Owing to their capability to produce reactive oxygen species (ROS) under solar irradiation, covalent organic frameworks (COFs) with pre-designable structure and unique architectures show great potentials for water purification. However, the sluggish charge separation, inefficient oxygen activation and poor structure stability in COFs restrict their practical applications to decontaminate water. Herein, via a facile one-pot synthetic strategy, we show the direct conversion of reversible imine linkage into rigid thiazole linkage can adjust the $π$-conjugation and local charge polarization of skeleton to boost the exciton dissociation on COFs. The rigid linkage can also improve the robustness of skeleton and the stability of COFs during the consecutive utilization process. More importantly, the thiazole linkage in COFs with optimal C 2p states (COF-S) effectively increases the activities of neighboring benzene unit to directly modulate the O2-adsorption energy barrier and improve the ROS production efficiency, resulting in the excellent photocatalytic degradation efficiency of seven toxic emerging contaminants (e.g. degrading \textasciitilde99% of 5þinspace}mgþinspace}L−1 paracetamol in only 7þinspace}min) and effective bacterial/algal inactivation performance. Besides, COF-S can be immobilized in continuous-flow reactor and in enlarged reactor to efficiently eliminate pollutants under natural sunlight irradiation, demonstrating the feasibility for practical application.

The successful implementation of in-situ bioremediation of nonaqueous-phase liquid (NAPL) contamination in soil-groundwater systems is greatly influenced by the migration performance of NAPL-degrading bacteria. However, the impact and mechanisms of NAPL on the migration/retention of pollutant-degrading bacteria remain unclear. This study investigated the migration/retention performance of A. lwoffii U1091, a strain capable of degrading diesel while producing surfactants, in porous media without and with the presence of mono- and multicomponent NAPL (n-dodecane and diesel) under environmentally relevant conditions. The results showed that under all examined conditions (5 and 50 mM NaCl solution at flow rates of 4 and 8 m/d), the presence of n-dodecane/diesel in porous media could reduce the migration and enhance retention of A. lwoffii in quartz sand columns. Moreover, comparing with mutlicomponent NAPLs of n-dodecane, the monocomponent NAPLs (diesel) exhibited a greater reduction effect on the retention of A. lwoffii in porous media. Through systemically investigating the potential mechanisms via tracer experiment, visible chamber experiment, and theoretical calculation, we found that the reduction in porosity, repulsive forces and movement speeds, the presence of stagnant flow zones in porous media, particularly the biosurfactants generated by A. lwoffii contributed to the enhanced retention of bacteria in NAPL-contaminated porous media. Moreover, owing to presence of the greater amount of hydrophilic components in diesel than in n-dodecane, the available binding sites for the adsorption of bacteria were lower in diesel, resulting in the slightly decreased retention of A. lwoffii in porous media containing diesel than n-dodecane. This study demonstrated that comparing with porous media without NAPL contamination, the retention of strain capable of degrading NAPL in porous media with NAPL contamination was enhanced, beneficial for the subsequent biodegradation of NAPL.

Antibiotic-resistant bacteria (ARB) and antibiotic-resistant genes (ARGs) pose a significant threat to both ecosystems and human health. Owing to the excellent catalytic activity, eco-safety, and convenience for defect engineering, BiOBr with oxygen vacancies (OVs) of different density thus were fabricated and employed to activate H2O2 for ARB disinfection/ARGs degradation in present study. We found that BiOBr with OVs of appropriate density induced via ethanol reduction (BOB-E) could effectively activate H2O2, achieving excellent ARB disinfection and ARGs degradation efficiency. Moreover, this disinfection system exhibited remarkable tolerance to complex water environments and actual water conditions. In-situ characterization and theoretical calculations revealed that OVs in BOB-E could effectively capture and activate aqueous H2O2 into HO· and O2·−. The generated reactive oxygen species combined with electron transfer could damage the cell membrane system and degrade genetic materials of ARB, leading to effective disinfection. The impressive reusability, high performance achieved in two immobilized reaction systems (packed column and baffled ditch reactor), excellent degradation of emerging organic pollutants supported the feasibility of BOB-E/H2O2 system towards practical water decontamination. Overall, this study not only provides insights into fabrication of bismuth-based catalysts for efficient ARB disinfection/ARGs degradation via OVs regulation, but also paves the way for their practical applications.

The influence and mechanisms of starvation on the bacterial mobile performance in porous media with different nutrition conditions are not well understood. The present study systematically investigated the impacts of starvation on the mobility and attachment of both Gram-negative and Gram-positive strains in porous media without and with nutrients on surfaces in both simulated and real water samples. We found that regardless of strain types and water chemistries, starvation would greatly inhibit bacterial attachment onto bare porous media without nutrients yet could significantly enhance cell attachment onto porous media with nutrients on their surfaces. The mechanisms driving the opposite transport behaviors induced by starvation in porous media without and with nutrients were totally different. We found that the starvation process decreased cell motility and increased repulsive force between bacteria and porous media via decreasing cell sizes and zeta potentials, reducing EPS secretion and cell hydrophobicity, thus increasing transport/inhibiting attachment of bacteria in porous media without nutrients on sand surfaces. In contrast, through strengthening the positive chemotactic response of bacteria to nutrients, the starvation process greatly enhanced bacterial attachment onto porous media with nutrients on sand surfaces. Clearly, via modification of the nutrient conditions in porous media, the mobility/attachment performance of bacteria could be regulated.

Harmful algal blooms pose tremendous threats to ecological safety and human health. In this study, simulated solar light (SSL) irradiation was used to activate periodate (PI) for the inactivation of Microcystis aeruginosa and degradation of microcystin-LR (MC-LR). We found that PI-SSL system could effectively inactivate 5 × 106 cells·mL−1 algal cells below the limit of detection within 180 min. ·OH and iodine (IO3· and IO4·) radicals generated in PI-SSL system could rupture cell membranes, releasing intracellular substances including MC-LR into the reaction system. However, the released MC-LR could be degraded into non-toxic small molecules via hydroxylation and ring cleavage processes in PI-SSL system, reducing their environmental risks. High algae inactivation performance of PI-SSL system in solution with a wide pH range (3–9), with the coexisting anions (Cl−, NO3− and SO42−) and the copresence of natural organic matters (humic acid and fulvic acid), real water (lake water and river water), as well as in continuous-flow reactor (14 h) were also achieved. In addition, under natural sunlight irradiation, effective algae inactivation could also be achieved in an enlarged reactor (1 L). Overall, our study showed that PI-SSL system could avoid the inference by the background substances and could be employed as a feasible technique to treat algal bloom water.

Abstract The insufficient exciton (e−-h+ pair) separation/transfer and sluggish two-electron water oxidation are two main factors limiting the H2O2 photosynthetic efficiency of covalent organic frameworks (COFs) photocatalysts. Herein, we present an alternative strategy to simultaneously facilitate exciton separation/transfer and reduce the energy barrier of two-electron water oxidation in COFs via a dicyano functionalization. The in situ characterization and theoretical calculations reveal that the dicyano functionalization improves the amount of charge transfer channels between donor and acceptor units from two in COF-0CN without cyano functionalization to three in COF-1CN with mono-cyano functionalization and four in COF-2CN with dicyano functionalization, leading to the highest separation/transfer efficiency in COF-2CN. More importantly, the dicyano group activates the neighbouring C atom to produce the key *OH intermediate for effectively reducing the energy barrier of rate-determining two-electron water oxidation in H2O2 photosynthesis. The simultaneously enhanced exciton separation/transfer and two-electron water oxidation in COF-2CN result in high H2O2 yield (1601 μmol g−1 h−1) from water and oxygen without using sacrificial reagent under visible-light irradiation. COF-2CN can effectively yield H2O2 in water with wide pH range, in different real water samples, in scaled-up reactor under natural sunlight irradiation, and in continuous-flow reactor for consecutively producing H2O2 solution for water decontamination.

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.

As novel metal-free photocatalysts, covalent organic frameworks (COFs) have great potential to decontaminate pollutants in water. Fast charge recombination in COFs yet inhibits their photocatalytic performance. We found that the intramolecular charge transfer within COFs could be modulated via constructing a donor–acceptor (D–A) structure, leading to the improved photocatalytic performance of COFs toward pollutant degradation. By integrating electron donor units (1,3,4-thiadiazole or 1,2,4-thiadiazole ring) and electron acceptor units (quinone), two COFs (COF-TD1 and COF-TD2) with robust D–A characteristics were fabricated as visible-light-driven photocatalysts to decontaminate paracetamol. With the readily excited electrons in 1,3,4-thiadiazole rings, COF-TD1 exhibited efficient electron–hole separation through a push–pull electronic effect, resulting in superior paracetamol photodegradation performance (>98% degradation in 60 min) than COF-TD2 (∼60% degradation within 120 min). COF-TD1 could efficiently photodegrade paracetamol in complicated water matrices even in river water, lake water, and sewage wastewater. Diclofenac, bisphenol A, naproxen, and tetracycline hydrochloride were also effectively degraded by COF-TD1. Efficient photodegradation of paracetamol in a scaled-up reactor could be achieved either by COF-TD1 in a powder form or that immobilized onto a glass slide (to further ease recovery and reuse) under natural sunlight irradiation. Overall, this study provided an effective strategy for designing excellent COF-based photocatalysts to degrade emerging contaminants.

The release of microplastics (MPs) especially those with sizes less than 10 μm from effluent of wastewater treatment plants (WWTPs) is one of the major sources of plastics into aquatic environment. To reduce the discharge of MPs into environment, it is essential to further enhance their removal efficiencies in WWTPs. In present study, to boost the removal performance of MPs in sand filtration systems (units that commonly employed in WWTPs to remove colloidal pollutants), six types of biochar fabricated from three raw biomass materials (i.e. lignin, cellulose, and woodchips) at two pyrolysis temperatures (400 °C and 700 °C) was respectively amended into sand columns as thin permeable layer. We found that adding all six types of biochar into sand columns as thin permeable layer could greatly improve the retention of MPs with the diameter of 1 μm under either slow (4 m/d) or fast flow rates (160 m/d) due to the high adsorption capability of biochar. Woodchip-derived biochar exhibited the highest MPs retention performance, which was followed by cellulose-derived biochar and then lignin-derived biochar. Moreover, for biochar derived from three raw biomasses, increasing pyrolysis temperature could improve MPs retention performance. The direct observation of real-time plastics retention processes on different types of biochar via a visible flow chamber showed that woodchip-derived biochar especially that fabricated at 700 °C exhibited more MPs trapping processes relative to lignin and cellulose-derived biochar due to their more complex surface morphology. Thus, the highest MPs retention performance was achieved in sand columns with amendment by 1 wt% woodchip-derived biochar fabricated at 700 °C. More importantly, we found that for these modified sand filtration column systems, complete MPs removal could be achieved in real river water and actual sewage water, in multiple filtration cycles, longtime filtration process (100 pore volumes injection) as well as with interval flow conditions. Moreover, biochar could be regenerated and reused as thin permeable layer to effectively remove MPs. The results of this study clearly showed that biochar especially woodchip-derived biochar fabricated at 700 °C had the potential to immobilize MPs especially those with small sizes in WWTPs.

Bacteria present in natural environment especially those in cold regions would experience freeze-thaw (FT) process during day-night and season turns. However, knowledge about the influence of FT on bacteria release behaviors in porous media was limited. In present study, the bacteria release behaviors from quartz sand columns without and with 1 and 3 FT treatment cycles under three water saturations (θ=100%, 90%, and 60%) were investigated. We found that for all three water saturated columns without FT treatment, negligible bacteria released from columns via background salt solution elution, while the subsequent release of bacteria from sand columns via low ionic strength (IS) solution elution decreased with decreasing column water saturations. More importantly, we found unlike the negligible bacteria release in columns without FT treatment, for columns with high saturations (θ=100% and 90%), FT treatment could promote bacteria release with background salt solution elution. Moreover, for high saturated columns, FT treatment would decrease subsequent bacteria release with low IS solution elution. This phenomenon was more obvious with increasing FT treatment cycles. In contrast, FT treatment had negligible influence on bacteria release from columns with lower saturation (θ=60%). The decreased bacterial sizes, the loss of bacterial flagella, as well as the change of local configuration of porous media (via changing water into ice and ice back into water) during the FT processes contributed to increased bacteria release via background salt solution elution from high saturated sand columns. While, the reduced amount of bacteria being retained at secondary energy minima drove to the subsequently decreased bacteria release via low IS solution elution. The results of this study clearly showed that for porous media with high saturations, FT cycles would increase the risk of bacteria detaching from porous media with flushing by the background solution.

Periodate (PI)-based advanced oxidation process has recently attracted great attention in the water treatment processes. In this study, solar irradiation was used for PI activation to disinfect waterborne bacteria. The PI/solar irradiation system could inactivate Escherichia coli below the limit of detection (LOD, 10 CFU mL–1) with initial concentrations of 1 × 106, 1 × 107, and 1 × 108 CFU mL–1 within 20, 40, and 100 min, respectively. •O2– and •OH radicals contributed to the bacterial disinfection. These reactive radicals could attack and penetrate the cell membrane, thereby increasing the amount of intracellular reactive oxygen species and destroying the intracellular defense system. The damage of the cell membrane caused the leakage of intracellular K+ and DNA (that could be eventually degraded). Excellent bacterial disinfection performance in PI/solar irradiation systems was achieved in a wide range of solution pH (3–9), with coexisting humic acid (0.1–10 mg L–1) and broad solution ionic strengths (15–600 mM). The PI/solar irradiation system could also efficiently inactivate Gram-positive Bacillus subtilis. Moreover, PI activated by natural sunlight irradiation could inactivate 1 × 107 CFU mL–1 viable E. coli below the LOD in the river and sea waters with a working volume of 1 L in 40 and 50 min, respectively. Clearly, the PI/solar system could be potentially applied to disinfect bacteria in water.

Bacterial removal by sand filtration system is commonly inefficient due to the low bacterial adsorption capacity of sand. To improve the bacterial removal performance, biochar fabricated at different temperatures (400 °C, 550 °C and 700 °C) and arginine modified biochar were added into sand filtration columns as filter layers (0.5 and 1 wt%). Addition of biochar into sand columns could improve the removal efficiency for both Escherichia coli and Bacillus subtilis under both slow (4 m/day) and fast (240 m/day) filtration conditions. Bacterial removal efficiency in sand columns with the addition of biochar fabricated at 700 °C were higher than those fabricated at 400 °C and 550 °C due to its best bacterial adsorption capacity. Modification of biochar with arginine could further improve the bacterial removal performance. Specifically, complete bacterial removal (1.35 × 107 ± 10% cells/mL) could be achieved under both slow and fast filtration conditions in sand columns with 1 wt% arginine functionalized biochar amendment. The enhanced bacterial adsorption capacity mainly contributed to the increased bacterial capture performance in columns with addition of arginine-modified biochar. Bacteria more tightly bounded with arginine-modified biochar than bulk biochar. Moreover, complete bacterial removal with the copresence of 5 mg/L humic acid in suspensions was acquired in columns with addition of 1 wt% arginine-modified biochar. Efficient bacterial removal in actual river water, multiple filtration cycles as well as longtime injection duration (100 pore volumes injection) was also obtained. The results of this study demonstrated that arginine-modified biochar had great potential to treat water contaminated by pathogenic bacteria.

The effects of flagella and their properties on bacterial transport and deposition behaviors were examined by using four types of Escherichia coli (E. coli) with or without flagella, as well as with normal or sticky flagella. Packed column, quartz crystal microbalance with dissipation, visible parallel-plate flow chamber system, and visible flow chamber packed with porous media system were employed to investigate the deposition mechanisms of bacteria with different properties of flagella. We found that the presence of flagella favored E. coli deposition onto quartz sand/silica surfaces. Moreover, by changing the porous media porosity and directly observing the bacterial deposition process, local sites with high roughness, narrow flow channels, and grain-to-grain contacts were found to be the major sites for bacterial deposition. Particularly, flagella could help bacteria swim near and then deposit at these sites. In addition, we found that due to the stronger adhesive forces, sticky flagella could further enhance bacterial deposition onto quartz sand/silica surfaces. Elution experiments indicated that flagella could help bacteria attach onto sand surfaces more irreversibly. Clearly, flagella and their properties would have obvious impacts on the transport/deposition behaviors of bacteria in porous media. © 2021 American Chemical Society.

Covalent organic frameworks (COFs) have great application potentials in photocatalytic water treatment. By using p-phenylenediamine with different numbers and locations of heterocyclic nitrogen atoms as a precursor, five types of COFs with different nitrogen positions were synthesized. We found that Cr(VI) photoreduction,Escherichia coli inactivation, and paracetamol degradation by COFs were heterocyclic nitrogen location-dependent. Particularly, the photocatalytic performance for all three tested pollutants by five types of COFs followed the order of the best performance for COF-PDZ with two ortho position heterocyclic N atoms, medium for COF-PMD with two meta position heterocyclic N atoms, and COF-PZ with two para position heterocyclic N atoms, and COF-PD with a single heterocyclic N atom, the worst performance for COF-1 without a heterocyclic N atom. Compared to the other COFs, COF-PDZ contained improved quantum efficiency and thus enhanced generation of electrons. The lower energy barriers and larger energy gaps of COF-PDZ contributed to its improved quantum efficiencies. The stronger affinity to Cr(VI) with lower adsorption energy of COF-PDZ also contributed to its excellent Cr(VI) reduction performance. By transferring into a more stable keto form, COF-PDZ showed great stability through five regeneration and reuse cycles. Overall, this study provided an insight into the synthesis of high-performance structure-dependent COF-based photocatalysts. © 2021 American Chemical Society.

Biofilm, community of bacteria ubiquitously present in natural environment, may interact with plastic particles and affect the transport of plastic particles in environment. The significance of biofilm (Escherichia coli) on the transport and deposition behaviors of three different sized plastic particles (0.02 μm NPs, 0.2 μm MP and 2 μm MP) were examined under both 10 mM and 50 mM NaCl solutions by comparing the breakthrough curves and retained profiles of plastic particles in bare sand versus those in biofilm-coated sand. Regardless of ionic strengths, the presence of biofilm increases the deposition of all three sized plastic particles in porous media. Via employing X-ray microtomography imaging (XMT) and Scanning electron microscope (SEM), we find that the presence of biofilm could narrow the flow path especially near to the inlet of the column and increase the surface roughness of porous media (by decreasing DLVO repulsive interaction), which contributes to the enhanced the deposition of plastic particles. Extracellular polymeric substances (EPS) present on the biofilm are found to contribute to the enhanced deposition of plastic particles. Packed column experiments, quartz crystal microbalance with dissipation (QCM-D) as well as parallel plate flow chamber experiments all show that three major components of EPS, proteins, polysaccharide, and humic substances all contribute to the enhanced deposition of plastic particles. O–H and N–H groups present on cell surfaces are highly likely to form hydrogen bond with plastic particles and increase the deposition plastic particles. Elution experiments show that decreasing solution ionic strength could release small portion of plastic particles from both bare and biofilm-coated sand columns especially from the segments near to the column inlet (with slighter lower percentage from biofilm-coated columns based on the total mass of retained plastics). In contrast, increasing flow rate does not obviously detach the plastic particles that already deposited onto porous media. The results of this study clearly show that the presence of biofilm in natural environment could enhance the deposition and decrease the transport of plastic particles. © 2020