Low-voltage stimulated denitrification performance of high-salinity wastewater using halotolerant microorganisms.

Nitrate is a common contaminant in high-salinity wastewater, which has adverse effects on both the environment and human health. However, conventional biological treatment exhibits poor denitrification performance due to the high-salinity shock. In this study, an innovative approach using an electrostimulating microbial reactor (EMR) was explored to address this challenge. With a low-voltage input of 1.2 V, the EMR reached nitrate removal kinetic parameter (kNO3-N) of 0.0166-0.0808 h-1 under high-salinities (1.5 %-6.5 %), which was higher than that of the microbial reactor (MR) (0.0125-0.0478 h-1). The mechanisms analysis revealed that low-voltage significantly enhanced microbial salt-in strategy and promoted the secretion of extracellular polymeric substances. Halotolerant denitrification microorganisms (Pseudomonas and Nitratireductor) were also enriched in EMR. Moreover, the EMR achieved a NO3-N removal efficiency of 73.64 % in treating high-salinity wastewater (salinity 4.69 %) over 18-cycles, whereas the MR only reached 54.67 %. In summary, this study offers an innovative solution for denitrification of high-salinity wastewater.

Enhancing microbial salt tolerance through low-voltage stimulation for improved p-chloronitrobenzene (p-CNB) removal in high-salinity wastewater.

As an important raw material for the synthesis of chemical and pharmaceutical, hazardous carcinogen p-chloronitrobenzene (p-CNB) has been widely found in high-salinity wastewater which need to be treated carefully. Due to the high-salinity shock on microorganisms, conventional microbial treatment technologies usually show poor effluent quality. This study initially investigated the p-CNB removal performance of microorganisms stimulated by 1.2 V low-voltage in high-salinity wastewater under facultative anaerobic conditions and further revealed the enhanced mechanisms. The results showed that the p-CNB removal kinetic parameter kp-CNB in the electrostimulating microorganism reactor (EMR) increased by 104.37 % to 155.30 % compared to the microorganism reactor (MR) as the control group under the varying salinities (0-45 g/L NaCl). The secretion of extracellular polymeric substances (EPS) in halotolerant microorganisms mainly enhanced by 1.2 V voltage stimulation ranging from 0 g/L NaCl to 30 g/L NaCl. Protein concentration ratio of EMR to MR in loosely bound EPS achieved maximum value of 1.77 at the salinity of 15 g/L NaCl, and the same ratio in tightly bound EPS also peaked at 1.39 under the salinity of 30 g/L NaCl. At the salinity of 45 g/L NaCl, 1.2 V voltage stimulation mainly enhanced salt-in strategy of halotolerant microorganisms, and the intracellular Na+ and K+ concentration ratio of EMR to MR reached maximum and minimum values of 0.65 and 1.92, respectively. Furthermore, the results of microbial metagenomic and metatranscriptomic analysis showed the halotolerant microorganisms Pseudomonas_A and Nitratireductor with p-CNB removal ability were enriched significantly under 1.2 V voltage stimulation. And the gene expression of p-CNB removal, salt-in strategy and betaine transporter were enhanced under voltage stimulation at varying salinities. Our investigation provided a new solution which combined with 1.2 V voltage stimulation and halotolerant microorganisms for the treatment of high-salinity wastewater.

The impact of powdered activated carbon types on membrane anti-fouling mechanism in membrane bioreactors.

Dosing powdered activated carbon (PAC) has been proven to be an economical and effective method to mitigate membrane fouling. However, the effects of pretreated PAC with different redox properties on membrane fouling still need to be further investigated. Here, the impact of commercial PAC, oxidized-PAC, and reduced-PAC on membrane fouling was investigated in membrane bioreactors (MBRs). Surprisingly, the filtration cycles were extended from 12-36 h to 132-156 h only by dosing reduced-PAC and commercial PAC with a finial dosage of 3 g/L, which were provided with reductive properties. However, few improvements of filtration cycle (less than 50 h) were achieved by dosing oxidized-PAC in the same dosage, which had the same adsorption performance as reduced-PAC and commercial PAC. The biomass and foulant concentration suggested that the enhanced anti-fouling performances by PAC with reductive properties were mainly attributed to the reduction of extracellular polymer substances (EPS) and soluble microbial products (SMP) content in the bulk solutions after 14 days of continuous operation. The model foulant degradation tests and the confocal laser scanning microscope (CLSM) images of activated sludge further demonstrated that PAC with reductive properties directly affected the microbial activities by controlling the EPS and SMP concentrations in the bulk solution, thereby suppressing membrane fouling. Such a finding provides new insights into anti-fouling mechanisms that the redox properties of PAC played a decisive role in membrane fouling mitigation, and also provides a strategy to prolong the anti-fouling effects by restoring the reductive properties of PAC. KEY POINTS: • The anti-fouling mechanisms of PAC with reductive property were investigated. • Reductive property was the main reason for fouling control instead of adsorption. • PAC with reductive property hindered the sludge activity to produce fewer foulants.

Mechanism on the microbial salt tolerance enhancement by electrical stimulation.

The application of biological methods in industrial saline wastewater treatment is limited, since the activities of microorganisms are strongly inhibited by the highly concentrated salts. Acclimatized halotolerant and halophilic microorganisms are of high importance since they can resist the environmental stresses of high salinity. The acclimation to salinity can be passive or active based on whether external simulation is used. However, there is a need for development of economic, efficient and reliable active biological stimulation technologies to accelerate salinity acclimation. Recent studies have shown that electrical stimulation can effectively enhance microbial salt tolerance and pollutant removal ability. However, there have been no comprehensive reviews of the mechanisms involved. Therefore, this mini-review described the mechanisms of electrical stimulation that can significantly improve microbial bioactivity and biodiversity. These mechanisms include regulation of Na+ and K+ transporters by changing membranepotential and promoting ATP production, as well as regulation of extracellular polymer substances through enhanced release of low molecular weight EPS and quorum sensing molecules. The information provided herein will facilitate the application of biological high-salinity wastewater treatment.

Evaluating the effect of fenton pretreated pyridine wastewater under different biological conditions: Microbial diversity and biotransformation pathways.

Pyridine contamination poses a significant threat to human and environmental health. Due to the presence of nitrogen atom in the pyridine ring, the pi bond electrons are attracted toward it and make difficult for pyridine treatment with biological and chemical methods. In this study, coupling Fenton treatment with different biological process was designed to enhance pyridine biotransformation and further mineralization. After Fenton oxidation process optimized, pretreated pyridine was evaluated under three biological (anaerobic, aerobic and microaerobic) operating conditions. Under optimum Fenton oxidation, pyridine (30-75%) and TOC (5-25%) removal efficiencies were poor. Biological process alone also showed insignificant removal efficiency, particularly anaerobic (pyridine = 8.2%; TOC = 5.3%) culturing condition. However, combining Fenton pretreatment with biological process increased pyridine (93-99%) and TOC (87-93%) removals, suggesting that hydroxyl radical generated during Fenton oxidation enhanced pyridine hydroxylation and further mineralization in the biological (aerobic > microaerobic > anaerobic) process. Intermediates were analyzed with UPLC-MS and showed presence of maleic acid, pyruvic acid, glutaric dialdehyde, succinic semialdehyde and 4-formylamino-butyric acid. High-throughput sequencing analysis also indicated that Proteobacteria (35-43%) followed by Chloroflexi (10.6-24.3%) and Acidobacteria (8.0-29%) were the dominant phyla detected in the three biological treatment conditions. Co-existence of dominant genera under aerobic/microaerobic (Nitrospira > Dokdonella > Caldilinea) and anaerobic (Nitrospira > Caldilinea > Longilinea) systems most probably play significant role in biotransformation of pyridine and its intermediate products. Overall, integrating Fenton pretreatment with different biological process is a promising technology for pyridine treatment, especially the combined system enhanced anaerobic (>10 times) microbial pyridine biotransformation activity.

Enhanced treatment of coal gasification wastewater in a membraneless sleeve-type bioelectrochemical system.

A bioelectrochemical system (BES) is a technology with potential for accelerating the degradation of recalcitrant compounds, the components and configurations of which are important for treatment performance. In the present work, a membraneless sleeve-type BES (termed BioE) was designed for the treatment of synthetic coal gasification wastewater (CGW, phenol as a model pollutant) and real CGW. Compared with the biological control (termed Bio), the phenol removal rate and COD removal efficiency increased by 2.6 and 2.1 fold in the BioE, respectively. However, the coulombic efficiency of this system was relatively low, ranging from 0.42% to 2.6%. This combination of results indicated that anode respiration was not the main process in the BioE. The increased CH4 production and higher levels of methanogens obtained from the BioE confirmed that the methanogenic process proceeded, possibly facilitated by the diffusion of H2 from the cathode to the anode. This study provides new insight into biocathode function for COD oxidation removal in BESs. Moreover, this study indicates that pursuing a high coulombic efficiency may not be necessary for wastewater treatment, as it consumes less energy at the lower value.

Borate Inorganic Cross-Linked Durable Graphene Oxide Membrane Preparation and Membrane Fouling Control.

Graphene oxide (GO) membranes have the potential to be next-generation membranes. However, the GO layer easily swells in water and risks shedding during the long-term filtration. Organic GO interlayer organic cross-linking agent was not resistant to oxidation, which limits the application scope of GO membrane. In this study, an inorganic cross-linked GO membrane was prepared via the reaction of sodium tetraborate and GO hydroxyl groups, and a -B-O-C- cross-linking bond was detected by X-ray photoelectron spectroscopy (XPS). Additionally, a new atomic force microscope scratch method to evaluate the cross-linking force of a nanoscale GO layer was proposed. It showed that the critical destructive load of the inorganic cross-linked GO membrane increased from 8 to 80 nN, which was a 10-fold increase from that of the nonlinked sample. During the NaOH/sodium dodecyl sulfate (SDS) destructive wash tests, morphology, flux and retention rate of inorganic cross-linked GO remained stable while the comparative membranes showed significant destruction. At the same time, based on the better oxidation resistance, organic membrane fouling was effectively controlled by the introduction of trace ·OH radicals. This study provides a new perspective for GO membrane preparation, interlayer cross-linking force testing and membrane fouling control.

Graphene Modified Electro-Fenton Catalytic Membrane for in Situ Degradation of Antibiotic Florfenicol.

The removal of low-concentration antibiotics from water to alleviate the potential threat of antibiotic-resistant bacteria and genes calls for the development of advanced treatment technologies with high efficiency. In this study, a novel graphene modified electro-Fenton (e-Fenton) catalytic membrane (EFCM) was fabricated for in situ degradation of low-concentration antibiotic florfenicol. The removal efficiency was 90%, much higher than that of electrochemical filtration (50%) and single filtration process (27%). This demonstrated that EFCM acted not only as a cathode for e-Fenton oxidation process in a continuous mode but also as a membrane barrier to concentrate and enhance the mass transfer of florfenicol, which increased its oxidation chances. The removal rate of florfenicol by EFCM was much higher (10.2 ± 0.1 mg m-2 h-1) than single filtration (2.5 ± 0.1 mg m-2 h-1) or batch e-Fenton processes (4.3 ± 0.05 mg m-2 h-1). Long-term operation and fouling experiment further demonstrated the durability and antifouling property of EFCM. Four main degradation pathways of florfenicol were proposed by tracking the degradation byproducts. The above results highlighted the feasibility of this integrated membrane catalysis process for advanced water purification.

Functional graphene oxide membrane preparation for organics/inorganic salts mixture separation aiming at advanced treatment of refractory wastewater.

Some refractory organic matters or soluble microbial products remained in the effluents of refractory organic wastewater after biological secondary treatment and need an advanced treatment before final disposal. Graphene oxide (GO) was known to have potential to be the next generation membrane material. The functional organics/inorganic salts separation GO membrane preparation and application in wastewater advanced treatment could reduce energy or chemicals consumption and avoid organics/inorganic salts mixed concentrate waste problems after nanofiltration or reverse osmosis. In this study, we developed a novelty GO membrane aiming at advanced purification of organic matters in the secondary effluents of refractory organic wastewater and avoiding the organics/inorganic salts mixed concentrate waste problem. The influence of preparation conditions including pore size of support membrane, the number of GO layers and the applied pressure was investigated. It was found that for organics/inorganic salts mixture separation membrane preparation, the rejection and flux would achieve balance for the support membrane at a pore size of ~0.1µm and the number of GO layers of has an optimization value (~10 layers). A higher assemble pressure (~10bar) contributed to the acquisition of a higher rejection efficiency and lower roughness membrane. This as prepared GO membrane was applied to practical secondary effluent of a chemical synthesis pharmaceuticals wastewater. A good organic matter rejection efficiency (76%) and limited salt separation (<14%) was finally obtained. These results can promote the practical application of GO membrane and the resourcelized treatment of industrial wastewater.

Increasing the bio-electrochemical system performance in azo dye wastewater treatment: Reduced electrode spacing for improved hydrodynamics.

The electrodes spacing would exert a pronounced effect on bio-electrochemical systems (BESs) performance, especially for the scaling-up of reactors and practical applications. In this study, we traced the effect of electrode spacing on wastewater treatment performances from the aspects of hydrodynamics and electrochemical characteristics. Three series of folded stainless steel mesh (f-SSM) electrodes with electrode spacing of 2, 4 and 8mm were designed for azo dye (acid orange 7 (AO7)) wastewater treatment. Results showed that BES with electrode spacing of 2mm (RS2) obtained the highest efficiencies of AO7 decolorization (90.9±0.4%) and COD removal (36.8±3.8%) at HRT of 8h, which was 30.7% and 15.2% higher than that in BES with electrode spacing of 8mm (RS8), respectively. Moreover, the relationship between pollutants removal, internal resistance and hydrodynamics of BESs with different electrode spacing supported the hydrodynamics was significantly influence the pollutants removal performance.

A new method for rapid construction of a Pseudomonas sp. HF-1 bioaugmented system: accelerating acylated homoserine lactones secretion by pH regulation.

Pseudomonas sp. HF-1 bioaugmented systems were operated to treat tobacco wastewater under pH 5.5 for three cycles and pH 8.0 for the rest, which was suitable for HF-1 biofilm formation. The results showed that, under pH control, the contents of 3-oxo-C6-HSL, C6-HSL and 3-oxo-C8-HSL were significantly higher than HF-1 thresholds for biofilm formation. Compared with non-pH controlled reactors, HF-1 showed greater colonization in pH controlled reactors, primarily owing to the high extracellular polymeric substances secretion induced by quorum sensing. Accordingly, high indigenous community activity and granular sludge were observed. Sludge granulation occurred from the seventh cycle, and the average diameter was greater than 400 µm. These systems were also highly efficient with nearly 100% nicotine degradation and 60% total organic carbon removal. Overall, the results indicate that pH regulation is a new and feasible method for acceleration of releasing of auto-inducers, which is beneficial to construction of HF-1 bioaugmented systems.