Hydrogen generated by electrochemical water splitting as electron donor for nitrate removal from micro-polluted reservoir water.

Extremely limited organic carbon sources and aerobic environment in micro-polluted reservoir water make conventional denitrification exceptionally challenging. As a result, total nitrogen (TN) concentration in most reservoir waters exceeds standard value year-round. In this study, for the first time, we constructed a mini water-lifting and aeration system (mini-WLAS) to remove nitrate in actual reservoir water. In the mini-WLAS, H2 was produced through electrolysis of reservoir water without adding any electrolyte, and the ascending water flow carried the generated H2 from lower layer to upper bacteria layer. The maximum denitrification rate reached 0.29 mg (L·d)-1 under dissolved oxygen (DO) concentration of 6-8 mg L-1, 6.04 times higher than that of the control group. There is almost no accumulation of NH4+-N, NO2--N, and N2O, and the concentration of CODMn decreased by 55.2 %. More importantly, the pH stayed near-neutral steadily throughout the whole process. Microbial community analysis showed that the abundances of hydrogenotrophic denitrifying bacteria (HDB) were 2 orders higher than those in the control system. Some HDB could work under aerobic conditions, providing an explanation for the excellent denitrification performance under high DO. This study provides a novel perspective for TN removal from reservoir water.

Impact of metal ions on PMS/Cl- disinfection efficacy: Enhancing or impeding microbial inactivation?

Peroxymonosulfate (PMS) is an eco-friendly disinfectant gaining attention. This study examined the influence of metal ions (Co(II), Cu(II), Fe(II)) on PMS disinfection with chloride ions (Cl-) against waterborne microorganisms, encompassing both bacteria and fungal spores. The findings elucidated that metal ions augment the inactivation of bacteria in the PMS/Cl- system while concurrently impeding the inactivation of fungal spores. Specifically, the PMS/Co(II)/Cl- process increased E. coli inactivation rates by 2.25 and 2.75 times compared to PMS/Co(II) and PMS/Cl-, respectively. Conversely, PMS/Me(II)/Cl- generally exhibited a diminished inactivation capacity against the three fungal spores compared to PMS/Cl-, albeit surpassing the efficacy of PMS/Me(II). For instance, the inactivation levels of A. niger by PMS/Cl-, PMS/Cu(II)/Cl-, and PMS/Cu(II) are 4.47-log, 1.92-log, and 0.11-log, respectively. Notably, fungal spores demonstrated a substantially higher resistance to disinfectants compared to bacteria. Differences in microbial susceptibility were linked to cell wall structure, composition, antioxidant defenses, and reactive species generation, such as hydroxyl radicals (•OH), sulfate radicals (SO4•-), and reactive chlorine species (RCS). This study demonstrated the novel and unique phenomenon of metal ions' dual role in modulating the PMS/Cl- disinfection process, which has not been reported before and has important implications for the field of water treatment.

Insights into the pH effect on hydrogen electrocatalysis.

Hydrogen electrocatalytic reactions, including the hydrogen evolution reaction (HER) and the hydrogen oxidation reaction (HOR), play a crucial role in a wide range of energy conversion and storage technologies. However, the HER and HOR display anomalous non-Nernstian pH dependent kinetics, showing two to three orders of magnitude sluggish kinetics in alkaline media compared to that in acidic media. Fundamental understanding of the origins of the intrinsic pH effect has attracted substantial interest from the electrocatalysis community. More critically, a fundamental molecular level understanding of this effect is still debatable, but is essential for developing active, stable, and affordable fuel cells and water electrolysis technologies. Against this backdrop, in this review, we provide a comprehensive overview of the intrinsic pH effect on hydrogen electrocatalysis, covering the experimental observations, underlying principles, and strategies for catalyst design. We discuss the strengths and shortcomings of various activity descriptors, including hydrogen binding energy (HBE) theory, bifunctional theory, potential of zero free charge (pzfc) theory, 2B theory and other theories, across different electrolytes and catalyst surfaces, and outline their interrelations where possible. Additionally, we highlight the design principles and research progress in improving the alkaline HER/HOR kinetics by catalyst design and electrolyte optimization employing the aforementioned theories. Finally, the remaining controversies about the pH effects on HER/HOR kinetics as well as the challenges and possible research directions in this field are also put forward. This review aims to provide researchers with a comprehensive understanding of the intrinsic pH effect and inspire the development of more cost-effective and durable alkaline water electrolyzers (AWEs) and anion exchange membrane fuel cells (AMFCs) for a sustainable energy future.

Enhanced inactivation of Aspergillus niger biofilms by the combination of UV-LEDs with chlorine-based disinfectants.

The presence of pathogenic fungal biofilms in drinking water distribution systems poses significant challenges in maintaining the safety of drinking water. This research delved into the formation of Aspergillus niger (A. niger) biofilms and evaluated their susceptibility to inactivation using combinations of ultraviolet light emitting diodes (UV-LEDs) with chlorine-based disinfectants, including UV-LEDs/chlorine (Cl2), UV-LEDs/chlorine dioxide (ClO2), and UV-LEDs/chloramine (NH2Cl) at 265 nm, 280 nm and 265/280 nm. Results indicated that A. niger biofilms reached initial maturity within 24 h, with matured three-dimensional filamentous structures and conidiospores by 96 h. UV-LEDs combined with chlorine-based disinfectants enhanced A. niger biofilm inactivation compared to UV-LEDs alone and low-pressure UV combined with chlorine-based disinfectants. At an UV fluence of 400 mJ/cm2, log reductions of UV265, UV280, and UV265/280 combined with chlorine-based disinfectants were 2.95-fold, 3.20-fold, and 2.38-fold higher than that of UV265, UV280, and UV265/280, respectively. During the inactivation, A. niger biofilm cells experienced increased membrane permeability and intracellular reactive oxygen species levels, resulting in cellular apoptosis. Extracellular polymeric substances contributed to the higher resistance of biofilms. Regarding electrical energy consumption, the order was: UV-LEDs/ClO2 > UV-LEDs/NH2Cl > UV-LEDs/Cl2. These findings provide insights into the effective utilization of UV-LEDs for fungal biofilm disinfection.

Qing-Luo-Yin Eased Adjuvant-Induced Arthritis by Inhibiting SIRT1-Controlled Visfatin Production in White Adipose Tissues.

Background: Nicotinamide adenine dinucleotide (NAD)-dependent deacetylase SIRT1 regulates both metabolism and immune functions. This study investigated if SIRT1 inhibitory property of herbal formula Qing-Luo-Yin (QLY) contributed to its anti-rheumatic effects. Methods: Adjuvant-induced arthritis (AIA) rats were treated by QLY and nicotinamide mononucleotide (NMN, a biosynthesis precursor of NAD) for 38 days. After sacrifice, blood, paws, liver and white adipose tissues (WAT) were collected. Pre-adipocytes were cultured by the rats' serum. The medium was used for monocytes culture. Some pre-adipocytes were treated by QLY-derived SIRT1 inhibitors. SIRT1 was silenced or overexpressed beforehand. The samples were subjected to kits-based quantification, polymerase-chain reaction, western-blot, immunofluorescence, and histology experiments. Results: AIA rats experienced significant fat loss in liver and WAT. Expression of many SIRT1-related signals like PPARγ, PGC-1α, HSL, ATGL and CPT-1A were altered. QLY attenuated all these abnormalities and joint injuries. By pan-acetylation up-regulation, visfatin was obviously reduced in QLY-treated AIA rats' blood (from 191.8 to 127.0 pg/mL). NMN sustained SIRT1 activation by replenishing NAD, and weakened these effects. QLY-containing serum and the related compounds showed similar impacts on pre-adipocytes, resembling the changes in QLY-treated AIA rats' WAT. These treatments suppressed AIA serum-induced visfatin secretion (from 49.3 to 36.1 and 30.7 pg/mL). This effect was impaired by SIRT1 overexpression. The medium from the compounds-treated pre-adipocytes impaired NF-κB activation in AIA serum-cultured monocytes. Conclusion: Besides fat depletion, SIRT1 up-regulation in rheumatic subjects' WAT promotes visfatin production, and exacerbates inflammation. SIRT1 inhibition in WAT is an anti-rheumatic way of QLY independent of immune regulation.

Enhanced ammonia nitration by Bio-Electrochemical systems with constructed wetlands.

The insufficient abundance of electron acceptors for ammonia during electron transfer in constructed wetlands (CWs) results in low nitrification rates. This study developed a green, low-carbon CWs enhanced by a bio-electrochemical systems (BESs-CWs) to achieve efficient ammonia (NH4+-N) removal. Electrode enhancement significantly promoted NH4+-N removal. Compared with traditional CWs, the average removal efficiency of NH4+-N in the BESs-CWs increased from 62.9 % to 90.6 %. The intermittent voltage driven by the photovoltaic power system caused minimal plant stress. However, electrode enhancement significantly affected microbial communities involved in short-path nitrification and denitrification within the biofilm. Specifically, the removal rate of NH4+-N by BESs-CWs under electrode enhancement was increased by 27.7 % compared to traditional CWs, enhancing the electron output of NH4+-N in the BESs-CWs. This system provides a method of ammonia nitration for CWs under poor electron acceptor conditions.

Aerobic denitrifying bacterial community with low C/N ratio remove nitrate from micro-polluted water: Metagenomics unravels denitrification pathways.

The efficient nitrogen removal from micro-polluted source water is an international challenge to be solved urgently. However, the inner denitrification mechanism of native aerobic denitrifying bacterial communities in response to carbon scarcity remains relatively unclear. Here, the bacterial community XT6, screened from an oligotrophic reservoir, exhibited aerobic denitrifying capacity under low-carbon environments. Up to 76.79-81.64 % of total organic carbon (TOC) and 51.48-67.60 % of NO3--N were removed by XT6 within 48 h at C/N ratios of 2.0-3.0. Additionally, the nitrogen balance experiments further manifested that 26.27-38.13 % of NO3--N was lost in gaseous form. As the C/N ratio decreased, XT6 tended to generate more extracellular polymeric substances (EPS), with the tightly bound EPS showing the largest increase. Pseudomonas and Variovorax were quite abundant in XT6, constituting 59.69 % and 28.65 % of the total sequences, respectively. Furthermore, metagenomics analysis evidenced that XT6 removed TOC and nitrate mainly through the tricarboxylic acid cycle and aerobic denitrification. Overall, the abovementioned results provide a deeper understanding of the nitrogen metabolic pathways of indigenous aerobic denitrifying bacterial communities with low C/N ratios and offer useful guidance for controlling nitrogen pollution in oligotrophic ecosystems.

Emergency control of dinoflagellate bloom in freshwater with chlorine enhanced by solar radiation: Efficiency and mechanism.

Dinoflagellate requires a lower temperature and blooms frequently in the spring and autumn compared to regular cyanobacteria. The outbreak of dinoflagellate bloom will also lead to the death of some aquatic organisms. However, research on freshwater dinoflagellates is still lacking due to the challenges posed by classification and culture in laboratory. The removal effect and mechanism of Peridinium umbonatum (P. umbonatum, a typical dinoflagellate) were investigated using solar/chlorine in this study. The effect of simulated solar alone on the removal of algae was negligible, and chlorine alone had only a slight effect in removing algae. However, solar/chlorine showed a better removal efficiency with shoulder length reduction factor and kmax enhancement factor of 2.80 and 3.8, respectively, indicating a shorter latency period and faster inactivation rate for solar/chlorine compared to solar and chlorine alone. The removal efficiency of algae gradually increased with the chlorine dosage, but it dropped as the cell density grew. When the experimental temperature was raised to 30 °C, algal removal efficiency significantly increased, as the temperature was unsuitable for the survival of P. umbonatum. Attacks on cell membranes by chlorine and hydroxyl radicals (•OH) produced by solar/chlorine led to a decrease in cell membrane integrity, leading to a rise in intracellular reactive oxygen species and an inhibition of photosynthetic and antioxidant systems. Cell regeneration was not observed in either the chlorine or solar/chlorine systems due to severe cell damage or cysts formation. In addition, natural solar radiation was demonstrated to have the same enhancing effect as simulated solar radiation. However, the algal removal efficiency of solar/chlorine in real water was reduced compared to 119 medium, mainly due to background material in the real water substrate that consumed the oxidant or acted as shading agents.

Transformation of p-arsanilic acid by dissolved Mn(III) and enhanced arsenic removal: Mechanism, toxicity and performance in complicated water matrices.

Dissolved Mn(III), as a potent one-electron transfer oxidant, is ubiquitous in natural waters and sediments and actively involved in the transformation of organics in biogeochemical processes and water treatment. However, the important role of Mn(III) has long been overlooked because of its short life. This study was the first to investigate the performance of Mn(III) in organoarsenic transformation and to highlight the environmental implications. Both homogeneous and heterogeneous Mn(III)-based systems were effective to remove p-arsanilic acid (p-ASA, 15 µM) with degradation efficiency approaching 40.4 %-98.3 %. Two degradation pathways of p-ASA were proposed, in which As-C bond and amino group were vulnerable sites to Mn(III) attack, leading to the formation of more toxic arsenate (As(V)) and nitarsone. Through transforming organoarsenic to inorganic arsenic species, the removal efficiency of total arsenic and dissolved organics were enhanced to 65.1 %-95.5 % and 16.6 %-36.6 %, respectively, by post-treatment of coagulation or adsorption, accompanied with significant reduction of cytotoxicity and environmental risks. Particularly, polymeric ferric sulfate and granular activated alumina showed superior performance in the total As removal. Moreover, oxidation efficiency of Mn(III) was hardly affected by common cations and anions (e.g., Ca2+, Mg2+, NH4+, NO3-, SO4-), halide ions (e.g., Cl-, Br-) and natural organic matter, showing high robustness for organoarsenic removal under complicated water matrices. Overall, this study shed light on the significance of Mn(III) to the fate of organoarsenics in manganese-rich environments, and demonstrated the promising potential of Mn(III)-based strategies to achieve targeted decontamination in water/wastewater purification.

Modulating the RPS27A/PSMD12/NF-κB pathway to control immune response in mouse brain ischemia-reperfusion injury.

BACKGROUND: Investigating immune cell infiltration in the brain post-ischemia-reperfusion (I/R) injury is crucial for understanding and managing the resultant inflammatory responses. This study aims to unravel the role of the RPS27A-mediated PSMD12/NF-κB axis in controlling immune cell infiltration in the context of cerebral I/R injury. METHODS: To identify genes associated with cerebral I/R injury, high-throughput sequencing was employed. The potential downstream genes were further analyzed using Gene Ontology (GO), Kyoto Encyclopedia of Genes and Genomes (KEGG), and Protein-Protein Interaction (PPI) analyses. For experimental models, primary microglia and neurons were extracted from the cortical tissues of mouse brains. An in vitro cerebral I/R injury model was established in microglia using the oxygen-glucose deprivation/reoxygenation (OGD/R) technique. In vivo models involved inducing cerebral I/R injury in mice through the middle cerebral artery occlusion (MCAO) method. These models were used to assess neurological function, immune cell infiltration, and inflammatory factor release. RESULTS: The study identified RPS27A as a key player in cerebral I/R injury, with PSMD12 likely acting as its downstream regulator. Silencing RPS27A in OGD/R-induced microglia decreased the release of inflammatory factors and reduced neuron apoptosis. Additionally, RPS27A silencing in cerebral cortex tissues mediated the PSMD12/NF-κB axis, resulting in decreased inflammatory factor release, reduced neutrophil infiltration, and improved cerebral injury outcomes in I/R-injured mice. CONCLUSION: RPS27A regulates the expression of the PSMD12/NF-κB signaling axis, leading to the induction of inflammatory factors in microglial cells, promoting immune cell infiltration in brain tissue, and exacerbating brain damage in I/R mice. This study introduces novel insights and theoretical foundations for the treatment of nerve damage caused by I/R, suggesting that targeting the RPS27A and downstream PSMD12/NF-κB signaling axis for drug development could represent a new direction in I/R therapy.

Response of the algal-bacterial community to thermal stratification succession in a deep-water reservoir: Community structure, co-assembly patterns, and functional groups.

Thermal stratification in lakes and reservoirs may intensify and become more persistent with global warming. Periodic thermal stratification is a naturally occurring phenomenon that indicates a transition in aquatic ecosystem homeostasis, which could lead to the deterioration of water quality and impaired aquatic communities. However, the responses of communities and associated nutrient cycling processes to periodic thermal stratification are still poorly understood. This study delved into the changes in water quality, algal-bacterial communities, and functional diversity influenced by thermal stratification succession, and their relationship with nutrient cycling. The results indicated that the apparent community dynamics were driven by environmental factors, with ammonium (NH4+) and nitrate (NO3--N) being the most important factors that influenced the algal and bacterial community structure, respectively. Ecological niche widths were narrower during thermal stratification, exacerbating the antagonism of the communities, and stochastic processes dominated community assembly. Then, the complexities of the co-occurrence network decreased with succession. Algal community assembly became more deterministic, while bacterial assembly became more stochastic. Moreover, the roles of algal-bacterial multidiversity in nutrient cycling differed: bacterial diversity enhanced nutrient cycling, whereas algal diversity had the opposite effect. These findings broadened our understanding of microbial ecological mechanisms to environmental change and provided valuable ecological knowledge for securing water supplies in drinking water reservoirs.

Review of cathodic electroactive bacteria: Species, properties, applications and electron transfer mechanisms.

Cathodic electroactive bacteria (C-EAB) which are capable of accepting electrons from solid electrodes provide fresh avenues for pollutant removal, biosensor design, and electrosynthesis. This review systematically summarized the burgeoning applications of the C-EAB over the past decade, including 1) removal of nitrate, aromatic derivatives, and metal ions; 2) biosensing based on biocathode; 3) electrosynthesis of CH4, H2, organic carbon, NH3, and protein. In addition, the mechanisms of electron transfer by the C-EAB are also classified and summarized. Extracellular electron transfer and interspecies electron transfer have been introduced, and the electron transport mechanism of typical C-EAB, such as Shewanella oneidensis MR-1, has been combed in detail. By bringing to light this cutting-edge area of the C-EAB, this review aims to stimulate more interest and research on not only exploring great potential applications of these electron-accepting bacteria, but also developing steady and scalable processes harnessing biocathodes.

Asymmetric dearomatization of benzyl 1-naphthyl ethers via [1,3] O-to-C rearrangement.

A catalytic asymmetric dearomatization reaction of benzyl 1-naphthyl ethers accelerated by a chiral N,N'-dioxide/Co(II) complex is disclosed. The reaction proceeds via an enantioselective [1,3] O-to-C rearrangement through a tight ion-pair pathway, providing a wide array of α-naphthalenone derivatives bearing an all-carbon quaternary center in high yields with excellent ee values.

Disentangling the assembly patterns and drivers of microbial communities during thermal stratification and mixed periods in a deep-water reservoir.

Effect of periodic thermal stratification in deep-water reservoirs on aquatic ecosystems has been a research hotspot. Nevertheless, there is limited information on the response patterns of microbial communities to environmental changes under such specialized conditions. To fill this gap, samples were collected from a typical deep-water reservoir during the thermal stratification period (SP) and mixed period (MP). Three crucial questions were answered: 1) How microbial communities develop with stratified to mixed succession, 2) how the relative importance of stochastic and deterministic processes to microbial community assembly, shifted in two periods, and 3) how environmental variables drive microbial co-occurrence networks and functional group alteration. We used Illumina Miseq high-throughput sequencing to investigate the dynamics of the microbial community over two periods, constructed molecular ecological networks (MENs), and unraveled assembly processes based on null and neutral models. The results indicated that a total of 33.9 % and 27.7 % of bacterial taxa, and 23.1 % and 19.4 % of fungal taxa were enriched in the stratified and mixed periods, respectively. Nitrate, water temperature, and total phosphorus drove the variation of microbial community structure. During the thermal stratification period, stochastic processes (dispersal limitation) and deterministic processes (variable selection) dominated the assembly of bacterial and fungal communities, followed by a shift to stochastic processes dominated by dispersal limitation in two communities. The MENs results revealed that thermal stratification-induced environmental stresses increased the complexity of microbial networks but decreased its robustness, resulting in more vulnerable ecological networks. Therefore, this work provides critical ecological insights for the longevity and sustainability of water quality management in an artificially regulated engineered system.

Exserolide J ameliorates lipid accumulation in vitro by regulating liver X receptor alpha and peroxisome proliferator-activated receptor alpha proteins.

Exserolides are isocoumarin derivatives containing lactone moiety. Recently, some isocoumarins have been demonstrated to ameliorate hyperlipidemia, a major factor for inducing cardiovascular diseases. However, the effects and mechanisms of action of exserolides on hyperlipidemia are not known. The aim of this study is to investigate whether the marine fungus Setosphaeria sp.-derived exserolides (compounds I, J, E, and F) exert lipid-lowering effects via improving reverse cholesterol transport (RCT) in vitro. RAW264.7 macrophages and HepG2 cells were used to establish lipid-laden models, and the levels of intracellular lipids and RCT-related proteins were determined by assay kits and Western blotting, respectively. We observed that exserolides (at a 5 µM concentration) significantly decreased intracellular cholesterol and triglyceride levels in oxidized low-density lipoprotein-laden RAW264.7 cells and markedly improved [3H]-cholesterol efflux. Among the four tested compounds, exserolide J increased the protein levels of ATP-binding cassette transporter A1, peroxisome proliferator-activated receptor α (PPARα), and liver X receptor α (LXRα). Furthermore, treatment with exserolides significantly decreased oleic acid-laden lipid accumulation in HepG2 hepatocytes. Mechanistically, exserolides enhance PPARα protein levels; furthermore, compound J increases cholesterol 7 alpha-hydroxylase A1 and LXRα protein levels. Molecular docking revealed that exserolides, particularly compound J, can interact with PPARα and LXRα proteins. These data suggest that the terminal carboxyl group of compound J plays a key role in lowering lipid levels by stimulating LXRα and PPARα proteins. In conclusion, compound J exhibits powerful lipid-lowering effects in vitro. However, its hypolipidemic effects in vivo should be investigated in the future.

Formation of filamentous fungal biofilms in water and the transformation of resistance to chlor(am)ine disinfection.

Biofilms are composed of complex multi-species in nature, potentially threatening drinking water safety. In this work, the formation of single- and multi-species fungal biofilms formed by Aspergillus niger (A. niger) and Aspergillus flavus (A. flavus), and the inactivation of mature biofilms using chlor(am)ine were firstly investigated. Results revealed that the antagonistic interaction occurred between A. niger and A. flavus. Chloramination at 20 mg/L for 30 min achieved 74.74 % and 76.04 % inactivation of A. flavus and multi-species biofilm, which were 1.69- and 1.84-fold higher than that of chlorine at the same condition. However, no significant difference was observed in the inactivation of A. niger biofilm between chlorine and monochloramine disinfection due to the lower amount of extracellular polymeric substance produced by it (p > 0.05). The inactivation of biofilm by monochloramine fitted the Weibull model well. According to the Weibull model, the monochloramine resistance of biofilm were as follows: A. flavus > multi-species > A. niger biofilm. Besides, an increase in reactive oxygen levels, damage of cell membrane, and leakage of intracellular substances in biofilms were observed after chlor(am)ination. More intracellular polysaccharides and proteins were leaked in chloramination inactivation (p < 0.05). This study provides important implications for controlling fungal biofilm.

Solar/ClO2 system inactivates fungal spores in drinking water: Synergy, efficiency and mechanisms.

The risk of fungal pollution in drinking water has been paid attention. Solar/chlorine dioxide (ClO2) combined system is an environment-friendly, economical and efficient disinfection method, especially for countries and regions that are economically backward and still exposed to unsafe drinking water. In this paper, the kinetics, influencing factors, mechanism and regrowth potential of inactivated Aspergillus niger (A. niger) spores by solar/ClO2 were reported for the first time. The inactivation curve can be divided into three stages: instant inactivation within 1-2 min, slow linear inactivation and finally a tail. The synergistic factors produced by solar/ClO2 in terms of log reduction and maximum inactivation rate were 1.194 and 1.112, respectively. The inhibitory effect on the regrowth of A. niger spores inactivated by solar/ClO2 was also stronger than that by ClO2 alone. Strongly oxidizing reactive species produced by solar/ClO2 accelerated the accumulation of endogenic reactive oxygen species (ROS) caused by oxidation stress of A. niger spores, improving the inactivation ability of the system. The inactivation order of A. niger spores was: loss of culturability, accumulation of intracellular ROS, loss of membrane integrity, leakage of intracellular species and change of morphology. The inactivation performance of solar/ClO2 was better than solar/chlor(am)ine according to the comparison of inactivation efficiency and regrowth potential. Results also suggested that solar/ClO2 process was more suitable for the treatment of ground water sources.