mM and 0.05 mM) and Fe:EDDS ratio (1:2 and 1:1). Subsequently, sunlight/H2O2 and solar photo-Fenton with EDDS (molar ratio 1:1, Fe(III) 0.1 mM) at neutral pH were singularly and sequentially investigated at pilot scale in a raceway pond reactor. Sunlight/H2O2 (50 mg L-1) tests resulted in total bacteria inactivation in 60 min (0.69 kJ L-1) but low CECs removal efficiency. On the opposite, solar photo-Fenton was effective in the removal of the total CECs (87% removal after 20 min and 0.14 kJ L-1) but not in E. faecalis inactivation (the initial concentration did not change even after 180 min). However, when the two processes were operated sequentially, a complete bacteria inactivation was observed in 15 min (0.17 kJ L-1), 20 min (0.23 kJ L-1) and 60 min (0.70 kJ L-1) of treatment for E. coli, S. enteritidis and E. faecalis, respectively and 80% removal of total CECs was achieved after 10 min of Fe:EDDS addition. Sequential combination of sunlight/H2O2 and solar photo-Fenton would be an effective solution for simultaneous CECs removal and bacteria inactivation in the same photo-reactor.