Lake sediments represent a typical reservoir of antibiotic resistance genes (ARGs), an emerging contaminant. As a key nutrient for sediment microorganisms, elevated sulfate levels can profoundly influence sulfur cycling and related microbial processes. However, the impact of sulfate loads on the profiles of ARGs in lake sediments remains poorly understood. This study utilized a microcosm experiment to examine how sulfate addition at various concentrations (200, 400, and 600 mg/kg dry weight) affects the sediment resistome, via metagenomic analysis. Sulfate addition significantly increased sediment sulfides and the relative abundance of sulfate-reducing genes (SRGs). Notably, the high sulfate treatment (600 mg/kg) resulted in a significant rise in the relative abundance of ARGs, virulence factor genes (VFGs), and mobile genetic elements (MGEs), indicating an increased potential for resistance dissemination under high sulfate loading. The relative abundance of horizontal transfer related genes, including those mediating cell membrane permeability and type IV secretion system, was enhanced by sulfate addition, potentially promoting ARG dissemination. Linear regression identified strong positive relationships between the abundance of ARGs and abundances of both MGEs and VFGs. Sulfate addition enriched specific antibiotic-resistant bacteria (ARBs) carrying SRGs that were identified via network analysis. The genera Burkholderia, JACDDX01, and Hylemonella showed marked enrichment, with increases of 16.7 %, 13.2 %, and 94.6 %, respectively. Overall, the rise in ARG abundance under sulfate addition shows close links to specific ARBs and enhanced horizontal transfer. These findings have implications for understanding sulfate-driven changes in sediment resistome and assessing environmental risk in sulfate-enriched lake ecosystems.
Piezo-photocatalytic H2O2 production faces a central challenge: inadequate visible-light absorption and insufficient driving forces for charge separation, especially in wide-bandgap nonpolar semiconductors. To address this, we propose a strategy that constructs Cu+-oxygen vacancy defect dipoles within nonpolar ZrO2 to enable piezo-photo coupling. Under ultrasonic excitation, these defect dipoles produce a robust piezoelectric polarization field that facilitates directional separation of photogenerated carriers. As a result, charge recombination at visible-light-absorbing defect states is effectively suppressed, enabling synergistic utilization of mechanical and optical energy. The optimized catalyst exhibits a remarkable H2O2 production rate of 415.36 μmol·g-1·hour-1 under ambient air/water conditions and achieves near-complete degradation (88.7%) of rhodamine B in continuous-flow wastewater treatment (1 liter within 60 min). Theoretical calculations further reveal that the defect dipoles lower the d-band center of the active sites, thereby promoting *OH desorption and accelerating H2O2 formation kinetics. This study offers a viable strategy for inducing piezoelectricity in nonpolar semiconductors, thereby establishing design principles for high-performance piezo-photocatalytic systems.
Animal husbandry tailwater represents a significant contributor to phosphorus (P) release and antibiotic resistance genes (ARGs) dissemination in agricultural non-point source pollution. Conventional P adsorption nanomaterials may unintentionally act as carriers that promote ARGs propagation. This phenomenon is analogous to the "Trojan horse effect", attributed their large specific surface area and weaken oxidative activity. To address this limitation, we developed a novel dual-light-driven agent (Biochar/LaFeO3/TiO2, BLFT) that is capable of simultaneous P adsorption and ARGs inactivation. This material integrates the specific affinity of La sites for phosphate groups with the photocatalytic degradation capacity of a constructed S-scheme heterojunction. Characterization verified the successful loading of LaFeO3 and TiO2 as "grape - cluster" - like aggregates. These aggregates formed an S-scheme heterojunction that effectively promoted the separation and transfer of photogenerated charges. In actual animal husbandry tailwater, BLFT achieved removal rates of 91.17%-96.97% (ARGs) and 72.68%-76.96% (P) with both processes being light-driven. Mechanistic studies revealed that the synergistic effect stems from P adsorption via La-O-P Lewis acid-base interaction, coupled with oxidative degradation by a four-electron transfer pathway. Ultimately, energy consumption analysis estimated that BLFT production generated a surplus energy of 1017.2 kW & sdot;h/t for external supply. Moreover, its cost-benefit cost for water treatment remains lower than the combined expenses of conventional advanced oxidation process and flocculation P process. This study provides a cost-effective and efficient strategy to simultaneously mitigate both traditional and emerging pollutants, presenting a promising win-win solution for sustainable agricultural water management.
Integrated irrigation-aquaculture (IIA) systems recycle aquaculture wastewater for crop irrigation, yet the ecological risks of fishery drugs under protein-rich dissolved organic matter (DOM) remain unclear. To evaluate crop responses, rice seedlings were exposed to florfenicol (FF) with lysine, simulating high-protein DOM matrix effects. A clear dose-response relationship was observed for FF exposure, with an EC10 of 1.58 mg·L-1. At 1/4 EC10, FF promoted growth while inducing oxidative stress, glutathione S-transferase activation, and lignin synthesis. At EC10, FF suppressed root development by down-regulating sulfur and ethylene pathways, disrupting antioxidant balance, and triggering defensive lignification that constrained growth. Notably, lysine did not merely coexist with FF but significantly enhanced its uptake and translocation, thus enhancing the oxidative stress and transcriptional response caused by FF. Molecular interaction analysis indicated that lysine facilitated FF absorption through hydrogen bonding, halogen bonding, and hydrophobic interactions with lysine-histidine transporters, lowering the binding energy and increasing FF bioaccumulation. Although lysine upregulated amino acid metabolism pathways, this partial metabolic adjustment was insufficient to offset the increased internal FF burden. This study delves into the molecular mechanisms underlying rice ecological disorders in the IIA system, providing a scientific basis for agricultural water management.
Antibiotic resistance genes (ARGs) in agricultural systems could pose potential threats to food safety and human health, their migration pathways and drivers across water-soil-crop environments require further elucidation. In this study, we selected three paddy fields irrigated with representative water sources in the lower Yangtze River region and collected 7 sample types from water, soil, and rice-associated compartments. The results showed that 10 ARGs and 2 mobile genetic elements (MGEs) were widely detected across the multi-media of paddy, with relative abundances ranging from 24.60 to 33.52 copies/16S copies. Bioaccumulation factors (BAF) ranged from 1.00 to 1.12, indicating that the soil-root represents a key interface for ARGs migration. Notably, SourceTracker identified two dominant sources of the leaf endophytic microbiome, with root endophytes contributing 55-77% and leaf epiphytes contributing 8-41%, suggesting that microorganisms can be transmitted through dual pathways involving internal plant transport and external surface colonization. PLS-PM further showed that differences in soil physicochemical properties induced by overlying water influenced ARGs occurrence by regulating leaf endophytic host bacterial communities. Overall, this study outlines a potential ARGs transmission pathway across water-soil-crop compartments and provides a microbially mediated framework for understanding ARGs migration and establishment in aboveground rice tissues.
Osmotic energy conversion offers a sustainable route to harvest electricity from salinity gradients. Beyond natural seawater/riverwater systems, saline waste streams rich in dissolved ions and persistent organic pollutants remain an underutilized resource for simultaneous energy recovery and remediation. Here, we report an asymmetric MoS2/oxygen-doped ZIF-8 membrane (MS-ZIF-A) that incorporates a built-in electric field (IEF) to accelerate selective ion transport and enhance osmotic energy conversion. Work function matching between the functional layers optimizes interfacial band alignment, strengthening the internal driving force for ion migration and enabling a peak power density of 9.4 W m-2 under a 50-fold NaCl salinity gradient. In simulated industrial wastewater containing NaCl and RhB, the membrane delivers power densities of up to 30 W m-2 while concurrently degrading organic pollutants. These results establish work function engineering as an effective strategy to construct interfacial IEF in asymmetric membranes, providing a general design principle for high-performance blue-energy devices and offering a promising route toward energy-positive treatment of saline wastewater.
Covalent organic framework (COF) membranes hold great promise for harvesting osmotic energy from the salinity gradient. However, their power output is often constrained by limited ion transport. Here, we report Schiff base COF-xSO3H membranes fabricated via interfacial polymerization, where tuning the sulfonate content induces a structural transition from AA stacking (COF-1SO3H) to AB stacking (COF-2SO3H), reducing the pore size from 0.93 to 0.59 nm. The COF-2SO3H membrane, with subnanometer channels and high charge density, exhibited strong dehydration capability, thereby significantly enhancing ion transport. Under a 50-fold salinity gradient, it achieved a maximum power density of 10.5 W m-2, 2.7 times higher than that of the COF-1SO3H membrane. These findings highlight a biomimetic strategy for tailoring subnanometer pores to enable selective ion dehydration and boost osmotic energy conversion efficiency.
Aquaculture activities discharge large amounts of antibiotics, with protein-like dissolved organic matter (DOM) coexisting in wastewater, whose impact on FF degradation remains unclear. An efficient advanced oxidation process (AOP) was established by Mn(II), nitrilotriacetic acid (NTA), and peroxymonosulfate (PMS) for degrading the typical aquaculture antibiotic florfenicol (FF), achieving removal efficiency of (97.38±1.02)% within 20 min primarily via Mn(V)=O, in which •OH, •SO4-, and 1O2 made minor contributions. The inhibitory effects of fishery amino acids on FF degradation followed the order: poly lysine > tryptophan > methionine > lysine. Based on electrochemical measurements and density functional theory (DFT) calculations, tryptophan and methionine competed for PMS binding sites, with methionine being preferentially oxidized by Mn(V)=O, thereby delaying FF degradation. Primary degradation pathways involved defluorination, dechlorination, and aromatic ring hydroxylation, exhibiting a reduced toxicity. Overall, this study developed a sustainable strategy to remove typical fishery antibiotics, highlighting the critical role of Mn(V)=O and the interference mechanism of protein-like DOM.
Benzotriazole ultraviolet stabilizers (BUVSs) are widespread emerging pollutants in sediments. However, studies on the effects of BUVSs on benthic gut microbiota, particularly under co-exposure with salinity fluctuations, remain underexplored. This is significant as salinity is a contributing factor to saline intrusion attributed to climate change. Therefore, this research was conducted to investigate the combined effects of benzotriazole ultraviolet stabilizer-329 (UV-329) and salinity on the gut microbiota of Corbicula fluminea in sediments. The metabolic function of gut microbiota evaluated by Biolog ECO microplates showed that co-exposure to UV-329 and salt stress reduced microbial metabolic activity (from 0.731 to 0.192, average well color development). Self-organizing map algorithm further revealed shifts in carbon sources utilization, with salt stress exerting a greater metabolic influence compared to UV-329. Compared to UV-329, co-exposure was more conducive to the survival of pathogens (e.g., Mycoplasma). Molecular docking demonstrated that UV-329-Na complexes had a stronger binding affinity for diamine oxidase than UV-329 alone, suggesting a mechanistic basis for enhanced intestinal inflammation under combined stress. Microbial source tracking indicated an increased proportion of gut bacteria originating from sediments (from 16.2% to 26.4%) under UV-329 and salt stress. Neutral community model and null model analyses revealed that stochastic processes dominated gut microbial assembly, and co-exposure reduced bacterial immigration rate compared to UV-329 exposure. These results highlight that salinity modulates the toxicity of UV-329 by exacerbating gut microbiota dysbiosis, impairing intestinal barrier function, and altering the probability of bacterial dispersal.
Wetland interfaces regulate greenhouse-gas exchange and carbon retention, yet contaminant exposure may disrupt the relationship between these two processes. Whether aqueous perfluorooctane sulfonate (PFOS), a persistent aquatic contaminant, alters this relationship remains unclear. Here, we used a controlled rhizobox mesocosm with paired planted and unplanted treatments across an aqueous PFOS gradient (0, 10, 100, and 1000 μg L-1) to resolve plant-mediated and background soil responses. We combined endpoint, time-weighted 24-h CO2 and CH4 flux partitioning with 13CO2 tracing of root-derived carbon, rhizosphere priming estimates, soil organic carbon fractionation into particulate organic carbon (POC) and mineral-associated organic carbon (MAOC), and metagenomic profiling. PFOS induced clear exposure-dependent and non-linear responses. Low-to-medium PFOS stimulated root-associated CO2 fluxes and maintained positive rhizosphere priming, whereas high PFOS suppressed rhizosphere CO2 and root respiration, weakened net plant CO2 uptake, and shifted soil organic carbon priming to a net negative response. In contrast, at H-P, MAOC was significantly higher than the control in both bulk and rhizosphere compartments, indicating that mineral-associated carbon retention can persist even when biological carbon processing weakens. Metagenomic profiling further suggested compartment-specific microbial filtering, reduced genetic potential for polymer depolymerization, and reweighted methane-related functions under PFOS exposure. Together, these results show that aqueous PFOS exposure can decouple gaseous carbon loss from mineral-associated carbon retention in controlled wetland-interface mesocosms. These findings indicate that lower gaseous carbon release under PFOS exposure should not be interpreted straightforwardly as stronger carbon-retention function or enhanced carbon sequestration, particularly without longer-term field validation.
Sustainable design and implementation of wastewater reuse in China have to achieve an optimum compromise among water resources augmenting, pollutants reduction and economic profit. A systematic framework with a multiobjective optimization model is first developed considering the trade-offs among wastewater reuse supplies and demands, costs and profits, as well as pollutants reduction. Pareto fronts of wastewater reuse optimization for 31 provinces of China are obtained through nondominated sorting genetic algorithm trials. The control strategies for each province are selected on the basis of regional water resources and water environment status. On the national level, the control strategies of wastewater reuse scale, BOD5 reduction, and economic profit are 15.39 billion cubic meters, 176.31 kilotons, and 9.68 billion RMB Yuan, respectively. The driving forces of water resources augmenting and water pollution control play more important roles than economic profit during wastewater reuse expanding in China. According to the optimal allocations, reclaimed wastewater should be intensively used in municipal, domestic, and recreative sectors in the regions suffering from quantity-related water scarcity, while it should be focused on industrial users in the regions suffering from quality-related water scarcity. The results present a general picture of wastewater reuse for policy makers in China.
Azole-linked covalent organic frameworks have drawn a lot of attention in photocatalytic synthesis of hydrogen peroxide, yet remain challenged by complex and costly synthetic routes. Here, we present a light-induced structural transformation strategy to facilely construct azole-linked covalent organic frameworks. We find that benzisoxazole linkages can be in-situ formed from imine linkages under light irradiation. As expected, the evolved partially benzisoxazole-linked covalent organic framework achieves a high hydrogen peroxide yield rate of 1986.9 μmol·g-1·h-1 in pure water. Theoretical calculations and spectral characterizations reveal significantly enhanced charge carrier separation and transfer efficiency, due to the formation of donor-acceptor structure. Furthermore, the in-situ formed benzisoxazole unit acts as both electron acceptor and catalytic center, promoting the reduction of dioxygen to superoxide radical, which is then converted into hydrogen peroxide, ultimately enhancing the yield. This work demonstrates a pioneering strategy for constructing benzisoxazole-linked covalent organic frameworks with high performance on hydrogen peroxide photo-synthesis.
Through a systematic review of 94 pieces of literature related to the impact of floating photovoltaic power stations on aquatic ecological environments,the effects of such power stations on abiotic factors in water bodies(water temperature,dissolved oxygen concentration,nutrient concentration,and pollutant distribution)and aquatic organisms(phytoplankton,aquatic plants,zooplankton,fishes,and birds)were analyzed.It concludes that the photovoltaic panel coverage ratio is the core factor driving ecological effects.Floating photovoltaic power stations reshape phytoplankton community structures through light-thermal coupled stress,inhibit the photosynthesis of submerged plants,alter fish metabolic rhythms and birds'migration behaviors,and trigger cross-trophic-level ecological cascade effects.By combining zonal layout and material optimization while balancing power generation benefits and ecological protection,a dynamic regulatory strategy for the floating photovoltaic coverage ratio is used:Coverage ratio in core water areas should be less than 30%,while that in ecological buffer zones should be set between 30%and 60%.It also points out the need for future research to further analyze the superimposed response mechanisms of photothermal effects and climate change,construct hydrodynamic-ecological coupling models,and promote the development of floating photovoltaic power generation toward a sustainable model featuring multi-energy complementarity and ecological synergy.
Electrocatalytic nitrate reduction has paraded widening attentions in simultaneously mitigating nitrogen-contaminant and producing ammonia under ambient conditions. Lattice hydrogen (Hlat) is a promising alternative proton source to boost nitrate hydrogenation kinetics, but its selective activation and utilization remain challenging. Herein, we propose a tailored pulsed strategy to filter active hydrogen species in interfacial microenvironment, thereby maximizing the participation of Hlat for nitrate hydrogenation. The designed PdAlH metallene delivers an impressive ammonia Faradaic efficiency of 98.53% and a yield rate of 11.63mgh-1 cm-2. The Hlat-mediated proton-coupled electron transfer and rapid Hlat dynamical reconstruction are both validated by in-situ characterization and theoretical calculation. For scale-up actual utilization, a membrane electrode assembly incorporating PdAlH is also built for sequential ammonia production, ultimately achieving stable operation for over 100h at industrial-level current densities and outstanding economic feasibility. Our work provides a novel modulation mechanism for Hlat-involved electrochemical reaction, enabling efficient large-scale nitrate remediation and sustainable ammonia resource recovery.
Using manure compost can be an effective strategy to sustain crop production, mitigate greenhouse gas (GHG) emissions, and promote soil organic carbon (SOC) sequestration. However, in the North China Plain (NCP)-a key food hub in China-the disconnect between livestock farms and croplands limits manure recycling, obscuring its potential environmental benefits and economic costs. This study employs a life cycle assessment method to quantify GHG and ammonia emissions, SOC sequestration, economic performance, and the eco-efficiency of wheat-maize production in the NCP across six livestock-cropland coupling scenarios: farmers' practice (FP), traditional household farming (HF), modern intensive decoupled systems with low (L), medium (M), and high (H) manure returning rates, and an intensive coupled system with optimum manure returning rate (IC). The results show that increasing manure return rates in intensive systems decreases the net global warming potential (NGWP), emphasizing the importance of livestock-cropland re-coupling. Emissions embodied in the field input supply chain was identified as a major NGWP contributor, while SOC accumulation significantly contributed to net GHG mitigation. The IC scenario is both the most economically viable ($322.8 (t grain)-1) and eco-efficient (1.03 kg CO2-eq USD-1) system. With the same compost application rates, intensive farming reduced the NGWP by 26.1% compared to household farming, despite trade-offs between GHG and NH3 emissions. The FP scenario had the highest climate impact (722.8 kg CO2-eq (t grain)-1) and the lowest eco-efficiency (4.91 kg CO2-eq USD-1). These insights advance our understanding of sustainable management practices for pursuing synergistic progress in economic gains, environmental conservation, and sustainable agricultural production.
Reservoirs play a critical role in addressing water resources challenges. However, their vertical influence on the assembly mechanisms of different microbial communities, including prokaryotes and eukaryotes, remains unclear. This study examined the vertical diversity patterns of abundant and rare subcommunities of prokaryotes and eukaryotes in an urban reservoir, using water depth as a geographical gradient and employing high-throughput sequencing. The impact of vertical environmental heterogeneity on community structure was quantified, and key drivers of these dynamics were identified. The results indicated that the urban reservoir exhibited statistically significant differences in the vertical distribution of water temperature and oxidation/reduction potential. The α-diversity of the abundant subcommunity displayed an opposing vertical pattern compared to that of the rare subcommunity, while the β-diversity for both subcommunities of prokaryotes and eukaryotes increased with water depth. Moreover, the distinct diversity patterns of abundant and rare subcommunities were associated with environmental heterogeneity and species adaptability. Notably, the β-diversity of the rare subcommunity of eukaryotes was primarily driven by species turnover in surface water, whereas nestedness became the dominant factor in deeper water. Furthermore, eukaryotic microbes exhibited a more pronounced response to changes in water depth than prokaryotes, consistent with the importance of heterogeneous selection to the eukaryotic community. Water temperature significantly affected the community composition of all groups, highlighting its importance in shaping community dynamics. This study provides valuable insights into the vertical distribution and assembly mechanisms of microbial communities in urban reservoirs, contributing to the protection and management of aquatic ecosystems under river regulation.
Piezo‐photocatalytic production of hydrogen peroxide (H 2 O 2 ) from water and air is promising but its large‐scale application is still challenging as insufficient reaction active sites and low reaction efficiency. We have applied molecular engineering methods to design an anthraquinone molecularly (AQ) grafted metal–organic framework piezo‐photocatalyst (UiO‐66‐AQ) for H 2 O 2 generation from water and air. The catalyst achieves a peak H 2 O 2 yield of 7872.4 μM g −1 h −1 by facilitating two critical reactions: single‐electron water oxidation (WOR) and two‐electron oxygen reduction (ORR) on spatially separated redox sites. Experiments and computational simulations reveal efficient charge separation through a ligand‐to‐chain transfer mechanism. Electrons and holes are selectively transferred to AQ and UiO‐66 promoting ORR and WOR under ultrasound and visible light. The high reaction rate of ORR (rapid generation of endoperoxide) compensates for the slow kinetics of WOR (generation of OH*) and greatly increases the rate of full‐reaction of H 2 O 2 production. Additionally, a continuous flow tubular reactor equipped with UiO‐66‐AQ catalytic membranes affords 96 % removal of organic dyes by a in situFenton process under visible light and water flow, confirming the significant potential of the catalyst for practical applications. This work deepens the understanding of directional carrier migration at piezo‐photocatalytic spatial separation sites, opening new pathways for environmentally friendly and efficient H 2 O 2 synthesis.