A new strategy for enhanced electrochemically activation of persulfate on B and Co co-modified carbon felt in flow-through system for efficient organic pollutants degradation.

Electrochemical activation of persulfate (EA-PS) is gradually attracting attention as an emerging method for wastewater treatment. In this study, a novelty flow-through EA-PS system was first attempted for pollutants degradation using boron and cobalt co-doping carbon felt (B, Co-CF) as the cathode. SEM images, XPS and XRD spectra of B, Co-CF were investigated. The optimal doping ration between B and Co was 1:2. Increasing current density, PS concentration and flow rate, decreasing initial pH accelerated the removal of AO7. The mechanism involved in EA-PS were the comprehensive effect of DET, •OH and SO4•-. B, Co-CF cathode for flow-through system was stable with five cycles efficient AO7 decay performance. EA-PS in flow-through system was an efficient method with low cost and efficient pollutants degradation. This work provides a feasible strategy for synergistically enhancing PS activation and promoting the degradation of organic pollutants.

Is it possible for fulvic acid modified dredged sediment biochar to adsorb tetracycline and result in a novel method of resource utilization?

In this study, dredged sediment from Baiyang Lake was used as raw material to prepare DSB at a pyrolysis temperature of 600 °C and in an anoxic pyrolysis atmosphere. The adsorption and removal performance of tetracycline in water of DSB were investigated using fulvic acid (FA) as the activator. The biochar materials were first characterized (SEM, BET, XRD, FTIR, and XPS), and the elemental composition and surface functional groups of F-DSB were investigated. The maximum adsorption capacity of F-DSB, according to the Langmuir model, was 72.3 mg/g. Results demonstrated that F-DSB exhibited good adsorption performance. In conclusion, FA is a potential green modifier that can be used to improve the adsorption properties of DSB. This research will be useful in improving our understanding of the possible adsorption mechanism and process optimization of modified DSB. This work offers a novel approach to the resource utilization of dredged sediment.

Pyrolyzed sediment accelerates electron transfer and regulates rhodamine B biodegradation.

Electron transfer efficiency is a key factor that determined the removal of environmental pollution through biodegradation. Electron shuttles exogenously addition is one of the measures to improve the electron transfer efficiency. In this study, the sediment was pyrolyzed at different temperature to investigate its properties of mediating electron transfer and removing of rhodamine B (RhB) in microbial electrochemical systems (MESs). Sediments pyrolyzed at 300 °C (PS300) and 600 °C (PS600) have promoted electron transfer which led to 16 % enhancement of power generation while the result is reversed at 900 °C (PS900). Although power output of PS300 and PS600 are similar, the removal efficiency of RhB is not consistent, which may be caused by the biofilm structure difference. Microbial community analysis revealed that the abundance of EAB and toxicity-degrading bacteria (TDB) in PS600 was 6 % higher than that in PS300. The differentiation of microbial community also affected the metabolic pathway, the amino synthesis and tricarboxylic acid cycle were primarily upregulated with PS600 addition, which enhanced the intracellular metabolism. However, a more active cellular anabolism occurred with PS300, which may have been triggered by RhB toxicity. This study showed that pyrolytic sediment exhibits an excellent ability to mediate electron transport and promote pollutant removal at 600 °C, which provides a techno-economically feasible scenario for the utilization of low-carbon-containing solid wastes.

Photocatalytic degradation of organic pollutants by carbon quantum dots functionalized g-C3N4: A review.

Graphitic carbon nitride (g-C3N4) has received much attention due to its unique characteristics of stable physicochemical features, facile preparation, and inexpensive cost. However, the bulk g-C3N4 has a weak capacity for pollutant degradation and needs to be modified for real application. Therefore, extensive research has been done on g-C3N4, and the discovery of the novel zero-dimensional nanomaterials known as carbon quantum dots (CQDs) provided it with a unique modification option. In this review, the development for the removal of organic pollutants by g-C3N4/CQDs was discussed. Firstly, the preparation of g-C3N4/CQDs were introduced. Then, the application and the degradation mechanism of g-C3N4/CQDs were briefly described. And the discussion of the influencing factors on g-C3N4/CQDs' ability to degrade organic pollutants came in third. Finally, the conclusions of photocatalytic degradation of organic pollutants by g-C3N4/CQDs and future perspectives followed. This review will strengthen the understanding of the photocatalytic degradation of real organic wastewater by g-C3N4/CQDs, including their preparation, application, mechanism, and influencing factors.

Methane emission reduction oriented extracellular electron transfer and bioremediation of sediment microbial fuel cell: A review.

Sediment is the internal and external source of water environment pollution, so sediment remediation is the premise of water body purification. Sediment microbial fuel cell (SMFC) can remove the organic pollutants in sediment by electroactive microorganisms, compete with methanogens for electrons, and realize resource recycling, methane emission inhibiting and energy recovering. Due to these characteristics, SMFC have attracted wide attention for sediment remediation. In this paper, we comprehensively summarized the recent advances of SMFC in the following areas: (1) The advantages and disadvantages of current applied sediment remediation technologies; (2) The basic principles and influencing factors of SMFC; (3) The application of SMFC for pollutant removal, phosphorus transformation and remote monitoring and power supply; (4) Enhancement strategies for SMFC in sediments remediation such as SMFC coupled with constructed wetland, aquatic plant and iron-based reaction. Finally, we have summarized the drawback of SMFC and discuss the future development directions of applying SMFC for sediment bioremediation.

A comprehensive review on the photocatalytic inactivation of Microcystis aeruginosa: Performance, development, and mechanisms.

Harmful algae blooms (HABs), caused by severe eutrophication and extreme weather, have spread all over the world, posing adverse effects on eco-environment and human health. Microcystis aeruginosa is the dominant harmful cyanobacterial species when HABs occur, and the toxic metabolites produced by it, microcystins, are even fatal to humans. Photocatalytic technology has received wide attention from researchers for its clean and energy-efficient features, while the basic mechanisms and modification methods of photocatalysts have also been widely reported. In recent years, photocatalytic technology has shown great promise in the inhibition of HABs. In this article, we systematically reviewed the progress in photocatalytic performance and algae removal efficiency, discuss the damage mechanisms of photocatalysts for algae removal, including physical damage and various oxidative stresses, and also explore the degradation rates and possible pathways of microcystins. It can be concluded that during the photocatalytic process, the cytoarchitectural integrity of algae cells was damaged, a variety of important protein and enzyme systems were disrupted, and the antioxidant systems collapsed due to the continuous attack of ROS, which adversely affected the normal physiological activities and growth, resulting in the inactivation of algae cells. Moreover, photocatalysts have a degrading effect on microcystins, thus reducing the adverse effects of HAB. Finally, a brief summary of future research priorities regarding the photocatalytic degradation of algae cells is presented. This study helps to enhance the understanding of the destruction mechanism of Microcystis aeruginosa during the photocatalytic process, and provides a reference for the photodegradation of HAB in water bodies.

Fabrication of g-C3N4@Bi2MoO6@AgI floating sponge for photocatalytic inactivation of Microcystis aeruginosa under visible light.

In this work, a floating photocatalyst was constructed by loading g-C3N4@Bi2MoO6@AgI (GBA) nanocomposite on a modified polyurethane sponge via a simple dip-coating method and applied for the inactivation of Microcystis aeruginosa under visible light. GBA ternary photocatalyst was fabricated successfully and the morphology, structure, chemical state, and optical properties were characterized systematically. The floating catalyst achieved near 100% removal efficiency of algae cells under 6 h visible light irradiation and also could be retrieved and used at least three times repeatedly. The influences of various conditions on photocatalytic performance such as loading content of nanoparticles, algae density, and concentration of natural organic matters were also studied, which revealed that the GBA floating catalyst exhibited excellent photocatalytic performance of algae removal under different conditions. Furthermore, the physiological characteristics of algae cells during the photocatalytic process, including cell morphology, membrane permeability, Zeta potential, photosynthetic system, antioxidant system, and the metabolic activity were investigated. Results confirmed that the algae cells were severely damaged during the photocatalytic inactivation and the normal physiological functions were significantly affected, which resulted in the death of algae cells at last. Finally, a possible photocatalytic inactivation mechanism of algae cells was proposed. In summary, GBA floating catalyst can effectively inactivate Microcystis aeruginosa under visible light, which confirmed the high efficiency of the novel photocatalytic algae removal technology. Meanwhile, the recyclable floating material also makes the practical application in eutrophic waters of the algae removal technology possible.

Efficient adsorption of tetracycline in aquatic system by thermally-treated sediment.

The disposal of dredged sediment is a considerable challenge for environmental protection and resource utilization. In this study, the dredged sediment was thermally-treated to prepare as adsorbent and utilized for tetracycline adsorption. Sediments based adsorbents under different pyrolysis temperature and atmosphere (N2 and limited oxygen) were obtained and 600 °C and N2 atmosphere (600AN) exhibited maximum TC adsorption capacity (15.45 mg/g). SEM, N2 adsorption-desorption isotherm, XRD, FTIR and XPS analysis suggested larger pore volume, relatively higher surface area, effective pore size distribution and abundant surface functional groups were the main reasons. Moreover, the influence of key adsorption parameters, including adsorbent dosage, initial pH, coexisting ions, ionic strength, contact time, initial TC concentration and ambient temperature had also been investigated. Results revealed that TC adsorption by 600AN were more consistent with pseudo-second order kinetic and Freundlich isothermal models. Combined with characterization results, which reasonably inferred that the adsorption mechanisms of 600AN were mainly involved pore-filling effect, hydrogen bonding interaction and π-π EDA interaction. This work has provided a low-cost, high efficiency and promising method for the dredged sediment reduction and resource recovery.

Laboratory-scale study of a biodegradable microplastic polylactic acid stabilizing aerobic granular sludge system.

The effects of microplastics on aerobic granular sludge technology are an emerging issue, although the impact of degradable microplastics (DMPs) on the aerobic granular system is still unexplored. In this study, degradable microplastic polylactic acid (DMP-PLA) was added at three concentrations (5, 15, 40 mg/L), which strengthened the granular stability and consequently stabilized pollutant removal compared to the control (without DMP-PLA). The experiment showed that adding DMP-PLA made cells secrete more extracellular polymeric substances [64.8 mg/g MLVSS (mixed liquor suspended solids)], particularly retaining ß-D-glucopyranose polysaccharides in experimental group. In addition, abundant hydrogen bonds were also maintained. The reactor under the stress of DMP-PLA exhibited high pollutant removal efficiency (COD>88%, TP>91%, TIN>86%), indicating high performance of the microbes. Microbial analysis at the genus level indicated that Defuviicoccus and Candidatus_Competibacter were dominant after DMP-PLA addition, which identified denitrifying glycogen-accumulating organisms as beneficial for nitrogenous compound removal. Redundancy analysis showed that the abundance of Candidatus_Competibacter was positively related to the addition of DMP-PLA. This study demonstrated that DMP-PLA was feasibly employed in the aerobic granular water treatment process, and presents a new method to optimize the stability and extracellular secretion of the microbial community.

Two key Geobacter species of wastewater-enriched electroactive biofilm respond differently to electric field.

Electroactive biofilms have attracted increasing attention due to their unique ability to exchange electrons with electrodes. Geobacter spp. are widely found to be dominant in biofilms in acetate-rich environments when an appropriate voltage is applied, but it is still largely unknown how these bacteria are selectively enriched. Herein, two key Geobacter spp. that have been demonstrated predominant in wastewater-enriched electroactive biofilm after long-term operation, G. sulfurreducens and G. anodireducens, responded to electric field (EF) differently, leading to a higher abundance of EF-sensitive G. anodireducens in the strong EF region after cocultivation with G. sulfurreducens. Transcriptome analysis indicated that two-component systems containing sensor histidine kinases and response regulators were the key for EF sensing in G. anodireducens rather than in G. sulfurreducens, which are closely connected to chemotaxis, c-di-GMP, fatty acid metabolism, pilus, oxidative phosphorylation and transcription, resulting in an increase in extracellular polymeric substance secretion and rapid cell proliferation. Our data reveal the mechanism by which EF select specific Geobacter spp. over time, providing new insights into Geobacter biofilm formation regulated by electricity.

Exploring the photocatalytic inactivation mechanism of Microcystis aeruginosa under visible light using Ag3PO4/g-C3N4.

In this work, a series of Ag3PO4/g-C3N4 (AG) photocatalysts were synthesized. After characterizing the properties, the effects of mass ratio, light intensity, and material dosages on photodegradation were investigated. The material with a 1/2 mass ratio of Ag3PO4/g-C3N4 showed the highest photocatalytic activity under visible light, and the removal efficiency reached 90.22% for an initial suspended algae concentration of 2.7 × 106 cells/mL, 0.1 g of AG, and 3 h of irradiation. These results showed that the conductivity was increased while the total protein and COD contents of the algae suspension were declined rapidly. In contrast, the variations in the malondialdehyde (MDA) level suggested that the algae cell wall was severely damaged and that selective permeability of the membrane was significantly affected. A possible photocatalytic mechanism was proposed and •O2- was shown to be the major reactive oxygen species in the photocatalysis. In summary, during the visible light photocatalytic process, the cell structure was destroyed, which caused the leakage of electrolyte, the inactivation of protein, and the inhibition of photosynthesis; finally, the cells died. This study provides a reference for photodegradation of algae pollution in water bodies.

Insight of bacteria and archaea in Feammox community enriched from different soils.

Anaerobic ammonium oxidation coupled to Fe(III) reduction, known as Feammox, is a newly discovered nitrogen-cycling process, which serves an important role in the pathways of nitrogen loss in the environment. However, the specific types of microorganisms involved in Feammox currently remain unclear. In this study, we selected two groups of soil samples (paddy and mine), from considerably different habitats in South China, to acclimate Feammox colonies. The Paddy Group had a shorter lag period than the Mine Group, while the ammonium transformation rate was nearly equal in both groups in the mature period. The emergence of the Feammox activity was found to be associated with the increased abundance of iron-reducing bacteria, especially Clostridium_sensu_stricto_12, Desulfitobacterium, Thermoanaerobaculum, Anaeromyxobacter and Geobacter. Ammonium oxidizing archaea and methanogens were dominant among the known archaea. These findings extend our knowledge of the microbial community composition of the potential Feammox microbes from soils under different environmental conditions, which broadens our understanding of this important Fe/N transformation process.

The aggregation behaviour and mechanism of commercial graphene oxide in surface aquatic environments.

In this study, we comprehensively and critically discuss the aggregation mechanism of commercial graphene oxide (CGO) in surface aquatic environments. The aggregation kinetics and critical coagulation concentration of CGO were obtained through time-resolved dynamic light scattering and batch techniques over a wide range of water types. By employing transmission electron microscopy and elemental mapping, Fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy, we studied the effects of cations in natural waters on the microstructure transformation, element content and distribution, and oxygen-containing functional group vibrations of CGO. The aggregation of CGO in natural water is induced mainly by Ca2+ by complexing; Na+, with a higher concentration, plays a more important role than Mg2+ in inducing aggregation via electric double layer suppression. Ca2+ mainly interacts with C - COOH, while Mg2+ has a greater effect on C - OH. Na+ has less effect on the oxygen-containing functional group but decreases the C/O ratio in contrast with Mg2+/Ca2+/natural water, indicating the different inducing mechanisms. This study looks forward to providing pivotal knowledge to predict the environmental fate of CGO more accurately in natural surface water.

Applying fulvic acid for sediment metals remediation: Mechanism, factors, and prospect.

Fulvic acid (FA) has been shown to play a decisive role in controlling the environmental geochemical behavior of metals. As a green and natural microbial metabolite, FA is widely used in environmental remediation because of its good adsorption complexation and redox ability. This paper introduces the reaction mechanism and properties of FA with metals, and reviews the progress of research on the remediation of metal pollutant by FA through physicochemical remediation and bioremediation. FA can control the biotoxicity and migration ability of some metals, such as Pb, Cr, Hg, Cd, and As, through adsorption complexation and redox reactions. The concentration, molecular weight, and source are the main factors that determine the remediation ability of FA. In addition, the ambient pH, temperature, metal ion concentrations, and competing components in sediment environments have significant effects on the extent and rate of a reaction between metals and FA during the remediation process. Finally, we summarize the challenges that this promising environmental remediation tool may face. The research directions of FA in the field of metals ecological remediation are also prospected. This review can provide new ideas and directions for the research of remediation of metals contaminants in sediments.

Long-Term Succession Shows Interspecies Competition of Geobacter in Exoelectrogenic Biofilms.

Geobacter spp. are well-known exoelectrogenic microorganisms that often predominate acetate-fed biofilms in microbial fuel cells (MFCs) and other bioelectrochemical systems (BESs). By using an amplicon sequence variance analysis (at one nucleotide resolution), we observed a succession between two closely related species (98% similarity in 16S RNA), Geobacter sulfurreducens and Geobacter anodireducens, in the long-term studies (20 months) of MFC biofilms. Geobacter spp. predominated in the near-electrode portion of the biofilm, while the outer layer contained an abundance of aerobes, which may have helped to consume oxygen but reduced the relative abundance of Geobacter. Removal of the outer aerobes by norspermidine washing of biofilms revealed a transition from G. sulfurreducens to G. anodireducens. This succession was also found to occur rapidly in co-cultures in BES tests even in the absence of oxygen, suggesting that oxygen was not a critical factor. G. sulfurreducens likely dominated in early biofilms by its relatively larger cell size and production of extracellular polymeric substances (individual advantages), while G. anodireducens later predominated due to greater cell numbers (quantitative advantage). Our findings revealed the interspecies competition in the long-term evolution of Geobacter genus, providing microscopic insights into Geobacter's niche and competitiveness in complex electroactive microbial consortia.

Efficient heavy metal removal from water by alginate-based porous nanocomposite hydrogels: The enhanced removal mechanism and influencing factor insight.

Novel porous alginate-based nanocomposite hydrogels were prepared by incorporating polyaniline-polypyrrole modified graphene oxide (GO@PAN-PPy) as reinforcing fillers into the alginate matrix (GO@PAN-PPy/SA) for Cr(VI) and Cu(II) removal from water. Different in-situ co-polymerization functionalized GO with Py-to-An mass ratios of monomers (from nil to 1:1) and contents of GO@PAN-PPy (from nil to 2.0%(w/v)) were embedded into the alginate backbone to improve the sorption performance. Key factors, such as pH, coexisting metal ions, and swelling states were investigated in batch adsorption modes. The synergistic effect combined from polymer backbone and fillers could lower the impact of the pH-dependent adsorption reaction. With an adsorption ability superior to that of plain SA and GO/SA, the optimized GO@PAN-PPy-2(1)/SA exhibited good experimental maximum adsorption capacities for Cr(VI) (~133.7 mg/g) and Cu(II) (~87.2 mg/g) at pH 3.0, which were better than those of many other similar sorbents. The sorbents possessed excellent adaptability for 0.2 M salt for Cr(VI) removal but poor for Cu(II) removal. Pre-swelling treatment and co-adsorption could enhance the adsorption performance. The excellent reusability of hydrogel was demonstrated after five cycles in single/binary system. Overall, this work reveals that the resultant hydrogel holds potential as candidate sorbent to remove anionic-cationic heavy metal ions from water.

Excessive extracellular polymeric substances induced by organic shocks accelerate electron transfer of oxygen reducing biocathode.

Electrotrophic bacteria on cathodes are promising substitutes to precious metals as oxygen reduction reaction catalysts in bioelectrochemical systems (BESs). Leading the anodic effluent to the biocathode has additional benefits of neutralizing pH and removing residual pollutants. However, the overflow of excessive organic pollutants inhibits the activity of autotrophic biocathodes. Adding glucose as an organic shock, we confirm that the startup time of biocathodes is initially prolonged by 1.2 times with a decrease in current. However, the currents inversely surpass the control in glucose-added BESs when the biofilm is mature, and the maximum current density increase by 5.5 times with a relatively stable performance. This increase is mainly attributed to the production of agglomerates dominated by polysaccharides and proteins as extracellular polymeric substances. These agglomerates wrap additional redox shuttles that accelerated the electron transfer between electrotrophic bacteria and the cathode. This study demonstrates for the first time that organic shocks enhance the electroactivity of autotrophic biocathodes and provides insights into the feedback mechanisms of electrotrophic microbial community to environmental changes.

A highly sensitive bioelectrochemical toxicity sensor and its evaluation using immediate current attenuation.

Electroactive biofilm (EAB) sensor had shown great potential in the field of early warning of toxicants in water because of the low-cost and broad-spectrum. However, the traditional calculation of sensitivity strongly relied on the time and concentration gradient which weakened time-efficiency of the sensor. Moreover, the sensitivity could be further improved to respond trace concentrations. Here EAB sensors with different substrate concentrations were formed to respond different concentrations formaldehyde ranging from 1 ppm to 50 ppm and immediate current attenuation (ICA) was induced to evaluate the sensitivity. The ICA (~70 s) exhibited a shorter time than that calculated by calculable sensitivity (CS) and current attenuation (CA), which not only achieved the response of trace concentration but also improved the time-efficiency of the sensor. The EAB formed with 0.1 g/L acetate (EAB-0.1) had a 380% higher sensitivity than that formed with 1.0 g/L acetate (EAB-1.0), leading to a significant electrochemical toxicity response to 1 ppm of formaldehyde. The results of electrochemical response coefficient confirmed that EAB-0.1 was 1.5-6.3 times of that formed with acetate from 0.2 to 1.0 g/L, which was related with microbial community and component of EAB as described in our previous study. Our findings demonstrated that calculation of sensitivity could be optimized to reflect time-efficiency and EAB with limit acetate could be applied in trace toxicant detection.

Revealing Decay Mechanisms of H2O2-Based Electrochemical Advanced Oxidation Processes after Long-Term Operation for Phenol Degradation.

Hydrogen peroxide (H2O2)-based electrochemical advanced oxidation processes (EAOPs) have been widely attempted for various wastewater treatments. So far, stability tests of EAOPs are rarely addressed and the decay mechanism is still unclear. Here, three H2O2-based EAOP systems (electro-Fenton, photoelectro-Fenton, and photo+ electro-generated H2O2) were built for phenol degradation. More than 97% phenol was removed in all three EAOPs in 1 h at 10 mA·cm-2. As a key component in EAOPs, the cathodic H2O2 productivity is directly related to the performance of the system. We for the first time systematically investigated the decay mechanisms of the active cathode by operating the cathodes under multiple conditions over 200 h. Compared with the fresh cathode (H2O2 yield of 312 ± 22 mg·L-1·h-1 with a current efficiency of 84 ± 5% at 10 mA·cm-2), the performance of the cathode for H2O2 synthesis alone decayed by only 17.8%, whereas the H2O2 yields of cathodes operated in photoelectro-generated H2O2, electro-Fenton, and photoelectro-Fenton systems decayed by 60.0, 90.1, and 89.6%, respectively, with the synergistic effect of salt precipitation, •OH erosion, organic contamination, and optional Fe contamination. The lower current decay of 16.1-32.3% in the electrochemical tests manifested that the cathodes did not lose activity severely. Therefore, the significant decrease of H2O2 yield was because the active sites were altered to catalyze the four-electron oxygen reduction reaction, which was induced by the long-term erosion of •OH. Our findings provided new insights into cathode performance decay, offering significant information for the improvement of cathodic longevity in the future.