New method for efficient control of hydrogen sulfide and methane in gravity sewers: Combination of NaOH and nitrite

• The combination of NaOH and nitrite was used to control harmful gas in sewers. • Hydrogen sulfide and methane in airspace were reduced by 96.01% and 91.49%. • Changes in sewage quality and greenhouse effect by chemical dosing were negligible. • The strong destructive effects on biofilm slowed down the recovery of harmful gases. • The cost of the method was only 3.92 × 10⁻³ $/m³. An innovative treatment method by the combination of NaOH and nitrite is proposed for controlling hydrogen sulfide and methane in gravity sewers and overcome the drawbacks of the conventional single chemical treatment. Four reactors simulating gravity sewers were set up to assess the effectiveness of the proposed method. Findings demonstrated hydrogen sulfide and methane reductions of about 96.01% and 91.49%, respectively, by the combined addition of NaOH and nitrite. The consumption of NaNO₂ decreased by 42.90%, and the consumption rate of NaOH also showed a downward trend. Compared with a single application of NaNO₂, the C/N ratio of wastewater was increased to about 0.61 mg COD/mg N. The greenhouse effect of intermediate N₂O and residual methane was about 48.80 gCO₂/m³, which is far lower than that of methane without control (260 gCO₂/m³). Biofilm was destroyed to prevent it from entering the sewage by the chemical additives, which reduced the biomass and inhibited the recovery of biofilm activity to prolong the control time. The sulfide production rate and sulfate reduction rate were reduced by 92.32% and 85.28%, respectively. Compared with conventional control methods, the cost of this new method was only 3.92 × 10⁻³ $/m³, which is potentially a cost-effective strategy for sulfide and methane control in gravity sewers.     

Enhanced triallyl isocyanurate (TAIC) degradation through application of an O3/UV process: Performance optimization and degradation pathways

• UV/O₃ process had higher TAIC mineralization rate than O₃ process. • Four possible degradation pathways were proposed during TAIC degradation. • pH impacted oxidation processes with pH of 9 achieving maximum efficiency. • CO₃^2– negatively impacted TAIC degradation while HCO₃^– not. • Cl^– can be radicals scavenger only at high concentration (over 500 mg/L Cl^–). Triallyl isocyanurate (TAIC, C₁₂H₁₅N₃O₃) has featured in wastewater treatment as a refractory organic compound due to the significant production capability and negative environmental impact. TAIC degradation was enhanced when an ozone(O₃)/ultraviolet(UV) process was applied compared with the application of an independent O₃ process. Although 99% of TAIC could be degraded in 5 min during both processes, the O₃/UV process had a 70%mineralization rate that was much higher than that of the independent O₃ process (9%) in 30 min. Four possible degradation pathways were proposed based on the organic compounds of intermediate products identified during TAIC degradation through the application of independent O₃ and O₃/UV processes. pH impacted both the direct and indirect oxidation processes. Acidic and alkaline conditions preferred direct and indirect reactions respectively, with a pH of 9 achieving maximum Total Organic Carbon (TOC) removal. Both CO₃^2– and HCO₃^– decreased TOC removal, however only CO₃^2– negatively impacted TAIC degradation. Effects of Cl^– as a radical scavenger became more marked only at high concentrations (over 500 mg/L Cl^–). Particulate and suspended matter could hinder the transmission of ultraviolet light and reduce the production of HO· accordingly.     

Evaluation of the technoeconomic feasibility of electrochemical hydrogen peroxide production for decentralized water treatment

• Gas diffusion electrode (GDE) is a suitable setup for practical water treatment. • Electrochemical H₂O₂ production is an economically competitive technology. • High current efficiency of H₂O₂ production was obtained with GDE at 5–400 mA/cm². • GDE maintained high stability for H₂O₂ production for ~1000 h. • Electro-generation of H₂O₂ enhances ibuprofen removal in an E-peroxone process. This study evaluated the feasibility of electrochemical hydrogen peroxide (H₂O₂) production with gas diffusion electrode (GDE) for decentralized water treatment. Carbon black-polytetrafluoroethylene GDEs were prepared and tested in a continuous flow electrochemical cell for H₂O₂ production from oxygen reduction. Results showed that because of the effective oxygen transfer in GDEs, the electrode maintained high apparent current efficiencies (ACEs,>80%) for H₂O₂ production over a wide current density range of 5–400 mA/cm², and H₂O₂ production rates as high as ~202 mg/h/cm² could be obtained. Long-term stability test showed that the GDE maintained high ACEs (>85%) and low energy consumption (<10 kWh/kg H₂O₂) for H₂O₂ production for 42 d (~1000 h). However, the ACEs then decreased to ~70% in the following 4 days because water flooding of GDE pores considerably impeded oxygen transport at the late stage of the trial. Based on an electrode lifetime of 46 days, the overall cost for H₂O₂ production was estimated to be ~0.88 $/kg H₂O₂, including an electricity cost of 0.61 $/kg and an electrode capital cost of 0.27 $/kg. With a 9 cm² GDE and 40 mA/cm² current density, ~2–4 mg/L of H₂O₂ could be produced on site for the electro-peroxone treatment of a 1.2 m³/d groundwater flow, which considerably enhanced ibuprofen abatement compared with ozonation alone (~43%–59% vs. 7%). These findings suggest that electrochemical H₂O₂ production with GDEs holds great promise for the development of compact treatment technologies for decentralized water treatment at a household and community level.     

Electro-catalytic activity of CeOx modified graphite felt for carbamazepine degradation via E-peroxone process

•CeO_x/GF-EP process had the better degradation efficiency than GF-EP process. •CeO_x/GF-EP process had the flexible application in the pH range from 5.0 to 9.0. •CeO_x could enhance surface hydrophilicity and reduce the charge-transfer resistance. •The interfacial electron transfer process was revealed. E-peroxone (EP) was one of the most attractive AOPs for removing refractory organic compounds from water, but the high energy consumption for in situ generating H₂O₂ and its low reaction efficiency for activating O₃ under acidic conditions made the obstacles for its practical application. In this study, cerium oxide was loaded on the surface of graphite felt (GF) by the hydrothermal method to construct the efficient electrode (CeO_x/GF) for mineralizing carbamazepine (CBZ) via EP process. CeO_x/GF was an efficient cathode, which led to 69.4% TOC removal in CeO_x/GF-EP process with current intensity of 10 mA in 60 min. Moreover, CeO_x/GF had the flexible application in the pH range from 5.0 to 9.0, TOC removal had no obvious decline with decrease of pH. Comparative characterizations showed that CeO_x could enhance surface hydrophilicity and reduce the charge-transfer resistance of GF. About 5.4 mg/L H₂O₂ generated in CeO_x/GF-EP process, which was 2.1 times as that in GF-EP process. The greater ozone utility was also found in CeO_x/GF-EP process. More O₃ was activated into hydroxyl radicals, which accounted for the mineralization of CBZ. An interfacial electron transfer process was revealed, which involved the function of oxygen vacancies and Ce³⁺/Ce⁴⁺ redox cycle. CeO_x/GF had the good recycling property in fifth times’ use.     

Techno-economic characteristics of wastewater treatment plants retrofitted from the conventional activated sludge process to the membrane bioreactor process

• Retrofitting from CAS to MBR increased effluent quality and environmental benefits. • Retrofitting from CAS to MBR increased energy consumption but not operating cost. • Retrofitting from CAS to MBR increased the net profit and cost efficiency. • The advantage of MBR is related to the adopted effluent standard. • The techno-economy of MBR improves with stricter effluent standards. While a growing number of wastewater treatment plants (WWTPs) are being retrofitted from the conventional activated sludge (CAS) process to the membrane bioreactor (MBR) process, the debate on the techno-economy of MBR vs. CAS has continued and calls for a thorough assessment based on techno-economic valuation. In this study, we analyzed the operating data of 20 large-scale WWTPs (capacity≥10000 m³/d) and compared their techno-economy before and after the retrofitting from CAS to MBR. Through cost-benefit analysis, we evaluated the net profit by subtracting the operating cost from the environmental benefit (estimated by the shadow price of pollutant removal and water reclamation). After the retrofitting, the removal rate of pollutants increased (e.g., from 89.0% to 93.3% on average for NH₃-N), the average energy consumption increased from 0.40 to 0.57 kWh/m³, but the operating cost did not increase significantly. The average marginal environmental benefit increased remarkably (from 0.47 to 0.66 CNY/g for NH₃-N removal), leading to an increase in the average net profit from 19.4 to 24.4 CNY/m³. We further scored the technical efficiencies via data envelopment analysis based on non-radial directional distance functions. After the retrofitting, the relative cost efficiency increased from 0.70 to 0.73 (the theoretical maximum is 1), while the relative energy efficiency did not change significantly. The techno-economy is closely related to the effluent standard adopted, particularly when truncating the extra benefit of pollutant removal beyond the standard in economic modeling. The modeling results suggested that MBR is more profitable than CAS given stricter effluent standards.     

Electricity-driven ammonia oxidation and acetate production in microbial electrosynthesis systems

• MES was constructed for simultaneous ammonia removal and acetate production. • Energy consumption was different for total nitrogen and ammonia nitrogen removal. • Energy consumption for acetate production was about 0.04 kWh/g. • Nitrate accumulation explained the difference of energy consumption. • Transport of ammonia and acetate across the membrane deteriorated the performance. Microbial electrosynthesis (MES) is an emerging technology for producing chemicals, and coupling MES to anodic waste oxidation can simultaneously increase the competitiveness and allow additional functions to be explored. In this study, MES was used for the simultaneous removal of ammonia from synthetic urine and production of acetate from CO₂. Using graphite anode, 83.2%±5.3% ammonia removal and 28.4%±9.9% total nitrogen removal was achieved, with an energy consumption of 1.32 kWh/g N for total nitrogen removal, 0.45 kWh/g N for ammonia nitrogen removal, and 0.044 kWh/g for acetate production. Using boron-doped diamond (BDD) anode, 70.9%±12.1% ammonia removal and 51.5%±11.8% total nitrogen removal was obtained, with an energy consumption of 0.84 kWh/g N for total nitrogen removal, 0.61 kWh/g N for ammonia nitrogen removal, and 0.043 kWh/g for acetate production. A difference in nitrate accumulation explained the difference of total nitrogen removal efficiencies. Transport of ammonia and acetate across the membrane deteriorated the performance of MES. These results are important for the development of novel electricity-driven technologies for chemical production and pollution removal.     

One-pot hydrothermal fabrication of BiVO4/Fe3O4/rGO composite photocatalyst for the simulated solar light-driven degradation of Rhodamine B

• BiVO₄/Fe₃O₄/rGO has excellent photocatalytic activity under solar light radiation. • It can be easily separated and collected from water in an external magnetic field. • BiVO₄/Fe₃O₄/0.5% rGO exhibited the highest RhB removal efficiency of over 99%. • Hole (h⁺) and superoxide radical (O₂^•−) dominate RhB photo-decomposition process. • The reusability of this composite was confirmed by five successive recycling runs. Fabrication of easily recyclable photocatalyst with excellent photocatalytic activity for degradation of organic pollutants in wastewater is highly desirable for practical application. In this study, a novel ternary magnetic photocatalyst BiVO₄/Fe₃O₄/reduced graphene oxide (BiVO₄/Fe₃O₄/rGO) was synthesized via a facile hydrothermal strategy. The BiVO₄/Fe₃O₄ with 0.5 wt% of rGO (BiVO₄/Fe₃O₄/0.5% rGO) exhibited superior activity, degrading greater than 99% Rhodamine B (RhB) after 120 min solar light radiation. The surface morphology and chemical composition of BiVO₄/Fe₃O₄/rGO were studied by scanning electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, UV–visible diffuse reflectance spectroscopy, Fourier transform infrared spectroscopy, and Raman spectroscopy. The free radicals scavenging experiments demonstrated that hole (h⁺) and superoxide radical (O₂^•−) were the dominant species for RhB degradation over BiVO₄/Fe₃O₄/rGO under solar light. The reusability of this composite catalyst was also investigated after five successive runs under an external magnetic field. The BiVO₄/Fe₃O₄/rGO composite was easily separated, and the recycled catalyst retained high photocatalytic activity. This study demonstrates that catalyst BiVO₄/Fe₃O₄/rGO possessed high dye removal efficiency in water treatment with excellent recyclability from water after use. The current study provides a possibility for more practical and sustainable photocatalytic process.     

Optimization of the O3/H2O2 process with response surface methodology for pretreatment of mother liquor of gas field wastewater

• Real ML-GFW with high salinity and high organics was degraded by O₃/H₂O₂ process. • Successful optimization of operation conditions was attained using RSM based on CCD. • Single-factor experiments in advance ensured optimal experimental conditions. • The satisfactory removal efficiency of TOC was achieved in spite of high salinity. • The initial pH plays the most significant role in the degradation of ML-GFW. The present study reports the use of the O₃/H₂O₂ process in the pretreatment of the mother liquor of gas field wastewater (ML-GFW), obtained from the multi-effect distillation treatment of the gas field wastewater. The range of optimal operation conditions was obtained by single-factor experiments. Response surface methodology (RSM) based on the central composite design (CCD) was used for the optimization procedure. A regression model with Total organic carbon (TOC) removal efficiency as the response value was established (R² = 0.9865). The three key factors were arranged according to their significance as: pH>H₂O₂ dosage>ozone flow rate. The model predicted that the best operation conditions could be obtained at a pH of 10.9, an ozone flow rate of 0.8 L/min, and H₂O₂ dosage of 6.2 mL. The dosing ratio of ozone was calculated to be 9.84 mg O₃/mg TOC. The maximum removal efficiency predicted was 75.9%, while the measured value was 72.3%. The relative deviation was found to be in an acceptable range. The ozone utilization and free radical quenching experiments showed that the addition of H₂O₂ promoted the decomposition of ozone to produce hydroxyl radicals (·OH). This also improved the ozone utilization efficiency. Gas chromatography-mass spectrometry (GC-MS) analysis showed that most of the organic matters in ML-GFW were degraded, while some residuals needed further treatment. This study provided the data and the necessary technical supports for further research on the treatment of ML-GFW.     

Sulfur cycle as an electron mediator between carbon and nitrate in a constructed wetland microcosm

• Fe(III) accepted the most electrons from organics, followed by NO₃^‒, SO₄^2‒, and O₂. • The electrons accepted by SO₄^2‒ could be stored in the solid AVS, FeS₂-S, and S⁰. • The autotrophic denitrification driven by solid S had two-phase characteristics. • A conceptual model involving electron acceptance, storage, and donation was built. • S cycle transferred electrons between organics and NO₃^‒ with an efficiency of 15%. A constructed wetland microcosm was employed to investigate the sulfur cycle-mediated electron transfer between carbon and nitrate. Sulfate accepted electrons from organics at the average rate of 0.84 mol/(m³·d) through sulfate reduction, which accounted for 20.0% of the electron input rate. The remainder of the electrons derived from organics were accepted by dissolved oxygen (2.6%), nitrate (26.8%), and iron(III) (39.9%). The sulfide produced from sulfate reduction was transformed into acid-volatile sulfide, pyrite, and elemental sulfur, which were deposited in the substratum, storing electrons in the microcosm at the average rate of 0.52 mol/(m³·d). In the presence of nitrate, the acid-volatile and elemental sulfur were oxidized to sulfate, donating electrons at the average rate of 0.14 mol/(m³·d) and driving autotrophic denitrification at the average rate of 0.30 g N/(m³·d). The overall electron transfer efficiency of the sulfur cycle for autotrophic denitrification was 15.3%. A mass balance assessment indicated that approximately 50% of the input sulfur was discharged from the microcosm, and the remainder was removed through deposition (49%) and plant uptake (1%). Dominant sulfate-reducing (i.e., Desulfovirga, Desulforhopalus, Desulfatitalea, and Desulfatirhabdium) and sulfur-oxidizing bacteria (i.e., Thiohalobacter, Thiobacillus, Sulfuritalea, and Sulfurisoma), which jointly fulfilled a sustainable sulfur cycle, were identified. These results improved understanding of electron transfers among carbon, nitrogen, and sulfur cycles in constructed wetlands, and are of engineering significance.     

A pulsed switching peroxi-coagulation process to control hydroxyl radical production and to enhance 2,4-Dichlorophenoxyacetic acid degradation

• A new pulsed switching peroxi-coagulation (PSPC) system was developed. • The EC_T for 2,4-D removal in the PSPC was lower than that in the EF. • The iron consumption for 2,4-D removal in the PSPC was lower than that in the PC. The aim of this study was to develop a new pulsed switching peroxi-coagulation system to control hydroxyl radical (?OH) production and to enhance 2,4-Dichlorophenoxyacetic acid (2,4-D) degradation. The system was constructed with a sacrifice iron anode, a Pt anode, and a gas diffusion cathode. Production of H₂O₂ and Fe²⁺ was controlled separately by time delayers with different pulsed switching frequencies. Under current densities of 5.0 mA/cm² (H₂O₂) and 0.5 mA/cm² (Fe²⁺), the ?OH production was optimized with the pulsed switching frequency of 1.0 s (H₂O₂):0.3 s (Fe²⁺) and the ratio of H₂O₂ to Fe²⁺ molar concentrations of 6.6. Under the optimal condition, 2,4-D with an initial concentration of 500 mg/L was completely removed in the system within 240 min. The energy consumption for the 2,4-D removal in the system was much lower than that in the electro-Fenton process (68±6 vs. 136±10 kWh/kg TOC). The iron consumption in the system was ~20 times as low as that in the peroxi-coagulation process (196±20 vs. 3940±400 mg/L) within 240 min. The system should be a promising peroxi-coagulation method for organic pollutants removal in wastewater.     

Evolution of humic substances in polymerization of polyphenol and amino acid based on non-destructive characterization

• Humification evolution was identified with non-destructive characterization method. • Humification process from precursors to fulvic and humic acid was confirmed. • MnO₂ alone had limited oxidation ability to form HA. • MnO₂ played a key role as a catalyst to transform FA to HA in the presence of O₂. • MnO₂ could affect the structure of the humification products. Abiotic humification is important in the formation and evolution of organic matter in soil and compost maturing processes. However, the roles of metal oxides in abiotic humification reactions under micro-aerobic remain ambiguous. The aim of this study was to use non-destructive measurement methods to investigate the role of MnO₂ in the evolution of humic substances (HSs) during oxidative polymerization of polyphenol-amino acid. Our results suggested a synergistic effect between MnO₂ and O₂ in promoting the polymerization reaction and identified that MnO₂ alone had a limited ability in accelerating the transformation of fulvic acid (FA) to humic acid (HA), whereas O₂ was the key factor in the process. Two-dimensional correlation spectroscopy (2D-COS) showed that the evolution in the UV-vis spectra followed the order of 475–525 nm>300–400 nm>240–280 nm in the humification process, indicating the formation of simple organic matter followed by FA and then HA. ¹³C nuclear magnetic resonance (¹³C NMR) analysis revealed that the products under both air and N₂ conditions in the presence of MnO₂ had greater amounts of aromatic-C than in the absence of MnO₂, demonstrating that MnO₂ affected the structure of the humification products. The results of this study provided new insights into the theory of abiotic humification.     

Submerged arc plasma system combined with ozone oxidation for the treatment of wastewater containing non-degradable organic compounds

• Submerged arc plasma was introduced in terms of wastewater treatment. • Ozone oxidation was coupled with submerged arc plasma system. • Ozone was converted into O and O₂ by submerged arc plasma. • Decomposition rate was accelerated by submerged arc plasma. • Introduction of ozone led to significant increase in mineralization. Submerged arc plasma technology was assessed for the removal of phenols from wastewater. The OH radicals generated from the boundary between the plasma and waste solution were considered as a significant factor on the degradation reaction. In this study, the effects of highly energetic electrons released from the submerged arc plasma were mainly studied. The highly energetic electrons directly broke the strong chemical bond and locally increased the reaction temperatures in solution. The effects of the submerged-arc plasma on the decomposition of phenol are discussed in terms of the input energy and initial concentration. The single use of submerged arc plasma easily decomposed the phenol but did not increase the mineralization efficiency. Therefore, the submerged arc plasma, coupled with the ozone injection, was investigated. The submerged arc plasma combined with ozone injection had a synergic effect, which led to significant improvements in mineralization with only a small increase in input energy. The decomposition mechanism of phenol by the submerged arc plasma with the ozone was analyzed.     

Performance and mechanistic study on electrocoagulation process for municipal wastewater treatment based on horizontal bipolar electrodes

• EC modified with BPEs enhances pollutant removal and reduce energy consumption. • Increasing BPE number cannot increase flocculants yield exponentially. • Simulations help to predict the distribution of electrochemical reactions on BPEs. The design of electrodes is crucial to electrocoagulation process (EC), specifically, with respect to pollutant removal and energy consumption. During EC, the mechanisms for interaction between different electrode arrangement and electrode reactions remain unclear. This work presents an integrated EC process based on horizontal bipolar electrodes (BPEs). In the electrochemical cell, the graphite plates are used as driving cathode while either Fe or Al plates serves as driving anode and BPEs. The BPEs are placed horizontally between the driving electrodes. For municipal wastewater treatment, the pollutant removal efficiency and energy consumption in different configurations of two-dimension electrocoagulation (2D-EC) system with horizontal BPEs were investigated. The removal efficiency of turbidity, total phosphorus and total organic carbon increased significantly with the number of BPEs. Noted that the energy consumption for TP removal decreased by 75.2% with Fe driving anode and 81.5% with Al driving anode than those of 2D-EC, respectively. In addition, the physical field simulation suggested the distributions of potential and current in electrolyte and that of induced charge density on BPE surface. This work provides a visual theoretical guidance to predict the distribution of reactions on BPEs for enhanced pollutant removal and energy saving based on electrocoagulation process for municipal wastewater treatment.     

Mercury removal from aqueous solution using petal-like MoS2 nanosheets

• Synthesized few-layered MoS₂ nanosheets via surfactant-assisted hydrothermal method. • Synthesized MoS₂ nanosheets show petal-like morphology. • Adsorbent showed 93% of mercury removal efficiency. • The adsorption of mercury is attributed to negative zeta potential (-21.8 mV). Recently, different nanomaterial-based adsorbents have received greater attention for the removal of environmental pollutants, specifically heavy metals from aqueous media. In this work, we synthesized few-layered MoS₂ nanosheets via a surfactant-assisted hydrothermal method and utilized them as an efficient adsorbent for the removal of mercury from aqueous media. The synthesized MoS₂ nanosheets showed petal-like morphology as confirmed by scanning electron microscope and high-resolution transmission electron microscopic analysis. The average thickness of the nanosheets is found to be about 57 nm. Possessing high stability and negative zeta potential makes this material suitable for efficient adsorption of mercury from aqueous media. The adsorption efficiency of the adsorbent was investigated as a function of pH, contact time and adsorbent dose. The kinetics of adsorption and reusability potential of the adsorbent were also performed. A pseudo-second-order kinetics for mercury adsorption was observed. As prepared MoS₂ nanosheets showed 93% mercury removal efficiency, whereas regenerated adsorbent showed 91% and 79% removal efficiency in the respective 2^nd and 3^rd cycles. The adsorption capacity of the adsorbent was found to be 289 mg/g at room temperature.     

Enhanced methane production during long-term UASB operation at high organic loads as enabled by the immobilized Fungi

• Fungi enable the constant UASB operation even at OLR of 25.0 kg/(m³×d). • The COD removal of 85.9% and methane production of 5.6 m³/(m³×d) are achieved. • Fungi inhibit VFAs accumulation and favor EPS generation and sludge granulation. • Fungi enrich methanogenic archaea and promote methanogenic pathways. Anaerobic digestion is widely applied in organic wastewater treatment coupled with bioenergy production, and how to stabilize its work at the high organic loading rate (OLR) remains a challenge. Herein, we proposed a new strategy to address this issue via involving the synergetic role of the Aspergillus sydowii 8L-9-F02 immobilized beads (AEBs). A long-term (210-day) continuous-mode operation indicated that the upflow anaerobic sludge bed (UASB) reactor (R1, with AEBs added) could achieve the OLR as high as 25.0 kg/(m³×d), whereas the control reactor (R0, with AEBs free) could only tolerate the maximum OLR of 13.3 kg/(m³×d). Remarkably, much higher COD removal (85.9% vs 23.9%) and methane production (5.4 m³/(m³×d) vs 2.2 m³/(m³×d)) were achieved in R1 than R0 at the OLR of 25.0 kg/(m³×d). Such favorable effect results from the facts that fungi inhibit VFAs accumulation, favor the pH stabilization, promote the generation of more extracellular polymeric substance, and enhance the sludge granulation and settleability. Moreover, fungi may enhance the secretion of acetyl-coenzyme A, a key compound in converting organic matters to CO₂. In addition, fungi are favorable to enrich methanogenic archaea even at high OLR, improving the activity of acetate kinase and coenzyme F₄₂₀ for more efficient methanogenic pathway. This work may shed new light on how to achieve higher OLR and methane production in anaerobic digestion of wastewater.     

One-step ball milling-prepared nano Fe2O3 and nitrogen-doped graphene with high oxygen reduction activity and its application in microbial fuel cells

• Nano Fe₂O₃ and N-doped graphene was prepared via a one-step ball milling method. • The maximum power density of Fe-N-G in MFC was 390% of that of pristine graphite. • Active sites like nano Fe₂O₃, pyridinic N and Fe-N groups were formed in Fe-N-G. • The improvement of Fe-N-G was due to full exposure of active sites on graphene. Developing high activity, low-cost and long durability catalysts for oxygen reduction reaction is of great significance for the practical application of microbial fuel cells. The full exposure of active sites in catalysts can enhance catalytic activity dramatically. Here, novel Fe-N-doped graphene is successfully synthesized via a one-step in situ ball milling method. Pristine graphite, ball milling graphene, N-doped graphene and Fe-N-doped graphene are applied in air cathodes, and enhanced performance is observed in microbial fuel cells with graphene-based catalysts. Particularly, Fe-N-doped graphene achieves the highest oxygen reduction reaction activity, with a maximum power density of 1380±20 mW/m² in microbial fuel cells and a current density of 23.8 A/m² at –0.16 V in electrochemical tests, which are comparable to commercial Pt and 390% and 640% of those of pristine graphite. An investigation of the material characteristics reveals that the superior performance of Fe-N-doped graphene results from the full exposure of Fe₂O₃ nanoparticles, pyrrolic N, pyridinic N and excellent Fe-N-G active sites on the graphene matrix. This work not only suggests the strategy of maximally exposing active sites to optimize the potential of catalysts but also provides promising catalysts for the use of microbial fuel cells in sustainable energy generation.     

Experimental and computational assessment of 1,4-Dioxane degradation in a photo-Fenton reactive ceramic membrane filtration process

• 1,4-Dioxane was degraded via the photo-Fenton reactive membrane filtration. • Degradation efficiency and AQY were both enhanced in photocatalytic membrane. • There is a tradeoff between photocatalytic degradation and membrane permeation flux. • Degradation pathways of 1,4-Dioxane is revealed by DFT analysis. The present study evaluated a photo-Fenton reactive membrane that achieved enhanced 1,4-Dioxane removal performance. As a common organic solvent and stabilizer, 1,4-Dioxane is widely used in a variety of industrial products and poses negative environmental and health impacts. The membrane was prepared by covalently coating photocatalyst of goethite (α-FeOOH) on a ceramic porous membrane as we reported previously. The effects of UV irradiation, H₂O₂ and catalyst on the removal efficiency of 1,4-Dioxane in batch reactors were first evaluated for optimized reaction conditions, followed by a systematical investigation of 1,4-Dioxane removal in the photo-Fenton membrane filtration mode. Under optimized conditions, the 1,4-Dioxane removal rate reached up to 16% with combination of 2 mmol/L H₂O₂ and UV₃₆₅ irradiation (2000 µW/cm²) when the feed water was filtered by the photo-Fenton reactive membrane at a hydraulic retention time of 6 min. The removal efficiency and apparent quantum yield (AQY) were both enhanced in the filtration compared to the batch mode of the same photo-Fenton reaction. Moreover, the proposed degradation pathways were analyzed by density functional theory (DFT) calculations, which provided a new insight into the degradation mechanisms of 1,4-Dioxane in photo-Fenton reactions on the functionalized ceramic membrane.     

Temporal variation of PM2.5-associated health effects in Shijiazhuang,Hebei

•Annual mean PM_2.5 in Shijiazhuang were 87, 95, and 82 µg/m³ in 2015–2017. •Health risk of cardiovascular system was higher than respiratory system. •Premature mortality attributed to PM_2.5 was 5088 people in 2017. •ΔMort and YLL reduced by 84.2% and 84.6% when PM_2.5 reduced to 10 µg/m³. •Health risks due to PM_2.5 were severe in Shijiazhuang in 2015–2017. Shijiazhuang is one of the cities in the North China Plain. In recent decades, this city has experienced high levels of fine particulate matter (PM_2.5), which have potentially significant effects on human health. In this study, the health effects of PM_2.5 exposure in Shijiazhuang were estimated by applying an integrated exposure-response model. Premature mortality, years of life lost (YLL), and the mortality benefits linked to reduced levels of PM_2.5 were quantified for the period 2015–2017. In 2015, 2016, and 2017, cerebrovascular diseases caused the highest premature mortality (2432, 2449, and 2483, respectively), followed by ischemic heart diseases (1391, 1479, and 1493, respectively), lung cancer (639,660, and 639, respectively), and chronic obstructive pulmonary diseases (533, 519, and 473, respectively). Notably, the total number of premature deaths caused by PM_2.5 exposure in Shijiazhuang in 2015, 2016, and 2017 were 4994, 5107, and 5088, respectively. Moreover, the YLL in the same years were 47001, 47880 and 47381, respectively. Interestingly, the YLL per 1000 females was lower than that per 1000 males. Finally, we noted that premature mortality and YLL decreased by 84.2% and 84.6% when the PM_2.5 levels diminished to 10 µg/m³. Overall, the results of this study improve our understanding of how high PM_2.5 concentrations affect human health and suggest the application of more stringent measures in Shijiazhuang to alleviate the associated health risks.     

The performance of nitrate-reducing Fe(II) oxidation processes under variable initial Fe/N ratios: The fate of nitrogen and iron species

•Bacterially-mediated coupled N and Fe processes examined in incubation experiments. •NO₃⁻ reduction was considerably inhibited as initial Fe/N ratio increased. •The maximum production of N₂ occurred at an initial Fe/N molar ratio of 6. •Fe minerals produced at Fe/N ratios of 1–2 were mainly easily reducible oxides. The Fe/N ratio is an important control on nitrate-reducing Fe(II) oxidation processes that occur both in the aquatic environment and in wastewater treatment systems. The response of nitrate reduction, Fe oxidation, and mineral production to different initial Fe/N molar ratios in the presence of Paracoccus denitrificans was investigated in 132 h incubation experiments. A decrease in the nitrate reduction rate at 12 h occurred as the Fe/N ratio increased. Accumulated nitrite concentration at Fe/N ratios of 2–10 peaked at 12–84 h, and then decreased continuously to less than 0.1 mmol/L at the end of incubation. N₂O emission was promoted by high Fe/N ratios. Maximum production of N₂ occurred at a Fe/N ratio of 6, in parallel with the highest mole proportion of N₂ resulting from the reduction of nitrate (81.2%). XRD analysis and sequential extraction demonstrated that the main Fe minerals obtained from Fe(II) oxidation were easily reducible oxides such as ferrihydrite (at Fe/N ratios of 1–2), and easily reducible oxides and reducible oxides (at Fe/N ratios of 3–10). The results suggest that Fe/N ratio potentially plays a critical role in regulating N₂, N₂O emissions and Fe mineral formation in nitrate-reducing Fe(II) oxidation processes.     

Enhanced catalytic oxidation of 2,4-dichlorophenol via singlet oxygen dominated peroxymonosulfate activation on CoOOH@Bi2O3 composite

• Bi₂O₃ cannot directly activate PMS. • Bi₂O₃ loading increased the specific surface area and conductivity of CoOOH. • Larger specific surface area provided more active sites for PMS activation. • Faster electron transfer rate promoted the generation of reactive oxygen species. • ¹O₂ was identified as dominant ROS in the CoOOH@Bi₂O₃/PMS system. Cobalt oxyhydroxide (CoOOH) has been turned out to be a high-efficiency catalyst for peroxymonosulfate (PMS) activation. In this study, CoOOH was loaded on bismuth oxide (Bi₂O₃) using a facile chemical precipitation process to improve its catalytic activity and stability. The result showed that the catalytic performance on the 2,4-dichlorophenol (2,4-DCP) degradation was significantly enhanced with only 11 wt% Bi₂O₃ loading. The degradation rate in the CoOOH@Bi₂O₃/PMS system (0.2011 min⁻¹) was nearly 6.0 times higher than that in the CoOOH/PMS system (0.0337 min⁻¹). Furthermore, CoOOH@Bi₂O₃ displayed better stability with less Co ions leaching (16.4% lower than CoOOH) in the PMS system. These phenomena were attributed to the Bi₂O₃ loading which significantly increased the conductivity and specific surface area of the CoOOH@Bi₂O₃ composite. Faster electron transfer facilitated the redox reaction of Co (III) / Co (II) and thus was more favorable for reactive oxygen species (ROS) generation. Meanwhile, larger specific surface area furnished more active sites for PMS activation. More importantly, there were both non-radical (¹O₂) and radicals (SO₄⁻•, O₂⁻•, and OH•) in the CoOOH@Bi₂O₃/PMS system and ¹O₂ was the dominant one. In general, this study provided a simple and practical strategy to enhance the catalytic activity and stability of cobalt oxyhydroxide in the PMS system.