主要成果

2026
Limitation of carbon and nitrogen nutrients could induce contrasting bacterial transport performance in porous media
He L, Qin J, Wu D, Zhang X, Tong M. Limitation of carbon and nitrogen nutrients could induce contrasting bacterial transport performance in porous media. Water Research [Internet]. 2026;297:125641. 访问链接Abstract
The effects and mechanisms of carbon (C)- and nitrogen (N)-deficient nutrient conditions (prevalent in natural environment) on bacterial mobile performance in porous media are unclear. This study systematically investigated the transport/retention performance of Gram-negative Escherichia coli and Gram-positive Bacillus subtilis experiencing different nutrient conditions (i.e. nutrient-sufficient, C-deficient, or N-deficient conditions) in column, parallel plate flow chamber (PPFC) and microfluidic chamber systems. We found that compared to those in nutrient-sufficient condition, bacteria (regardless of their type) exposure to C-deficient nutrient condition exhibited 7–14% reduced mobility in porous media, whereas those experienced N-deficient condition had 7–20% enhanced transport in both simulated electrolyte solutions and real groundwater samples. The underlying mechanisms driving to different mobile performance of bacteria exposure to different nutrient conditions were correlated with the composition of proteins (one major component of extracellular polymeric substances (EPS)). Compared to nutrient-sufficient condition, C-deficient condition increased EPS hydrophobicity via enhancing hydrophobic amino acids contents and altering secondary structure within proteins thus decreased bacterial transport, while N-deficient condition decreased EPS hydrophobicity through decreasing the abundance of hydrophobic amino acids within proteins and increased cell mobility. The results showed that via changing cell surface hydrophobicity, exposure bacteria to different nutrient conditions could induce different mobile performance of bacteria.
Ultrafast antibiotic resistance removal from water via activation of low-dose percarbonate by bismuth oxyiodide with optimal Bi3-oxygen vacancy sites
Li Z, Hou Y, Liu F, Liang J, Tong M. Ultrafast antibiotic resistance removal from water via activation of low-dose percarbonate by bismuth oxyiodide with optimal Bi3-oxygen vacancy sites. Water Research [Internet]. 2026;297:125661. 访问链接Abstract
Antibiotic-resistant bacteria (ARB) and antibiotic-resistant genes (ARGs) pose global threats to human health and ecological safety. Activation of percarbonate (PC) by eco-friendly bismuth oxyiodide (BiOI) is a promising ARB/ARGs removal technique, yet its efficiency is hindered by the insufficient exposure of reactive Bi sites. Herein, we provide a facile protocol to fabricate BiOI with remarkable PC activation efficiency (BOI-C) for the ultrafast ARB/ARGs removal via modulating reactive Bi sites through introducing optimal Bi3-oxygen vacancy (OV) sites on the unsaturated facets. We show that BOI-C with optimal amount of Bi3-OV site can efficiently activate 50 µM PC to rapidly disinfect 7-log ARB to the limit of detection within only 4 min. Moreover, this reaction system can effectively degrade the released ARG and suppress the horizontal gene transfer process, greatly decreasing the risks of ARG dissemination. Negligible toxic halogen-containing disinfection byproducts is generated during the disinfection process, indicating the outstanding ecological safety of BOI-C/PC system. The reaction system can also effectively disinfect ARB under complex water chemistries including a broad pH range (3–9), high ionic strengths (up to 150 mM), copresence of natural organic matter (up to 10 mg L−1), and diverse actual water samples including tap water, lake water, groundwater and aquaculture tailwater. Furthermore, it can also be assembled into a filtration system for successive ARB disinfection, demonstrating the feasibility for practical application. The catalytic system also exhibits excellent ARB disinfection performance across various bacterial strains and effective degradation performance towards different types of emerging organic pollutants, suggesting its universal decontamination capability. Combining in-situ characterizations and theoretical calculations, we reveal that Bi3-OV sites on the unsaturated facets of BOI-C facilitate the p-p interaction with peroxy O atoms of PC molecules and trigger the electron transfer as well as the subsequent cleavage of peroxy bonds, generating abundant CO3•− for the ultrafast ARB disinfection. The results of this study show that BOI-C/PC system can be employed to effectively remove antibiotic resistance in real water.
2025
Constructing dual charge-transfer tunnels within highly charge-confined COFs for efficient photosynthesis of hydrogen peroxide from water and air
Hou Y, Liu F, Li Z, Liang J, Zhou P, Tong M. Constructing dual charge-transfer tunnels within highly charge-confined COFs for efficient photosynthesis of hydrogen peroxide from water and air. National Science Review [Internet]. 2025;13:nwaf444. 访问链接Abstract
Insufficient charge separation and sluggish two-electron water-oxidation reaction are two critical factors restricting the photosynthesis performance of metal-free covalent organic frameworks (COFs) for hydrogen peroxide (H2O2) generation from naturally abundant water and air. Herein, we develop a facile strategy to simultaneously boost the charge-separation efficiency and water-oxidation capability through constructing short and rapid charge-transfer tunnels within highly charge-confined COFs via replacing the phenyl with pyrimidine. Compared with a single charge-transfer tunnel within a lowly charge-confined COF-5-(4-aminophenyl)pyrimidin-2-amine (APM) with pyrimidine, dual charge-transfer tunnels are constructed within a highly charge-confined COF-5,5′-bipyrimidine-2,2′-diamine (BPM) with bipyrimidine due to the ground-state charge transfer between para-carbon and meta-nitrogen, which significantly accelerates the intermolecular charge-transfer process and prevents charge recombination. This strategy also decreases the energy barrier of rate-determining water oxidation in H2O2 photosynthesis and thus promotes the effective generation of the key *OH intermediates, facilitating the generation of H2O2 at a production rate of 5521 μmol g−1 h−1 from water, oxygen and light without sacrificial reagents or additional energy consumption by COF-BPM. Furthermore, COF-BPM can also efficiently produce H2O2 under broad pH conditions, in widely available real water, on a floatable foam sheet, in a continuous-flow reactor and in a scaled-up reactor by using natural solar light for water decontamination.
Activation of Chlorite with Sunlight for the Efficient Disinfection of Antibiotic-Resistant Bacteria: the Overlooked Contribution of Cytomembrane-Bound Chlorite
Shen Y, Liu F, Liang J, Li Z, Hou Y, Wu J, Ting Y, Guo R, Liu Y, Han P, et al. Activation of Chlorite with Sunlight for the Efficient Disinfection of Antibiotic-Resistant Bacteria: the Overlooked Contribution of Cytomembrane-Bound Chlorite. Environmental Science & Technology [Internet]. 2025;59:19526-19536. 访问链接Abstract
Current antibiotic-resistant bacteria (ARB) disinfection techniques commonly rely on large dosages of oxidants, resulting in the presence of considerable amounts of residuals and toxic disinfection byproducts (DBPs) in water. Herein, we propose a highly effective ARB disinfection approach via activating an ultralow concentration (10 μM) of chlorite (ClO2–) by naturally abundant sunlight to generate various reactive species (i.e., HO•, Cl•, ClO•, and ClO2) with negligible generation of halogenated DBPs. Combining in situ characterization with theoretical calculations, we reveal that, in addition to the photolysis of ClO2– in the bulk solution, ClO2– ions electrostatically adsorbed on the positive local sites of lipids can boost light absorption and facilitate the in situ generation of reactive species upon sunlight irradiation, enabling more efficient attacks toward cell membranes and the intracellular antioxidant enzyme system. The intracellular antibiotic resistance genes (ARGs) are then released and further degraded, inhibiting horizontal ARG transfer. This approach can also achieve excellent ARB disinfection performance in real water matrices (e.g., lake and river water) in 1 L tanks and 500 mL plastic bottles with natural sunlight irradiation. Overall, this work presents an efficient, safe, and sustainable method to inactivate ARB with deep insights into disinfection mechanisms at the subcellular level.
Boosting Low-Dose Ferrate(VI) Activation by Layered FeOCl for the Efficient Removal of Antibiotic-Resistant Bacteria and Antibiotic Resistance Genes via Enhancing Fe(IV)/Fe(V) Generation
Nie C, Liu F, Li Z, Shen Y, Hou Y, Han P, Tong M. Boosting Low-Dose Ferrate(VI) Activation by Layered FeOCl for the Efficient Removal of Antibiotic-Resistant Bacteria and Antibiotic Resistance Genes via Enhancing Fe(IV)/Fe(V) Generation. Environmental Science & Technology [Internet]. 2025;59:19559-19569. 访问链接Abstract
Antibiotic-resistant bacteria (ARB) and antibiotic resistance genes (ARGs) in aquatic environments pose threats to ecosystem safety and human health, which could not be efficiently removed by conventional disinfection techniques. Herein, layered FeOCl with coordinatively unsaturated Fe sites were fabricated and used to activate Fe(VI) for the efficient ARB/ARG removal in the present study. We found that highly reactive Fe(IV)/Fe(V) intermediates were generated in the FeOCl/Fe(VI) system, rapidly disinfecting 1 × 107 CFU mL–1 ARB to below the limit of detection within only 6 min. Via the combination of in situ characterization and theoretical calculations, we revealed that Fe(VI) was preferentially adsorbed onto Fe sites on the (010) plane of FeOCl and subsequently activated to produce reactive Fe(IV)/Fe(V) through direct electron transfer. Meanwhile, O2•– generated from O2 activation on the FeOCl surface enhanced Fe(VI) conversion to Fe(IV)/Fe(V). During the disinfection process, intracellular/extracellular ARGs and DNA bases were simultaneously degraded, inhibiting the potential horizontal gene transfer process. The FeOCl/Fe(VI) system could effectively disinfect ARB under complex water matrices and in real water samples including tap water, lake water, and groundwater. When integrated into a continuous-flow reactor, the FeOCl/Fe(VI) system with excellent stability successively disinfected ARB. Overall, the FeOCl/Fe(VI) system showed great promise for eliminating ARB/ARGs from water.
Contrasting chemotactic responses drive opposite transport behaviors of petroleum-degrading and non-degrading bacteria in petroleum-contaminated porous media
Qin J, He L, Chen C, Tong M. Contrasting chemotactic responses drive opposite transport behaviors of petroleum-degrading and non-degrading bacteria in petroleum-contaminated porous media. Water Research [Internet]. 2025;287:124462. 访问链接Abstract
Injection of bacteria with petroleum degrading capability into contaminated sites is one of the most cost-effective and environmental friendly strategies for the successful remediation of petroleum-contaminated groundwater. The successful in-situ bioremediation of petroleum contamination in subsurface is greatly impacted by the mobile/retention performance of petroleum-degrading bacteria in porous media, which yet is not well understood. The present study systematically investigated the mobile performance of petroleum-degrading strains in porous media with petroleum contamination under environmentally relevant solution and flow conditions. We found that although the mobile performance of petroleum-degrading bacteria was similar to petroleum non-degrading bacteria in uncontaminated porous media, bacteria containing different petroleum degrading function yet exhibited opposite transport behaviors in petroleum contaminated porous media. Enhanced mobility in porous media with petroleum contamination was achieved for petroleum non-degrading bacteria, while reduced mobility was obtained for petroleum-degrading bacteria. Combining the batch adsorption experiments, capillary chemotaxis assays, in-situ microfluidic chamber experiments together with theoretical calculation, we found that the opposite mobile performance observed for bacteria containing different petroleum degrading functions could be mainly attributed to their different chemotactic responses towards petroleum with negative and positive chemotaxis response respectively for non- and petroleum-degrading bacteria. Clearly, pollutant-degrading bacteria exhibited different mobile performance from non-degrading bacteria in contaminated porous media. The previous findings achieved from the model bacteria without pollutant-degrading capability could not be simply used to predict the mobile performance of pollutant-degrading bacteria. To ensure the successful implementation of in-situ bioremediation, the mobility of pollutant-degrading bacteria in contaminated porous media should be fully understood.
N-Acyl-Homoserine Lactone (AHL)-Mediated Initial Adhesion Behaviors of Bacteria onto Plastics
Wang S, Su X, Qin J, He L, Tong M. N-Acyl-Homoserine Lactone (AHL)-Mediated Initial Adhesion Behaviors of Bacteria onto Plastics. Environmental Science & Technology [Internet]. 2025;59:13012-13021. 访问链接Abstract
The initial adhesion of microbes onto plastics is crucial for the subsequent formation of the plastisphere, which might be affected by signal molecules commonly present in bacteria-related environments that regulate cell-to-cell communication. Herein, the initial retention performance of E. coli onto six types of plastics, both without and with N-acyl-homoserine lactones (AHLs, a common signal molecule) at concentrations ranging from 10 ng/L to 100 μg/L in suspension, was determined to reveal the influence of signal molecules on the formation of the plastisphere. We found that AHLs coexisting in suspensions significantly enhanced bacterial adhesion performance onto plastics, regardless of plastic types and AHL types, with a more pronounced enhancement observed at higher AHL concentrations. This enhanced bacterial adhesion induced by AHLs also held true in solutions containing humic acid, in river water, and in sewage. AHLs stimulated the synthesis of EPS, enhanced EPS hydrophobicity by altering the protein/polysaccharide ratio and its secondary structures, and upregulated pathways related to flagellar assembly, quorum sensing, protein production, and biofilm formation, thereby enhancing bacterial adhesion capability onto plastics. Moreover, AHLs adsorbed onto plastic surfaces could induce chemoattraction effects, further promoting bacterial adhesion performance. Obviously, through various mechanisms, the signal molecules greatly influence the initial adhesion of bacteria onto plastics in aquatic systems.
Building a Confluence Charge Transfer Pathway in COFs for Highly Efficient Photosynthesis of Hydrogen Peroxide from Water and Air
Hou Y, Liu F, Liang J, Li Z, Zhou P, Tong M. Building a Confluence Charge Transfer Pathway in COFs for Highly Efficient Photosynthesis of Hydrogen Peroxide from Water and Air. Angewandte Chemie International Edition [Internet]. 2025:e202505621. 访问链接Abstract
Sunlight-driven photosynthesis by covalent organic frameworks (COFs) from water and air without using sacrificial reagents is a promising H2O2 fabrication approach, but is still restricted by the insufficient charge separation and sluggish 2e- water oxidation process. Herein, we provide a facile strategy to simultaneously improve charge separation and water oxidation in COFs via confining the charge transfer pathways from two diversion ones to a confluence one through regulating the site of nitrogen in bipyridine. Combining in-situ characterization with computational calculations, we reveal that compared to COF-BD1 containing two diversion charge transfer pathways, the charge transfer pathway in COF-BD2 is confined to a confluence one due to the electron-deficiency effect of nitrogen, which greatly accelerates the intermolecular and out-of-plane charge transfer. Via effectively reducing the energy barrier of rate-determining water oxidation reaction, the subsequent water oxidation process to produce key *OH intermediate in COF-BD2 is also greatly facilitated, boosting the yield of H2O2 (5211 μmol g-1 h-1) from water, oxygen, and light without sacrificial agents or additional energy consumption. We further demonstrate that H2O2 can be efficiently produced by COF-BD2 in broad pH range, in real water, and in enlarged reactor with using natural sunlight for water decontamination.
Green and efficient disinfection of antibiotic-resistant bacteria via PI/H2O2 homogeneous system
Zhang B, Li Z, Liu F, Zhang X, Hou Y, Tong M. Green and efficient disinfection of antibiotic-resistant bacteria via PI/H2O2 homogeneous system. Water Research [Internet]. 2025:123468. 访问链接Abstract
The proliferation and spread of antibiotic-resistant bacteria (ARB) significantly threaten human health and ecosystem. Periodate (PI) based advanced oxidation process has potentials for water purification but limited by complex activators or activation process. Herein, we demonstrated that H2O2 could be used to activate PI, achieving efficient ARB disinfection performance. Particularly, we found that the PI/H2O2 system (0.1 mM for both oxidants) could inactivate ARB (Escherichia coli) within 35 min. The intracellular defense system attacked by HO· radicals generated in the disinfection system, resulting in the inactivation of ARB. Antibiotic resistance genes (ARGs) released with the lysis of cell membrane could be further degraded by HO· radicals. Moreover, we found that the PI/H2O2 system was effective to inactivate ARB in a broad range of ionic strengths, with coexisting common ions and humic acid, as well as in four typical actual water bodies. The PI/H2O2 system could also efficiently disinfect other types of bacteria and degrade typical organic contaminants. In addition, under sunlight irradiation, the ARB inactivation performance of the PI/H2O2 system could be greatly improved. This study provided a practical and efficient way for decontaminating ARB/ARGs-polluted water.
2024
Rigid covalent organic frameworks with thiazole linkage to boost oxygen activation for photocatalytic water purification
Hou Y, Zhou P, Liu F, Tong K, Lu Y, Li Z, Liang J, Tong M. Rigid covalent organic frameworks with thiazole linkage to boost oxygen activation for photocatalytic water purification. Nature Communications [Internet]. 2024;15:7350. 访问链接Abstract
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.
Effects of Mono- and Multicomponent Nonaqueous-Phase Liquid on the Migration and Retention of Pollutant-degrading Bacteria in Porous Media
He L, Li O, Qin J, Chen C, Li Z, Tong M. Effects of Mono- and Multicomponent Nonaqueous-Phase Liquid on the Migration and Retention of Pollutant-degrading Bacteria in Porous Media. Water Research [Internet]. 2024:122673. 访问链接Abstract
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.
Oxygen vacancy-dependent synergistic disinfection of antibiotic-resistant bacteria by BiOBr nanoflower induced H2O2 activation
Li Z, Hou Y, Shen Y, Nie C, Zhang X, Liu F, Tong M. Oxygen vacancy-dependent synergistic disinfection of antibiotic-resistant bacteria by BiOBr nanoflower induced H2O2 activation. Water Research [Internet]. 2024;267:122524. 访问链接Abstract
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.
Starvation Process Would Induce Different Bacterial Mobilities and Attachment Performances in Porous Media without and with Nutrients on Surfaces
Qin J, He L, Su X, Wang S, Tong M. Starvation Process Would Induce Different Bacterial Mobilities and Attachment Performances in Porous Media without and with Nutrients on Surfaces. Environmental Science & Technology [Internet]. 2024;58(31):13879-13889. 访问链接Abstract
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.
Simultaneous inactivation of Microcystis aeruginosa and degradation of microcystin-LR in water by activation of periodate with sunlight
Zhang X, Zhang B, Shen Y, Li Z, Hou Y, Liu F, Tong M. Simultaneous inactivation of Microcystis aeruginosa and degradation of microcystin-LR in water by activation of periodate with sunlight. Water Research [Internet]. 2024;260:121948. 访问链接Abstract
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.
Efficient Photosynthesis of Hydrogen Peroxide by Cyano-Containing Covalent Organic Frameworks from Water, Air and Sunlight
Hou Y, Zhou P, Liu F, Lu Y, Tan H, Li Z, Tong M, Ni J. Efficient Photosynthesis of Hydrogen Peroxide by Cyano-Containing Covalent Organic Frameworks from Water, Air and Sunlight. Angewandte Chemie International Edition [Internet]. 2024;63:e202318562. 访问链接Abstract
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.
2023
Boosting Exciton Dissociation and Charge Transfer in Triazole-Based Covalent Organic Frameworks by Increasing the Donor Unit from One to Two for the Efficient Photocatalytic Elimination of Emerging Contaminants
Hou Y, Liu F, Nie C, Li Z, Tong M. Boosting Exciton Dissociation and Charge Transfer in Triazole-Based Covalent Organic Frameworks by Increasing the Donor Unit from One to Two for the Efficient Photocatalytic Elimination of Emerging Contaminants. Environmental Science & Technology [Internet]. 2023;57:11675-11686. 访问链接Abstract
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.
Covalent organic frameworks for direct photosynthesis of hydrogen peroxide from water, air and sunlight
Liu F, Zhou P, Hou Y, Tan H, Liang Y, Liang J, Zhang Q, Guo S, Tong M, Ni J. Covalent organic frameworks for direct photosynthesis of hydrogen peroxide from water, air and sunlight. Nature Communications [Internet]. 2023;14:4344. 访问链接Abstract
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.
Effects of Antibiotic Resistance Genes and Antibiotics on the Transport and Deposition Behaviors of Bacteria in Porous Media
Wang S, He L, Zhang M, Su X, Liu F, Chen Q, Yang J, Tong M. Effects of Antibiotic Resistance Genes and Antibiotics on the Transport and Deposition Behaviors of Bacteria in Porous Media. Environmental Science & Technology [Internet]. 2023;57:10426-10437. 访问链接Abstract
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.
Efficient peroxymonosulfate activation by magnetic MoS2@Fe3O4 for rapid degradation of free DNA bases and antibiotic resistance genes
Nie C, Hou Y, Liu F, Dong Q, Li Z, Han P, Tong M. Efficient peroxymonosulfate activation by magnetic MoS2@Fe3O4 for rapid degradation of free DNA bases and antibiotic resistance genes. Water Research [Internet]. 2023;239:120026. 访问链接Abstract
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.
Influence of flagella and their property on the initial attachment behaviors of bacteria onto plastics
Zhang M, He L, Qin J, Wang S, Tong M. Influence of flagella and their property on the initial attachment behaviors of bacteria onto plastics. Water Research [Internet]. 2023;231:119656. 访问链接Abstract
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.

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