Biodegradation Of Sulfamethoxazole Research Articles

Unveiling the influence of microaeration and sludge recirculation on enhancement of pharmaceutical removal and microbial community change of the novel anaerobic baffled biofilm - membrane bioreactor in treating building wastewater

This research aims to conduct a comparative investigation of the role played by microaeration and sludge recirculation in the novel anaerobic baffled biofilm-membrane bioreactor (AnBB-MBR) for enhancing pharmaceutical removal from building wastewater. Three AnBB-MBRs — R1: AnBB-MBR, R2: AnBB-MBR with microaeration and R3: AnBB-MBR with microaeration and sludge recirculation — were operated simultaneously to remove Ciprofloxacin (CIP), Caffeine (CAF), Sulfamethoxazole (SMX) and Diclofenac (DCF) from real building wastewater at the hydraulic retention time (HRT) of 30 h for 115 days. From the removal profiles of the targeted pharmaceuticals in the AnBB-MBRs, it was found that the fixed-film compartment (C1) could significantly reduce the targeted pharmaceuticals. The remaining pharmaceuticals were further removed with the microaeration compartment. R2 exhibited the utmost removal efficiency for CIP (78.0 %) and DCF (40.8 %), while SMX was removed most successfully by R3 (microaeration with sludge recirculation) at 91.3 %, followed by microaeration in R2 (88.5 %). For CAF, it was easily removed by all AnBB-MBR systems (>90 %). The removal mechanisms indicate that the microaeration in R2 facilitated the adsorption of CIP onto microaerobic biomass, while the enhanced biodegradation of CAF, SMX and DCF was confirmed by batch biotransformation kinetics and the adsorption isotherms of the targeted pharmaceuticals. The microbial groups involved in biodegradation of the targeted compounds under microaeration were identified as nitrogen removal microbials (Nitrosomonas, Nitrospira, Thiobacillus, and Denitratisoma) and methanotrophs (Methylosarcina, Methylocaldum, and Methylocystis). Overall, explication of the integration of AnBB-MBR with microaeration (R2) confirmed it as a prospective technology for pharmaceutical removal from building wastewater due to its energy-efficient approach characterized by minimal aeration supply.

Reduced graphene oxide promotes the biodegradation of sulfamethoxazole by white-rot fungus Phanerochaete chrysosporium under cadmium stress

The biodegradation of antibiotics in aquatic environment is consistently impeded by the widespread presence of heavy metals, necessitating urgent measures to mitigate or eliminate this environmental stress. This work investigated the degradation of sulfamethoxazole (SMX) by the white-rot fungus Phanerochaete chrysosporium (WRF) under heavy metal cadmium ion (Cd2+) stress, with a focus on the protective effects of reduced graphene oxide (RGO). The pseudo-first-order rate constant and removal efficiency of 5 mg/L SMX in 48 h by WRF decrease from 0.208 h−1 and 55.6% to 0.08 h−1 and 28.6% at 16 mg/L of Cd2+, while these values recover to 0.297 h−1 and 72.8% by supplementing RGO. The results demonstrate that RGO, possessing excellent biocompatibility, effectively safeguard the mycelial structure of WRF against Cd2+ stress and provide protection against oxidative damage to WRF. Simultaneously, the production of manganese peroxidase (MnP) by WRF decreases to 38.285 U/L in the presence of 24 mg/L Cd2+, whereas it recovers to 328.51 U/L upon the supplement of RGO. RGO can induce oxidative stress in WRF, thereby stimulating the secretion of laccase (Lac) and MnP to enhance the SMX degradation. The mechanism discovered in this study provides a new strategy to mitigate heavy metal stress encountered by WRF during antibiotic degradation.

Enhanced biodegradation of sulfamethoxazole by pyrogenic carbon derived from aquacultural waste sludge

Sulfamethoxazole (SMX) is a widely utilized antibiotic that exhibits a broad spectrum of antibacterial activity, but its inadvertent release into the environment poses a significant threat to human society. The inefficacy of SMX degradation in microbial pipelines constantly challenges the regulation of antibiotics, making it a pressing and compelling concern. Former research has demonstrated the enhancement of the waste sludge-derived materials on SMX biodegradation, but the impact of these materials on microbial behavior remains unclear. In this study, two pyrogenic carbon materials (FBC and RBC) were prepared from aquacultural waste sludge and its downstream river sediment, respectively, to collaborate with SMX degrading species, Alcaligenes sp., for highly efficient removal of SMX. The cells of Alcaligenes sp. successfully colonized onto the biocompatible surface of the materials, and this hybrid structure nearly doubled the SMX degradation efficiency of the group without the carbon materials. The transcriptome analysis revealed that the existence of carbon materials significantly upregulated the expression of SMX degrading-related genes, including metCF and paaCIK, which led to bond breaking and benzene ring breakdown for the degradation of sulfamethoxazole. This work provides new insights into the mechanisms and environmental significance of SMX degradation by microbial immobilization onto waste-derived carbon-rich materials.

Enzyme-induced reactive oxygen species trigger oxidative degradation of sulfamethoxazole within a methanotrophic biofilm

Although microorganisms carrying copper-containing membrane-bound monooxygenase (CuMMOs), such as particulate methane monooxygenase (pMMO) and ammonia monooxygenase (AMO), have been extensively documented for their capability to degrade organic micropollutants (OMPs), the underlying reactive mechanism remains elusive. In this study, we for the first time demonstrate biogenic reactive oxygen species (ROS) play important roles in the degradation of sulfamethoxazole (SMX), a representative OMP, within a methane-fed biofilm. Highly-efficient and consistent SMX biodegradation was achieved in a CH4-based membrane biofilm reactor (MBfR), manifesting a remarkable SMX removal rate of 1210.6 ± 39.0 μg·L−1·d−1. Enzyme inhibition and ROS clearance experiments confirmed the significant contribution of ROS, which were generated through the catalytic reaction of pMMO and AMO enzymes, in facilitating SMX degradation. Through a combination of density functional theory (DFT) calculations, electron paramagnetic resonance (EPR) analysis, and transformation product detection, we elucidated that the ROS primarily targeted the aniline group in the SMX molecule, inducing the formation of aromatic radicals and its progressive mineralization. In contrast, the isoxazole-ring was not susceptible to electrophilic ROS attacks, leading to accumulation of 3-amino-5-methylisoxazole (3A5MI). Furthermore, microbiological analysis suggested Methylosarcina (a methanotroph) and Candidatus Nitrosotenuis (an ammonia-oxidizing archaea) collaborated as the SMX degraders, who carried highly conserved and expressed CuMMOs (pMMO and AMO) for ROS generation, thereby triggering the oxidative degradation of SMX. This study deciphers SMX biodegradation through a fresh perspective of free radical chemistry, and concurrently providing a theoretical framework for the advancement of environmental biotechnologies aimed at OMP removal.

Comprehensive assessment of toxicity and environmental risk associated with sulfamethoxazole biodegradation in sulfur-mediated biological wastewater treatment

Incomplete mineralization of sulfamethoxazole (SMX) in wastewater treatment systems poses a threat to ecological health. The toxicity and environmental risk associated with SMX biodegradation in the sulfur-mediated biological process were examined for the first time through a long-term (180 days) bioreactor study and a series of bioassays. The results indicated that the sulfur-mediated biological system was highly resistant and tolerant to SMX toxicity, as evidenced by the enrichment of sulfate-reducing bacteria (SRB), the improved microbial metabolic activity, and the excellent performance on pollutants removal under long-term SMX exposure. SMX can be effectively biodegraded by the cleavage and rearrangement of the isoxazole ring, hydrogenation and hydroxylation reactions in sulfur-mediated biological wastewater system. These biodegradation pathways effectively reduced the acute toxicity, antibacterial activity, and ecotoxicities of SMX and its biotransformation products (TPs) in the effluent of the sulfur-mediated biological system. The TPs produced via hydrogenation (TP1), hydroxylation, and isoxazole ring cleavage (TP3, TP4, TP5, TP8, and TP9) exhibited lower toxicity than SMX. Under SMX stress, although the abundance of sulfonamide resistance genes increased, the total abundance of ARGs decreased due to the extrusion of some intracellular SMX by the efflux pump genes and the inactivation of some SMX through the biodegradation process. Efflux pump and inactivation, as the main resistance mechanisms of antibiotics in the sulfur-mediated biological system, play a crucial role in microbial self-defense. The findings of this study demonstrate the great potential of the sulfur-mediated biological system in SMX removal, detoxication, and ARGs environmental risk reduction.

Composting post-anaerobic digestion for emerging contaminant biodegradation: Impacts of operating conditions.

Sustainable manure management technologies are needed, and combining anaerobic digestion (AD) for energy generation and aerobic composting (AC) to stabilize digestate and remove emerging contaminants (ECs), including veterinary pharmaceuticals and steroid hormones, is promising. This study identified post-AD, AC operating conditions that maximized degradation of study ECs, expected to be present in cattle manure digested using treated municipal wastewater as the water source. Study ECs included sulfamethoxazole (SMX), chlortetracycline (CTC), oxytetracycline (OTC), estrone (E1), and naproxen (NPX). Composting conditions were simulated in bench-scale reactors, with microorganisms from digestate produced in an AD system (25L scale), by varying temperatures, pH, and carbon source compositions (representing food waste/manure co-digestion with different residence times). Results indicate maximum SMX biodegradation occurred at 35°C, pH 7, and with high levels of easily degradable carbon (≥99%, 99%, and 98%), and maximum E1 biodegradation occurred at 35°C, and with low levels of easily degradable carbon (≥97% and 99%). Abiotic degradation was responsible for the nearly complete removal of tetracyclines under all conditions and for partial degradation of NPX (between 20% and 48%). Microorganisms originating from the AD system putatively capable of SMX and E1 biodegradation, or of contributing to biodegradation during the AC phase, were identified, including phylotypes previously shown to biodegrade SMX (Brevundimonas and Alcaligenes).

The role of biochar and green compost amendments in the adsorption, leaching, and degradation of sulfamethoxazole in basic soil

The fate of the antibiotic sulfamethoxazole in amended soils remains unclear, moreover in basic soils. This work aimed to assess the adsorption, leaching, and biodegradation of sulfamethoxazole in unamended and biochar from holm oak pruning (BC)- and green compost from urban pruning (CG)-amended basic soil. Adsorption properties of the organic amendments and soil were determined by adsorption isotherms of sulfamethoxazole. The leachability of this antibiotic from unamended (Soil) and BC- (Soil + BC) and GC- (Soil + GC) amended soil was determined by leaching columns using water as solvent up to 250 mL. Finally, Soil, Soil + BC, and Soil + GC were spiked with sulfamethoxazole and incubated for 42 days. The degradation rate and microbial activity were periodically monitored. Adsorption isotherms showed poor adsorption of sulfamethoxazole in unamended basic soil. BC and CG showed good adsorption capacity. Soil + BC and Soil + GC increased the sulfamethoxazole adsorption capacity of the soil. The low sulfamethoxazole adsorption of Soil produced quick and intense sulfamethoxazole leaching. Soil + BC reduced the sulfamethoxazole leaching, unlike to Soil + GC which enhanced it concerning Soil. The pH of adsorption isotherms and leachates indicate that the anion of sulfamethoxazole was the major specie in unamended and amended soil. CG enhanced the microbial activity of the soil and promoted the degradability of sulfamethoxazole. In contrast, the high adsorption and low biostimulation effect of BC in soil reduced the degradation of sulfamethoxazole. The half-life of sulfamethoxazole was 2.6, 6.9, and 11.9 days for Soil + GC, Soil, and Soil + BC, respectively. This work shows the benefits and risks of two organic amendments, BC and GC, for the environmental fate of sulfamethoxazole. The different nature of the organic carbon of the amendments was responsible for the different effects on the soil.

Magnetic biochar derived from peanut shells facilitates antibiotic degradation and fouling control in anaerobic membrane bioreactor for antibiotic pharmaceutical wastewater treatment

Anaerobic membrane bioreactor is an attractive option for antibiotic pharmaceutical wastewater treatment, but the unsatisfied treatment performance and membrane fouling issue hindered its wide application. Herein, magnetic biochar (MBC) derived from peanut shells was added to AnMBR for synthetic pharmaceutical wastewater treatment containing sulfamethoxazole (SMX). The results indicated that the treatment performance was improved with 80 % of COD and over 90 % of SMX removal. This can be explained by the adsorption capacity of MBC and improved microbial activity due to the direct interspecies electron transfer enhancement with MBC addition. Membrane fouling was also alleviated due to the adsorption and magnetic bio-effect of MBC, leading to the reduced soluble microbial product (SMP) (22.2 to 6.3 mg/gVSS) and extracellular polymer substance (EPS) concentration (18.9 to 14.2 mg/gVSS), and enlarged particle size (60.6 to 113.4 μm). Microbial diversity analyses indicated that hydrolysis and acidogenesis bacteria (Bacteroidetes and Choloflexi phyla), methanogenic archaea (Methanobacterium and Methanosaeta), and bacteria related to electron transfers (unclassified_f_Geobacteraceae) were enriched due to the presence of MBC. Additionally, the SMX plausible biotransformation pathway and removal mechanism further validated that MBC addition can improve the SMX biodegradation and biotranformation. Importantly, the MBC addition facilitates antibiotic degradation and fouling alleviation of AnMBR, which makes AnMBR a more attractive choice treating for antibiotic pharmaceutical wastewater.

FDH/Hases-S-chain mediated electron redistributing in Citrobacter freundii JH@FeS during degradation of sulfamethoxazole and nitrate

Considering the negligent degradation of sulfamethoxazole (SMX) by Citrobacter freundii JH, the incorporation of bio-FeS could initiate the SMX biodegradation to 0.0444 (S-FeS), and further to 0.0564 mg L−1 mg−1 protein d−1 (SN-FeS) when coexisted with nitrate. Electrochemical (LSV, I-t, DPV, EIS and EDC) and respiratory inhibition experiments clarified that the bio-FeS could greatly switch/redistribute electron transmembrane-transfer from intracellular to extracellular mainly via FDH/Hases-S-chain, as revealed by the significant increase of ipa-FDH/Hases/ipa-FC-Cyts and ipc-FDH/Hases/ipc-FC-Cyts (from 1.09 and 1.07 (SN-native) to 1.50 and 3.58 (SN-FeS)), while nitrate (linear fitting with NADH (R2 = 0.9903)) mainly intensified CoQ-L-chain related INET from Complex I to CoQ to compensate for the electronic competition with SMX. SN-FeS system detoxified the SMX on microbial metabolism (such as membrane rupture and oxidative stress induction) with high SOD activity (737.93 U gFW−1). Structural equation modeling indicated that bio-FeS up-regulated PMF-mediated ATP synthesis (PPMF-ATPs from 0.12 (SN-native) to 0.74 (SN-FeS)) and PMF-mediated NADH (PPMF-NADH from -0.72 (SN-native) to 0.63 (SN-FeS)), and the nitrate addition intensified this positive feedback. Overall, this study provides a new perspective for bionanoparticles via electron transfer/redistribution to detoxify and launch the antibiotics biodegradation in ecological environment.

The sulfonamide-resistance dihydropteroate synthase gene is crucial for efficient biodegradation of sulfamethoxazole by Paenarthrobacter species.

Sulfonamide antibiotics (SAs) are serious pollutants to ecosystems and environments. Previous studies showed that microbial degradation of SAs such as sulfamethoxazole (SMX) proceeds via a sad-encoded oxidative pathway, while the sulfonamide-resistant dihydropteroate synthase gene, sul, is responsible for SA resistance. However, the co-occurrence of sad and sul genes, as well as how the sul gene affects SMX degradation, was not explored. In this study, two SMX-degrading bacterial strains, SD-1 and SD-2, were cultivated from an SMX-degrading enrichment. Both strains were Paenarthrobacter species and were phylogenetically identical; however, they showed different SMX degradation activities. Specifically, strain SD-1 utilized SMX as the sole carbon and energy source for growth and was a highly efficient SMX degrader, while SD-2 did could not use SMX as a sole carbon or energy source and showed limited SMX degradation when an additional carbon source was supplied. Genome annotation, growth, enzymatic activity tests, and metabolite detection revealed that strains SD-1 and SD-2 shared a sad-encoded oxidative pathway for SMX degradation and a pathway of protocatechuate degradation. A new sulfonamide-resistant dihydropteroate synthase gene, sul918, was identified in strain SD-1, but not in SD-2. Moreover, the lack of sul918 resulted in low SMX degradation activity in strain SD-2. Genome data mining revealed the co-occurrence of sad and sul genes in efficient SMX-degrading Paenarthrobacter strains. We propose that the co-occurrence of sulfonamide-resistant dihydropteroate synthase and sad genes is crucial for efficient SMX biodegradation. KEY POINTS: • Two sulfamethoxazole-degrading strains with distinct degrading activity, Paenarthrobacter sp. SD-1 and Paenarthrobacter sp. SD-2, were isolated and identified. • Strains SD-1 and SD-2 shared a sad-encoded oxidative pathway for SMX degradation. • A new plasmid-borne SMX resistance gene (sul918) of strain SD-1 plays a crucial role in SMX degradation efficiency.

Role of biochar-derived DOM compositions in enhanced biodegradation of sulfamethoxazole and chloramphenicol

In the study, we investigated the different compositions of biochar-derived dissolved organic matter (BDOM) that play a key role in the biodegradation of sulfamethoxazole (SMX) and chloramphenicol (CAP) by P. stutzeri and S. putrefaciens, and found that aliphatic compounds in Group 4, fulvic acid like in Region III, and solid microbial byproduct like in region IV are key common factors. The growth and antibiotic degradation efficiency of P. stutzeri and S. putrefaciens are positively correlated with the content of Group 4 and Region III, and negatively correlated with Region IV. This is consistent with the optimal biodegradation results of BDOM700 with the highest content of Group 4 and Region III. Additionally, the degradation efficiency of SMX by Pseudomonas stutzeri is negatively correlated with the percentage of polycyclic aromatics in Group 1, but not with CAP. Similarly, the percentage of fatty acids in S. putrefaciens was positively correlated with Group 1, whereas P. stutzeri did not. This indicates that some components of BDOM have varying effects on different bacteria or types of antibiotics. This study provides new insights into enhancing antibiotic biodegradation by controlling the composition of BDOM.

Combined use of strictly anaerobic MBBR and aerobic MBR for municipal wastewater treatment and removal of pharmaceuticals

An integrated lab-scale wastewater treatment system consisting of an anaerobic Moving Bed Biofilm Reactor (AnMBBR) and an aerobic Membrane Bioreactor (AeMBR) in series was used to study the removal and fate of pharmaceuticals during wastewater treatment. Continuous-flow experiments were conducted applying different temperatures to the AnMBBR (Phase A: 35 °C; Phase B: 20 °C), while batch experiments were performed for calculating sorption and biotransformation kinetics. The total removal of major pollutants and target pharmaceuticals was not affected by the temperature of the AnMBBR. In Phase A, the average removal of dissolved chemical oxygen demand (COD), biological oxygen demand (BOD), and ammonium nitrogen (NH4–N) was 86%, 91% and 96% while in Phase B, 91%, 96% and 96%, respectively. Removal efficiencies ranging between 65% and 100% were observed for metronidazole (MTZ), trimethoprim (TMP), sulfamethoxazole (SMX), and valsartan (VAL), while slight (<30%) or no removal was observed for carbamazepine (CBZ) and diclofenac (DCF), respectively. Application of a mass balance model showed that the predominant mechanism for the removal of pharmaceuticals was biotransformation, while the role of sorption was of minor importance. The AeMBR was critical for VAL, SMX and TMP biodegradation; the elimination of MTZ was strongly enhanced by the AnMBBR. In both bioreactors, Bacteroidetes was the dominant phylum in both bioreactors over time. In the AnMBBR, Cloacibacterium and Bacteroides had a higher abundance in the biocarriers compared to the suspended biomass.

Methanotrophic oxidation of organic micropollutants and nitrogen upcycling in a hybrid membrane biofilm reactor (hMBfR) for simultaneous O2 and CH4 supply

Pharmaceuticals and other organic micropollutants (OMPs) present in wastewater effluents are of growing concern, as they threaten environmental and human health. Conventional biological treatments lead to limited removal of OMPs. Methanotrophic bacteria can degrade a variety of OMPs. By employing a novel bubble-free hybrid membrane biofilm bioreactor (hMBfR), we grew methanotrophic bacteria at three CH4 loading rates. Biomass productivity and CH4 loading showed a linear correlation, with a maximum productivity of 372 mg-VSS·L−1·d−1, with corresponding biomass concentration of 1117.6 ± 56.4 mg-VSS·L−1. Furthermore, the biodegradation of sulfamethoxazole and 1H-benzotriazole positively correlated with CH4 oxidation rates, with highest biodegradation kinetic constants of 3.58 L·g−1·d−1 and 5.42 L·g−1·d−1, respectively. Additionally, the hMBfR recovered nutrients as microbial proteins, with an average content 39% DW. The biofilm community was dominated by Methylomonas, while the bulk was dominated by aerobic heterotrophic bacteria. The hMBfR removed OMPs, allowing for safer water reuse while valorising CH4 and nutrients.

Metabolite Cross-Feeding Promoting NADH Production and Electron Transfer during Efficient SMX Biodegradation by a Denitrifier and S. oneidensis MR-1 in the Presence of Nitrate.

Antibiotics often coexist with other pollutants (e.g., nitrate) in an aquatic environment, and their simultaneous biological removal has attracted widespread interest. We have found that sulfamethoxazole (SMX) and nitrate can be efficiently removed by the coculture of a model denitrifier (Paracoccus denitrificans, Pd) and Shewanella oneidensis MR-1 (So), and SMX degradation is affected by NADH production and electron transfer. In this paper, the mechanism of a coculture promoting NADH production and electron transfer was investigated by proteomic analysis and intermediate experiments. The results showed that glutamine and lactate produced by Pd were captured by So to synthesize thiamine and heme, and the released thiamine was taken up by Pd as a cofactor of pyruvate and ketoglutarate dehydrogenase, which were related to NADH generation. Additionally, Pd acquired heme, which facilitated electron transfer as heme, was the important composition of complex III and cytochrome c and the iron source of iron sulfur clusters, the key component of complex I in the electron transfer chain. Further investigation revealed that lactate and glutamine generated by Pd prompted So chemotactic moving toward Pd, which helped the two bacteria effectively obtain their required substances. Obviously, metabolite cross-feeding promoted NADH production and electron transfer, resulting in efficient SMX biodegradation by Pd and So in the presence of nitrate. Its feasibility was finally verified by the coculture of an activated sludge denitrifier and So.

Biochar-derived dissolved organic matters influencing bacterium characteristics during biodegradation of sulfamethoxazole and chloramphenicol under alternation of visible and avoiding light

The influence of biochar-released dissolved organic matter (BDOM) on the transcription of gene (DEG) in Pseudomonas stutzeri and Shewanella putrefacien during sulfamethoxazole (SMX) and chloramphenicol (CAP) biodegradation under visible light was investigated in this study. The results indicated that BDOM components would be nutrients for bacterial amplification and growth under the culture conditions of xenon lamp irradiation and avoiding light, especially BDOM from low temperatures. Additionally, visible light irradiation would improve the saturated fatty acid by stimulating the cell membrane of the microorganism, thus promoting the biodegradation of antibiotics through altering P. stutzeri and S. putrefaciens reoxidative and catabolism processes and significantly inhabiting the copy number of their genes. Moreover, the upregulated genes and enzymes related to SMX and CAP-metabolic and catabolic processes were enriched, which were involved in the pathways of biodegradation, further improving biodegradation efficiency. In particular, interaction network analysis between the top 100 dominant functional genes from P. stutzeri and S. putrefaciens and the molecular types of BDOM, e.g., CHO, CHON, and CHOS (p < 0.05), indicated that the genes of molecular function showed a high positive or negative correlation with the CHO type of BDOM. The results revealed that the CHO type of BDOM affected the functional genes of molecular function, cellular component, and biological process from P. stutzeri and S. putrefaciens, influencing the biodegradation of SMX and CAP. This study provided an basis for BDOM playing a role in antibiotic removal from the aqueous solution using biochar combined with photobiodegradation.Graphical

Characterization and shifting of microbial community to denitrification for anaerobic sulfamethoxazole biodegradation with different electron acceptors

This study investigated the interaction between function microbiota succession and three electron acceptors in anaerobic sulfamethoxazole (SMX) degradation. Over 20%–60% SMX was degraded biologically after antibiotics acclimation under co-electron acceptors. Under sulfate- and nitrate-reducing conditions, SMX removal followed a pseudo-zero-order kinetic model and related to the sludge adsorption site. Microbiological analyses showed syntrophic community, including autotrophic denitrifiyer, nitrate reducing-sulfate oxidizier, and heterotrophic denitrifier, were putative SMX reducers. As an electron acceptor, sulfate was more beneficial in degrading SMX and maintaining the system stability and the colony structure. However, autotrophic nitrate-reducing sulfate-oxidizing bacteria has a stronger substrate competition advantage than sulfate-reducing bacteria (SRB), resulting in invalid SMX degradation. Thus, for the system start-up, SRB and iron/sulfur-based denitrifier should be preferentially enriched with sulfate electron acceptors to assure the removals of antibiotics. These results uncovered crucial factors that may affect the fate of SMX and associated biochemicals in anaerobic degradation processes but were previously overlooked.

Analysis of the Comparative Growth Kinetics of Paenarthrobacter ureafaciens YL1 in the Biodegradation of Sulfonamide Antibiotics Based on Substituent Structures and Substrate Toxicity

The high consumption and emission of sulfonamide antibiotics (SAs) have a considerable threat to humans and ecosystems, so there is a need to develop safer and more effective methods than conventional strategies for the optimal removal of these compounds. In this study, four SAs with different substituents, sulfadiazine (SDZ), sulfamerazine (SMR), sulfamethoxazole (SMX), and sulfamethazine (SMZ) were removed by a pure culture of Paenarthrobacter ureafaciens YL1. The effect of the initial SAs concentration on the growth rate of strain YL1 was investigated. The results showed that the strain YL1 effectively removed various SAs in the concentration range of 0.05–2.4 mmol·L−1. The Haldane model was used to perform simulations of the experimental data, and the regression coefficient of the model indicated that the model had a good predictive ability. During SAs degradation, the maximum specific growth rate of strain YL1 was ranked as SMX &gt; SDZ &gt; SMR &gt; SMZ with constants of 0.311, 0.304, 0.302, and 0.285 h−1, respectively. In addition, the biodegradation of sulfamethoxazole (SMX) with a five-membered substituent was the fastest, while the six-membered substituent of SMZ was the slowest based on the parameters of the kinetic equation. Also, density functional theory (DFT) calculations such as frontier molecular orbitals (FMOs), and molecular electrostatic potential map analysis were performed. It was evidenced that different substituents in SAs can affect the molecular orbital distribution and their stability, which led to the differences in the growth rate of strain YL1 and the degradation rate of SAs. Furthermore, the toxicity of P. ureafaciens is one of the crucial factors affecting the biodegradation rate: the more toxic the substrate and the degradation product are, the slower the microorganism grows. This study provides a theoretical basis for effective bioremediation using microorganisms in SAs-contaminated environments.

Biotransformation of sulfamethoxazole by microalgae: Removal efficiency, pathways, and mechanisms

Recently, the biotransformation of sulfamethoxazole (SMX) by microalgae has attracted increasing interest. In particular, cytochrome P450 (CYP450) has been suggested to be the main enzymatic contributor to this biodegradation. However, the molecular evidence of CYP450 enzymes being involved in SMX biodegradation remains relatively unclear, hindering its applicability. Herein, the biodegradation of SMX by Chlorella sorokiniana (C. sorokiniana) was investigated, and comprehensively elucidated the reaction mechanism underlying CYP450-mediated SMX metabolism. C. sorokiniana was able to efficiently remove over 80% of SMX mainly through biodegradation, in which CYP450 enzymes responded substantially to metabolize SMX in cells. Additionally, screening of transformation products (TPs) revealed that N4-hydroxylation-SMX (TP270) was the main TP in the SMX biodegradation pathway of microalgae. Molecular dynamics (MD) simulation suggested that the aniline of SMX was the most prone to undergo metabolism, while density functional theory (DFT) indicated that SMX was metabolized by CYP450 enzymes through H-abstraction-OH-rebound reaction. Collectively, this work reveals key details of the hydroxylamine group of SMX, elucidates the SMX biodegradation pathway involving CYP450 in microalgae in detail, and accelerates the development of using microalgae-mediated CYP450 to eliminate antibiotics.

New biotransformation pathways from sulfamethoxazole and ciprofloxacin removal in sewage treatment along the spatial profile of an anaerobic fixed bed bioreactor

In this work, the biotransformation products (BTPs) from the removal of the antibiotics sulfamethoxazole (SMX) and ciprofloxacin (CIP) were assessed for the first time in an anaerobic packed bed biofilm reactor (APBBR) treating municipal sewage. Anaerobic batch assays at high concentrations of the antibiotics (5 mg·L−1) were performed to identify the BTPs generated during the SMX and CIP biodegradation. From the mass transitions of the identified BTPs, they were analyzed along the spatial profile of the APBBR fed with sewage (400 ngSMX·L−1 and 300 ngCIP·L−1). Three BTPs were identified: m/z 256 and m/z 270 from SMX, and m/z 316 from CIP. The molecular structures of the BTPs revealed that SMX biotransformation occurs in the isoxazole ring and a dehydroxylation in the CIP molecule. This study showed new biotransformation pathways of SMX and CIP during anaerobic digestion, contributing to the understanding of the fate of these pharmaceutical compounds in the environment.

Biological removal of sulfamethoxazole enhanced by S. oneidensis MR-1 via promoting NADH generation and electron transfer and consumption

The bio-removal efficiency of sulfamethoxazole (SMX) from wastewater is usually very poor. In this paper a new efficient method to biodegrade SMX was reported. The SMX biodegradation efficiency by Paracoccus denitrificans was observed to be remarkably enhanced from 48.9% to 94.2% after Shewanella oneidensis MR-1 addition. The mechanisms investigation revealed that P. denitrificans was the dominant microbe for SMX biodegradation. Although SMX biodegradation by S. oneidensis MR-1 alone was negligible, its presence advanced NADH generation. The proteomics assay revealed that the expression of key proteins relevant with complex I and III and cytochrome c in electron transfer chain were increased due to P. denitrificans acquiring iron from periplasm to cytoplasm being improved. In addition, the extracellular electron transfer capability was enhanced as S. oneidensis MR-1 not only produced flavin, but caused P. denitrificans to secret more extracellular polymeric substances. Further investigation indicated that the expression of key enzymes related to electron consumption in SMX biodegradation was up-regulated. Based on these findings, the pathways of S. oneidensis MR-1 promoting SMX biodegradation were proposed. As all nitrate could be removed with almost no nitrite accumulation, this study would also provide an attractive way for simultaneous bio-removal of multiple pollutants from wastewater.