• Fate of microplastics in integrated membrane system for water reuse was investigated. • Integrated membrane system has high removal efficiency (>98%) for microplastics. • Microplastics (>93%) were mainly removed through membrane bioreactor treatment. • Small scale fiber plastics (<200 μm) could break through reverse osmosis (RO) system. • The flux of microplastics maintained at 2.7 × 1011 MPs/d after the RO treatment.
Rare information on the fate of microplastics in the integrated membrane system (IMS) system in full-scale wastewater treatment plant was available. The fate of microplastics in IMS in a coastal reclaimed water plant was investigated. The removal rate of microplastics in the IMS system reached 93.2% after membrane bioreactor (MBR) treatment while that further increased to 98.0% after the reverse osmosis (RO) membrane process. The flux of microplastics in MBR effluent was reduced from 1.5 × 1013 MPs/d to 10.2 × 1011 MPs/d while that of the RO treatment decreased to 2.7 × 1011 MPs/d. Small scale fiber plastics (<200 μm) could break through RO system according to the size distribution analysis. The application of the IMS system in the reclaimed water plant could prevent most of the microplastics from being discharged in the coastal water. These findings suggested that the IMS system was more efficient than conventional activated sludge system (CAS) for the removal of microplastics, while the discharge of small scale fiber plastics through the IMS system should also not be neglected because small scale fiber plastics (<200 μm) could break through IMS system equipped with the RO system.
• The Chinese population exposure habits were surveyed. • The risks of three scenarios of reclaimed water utilization were evaluated by QMRA. • The risks were markedly higher than the threshold (10−4 pppy) recommended by WHO. • The risks were age-, educational background-, region- and gender-specific.
Reclaimed water utilization provides an effective way to alleviate water shortage. However, the residual pathogens in the recycled water like Legionella, could be spread into the air as aerosols through water-to-air transmission process. Inhaling the aerosols by the people nearby increases their susceptibility to diseases. For estimating the health risks associated with the potential exposure of airborne Legionella emitted from the urban use of reclaimed water in China, nationwide questionnaire was designed to investigate the exposure habits of Chinese population in different scenarios. Quantitative microbial risk assessment (QMRA) served as the suitable explanatory tool to estimate the risk. The results indicated that annual infection probability of populations exposed to Legionella for three scenarios, 0.0764 (95% CI: 0.0032–0.6880) for road cleaning, 1.0000 (95% CI: 0.1883–1.0000) for greenfield irrigation, 0.9981 (95% CI: 0.0784–1.0000) for landscape fountain, were markedly higher than the threshold recommended by WHO (10−4 per person per year (pppy)) according to the concentration distribution of Legionella in the reclaimed water. An age-, educational background-, region- and gender-specific data in annual infection probability also showed different tendencies for some subpopulations. This study provides some detailed information on the health risks from the water reuse in China and will be useful to promote the safe application of reclaimed water in water-deficient areas.
• Cellulose-based membrane separates oily wastewater mimicking the living things. • The three central surface mechanisms were reviewed. • Preparation, performance, and mechanism are critically evaluated. • First review of wettability based cellulose membrane as major material. • The current and future importance of the research are discussed.
It is challenging to purify oily wastewater, which affects water-energy-food production. One promising method is membrane-based separation. This paper reviews the current research trend of applying cellulose as a membrane material that mimics one of three typical biostructures: superhydrophobic, underwater superoleophobic, and Janus surfaces. Nature has provided efficient and effective structures through the evolutionary process. This has inspired many researchers to create technologies that mimic nature’s structures or the fabrication process. Lotus leaves, fish scales, and Namib beetles are three representative structures with distinct functional and surface properties: superhydrophobic, underwater superoleophobic, and Janus surfaces. The characteristics of these structures have been widely studied and applied to membrane materials to improve their performance. One attractive membrane material is cellulose, which has been studied from the perspective of its biodegradability and sustainability. In this review, the principles, mechanisms, fabrication processes, and membrane performances are summarized and compared. The theory of wettability is also described to build a comprehensive understanding of the concept. Finally, future outlook is discussed to challenge the gap between laboratory and industrial applications.
• Oxidation of methotrexate by high-valent metal-oxo species was first explored. • Fe(VI) presented a higher reactivity to MTX than Mn(VII) at pH 8.0. • Ketonization and cleavage of peptide bond were two initial reaction pathways. • Products of MTX were not genotoxic, neurotoxic, or endocrine-disrupting chemicals. • The less biodegradable products exhibited developmental and acute/chronic toxicity.
Accompanying an annual increase in cancer incidence, the global use of anticancer drugs has remarkably increased with their worldwide environmental prevalence and ecological risks. In this study, the oxidation of methotrexate (MTX), a typical anticancer drug with ubiquitous occurrence and multi-endpoint toxicity, by ferrate(VI) (Fe(VI)) and permanganate (Mn(VII))) was investigated in water. Fe(VI) exhibited a higher reactivity with MTX (93.34 M−1 s−1) than Mn(VII) (3.01 M−1 s−1) at pH 8.0. The introduction of Cu(II) and Fe(III) at 1.0 mM improved the removal efficiency of 5.0 μM MTX by 100.0 μM Fe(VI) from 80% to 95% and 100% after 4 min, respectively. Seven oxidized products (OPs) were identified during oxidative treatments, while OP-191 and OP-205 were characterized as specific products for Fe(VI) oxidation. Initial ketonization of the L-glutamic acid moiety and cleavage of the peptide bond of MTX were proposed. Additionally, a multi-endpoint toxicity evaluation indicated no genotoxicity, neurotoxicity, or endocrine-disrupting effects of MTX and its OPs. Particularly, serious developmental toxicity in zebrafish larvae was observed in the treated MTX solutions. Based on the acute and chronic aquatic toxicity prediction, OP-190, OP-192, OP-206, and OP-208 were deemed toxic or very toxic compared to harmful MTX. Furthermore, the reduced biodegradability index from 0.15 (MTX) to −0.5 to −0.2 (OP-192, OP-206, and OP-468) indicated the formation of lower biodegradable OPs. Overall, this study suggests that Fe(VI) and Mn(VII) oxidation are promising treatments for remediating anticancer drug-contaminated water. However, the environmental risks associated with these treatments should be considered in the evaluation of water safety.
•Addition of hindered amine increased thermal stability and viscosity of TTTM. •Addition of hindered amine improved the CO2 absorption performance of TTTM. •Good the CO2 absorption of recycled solvents after two regenerations. •Important role of amine group in CO2 absorption of TTTM confirmed by DFT analysis.
Is it possible to improve CO2 solubility in potassium carbonate (K2CO3)-based transition temperature mixtures (TTMs)? To assess this possibility, a ternary transition-temperature mixture (TTTM) was prepared by using a hindered amine, 2-amino-2-methyl-1,3-propanediol (AMPD). Fourier transform infrared spectroscopy (FT-IR) was employed to detect the functional groups including hydroxyl, amine, carbonate ion, and aliphatic functional groups in the prepared solvents. From thermogravimetric analysis (TGA), it was found that the addition of AMPD to the binary mixture can increase the thermal stability of TTTM. The viscosity findings showed that TTTM has a higher viscosity than TTM while their difference was decreased by increasing temperature. In addition, Eyring’s absolute rate theory was used to compute the activation parameters (ΔG*, ΔH*, and ΔS*). The CO2 solubility in liquids was measured at a temperature of 303.15 K and pressures up to 1.8 MPa. The results disclosed that the CO2 solubility of TTTM was improved by the addition of AMPD. At the pressure of about 1.8 MPa, the CO2 mole fractions of TTM and TTTM were 0.1697 and 0.2022, respectively. To confirm the experimental data, density functional theory (DFT) was employed. From the DFT analysis, it was found that the TTTM+ CO2 system has higher interaction energy (|ΔE |) than the TTM+ CO2 system indicating the higher CO2 affinity of the former system. This study might help scientists to better understand and to improve CO2 solubility in these types of solvents by choosing a suitable amine as HBD and finding the best combination of HBA and HBD.
• Manure fertilization resulted in antibiotic residues and increased metal contents. • The tet and sul genes were significantly enhanced with manure fertilization. • Soil physicochemical properties contributed to 12% of the variations in ARGs. • Soil metals and antibiotics co-select for ARGs.
Pig manure, rich in antibiotics and metals, is widely applied in paddy fields as a soil conditioner, triggering the proliferation of antibiotic resistance genes (ARGs) in soil. However, comprehensive studies on the effects of manure fertilization on the abundance of ARGs and their influencing factors are still insufficient. Here, pig manure and manure-amended and inorganic-amended soils were collected from 11 rice-cropping regions in eastern China, and the accumulation of antibiotics, metals, and ARGs was assessed simultaneously. The results showed that manure fertilization led to antibiotic residues and increased the metal content (i.e., Zn, Cu, Ni, and Cr). Tetracycline and sulfonamide resistance genes (tetM, tetO, sul1, and sul2) were also significantly enhanced with manure fertilization. According to variance partitioning analysis, the most important factors that individually influenced ARGs were soil physicochemical properties, accounting for 12% of the variation. Significant correlations between soil nutrients and ARGs indicated that manure application enhanced the growth of resistant microorganisms by supplying more nutrients. Metals and antibiotics contributed 9% and 5% to the variations in ARGs, respectively. Their co-occurrence also increased the enrichment of ARGs, as their interactions accounted for 2% of the variation in ARGs. Interestingly, Cu was significantly related to most ARGs in the soil (r = 0.26–0.52, p<0.05). Sulfapyridine was significantly related to sul2, and tetracycline resistance genes were positively related to doxycycline. This study highlighted the risks of antibiotic and ARG accumulation with manure fertilization and shed light on the essential influencing factors of ARGs in paddy soils.
• The autotrophic nitrogen removal combining Feammox and Anammox was achieved. • Activated carbon can be used as an electron shuttle to enhance Feammox activity. • Fe(III) was reduced to Fe(II) and the secondary Fe(II) mineral (FeOOH) was obtained. • The iron-reducing bacteria and Anammox consortium was enriched simultaneously.
Ferric iron reduction coupled with anaerobic ammonium oxidation (Feammox) is a novel ferric-dependent autotrophic process for biological nitrogen removal (BNR) that has attracted increasing attention due to its low organic carbon requirement. However, extracellular electron transfer limits the nitrogen transformation rate. In this study, activated carbon (AC) was used as an electron shuttle and added into an integrated autotrophic BNR system consisting of Feammox and anammox processes. The nitrogen removal performance, nitrogen transformation pathways and microbial communities were investigated during 194 days of operation. During the stable operational period (days 126–194), the total nitrogen (TN) removal efficiency reached 82.9%±6.8% with a nitrogen removal rate of 0.46±0.04 kg-TN/m3/d. The contributions of the Feammox, anammox and heterotrophic denitrification pathways to TN loss accounted for 7.5%, 89.5% and 3.0%, respectively. Batch experiments showed that AC was more effective in accelerating the Feammox rate than the anammox rate. X-ray photoelectron spectroscopy (XPS) analyses showed the presence of ferric iron (Fe(III)) and ferrous iron (Fe(II)) in secondary minerals. X-ray diffraction (XRD) patterns indicated that secondary iron species were formed on the surface of iron-AC carrier (Fe/AC), and Fe(III) was primarily reduced by ammonium in the Feammox process. The phyla Anaerolineaceae (0.542%) and Candidatus Magasanikbacteria (0.147%) might contribute to the Feammox process, and Candidatus Jettenia (2.10%) and Candidatus Brocadia (1.18%) were the dominative anammox phyla in the bioreactor. Overall, the addition of AC provided an effective way to enhance the autotrophic BNR process by integrating Feammox and anammox.
• Nanoparticle incorporation and anti-biofouling grafting were integrated. • Flux of modified membranes was enhanced without rejection sacrificing. • Anti-biofouling property of modified membranes was improved.
High performance is essential for the polyamide (PA) reverse osmosis (RO) membranes during the desalination process. Herein, RO membranes with high permselectivity and anti-biofouling properties were fabricated by nanoparticles incorporation and anti-biofouling grafting. Hydrotalcite (HT) incorporation was performed with a dual role, enhancing water flux and acting as grafting sites. The HT incorporation increased the water flux without sacrificing the salt rejection, compensating for the loss caused by the following grafting reaction. The exposed surface of HT acted as grafting sites for anti-biofouling agent dimethyloctadecyl[3-(trimethoxysilyl)propyl]ammonium chloride (DMOTPAC). The combination of HT incorporation and DMOTPAC grafting endowed RO membranes with high permselectivity and anti-biofouling properties. The water flux of the modified membrane PA-HT-0.06 was 49.8 L/m2·h, which was 16.4% higher than that of the pristine membrane. The salt rejection of PA-HT-0.06 was 99.1%, which was comparable to that of the pristine membrane. As to the fouling of negatively charged lysozyme, the modified membrane’s water flux recovery was superior to that of the pristine membrane (e.g. 86.8% of PA-HT-0.06 compared to 78.2% of PA-pristine). The sterilization rates of PA-HT-0.06 for E. coli and B. subtilis were 97.3% and 98.7%, much higher than those of the pristine membrane (24.0% for E. coli and 26.7% for B. subtilis).
• The optimum SCR activity was realized by tuning the acid pretreatment. • Optimized catalysts showed NOx conversion above 90%. • The NH3 and NO adsorption capacity of Al-O3-Fe is stronger than Fe-O3-Fe. • The formation of almandine consumes Fe3+ and Al3+ and weakens their interaction.
Red mud (RM), as an alkaline waste, was recently proved to be a promising substitute for the SCR catalyst. Dealkalization could improve the acidity and reducibility of red mud, which were critical for SCR reaction. However, the dealkalization effect depended on the reaction between acid solution and red mud. In this study, we realized the directional control of the chemical state of active sites through tuning the acid pretreatment (dealkalization) process. The pretreatment endpoint was controlled at pH values of 3–5 with diluted nitric acid. When the pH values of red mud were 3 and 5 (CRM-3 and CRM-5), activated catalysts showed NOx conversion above 90% at 275°C–475°C. The high initial reaction rate, Ce3+/(Ce3+ + Ce4+) ratio, and surface acidity accounted for the excellent SCR performance of CRM-5 catalyst. Meanwhile, more Fe3+ on the CRM-3 surface improved the NH3 adsorption. There was a strong interaction between Al and Fe in both CRM-5 and CRM-3 catalysts. DFT results showed that the adsorption capacity of the Al-O3-Fe for NH3 and NO is stronger than that of Fe-O3-Fe, which enhanced the NOx conversion of the catalyst. However, the almandine was formed in CRM-4, consumed part of Fe3+ and Al3+, and the interaction between Al and Fe was weakened. Also, deposited almandine on the catalyst surface covered the active sites, thus leading to lower NH3-SCR activity.
• Quorum sensing enhancement and inhibition methods are summarized. • Effects of quorum sensing regulation on biofilm are reviewed. • Current knowledge gaps and research challenges are proposed.
Quorum sensing (QS) plays an important role in microbial aggregation control. Recently, the optimization of biological waste treatment systems by QS regulation gained an increasing attention. The effects of QS regulation on treatment performances and biofilm were frequently investigated. To understand the state of art of QS regulation, this review summarizes the methods of QS enhancement and QS inhibition in biological waste treatment systems. Typical QS enhancement methods include adding exogenous QS molecules, adding QS accelerants and cultivating QS bacteria, while typical QS inhibition methods include additions of quorum quenching (QQ) bacteria, QS-degrading enzymes, QS-degrading oxidants, and QS inhibitors. The specific improvements after applying these QS regulation methods in different treatment systems are concluded. In addition, the effects of QS regulation methods on biofilm in biological waste treatment systems are reviewed in terms of biofilm formation, extracellular polymeric substances production, microbial viability, and microbial community. In the end, the knowledge gaps in current researches are analyzed, and the requirements for future study are suggested.
• A Passive Aeration Ditch was developed to treat decentralized wastewater. • A model was developed to describe the process performance. • A high C/N ratio facilitates microbial growth but nitrification deteriorates. • A high salinity decreases both organic and nitrogen contaminants removal.
Decentralized wastewater containing elevated salinity is an emerging threat to the local environment and sanitation in remote coastal communities. Regarding the cost and treatment efficiencies, we propose a passive aeration ditch (PAD) using non-woven polyester fabric as a feasible bubbleless aerator and biofilm carrier for wastewater treatment. Consideration has been first given to PAD’s efficacy in treating saline decentralized wastewater, and then to the impact of chemical oxygen demand-to-nitrogen (C/N) ratio and salinity on biofilm formation. A multispecies model incorporating the salinity effect has been developed to depict the system performance and predict the microbial community. Results showed that the PAD system had great capacity for pollutants removal. The biofilm thickness increased at a higher C/N ratio because of the boost of aerobic heterotrophs and denitrifying bacteria, which consequently improved the COD and total nitrogen removal. However, this led to the deterioration of ammonia removal. Moreover, while a higher salinity benefited the biofilm growth, the contaminant removal efficiencies decreased because the salinity inhibited the activity of aerobic heterotrophs and reduced the abundance of nitrifying bacteria inside the biofilm. Based on the model simulation, feed water with salinity below 2% and C/N ratio in a range of 1 to 3 forms a biofilm that can reach relatively high organic matter and ammonia removal. These findings not only show the feasibility of PAD in treatment of saline decentralized wastewater, but also offer a systematic strategy to predict and optimize the process performance.
• Adding kaolin/zeolite promotes the formation of stable heavy metals. • The potential ecological risk index of co-pyrolysis biochar is extremely low. • Increasing the pyrolysis temperature reduces the leaching toxicity of heavy metals. • The toxicity of biochar reduces with the increasing content of stable heavy metals.
Pyrolysis is a promising technique used for treating of sewage sludge. However, the application of pyrolysis products is limited due to the presence of heavy metals. In this study, sewage sludge mixed with kaolin/zeolite was pyrolyzed in a rotary kiln, aiming to improve the immobilization of heavy metals in pyrolytic carbon. The total concentrations, speciation distributions, leaching toxicities, and potential ecological risk indices of heavy metals in pyrolysis biochar were explored to examine the effects of kaolin/zeolite and pyrolytic temperature on immobilizing heavy metals. Further, mineral composition and surface morphology of biochar were characterized by X-ray diffraction and scanning electron microscopy to reveal the potential mechanism of immobilizing heavy metals. Increasing pyrolysis temperature facilitated the stabilization of heavy metals in pyrolysis biochar. The proportions of stable heavy metals in biochar obtained at 650℃ were 54.50% (Cu), 29.73% (Zn), 79.29% (Cd), 68.17% (Pb) and 86.70% (Cr). Compared to sewage sludge, the potential contamination risk index of pyrolysis biochar obtained at 650℃ was reduced to 17.01, indicating a low ecological risk. The addition of 7% kaolin/zeolite further reduced the risk index of co-pyrolysis biochar prepared at 650℃ to 10.86/15.28. The characterization of biochar revealed that increase in the pyrolysis temperature and incorporation of additives are conducive to the formation of stable heavy metal-inorganics. This study demonstrates that the formation of stable mineral compounds containing heavy metals is the key to stabilizing heavy metals in pyrolysis biochar.
• The PNA, denitratation/anammox, and DAMO/anammox process are reviewed together. • Denitratation/anammox-based process is promising in mainstream treatment. • DAMO and denitratation processes realize the higher nitrogen removal efficiency. • The utilization of metabolism diversity of functional microbe is worth exploring. • An effective waste treatment system concept is proposed.
Anammox technology has been widely researched over the past 40-year from the laboratory-scale to full-scale. It is well-known that in actual applications, the solo application of anammox is not feasible. Since both ammonium and nitrite are prerequisites based on the reaction mechanism, the pre-treatment of wastewater is necessary. With the combination of anammox process and other pre-treatment processes to treat the actual wastewater, many types of anammox-based processes have been developed with distinct nitrogen removal performance. Thus, in order to heighten the awareness of researchers to the developments and accelerate the application of these processes to the treatment of actual wastewater, the main anammox-based processes are reviewed in this paper. It includes the partial nitritation/anammox process, the denitratation/anammox (PD/A) process, the denitrifying anaerobic methane oxidation/anammox (DAMO/A) process, and more complex deuterogenic processes. These processes have made the breakthroughs in the application of the anammox technology, such as the combination of nitrification and PD/A process can achieve stability and reliability of nitrogen removal in the treatment of mainstream wastewater, the PD/A process and the DAMO/A have brought about further improvements in the total nitrogen removal efficiency of wastewater. The diversity of functional microbe characteristics under the specific condition indicate the wide application potential of anammox-based processes, and further exploration is necessary. A whole waste treatment system concept is proposed through the effective allocation of above mentioned processes, with the maximum recovery of energy and resources, and minimal environmental impact.
