As novel photocatalysts, covalent organic frameworks (COFs) have potential for water purification. Insufficient exciton dissociation and low charge mobility in COFs yet restricted their photocatalytic activity. Excitonic dissociation and charge transfer in COFs could be optimized via regulating the donor–acceptor (D–A) interactions through adjusting the number of donor units within COFs, yet relevant research is lacking. By integrating the 1,2,4-triazole or bis-1,2,4-triazole unit with quinone, we fabricated COF-DT (with a single donor unit) and COF-DBT (with double donor units) via a facile sonochemical method and used to decontaminate emerging contaminants. Due to the stronger D–A interactions than COF-DT, the exciton binding energy was lower for COF-DBT, facilitating the intermolecular charge transfer process. The degradation kinetics of tetracycline (model contaminant) by COF-DBT (k = (12.21 ± 1.29) × 10–2 min–1) was higher than that by COF-DT (k = (5.11 ± 0.59) × 10–2 min–1) under visible-light irradiation. COF-DBT could efficiently photodegrade tetracycline under complex water chemistry conditions and four real water samples. Moreover, six other emerging contaminants, both Gram-negative and Gram-positive strains, could also be effectively eliminated by COF-DBT. High tetracycline degradation performance achieved in a continuous-flow system and in five reused cycles in both laboratory and outdoor experiments with sunlight irradiation showed the stability and the potential for the practical application of COF-DBT.

Solar-driven photosynthesis is a sustainable process for the production of hydrogen peroxide, the efficiency of which is plagued by side reactions. Metal-free covalent organic frameworks (COFs) that can form suitable intermediates and inhibit side reactions show great promise to photo-synthesize H2O2. However, the insufficient formation and separation/transfer of photogenerated charges in such materials restricts the efficiency of H2O2 production. Herein, we provide a strategy for the design of donor-acceptor COFs to greatly boost H2O2 photosynthesis. We demonstrate that the optimal intramolecular polarity of COFs, achieved by using suitable amounts of phenyl groups as electron donors, can maximize the free charge generation, which leads to high H2O2 yield rates (605 μmol g−1 h−1) from water, oxygen and visible light without sacrificial agents. Combining in-situ characterization with computational calculations, we describe how the triazine N-sites with optimal N 2p states play a crucial role in H2O activation and selective oxidation into H2O2. We further experimentally demonstrate that H2O2 can be efficiently produced in tap, river or sea water with natural sunlight and air for water decontamination.

Antibiotics present in the natural environment would induce the generation of antibiotic-resistant bacteria (ARB), causing great environmental risks. The effects of antibiotic resistance genes (ARGs) and antibiotics on bacterial transport/deposition in porous media yet are unclear. By using E. coli without ARGs as antibiotic-susceptible bacteria (ASB) and their corresponding isogenic mutants with ARGs in plasmids as ARB, the effects of ARGs and antibiotics on bacterial transport in porous media were examined under different conditions (1–4 m/d flow rates and 5–100 mM NaCl solutions). The transport behaviors of ARB were comparable with those of ASB under antibiotic-free conditions, indicating that ARGs present within cells had negligible influence on bacterial transport in antibiotic-free solutions. Interestingly, antibiotics (5–1000 μg/L gentamicin) present in solutions increased the transport of both ARB and ASB with more significant enhancement for ASB. This changed bacterial transport induced by antibiotics held true in solution with humic acid, in river water and groundwater samples. Antibiotics enhanced the transport of ARB and ASB in porous media via different mechanisms (ARB: competition of deposition sites; ASB: enhanced motility and chemotaxis effects). Clearly, since ASB are likely to escape sites containing antibiotics, these locations are more likely to accumulate ARB and their environmental risks would increase.

Antibiotic resistance genes (ARGs) have become as emerging contaminant with great concerns worldwide due to their threats to human health. It is thus urgent to develop techniques to degrade ARGs in water. In this study, MoS2@Fe3O4 (MF) particles were fabricated and used to activate peroxymonosulfate (PMS) for the degradation of four types of free DNA bases (T, A, C, and G, major components of ARGs) and ARGs. We found that MF/PMS system could effectively degrade all four DNA bases (T within 10 min, A within 30 min, C within 5 min, and G within 5 min) in very short time. During the reaction process, MF could activate PMS to form the reactive radicals such as ·OH, SO4·−, O2·−, and 1O2, contributing to the degradation of DNA bases. Due to the low adsorption energy, high charge transfer, and great capability for PMS cleavage, MF exhibited excellent PMS adsorption and activation performances. MoS2 in MF could enhance the cycle of Fe(III)/Fe(II), improving the catalytic performance. Excellent catalytic performances of MF/PMS system were achieved in complex water matrix (including different solution pH, coexisting of anions and natural organic matter) as well as in real water samples (including tap water, river water, sea water, and sewage) especially under high salinity conditions due to the generation of Cl· radicals and HClO species. MF/PMS system could also efficiently degrade ARGs (chromosomal kanR and plasmid gmrA) and DNA extracted from antibiotic resistant bacteria (ARB) in super-short time. Moreover, complete disinfection of two types of model ARB (E. coli K-12 MG 1655 and E. coli S17–1) could also be achieved in MF/PMS system. The high degradation performances of MF/PMS system achieved in the reused experiments and the 14-day continuous flow reactor experiments indicated the stability of MF particles. Due to the magnetic property, it would be convenient to separate MF particles from water after use via using magnet, facilitating their reuse of MF and avoiding potential water contamination by catalysts. Overall, this study not only provided a deep insight on Fe/Mo-triggered PMS activation process, but also provided an effective and reliable approach for the treatment of DNA bases, ARGs, DNA, and ARB in water.

Flagella and their property would influence the initial attachment of bacteria onto plastics, yet their impacts have not been investigated. In present study, four types of E. coli with or without flagella as well as with normal or sticky flagella were utilized to investigate the effects of flagella and their property on the initial attachment behaviors of bacteria onto six types of plastics in freshwater systems. We found that E. coli with flagella exhibited better initial attachment performance onto all six types of plastics than strain without flagella. Flagella could help bacteria swim near to plastics, pierce the energy barrier, and subsequently attach onto plastics. With stronger adhesive force, sticky flagella could further facilitate bacterial attachment onto plastics. Moreover, flagella especially sticky flagella could help bacteria form more rigid attachment layer on plastics. Even with humic acid in suspensions or in river water, flagellar E. coli showed greater attachment onto plastics than E. coli without flagella. Humic acid might adsorb onto sticky flagella and thus decreased the attachment of bacteria with sticky flagella onto plastics. Obviously, flagella as well as their property would impact the initial attachment of bacteria onto plastics and the subsequent formation of plastisphere in freshwater.

The propagation of antibiotic-resistant bacteria (ARB) greatly endangers the ecological safety and human health. This study employed pyrite (FeS2, naturally abundant mineral) for periodate (PI) activation to disinfect ARB. FeS2/PI system could disinfect 1 × 107 CFU mL−1 of kanamycin-resistant E.coli below the limit of detection in 20 min. Efficient ARB inactivation performance was achieved in pH from 3 to 9, ionic strength from 0 to 300 mM, with HA (0.1–10 mg L−1) in suspension, and in real water samples including tap water, river water and sewage. FeS2/PI system could also efficiently disinfect gentamycin-resistant E.coli and Gram-positive B. subtilis. The generated reactive species including Fe(IV), ·O2– and ·OH would attack cell membrane and overwhelmed intracellular defense system. The intracellular kanamycin resistance genes in cells would be released and then degraded in FeS2/PI system. PI preferred to be adsorbed on Fe site of FeS2 (with lower adsorption energy, more occupancy of bonding state and stronger bonding strength). The subsequent transfer of electron cloud from Fe site to PI would cleave IO bond to generate reactive species. Moreover, FeS2/PI system could also combine with sand filtration system to efficiently capture and disinfect ARB. Therefore, FeS2/PI system is a promising approach to inactivate ARB in different scenarios.