Sulfamethoxazole degradation in anaerobic sulfate-reducing bacteria sludge system.

Sulfamethoxazole (SMX) is one of the most commonly used antibiotics. SMX degradation in sulfate-reducing bacteria (SRB) sludge systems has not been reported so far. This research investigated the SMX degradation using SRB sludge in a sulfate-reducing up-flow sludge bed reactor. Moreover, the mechanisms and kinetics of SMX removal were also investigated using SRB sludge via a series of batch experiments. The results showed that SMX removal was characterized by a rapid sorption onto SRB sludge, and desorption from SRB sludge to aqueous phase until achieving equilibrium, and then followed by slow biodegradation. Biodegradation was the dominant route for SMX removal. The sorption process conformed well to a pseudo-second-order kinetic model, meaning that the sorption occurred primarily via a chemical sorption process. The removal of SMX followed the pseudo-zero-order kinetic model with a specific removal rate of 13.2 ± 0.1 μg/L/d at initial SMX concentration 100 μg/L in batch tests. Based on the analysis of metabolites, most of the SMX biotransformation products' structures altered in the isoxazole ring, which were significantly different from that produced by aerobic and anaerobic sludge systems. Thus, SRB sludge system could play an important role in SMX biodegradation, especially in Sulfate-reduction Autotrophic denitrification and Nitrification Integrated (SANI) process for sewage treatment.

Jia Y ，Khanal SK ，Zhang H ，Chen GH ，Lu H ... -  《-》

Removal of sulfamethoxazole (SMX) in sulfate-reducing flocculent and granular sludge systems.

This study investigated sulfamethoxazole (SMX) removal and fate in sulfate-reducing up-flow sludge bed (SRUSB) reactors inoculated with sulfate-reducing bacteria (SRB) granules and flocs. The resilience of SRB granules and flocs against varying pHs and hydraulic retention times (HRTs) was also examined. SRB granules and flocs efficiently removed SMX from wastewater, which was significantly higher than the aerobic sludge. SRB granules achieved significantly (p < 0.05) higher SMX removal (∼13.3 μg/g suspended solids (SS)-d) than the SRB flocs (∼11.2 μg/g SS-d) during 150-day of SRUSB reactors operation. The SMX removal by both granules and flocs was mainly attributed to biodegradation. Sorption also contributed to SMX removal, in which aromatic protein-like substances of extracellular polymeric substances played important role in SMX removal. In addition, SRB granules showed higher resilience than SRB flocs against varying pHs and HRTs. Thus, SRB-mediated biological process, especially SRB granules, could be a promising biotechnology to remove SMX from wastewaters.

Qiu LQ ，Zhang L ，Tang K ，Chen G ，Kumar Khanal S ，Lu H ... -  《-》

Insights into pharmaceuticals removal in an anaerobic sulfate-reducing bacteria sludge system.

In this study, we examined eight typical and widely detected pharmaceuticals (PhAs) removal in an anaerobic sulfate-reducing bacteria (SRB) sludge system (five antibiotics: sulfadiazine (SD), sulfamethoxazole (SMX), trimethoprim (TMP), ciprofloxacin (CIP) and enoxacin (ENO), and three nonsteroidal anti-inflammatory drugs (NSAIDs): ibuprofen (IBU), ketoprofen (KET) and diclofenac (DIC)). The results showed that the SRB sludge had the higher removal efficacy (20 to 90%) for antibiotics (SD, SMX, TMP, CIP and ENO) than NSAIDs (<20%) via adsorption and biodegradation under different operating conditions. Based on a series of batch studies, fluoroquinolone antibiotics (CIP and ENO) were instantly (<15 min) removed (∼98%) via adsorption on SRB sludge with adsorption coefficient (Kd) as high as 25.3 ± 1.8 L/g-suspended solids (SS). And thermodynamics results indicated that the adsorption of CIP and ENO on SRB sludge was spontaneous (Gibbs free energy change (ΔG°) <0 kJ/mol), exothermic (enthalpy change (ΔH°) <0 kJ/mol), and the adsorption process involved both physisorption and chemisorption (absolute value of ΔH° = 20 to 80 kJ/mol). Three widely prescribed antibiotics (SMX, TMP and CIP) were further investigated for their possible biodegradation pathways along with functional enzymes involved through a series of batch experiments. The biotransformation intermediates indicated that biotransformations of SMX and CIP in SRB sludge system could be initiated from the cleavage of isoxazole and piperazinyl rings catalyzed by sulfite reductase (SR) and cytochrome P450 (CYP450) enzymes, respectively. TMP was likely biotransformed via O-demethylation and N-acetylation coupled with hydroxylation reactions with CYP450 enzymes as the main functional enzymes. This study provided new insight into PhAs removal in SRB sludge system, and has significant potential of implementing sulfur-mediated biological process for the treatment of PhAs containing wastewater.

Jia Y ，Zhang H ，Khanal SK ，Yin L ，Lu H ... -  《-》

Characterization of sulfate-reducing granular sludge in the SANI(®) process.

Hong Kong practices seawater toilet flushing covering 80% of the population. A sulfur cycle-based biological nitrogen removal process, the Sulfate reduction, Autotrophic denitrification and Nitrification Integrated (SANI(®)) process, had been developed to close the loop between the hybrid water supply and saline sewage treatment. To enhance this novel process, granulation of a Sulfate-Reducing Up-flow Sludge Bed (SRUSB) reactor has recently been conducted for organic removal and provision of electron donors (sulfide) for subsequent autotrophic denitrification, with a view to minimizing footprint and maximizing operation resilience. This further study was focused on the biological and physicochemical characteristics of the granular sulfate-reducing sludge. A lab-scale SRUSB reactor seeded with anaerobic digester sludge was operated with synthetic saline sewage for 368 days. At 1 h nominal hydraulic retention time (HRT) and 6.4 kg COD/m(3)-d organic loading rate, the SRUSB reactor achieved 90% COD and 75% sulfate removal efficiencies. Granular sludge was observed within 30 days, and became stable after 4 months of operation with diameters of 400-500 μm, SVI5 of 30 ml/g, and extracellular polymeric substances of 23 mg carbohydrate/g VSS. Fluorescence in situ hybridization (FISH) analysis revealed that the granules were enriched with abundant sulfate-reducing bacteria (SRB) as compared with the seeding sludge. Pyrosequencing analysis of the 16S rRNA gene in the sulfate-reducing granules on day 90 indicated that the microbial community consisted of a diverse SRB genera, namely Desulfobulbus (18.1%), Desulfobacter (13.6%), Desulfomicrobium (5.6%), Desulfosarcina (0.73%) and Desulfovibrio (0.6%), accounting for 38.6% of total operational taxonomic units at genera level, with no methanogens detected. The microbial population and physicochemical properties of the granules well explained the excellent performance of the granular SRUSB reactor.

Hao T ，Wei L ，Lu H ，Chui H ，Mackey HR ，van Loosdrecht MC ，Chen G ... -  《-》

Biological conversion of sulfamethoxazole in an autotrophic denitrification system.

Sulfamethoxazole (SMX) is a common antibiotic prescribed for treating infections, which is frequently detected in the effluent of conventional wastewater treatment plants (WWTPs). Its degradation and conversion in a laboratory-scale sulfur-based autotrophic denitrification reactor were for the first time investigated through long-term reactor operation and short-term batch experiments. Co-metabolism of SMX and nitrate by autotrophic denitrifiers was observed in this study. The specific SMX removal rate was 3.7 ± 1.4 μg/g SS-d, which was higher than those reported in conventional wastewater treatment processes. The removal of SMX by the enriched denitrifying sludge was mainly attributed to biodegradation. Four transformation products (three known with structures and one with unknown structure) were identified, of which the structures of the two transformation products (TPs) were altered in the isoxazole ring. Additionally, the presence of SMX significantly shaped the microbial community structures, leading to the dominant denitrifier shifting from Sulfuritalea to Sulfurimonas to maintain the stability of system. Collectively, the sulfur-based autotrophic denitrification process could effectively remove SMX in addition to efficient nitrate removal, and further polish the effluent from conventional WWTPs.

Zhang L ，Sun F ，Wu D ，Yan W ，Zhou Y ... -  《-》