Insights into the efficient mineralization of antibiotic trimethoprim in aqueous media by Fe2+ catalytically enhanced vacuum-UV irradiation: Kinetics, mechanisms, and toxicity evaluation.

The widespread existence of antibiotics in the environment has attracted growing concerns regarding the potential adverse effects on aquatic organisms, ecosystems, and human health even at low concentrations. Extensive efforts have been devoted to developing new methods for effective elimination of antibiotics from wastewater. Herein, a novel process of Fe2+ catalytically enhanced vacuum ultraviolet (VUV) irradiation was proposed as a promising approach for the removal of antibiotic trimethoprim (TMP) in water. Compared with UVC photolysis, VUV photolysis, and UVC/Fe2+, VUV/Fe2+ could increase the pseudo-first-order reaction rate constant of TMP removal by 6.6-38.4 times and the mineralization rate by 36.5%-59.9%. The excellent performance might originate from the synergistic effect of VUV and Fe2+, i.e., VUV irradiation could effectively split water and largely accelerate the Fe3+/Fe2+ cycle to generate more reactive oxygen species (ROS). EPR results indicated that •OH and O2•- were identified as the main ROS in the UVC/Fe2+ and VUV/Fe2+ processes, while •OH, O2•-, and 1O2 were involved in the VUV process. The operating parameters, such as Fe2+ dosage and initial TMP contents, were evaluated and optimized. Up to 8 aromatic intermediates derived from hydroxylation, demethylation, carbonylation, and methylene group cleavage were identified by UPLC-QTOF-MS/MS technique, the possible pathways of TMP degradation were proposed. Finally, the acute and chronic toxicity of intermediates formed during TMP degradation in the VUV/Fe2+ process were also evaluated.

Heterogeneous activation of self-generated H2O2 by Pd@UiO-66(Zr) for trimethoprim degradation: Efficiency and mechanism.

The Fenton reaction is recognized as an effective technique for degrading persistent organic pollutants, such as the emerging pollutant trimethoprim (TMP). Recently, due to the excellent reducibility of active hydrogen ([H]), Pd-H2 has been preferred for Fenton-like reactions and the specific H2 activation of Pd-based catalysts. Herein, a heterogeneous Fenton catalyst named the hydrogen-accelerated oxygen reduction Fenton (MHORF@UiO-66(Zr)) system was prepared through the strategy of building ships in the bottle. The [H] has been used for the acceleration of the reduction of Fe(III) and self-generate H2O2. The systematic characterization demonstrated that the nano Pd0 particle was highly dispersed into the UiO-66(Zr). The results found that 20 mg L-1 of TMP was thoroughly degraded within 90 min in the MHORF@UiO-66(Zr) system under conditions of initial pH 3, 30 mL min-1 H2, 2 g L-1 Pd@UiO-66(Zr) and 25 µM Fe2+. The hydroxyl radical as well as the singlet oxygen were evidenced to be the main reactive oxygen species by scavenging experiments and electron spin resonance. In addition, both reducing Fe(III) and self-generating H2O2 could be achieved due to the strong metal-support interaction (SMSI) between the nano Pd0 particles and UiO-66(Zr) confirmed by the correlation results of XPS and calculation of density functional theory. Finally, the working mechanism of the MHORF@UiO-66(Zr) system and the possible degradation pathway of the TMP have been proposed. The novel system exhibited excellent reusability and stability after six cyclic reaction processes.

Enhancing trimethoprim pollutant removal from wastewater using magnetic metal-organic framework encapsulated with poly (itaconic acid)-grafted crosslinked chitosan composite sponge: Optimization through Box-Behnken design and thermodynamics of adsorption parameters.

Trimethoprim (TMP), an antibiotic contaminant, can be effectively removed from water by using the innovative magnetic metal-organic framework (MOF) composite sponge Fe3O4@Rh-MOF@PIC, which is shown in this study. The composite is made up of magnetite (Fe3O4) nanoparticles and a rhodium MOF embedded in a poly(itaconic acid) grafted chitosan matrix. The structure and characteristics of the synthesized material were confirmed by thorough characterization employing SEM, FTIR, XPS, XRD, and BET techniques. Notably, the composite shows a high magnetic saturation of 64 emu g-1, which makes magnetic separation easier, according to vibrating sample magnetometry. Moreover, BET analysis revealed that the Fe3O4@Rh-MOF@PIC sponge had an incredibly high surface area of 1236.48 m2/g. Its outstanding efficacy was confirmed by batch adsorption tests, which produced a maximum adsorption capacity of 391.9 mg/g for the elimination of TMP. Due to its high porosity, magnetic characteristics, and superior trimethoprim uptake, this magnetic MOF composite sponge is a promising adsorbent for effective removal of antibiotics from contaminated water sources. An adsorption energy of 24.5 kJ/mol was found by batch investigations on the Fe3O4@Rh-MOF@PIC composite sponge for trimethoprim (TMP) adsorption. The fact that this value was up 8 kJ/mol suggests that the main mechanism controlling TMP absorption onto the sponge adsorbent is chemisorption. Chemisorption requires creating strong chemical interactions between adsorbate and adsorbent surface groups, unlike weaker physisorption. The magnetic composite sponge exhibited strong removal capabilities and high adsorption capacities for the antibiotic pollutant. The Fe3O4@Rh-MOF@PIC composite sponge also showed magnetism, which allowed for easy magnetic separation after adsorption. Over the course of 6 cycles, it showed outstanding reusability, and XRD confirmed that its composition was stable. The high surface area MOF's pore filling, hydrogen bonding, π-π stacking, and electrostatic interactions were the main trimethoprim adsorption mechanisms. This magnetic composite is feasible and effective for removing antibiotics from water because of its separability, reusability, and synergistic adsorption mechanisms via electrostatics, H-bonding, and π-interactions. The adsorption results were optimized using Box Behnken-design (BBD).

Migration and transformation behaviors of antibiotics in water-sediment system under simulated light and wind waves.

Antibiotics can generally be detected in the water-sediment systems of lakes. However, research on the migration and transformation of antibiotics in water-sediment systems based on the influences of light and wind waves is minimal. To address this research gap, we investigated the specific impacts of light and wind waves on the migration and transformation of three antibiotics, norfloxacin (NOR), trimethoprim (TMP), and sulfamethoxazole (SMX), under simulated light and wind waves disturbance conditions in a water-sediment system from Taihu Lake, China. In the overlying water, NOR was removed the fastest, followed by TMP and SMX. Compared to the no wind waves groups, the disturbance of big wind waves reduced the proportion of antibiotics in the overlying water. The contributions of light and wind waves to TMP and SMX degradation were greater than those of microbial degradation. However, the non-biological and biological contributions of NOR to degradation were almost equal. Wind waves had a significant impact on the microbial community changes in the sediment, especially in Methylophylaceae. These results verified the influence of light and wind waves on the migration and transformation of antibiotics, and provide assistance for the risk of antibiotic occurrence in water and sediments.

Trimethoprim-Based multicomponent solid Systems: Mechanochemical Screening, characterization and antibacterial activity assessment.

In this work, multicomponent trimethoprim-based pharmaceutical solid systems were developed by mechanochemistry, using coformers from the GRAS list and other active pharmaceutical ingredients. The choice of coformers took into account their potential to increase the aqueous solubility/dissolution rate of TMP or its antibacterial activity. All the binary systems were characterized by thermal analysis, powder X-ray diffraction and infrared spectroscopy, and 3 equimolar systems with FTIR pointing to salts, and 4 eutectic mixtures were identified. The intrinsic dissolution rate of TMP in combination with nicotinic acid (a salt) and with paracetamol (eutectic mixture) were 25% and 5% higher than for pure TMP, respectively. For both Gram-positive and -negative strains, the antibacterial activity of TMP with some of the coformers was improved, since the dosage used was lower than the TMP control. A significant increase in antibacterial activity against E. coli was found for the eutectic mixture with curcumin, with the best results being obtained for the eutectic and equimolar mixtures with ciprofloxacin. Combining trimethoprim with coformers offers an interesting alternative to using trimethoprim alone: multicomponent forms with enhanced TMP dissolution rates were identified, as well as combinations showing enhanced antibacterial activity relatively to the pure drug.