With the growth of the aquaculture industry, antibiotic residues in treated wastewater have become a serious ecological threat. The effects of supplementation with diethyl aminoethyl hexanoate (DA-6) on the removal of tetracycline (TC), ciprofloxacin (CPFX), and sulfamonomethoxine (SMM) from aquaculture wastewater by different microalgae-based systems were examined and systematically analyzed. The results demonstrated that C. vulgaris -S395-2-C. rosea symbiont performed best under 0.2 mg L-1 antibiotic treatment for antibiotic removal. At 10-7 M, DA-6 significantly enhanced C. vulgaris-S395-2-C. rosea symbiont removal of CPFX and SMM at 0.20 mg L-1. The removal of TC, CPFX and SMM by this strain under optimal conditions was 99.2 ± 0.4 %, 86.3 ± 6.3 %, and 91.3 ± 5.7 %, respectively. These results suggest that DA-6 may act on microalgae-bacteria-fungi three-phase symbionts for the removal of multiple antibiotics from aquaculture wastewater.

Herein, we present a high efficiency system based on biochar loaded with layered manganese dioxide to remove tetracycline and heavy metals from livestock wastewater. Under the optimal conditions, the degradation efficiencies of TC in the δ-MnO2/BC/PS system were 85.5% at 25 °C and 38.5% at 5 °C. Radical quenching experiments revealed that radical reactions in the δ-MnO2/BC/PS system were weak under 15 °C. Adsorption degradation experiments showed that the system maintained good adsorption performance at 5 °C. Galvanic cell experiments and cyclic voltammetry showed that the δ-MnO2/BC material had good electrochemical activity and high stability in response to temperature, indicating that TC was degraded by a nonradical pathway that was not limited by temperature, such as electron transfer. Copper ion was important coadsorbent and coactivator of the reaction system. Furthermore, FTIR, XPS, and X-ray diffraction (XRD) analyses showed that Cu(II) in the system was involved in changing the manganese valence state in the δ-MnO2/BC material and increasing the -OH content of BC. Comparison of the different products generated during metabolic testing revealed that the reaction pathway of the system at low temperature (5 °C) differed from that at normal temperature (25 °C). The δ-MnO2/BC material demonstrated good removal ability for antibiotics and heavy metals at normal and low temperatures in actual biogas slurry. The study provides insight for improving the efficiency of environmentally friendly treatments of aquaculture wastewater in cold regions, which is of great significance for resource utilization.

The efficient removal of antibiotics and its combined pollutants is essential for aquatic environment and human health. In this study, a lignin-based organic flocculant named PRL-VAc-DMC was synthesized using pulp reject as the raw material, with vinyl acetate (VAc) and methacryloxyethyltrimethyl ammonium chloride (DMC) as the grafting monomers. A series of modern characterization methods were used to confirm the successful preparation of PRL-VAc-DMC and elucidate its polymerization mechanism. It was found that the Ph-OH group and its contiguous carbon atoms of lignin served as the primary active sites to react with grafting monomers. Flocculation experiments revealed that PRL-VAc-DMC could react with tetracycline (TC) through π-π* interaction, hydrophobic interaction, hydrogen bonding, and electrostatic attraction. With the coexistence of humic acid (HA) and Kaolin, the aromatic ring, hydroxyl, and amide group of TC could react with the benzene ring, hydroxyl group, and carboxyl group of HA, forming TC@HA@Kaolin complexes with Kaolin particles acting as the hydrophilic shell. The increase in particle size, electronegativity, and hydrophily of TC@HA@Kaolin complexes facilitated their interaction with PRL-VAc-DMC through strong interfacial interactions. Consequently, the presence of HA and Kaolin promoted the removal of TC. The synergistic removal mechanism of TC, HA, and Kaolin by PRL-VAc-DMC was systematically analyzed from the perspective of muti-interface interactions. This paper is of great significance for the comprehensive utilization of pulp reject and provides new insights into the flocculation mechanism at the molecular scale.

Mariculture effluent polishing with microalgal biofilm could realize effective nutrients removal and resolve the microalgae-water separation issue via biofilm scraping or in-situ aquatic animal grazing. Ubiquitous existence of antibiotics in mariculture effluents may affect the remediation performances and arouse ecological risks. The influence of combined antibiotics exposure at environment-relevant concentrations towards attached microalgae suitable for mariculture effluent polishing is currently lack of research. Results from suspended cultures could offer limited guidance since biofilms are richer in extracellular polymeric substances that may protect the cells from antibiotics and alter their transformation pathways. This study, therefore, explored the effects of combined antibiotics exposure at environmental concentrations towards seawater Chlorella sp. biofilm in terms of microalgal growth characteristics, nutrients removal, anti-oxidative responses, and antibiotics removal and transformations. Sulfamethoxazole (SMX), tetracycline (TL), and clarithromycin (CLA) in single, binary, and triple combinations were investigated. SMX + TL displayed toxicity synergism while TL + CLA revealed toxicity antagonism. Phosphorus removal was comparable under all conditions, while nitrogen removal was significantly higher under SMX and TL + CLA exposure. Anti-oxidative responses suggested microalgal acclimation towards SMX, while toxicity antagonism between TL and CLA generated least cellular oxidative damage. Parent antibiotics removal was in the order of TL (74.5-85.2 %) > CLA (60.8-69.5 %) > SMX (13.5-44.1 %), with higher removal efficiencies observed under combined than single antibiotic exposure. Considering the impact of residual parent antibiotics, CLA involved cultures were identified of high ecological risks, while medium risks were indicated in other cultures. Transformation products (TPs) of SMX and CLA displayed negligible aquatic toxicity, the parent antibiotics themselves deserve advanced removal. Four out of eight TPs of TL could generate chronic toxicity, and the elimination of these TPs should be prioritized for TL involved cultures. This study expands the knowledge of combined antibiotics exposure upon microalgal biofilm based mariculture effluent polishing.

In this study, activated carbons were obtained from grape marc for tetracycline removal from wastewater. Activated carbons were obtained by subjecting them to pyrolysis at 300, 500, and 700 °C, respectively, and the effect of pyrolysis temperature on activated carbons was investigated. The physicochemical and surface properties of the activated carbons were evaluated by SEM, FTIR, XRD, elemental analysis, N2 adsorption/desorption isothermal, thermal gravimetric (TG) and derivative thermogravimetric (DTG), and BET surface area analysis. When the BET surface areas were examined, it was found that 4.25 m2/g for activated carbon was produced at 300 °C, 44.23 m2/g for activated carbon obtained at 500 °C and 44.23 m2/g at 700 °C, which showed that the BET surface areas increased with increasing pyrolysis temperatures. The pore volumes of the synthesized activated carbons were 0.0037 cm3/g, 0.023 cm3/g, and 0.305 cm3/g for pyrolysis temperatures of 300, 500, and 700 °C, respectively, while the average pore size was found to be 8.02 nm, 9.45 nm, and 10.29 nm, respectively. A better adsorption capacity was observed due to the decrease in oxygen-rich functional groups with increasing pyrolysis temperature. It was observed that the activated carbon obtained from grape skins can easily treat hazardous wastewater containing tetracycline due to its high carbon content and surface functional groups. It was also shown that the activated carbon synthesized in this study has a higher pore volume despite its low surface area compared to the studies in the literature. Thanks to the high pore volume and surface active groups, a successful tetracycline removal was achieved.

Ciprofloxacin (CIP), a broad-spectrum fluoroquinolone antibiotic, is commonly used in aquaculture to prevent and treat bacterial infections in aquatic animals. For this reason, aquatic environments contain CIP and its derivatives, which lead to the development of drug-resistant bacteria. In the present study, copper nanoparticles were prepared using Garcinia mangostana extract (GME-CuNPs) as a reducing agent and evaluated for their CIP removal efficiency (CRE). The results demonstrate that within 20 min, GME-CuNPs at 25 mM possess a CRE of 92.02 ± 0.09% from CIP-containing aqueous media with pH 6-7. The CRE is influenced by both monovalent and divalent salts. A high salt concentration significantly reduces the CRE. Contaminants in fish wastewater can reduce the CRE, but phenolics, flavonoids, tannins, and ammonia do not affect the CRE. Our results reveal that the CRE is controlled by electrostatic attraction between the negatively charged GME-CuNPs and the cationic species of CIP. The CRE is reduced by wastewater with a pH higher than 8.0, in which the CIP molecules have a negative charge, resulting in a repulsive force due to the negative charge of GME-CuNPs. In fish wastewater with a pH lower than 7.0, GME-CuNPs show the potential to achieve a CRE above 80%. Therefore, pH adjustment to a range of 6-7 in fish wastewater before treatment is deemed imperative. It is concluded that the newly developed GME-CuNPs possess excellent activity in CIP elimination from actual fish wastewater samples. Our findings suggest that GME-CuNPs can be a promising tool to effectively eliminate antibiotics from the environment.

Antibiotic residues in mariculture wastewater seriously affect the aquatic environment. Antibiotic Resistance Genes (ARGs) produced under antibiotic stress flow through the environment and eventually enter the human body, seriously affecting human health. Microalgal-bacterial symbiotic system (MBSS) can remove antibiotics from mariculture and reduce the flow of ARGs into the environment. This review encapsulates the present scenario of mariculture wastewater, the removal mechanism of MBSS for antibiotics, and the biomolecular information under metagenomic assay. When confronted with antibiotics, there was a notable augmentation in the extracellular polymeric substances (EPS) content within MBSS, along with a concurrent elevation in the proportion of protein (PN) constituents within the EPS, which limits the entry of antibiotics into the cellular interior. Quorum sensing stimulates the microorganisms to produce biological responses (DNA synthesis - for adhesion) through signaling. Oxidative stress promotes gene expression (coupling, conjugation) to enhance horizontal gene transfer (HGT) in MBSS. The microbial community under metagenomic detection is dominated by aerobic bacteria in the bacterial-microalgal system. Compared to aerobic bacteria, anaerobic bacteria had the significant advantage of decreasing the distribution of ARGs. Overall, MBSS exhibits remarkable efficacy in mitigating the challenges posed by antibiotics and resistant genes from mariculture wastewater.

Singlet oxygen (1O2) is extensively employed in the fields of chemical, biomedical and environmental. However, it is still a challenge to produce high- concentration 1O2 by dioxygen activation. Herein, a system of carbon-supported rare-earth oxide nanocluster and single atom catalysts (named as RE2O3/RE-C, RE=La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Sc and Y) with similar morphology, structure, and physicochemical characteristic are constructed to activate dissolved oxygen (DO) to enhance 1O2 production. The catalytic activity trends and mechanisms are revealed experimentally and are also proven by theoretical analyses and calculations. The 1O2 generation activity trend is Gd2O3/Gd-C>Er2O3/Er-C>Sm2O3/Sm-C>pristine carbon (C). More than 95.0% of common antibiotics (ciprofloxacin, ofloxacin, norfloxacin and carbamazepine) can be removed in 60 min by Gd2O3/Gd-C. Density functional theory calculations indicate that Gd2O3 nanoclusters and Gd single atoms exhibit the moderate adsorption energy of ·O2- to enhance 1O2 production. This study offers a universal strategy to enhance 1O2 production in dioxygen activation for future application and reveals the natural essence of basic mechanisms of 1O2 production via rare-earth oxide nanoclusters and rare-earth single atoms.

This study assessed the effect of gibberellins (GAs) concentrations on antibiotic and nutrient removal using diverse microalgal-bacterial-fungal consortia. Five systems (Chlorella vulgaris, T1; C. vulgaris + S395-2 + Clonostachys rosea, T2; C. vulgaris + S395-2 + Ganoderma lucidum, T3; C. vulgaris + S395-2 + Pleurotus pulmonarius, T4; and C. vulgaris + S395-2, T5) were established, and optimal conditions and effective symbiosis were applied to improve antibiotic and nutrient removal. Consortium growth was T2 > T3 > T5 > T4 > T1, while GA impact ranked 50 mg L-1 > 20 mg L-1 > 80 mg L-1 > 0 mg L-1. After 7 days at 50 mg L-1 GAs, total nitrogen (TN), NH4-N, NO3-N, and total phosphorous (TP) removal reached 85.97 %, 78.08 %, 86.59 %, and 94.39 %, respectively. Florfenicol, oxytetracycline hydrochloride, ofloxacin, and sulfamethoxazole removal efficiencies were 67.77 %, 98.29 %, 90.47 %, and 94.92 %, respectively. These findings highlight GAs\' significant role in enhancing antibiotic and nutrient removal.

The treatment of reverse osmosis concentrate generated from urban industrial sewage for resource recovery has been hot. In this research, a biofilm reactor was constructed by combining sycamore deciduous biochar, shell powder, and polyurethane sponge loaded with Zobellella denitrificans sp. LX16. For ammonia nitrogen (NH4+-N), calcium (Ca2+), chemical oxygen demand (COD), cadmium (Cd2+), and tetracycline (TC), the removal efficiencies were 98.69 %, 83.95 %, 97.26 %, 98.34 %, and 69.12 % at a hydraulic retention time (HRT) of 4 h, pH of 7.0, and influent salinity, Ca2+, and TC concentrations of 1.0, 180.0, and 3.0 mg/L, respectively. The biofilm reactor packing has a three-dimensional structure to ensure good loading of microorganisms while promoting electron transfer and metabolic activity of microorganisms and increasing the pollutant tolerance and removal efficiency. The reactor provides a practical reference for the sedimentation of reverse osmosis concentrate to remove Cd2+ and TC by microbial induced calcium precipitation (MICP).