The development of cost-effective and highly efficient anode materials for extracellular electron uptake is important to improve the electricity generation of bioelectrochemical systems. An effective approach to mitigate harmful algal bloom (HAB) is mechanical harvesting of algal biomass, thus subsequent processing for the collected algal biomass is desired. In this study, a low-cost biochar derived from algal biomass via pyrolysis was utilized as an anode material for efficient electron uptake. Electrochemical properties of the algal biochar and graphite plate electrodes were characterized in a bioelectrochemical system (BES). Compared with graphite plate electrode, the algal biochar electrode could effectively utilize both indirect and direct electron transfer pathways for current production, and showed stronger electrochemical response and better adsorption of redox mediators. The maximum current density of algal biochar anode was about 4.1 times higher than graphite plate anode in BES. This work provides an application potential for collected HAB to develop a cost-effective anode material for efficient extracellular electron uptake in BES and to achieve waste resource utilization.
In this research, supercritical carbon dioxide extraction (SFE) showed better extraction effect when compared with Solid- liquid extraction (SLE), Soxhlet extraction (SE) and Ultrasonic extraction (UE), not only in the rate but also the time. The comparison among these three extraction modifiers, including acetone, ethanol and methanol demonstrated that ethanol was preferred to SFE due to its high extraction effect and low toxicology. In addition, parameter of SFE, influence of temperature and pressure were investigated, and the best extraction effect was achieved at the optima conditions, temperature of 40°C and the pressure of 35 MPa. Thus, SFE is a highly effective method for flavonols extraction, requiring minimum energy and producing non-toxic byproduct. SFE-GC system is applied for the evaluation on flavonols that plays a key role in plant resistance to heavy metal, with its content and synthetase gene expression significantly increasing in plant when threatened by heavy metal. Besides, results indicated that flavonols can improve plant resistance to oxidative stress by quenching the redundant ROS in matrix.
Porous carbon material facilitates the reaction SO2 + O2 + H2O → H2SO4 in coal-burned flue gas for sulfur resources recovery at mild conditions. It draws a long-term mystery on its heterogeneous catalysis due to the complicated synergic effect between its microstructure and chemical components. To decouple the effects of geometric structure from chemical components, classical molecular dynamics method was used to investigate the static and dynamic characteristics of the reactants (H2O, SO2 and O2) in the confined space truncated by double-layer graphene (DLG). Strong adsorption of SO2 and O2 by the DLG was observed, which results in the filling of the solute molecules into the interior of the DLG and the depletion of H2O. This effect mainly results from the different affinity of the DLG to the species and can be tuned by the separation of the two graphene layers. Such dimension dependence of the static and dynamic properties like distribution profile, molecular cluster, hydrogen bond and diffusion coefficient were also studied. The conclusions drawn in this work could be helpful to the further understanding of the underlying reaction mechanism of desulfurization process in porous carbon materials and other applications of carbon-based catalysts.
First-principles calculations were performed to investigate the mechanism of Hg0 adsorption and oxidation on CeO2(111). Surface oxygen activated by the reduction of Ce4+ to Ce3+ was vital to Hg0 adsorption and oxidation processes. Hg0 was fully oxidized by the surface lattice oxygen on CeO2(111), without using any other oxidizing agents. HCl could dissociate and react with the Hg adatom on CeO2(111) to form adsorbed Hg–Cl or Cl–Hg–Cl groups, which promoted the desorption of oxidized Hg and prevented CeO2 catalyst deactivation. In contrast, O–H and H–O–H groups formed during HCl adsorption consumed the active surface oxygen and prohibited Hg oxidation. The consumed surface oxygen was replenished by adding O2 into the flue gas. We proposed that oxidized Hg desorption and maintenance of sufficient active surface oxygen were the rate-determining steps of Hg0 removal on CeO2-based catalysts. We believe that our thorough understanding and new insights into the mechanism of the Hg0 removal process will help provide guidelines for developing novel CeO2-based catalysts and enhance the Hg0 removal efficiency.
Heterogeneous photocatalysis has long been considered to be one of the most promising approaches to tackling the myriad environmental issues. However, there are still many challenges for designing efficient and cost-effective photocatalysts and photocatalytic degradation systems for application in practical environmental remediation. In this review, we first systematically introduced the fundamental principles on the photocatalytic pollutant degradation. Then, the important considerations in the design of photocatalytic degradation systems are carefully addressed, including charge carrier dynamics, catalytic selectivity, photocatalyst stability, pollutant adsorption and photodegradation kinetics. Especially, the underlying mechanisms are thoroughly reviewed, including investigation of oxygen reduction properties and identification of reactive oxygen species and key intermediates. This review in environmental photocatalysis may inspire exciting new directions and methods for designing, fabricating and evaluating photocatalytic degradation systems for better environmental remediation and possibly other relevant fields, such as photocatalytic disinfection, water oxidation, and selective organic transformations.
In this study, FeVO4 was prepared and used as Fenton-like catalyst to degrade orange G (OG) dye. The removal of OG in an aqueous solution containing 0.5 g·L–1 FeVO4 and 15 mmol·L–1 hydrogen peroxide at pH 7.0 reached 93.2%. Similar rates were achieved at pH 5.7 (k = 0.0471 min–1), pH 7.0 (k = 0.0438 min–1), and pH 7.7 (k = 0.0434 min–1). The FeVO4 catalyst successfully overcomes the problem faced in the heterogeneous Fenton process, i.e., the narrow working pH range. The data for the removal of OG in FeVO4 systems containing H2O2 conform to the Langmuir–Hinshelwood model (R2 = 0.9988), indicating that adsorption and surface reaction are the two basic mechanisms for OG removal in the FeVO4–H2O2 system. Furthermore, the irradiation of FeVO4 by visible light significantly increases the degradation rate of OG, which is attributed to the enhanced rates of the iron cycles and vanadium cycles.
Bioelectrochemical systems (BES) have been extensively studied for resource recovery from wastewater. By taking advantage of interactions between microorganisms and electrodes, BES can accomplish wastewater treatment while simultaneously recovering various resources including nutrients, energy and water (“NEW”). Despite much progress in laboratory studies, BES have not been advanced to practical applications. This paper aims to provide some subjective opinions and a concise discussion of several key challenges in BES-based resource recovery and help identify the potential application niches that may guide further technological development. In addition to further increasing recovery efficiency, it is also important to have more focus on the applications of the recovered resources such as how to use the harvested electricity and gaseous energy and how to separate the recovered nutrients in an energy-efficient way. A change in mindset for energy performance of BES is necessary to understand overall energy production and consumption. Scaling up BES can go through laboratory scale, transitional scale, and then pilot scale. Using functions as driving forces for BES research and development will better guide the investment of efforts.
A membrane-aerated biofilm reactor was employed to investigate the nitrogen removal of one typical municipal reverse osmosis(RO) concentrate with a high total nitrogen (TN) concentration and a low C/ N ratio. The effects of operational conditions, including the aeration pressure, the hydraulic retention time and the C/N ratio, on the systematic performance were evaluated. The nitrogen removal mechanism was evaluated by monitoring the effluent concentrations of nitrogen contents. Furthermore, the microbial tolerance with elevated salinity was identified. The results indicated that the optimal TN removal efficiency of 79.2% was achieved of the aeration pressure of 0.02 MPa, hydraulic retention time of 24 h, and the C/N ratio of 5.8, respectively. It is essential to supplement the carbon source for the targeted RO concentrate to promote the denitrification process. The inhibitory effect of salinity on denitrifying bacteria and nitrite oxidizing bacteria was significant, revealing the limited TN removal capacity of the conditions in this work. The TN removal efficiency remained more than 70% with the addition of salt (NaCl) amount below 20 g/L. This work preliminarily demonstrated the MABR feasibility for the nitrogen removal of municipal RO concentrate with low C/N ratio and provided technical guidance for further scale-up application.
Identifying source information after river chemical spill occurrences is critical for emergency responses. However, the inverse uncertainty characteristics of this kind of pollution source inversion problem have not yet been clearly elucidated. To fill this gap, stochastic analysis approaches, including a regional sensitivity analysis method, identifiability plot and perturbation methods, were employed to conduct an empirical investigation on generic inverse uncertainty characteristics under a well-accepted uncertainty analysis framework. Case studies based on field tracer experiments and synthetic numerical tracer experiments revealed several new rules. For example, the release load can be most easily inverted, and the source location is responsible for the largest uncertainty among the source parameters. The diffusion and convection processes are more sensitive than the dilution and pollutant attenuation processes to the optimization of objective functions in terms of structural uncertainty. The differences among the different objective functions are smaller for instantaneous release than for continuous release cases. Small monitoring errors affect the inversion results only slightly, which can be ignored in practice. Interestingly, the estimated values of the release location and time negatively deviate from the real values, and the extent is positively correlated with the relative size of the mixing zone to the objective river reach. These new findings improve decision making in emergency responses to sudden water pollution and guide the monitoring network design.
Ammonia has emerged as a promising hydrogen carrier with applications as an energy source in recent years. However, in addition to being toxic, gaseous ammonia is a precursor of secondary inorganic aerosols. The concentration of ambient fine particulate matter (PM2.5) is intrinsically connected to public health. In this study, PM2.5-related health impacts of utilizing ammonia-hydrogen energy in Kanto Region, Japan, were investigated. It was assumed that 20% of the electricity consumption in Kanto Region, the most populated area in Japan, was supplied by ammonia-hydrogen energy. The PM2.5 resulted from incomplete ammonia decomposition was simulated by a chemical transport model: ADMER-PRO (modified version). Based on the incremental PM2.5 concentration, health impacts on the elderly (individuals over 65 years old) were quantitatively evaluated. The ammonia emission in this scenario increased PM2.5 by 11.7% (0.16 μg·m–3·y–1) in winter and 3.5% (0.08 μg ·m–3·y–1) in summer, resulting in 351 premature deaths per year. This study suggests that costeffective emissions control or treatment and appropriate land planning should be considered to reduce the associated health impacts of this type of energy generation. In addition, further in-depth research, including cost-benefit analysis and security standards, is needed.
Effect of different carbon sources on purification performance and change of microbial community structure in a novel A2N-MBR process were investigated. The results showed that when fed with acetate, propionate or acetate and propionate mixed (1:1) as carbon sources, the effluent COD, NH4+-N, TN and TP were lower than 30, 5, 15 and 0.5 mg?L–1, respectively. However, taken glucose as carbon source, the TP concentration of effluent reached 2.6 mg?L–1. Process analysis found that the amount of anaerobic phosphorus release would be the key factor to determine the above effectiveness. The acetate was beneficial to the growth of Candidatus Accumulibacter associated with biological phosphorus removal, which was the main cause of high efficiency phosphorus removal in this system. In addition, it could eliminate the Candidatus Competibacter associated with glycogen-accumulating organisms and guarantee high efficiency phosphorus uptake of phosphorus accumulating organisms in the system with acetate as carbon source.
We implemented the online coupled WRF-Chem model to reproduce the 2013 January haze event in North China, and evaluated simulated meteorological and chemical fields using multiple observations. The comparisons suggest that temperature and relative humidity (RH) were simulated well (mean biases are–0.2K and 2.7%, respectively), but wind speeds were overestimated (mean bias is 0.5 m?s–1). At the Beijing station, sulfur dioxide (SO2) concentrations were overpredicted and sulfate concentrations were largely underpredicted, which may result from uncertainties in SO2 emissions and missing heterogeneous oxidation in current model. We conducted three parallel experiments to examine the impacts of doubling SO2 emissions and incorporating heterogeneous oxidation of dissolved SO2 by nitrogen dioxide (NO2) on sulfate formation during winter haze. The results suggest that doubling SO2 emissions do not significantly affect sulfate concentrations, but adding heterogeneous oxidation of dissolved SO2 by NO2 substantially improve simulations of sulfate and other inorganic aerosols. Although the enhanced SO2 to sulfate conversion in the HetS (heterogeneous oxidation by NO2) case reduces SO2 concentrations, it is still largely overestimated by the model, indicating the overestimations of SO2 concentrations in the North China Plain (NCP) are mostly due to errors in SO2 emission inventory.
Three acid-producing strains, AFB-1, AFB-2 and AFB-3, were isolated during this study, and their roles in anaerobic digestion of waste activated sludge (WAS) were evaluated. Data of 16S rRNA method showed that AFB-1 and AFB-2 were Bacillus coagulans, and AFB-3 was Escherichia coli. The removal in terms of volatile solids (VS) and total chemical oxygen demand (TCOD) was maximized at 42.7% and 44.7% by inoculating Bacillus coagulans AFB-1. Besides, the optimal inoculum concentration of Bacillus coagulans AFB-1 was 30% (v/v). Solubilization degree experiments indicated that solubilization ratios (SR) of WAS reached 20.8%±2.2%, 17.7%±1.48%, and 11.1%±1.53%. Volatile fatty acids (VFAs) concentrations and compositions were also explored with a gas chromatograph. The results showed that VFAs improved by 98.5%, 53.0% and 11.6% than those of the control, respectively. Biochemical methane potential (BMP) experiments revealed that biogas production increased by 90.7% and 75.3% when inoculating with Bacillus coagulans AFB-1 and AFB-2. These results confirmed that the isolated acid-producing bacteria, especially Bacillus coagulans, was a good candidate for anaerobic digestion of WAS.
Microwave irradiation has been used to prepare Al, Fe-pillared clays from a natural Tunisian smectite from the El Hicha deposit (province of Gabes). Chemical analysis, XRD spectra and surface properties evidenced the success of pillaring process. The obtained solids present higher surface area and pore volume than conventionally prepared Al-Fe pillared clays. The main advantages of the microwave methodology are the considerable reduction of the synthesis time and the consumption of water. The microwave-derived Al-Fe pillared clays have been tested for catalytic wet air oxidation (CWAO) of phenol in a stirred tank at 160°C and 20 bar of pure oxygen pressure. These materials are efficient for CWAO of phenol and are highly stable despite the severe operating conditions (acidic media, high pressure, high temperature). The catalyst deactivation was also significantly hindered when compared to conventionally prepared clays. Al-Fe pillared clays prepared by microwave methodology are promising as catalysts for CWAO industrial water treatment.
Investigation of demulsification of polybutadiene latex (PBL) wastewater by polyaluminum chloride (PAC) indicated that there was an appropriate dosage range for latex removal. The demulsification mechanism of PAC was adsorption-charge neutralization and its appropriate dosage range was controlled by zeta potential. When the zeta potential of the mixture was between -15 and 15 mV after adding PAC, the demulsification effect was good. Decreasing the latex concentration in chemical oxygen demand (COD) from 8.0 g/L to 0.2 g/L made the appropriate PAC dosage range narrower and caused the maximum latex removal efficiency to decrease from 95% to 37%. Therefore, more accurate PAC dosage control is required. Moreover, adding 50 mg/L sulfate broadened the appropriate PAC dosage range, resulting in an increase in maximum latex removal efficiency from 37% to 91% for wastewater of 0.2 g COD/L. The addition of sulfate will favor more flexible PAC dosage control in demulsification of PBL wastewater.
The feasibility of using Phragmites australis-JS45 system in removing nitrobenzene from sediments was conducted. However, it was observed that nitrobenzene degraded rapidly and was removed completely within 20 days in native sediments, raising the possibility that indigenous microorganisms may play important roles in nitrobenzene degradation. Consequently, this study aimed to verify this possibility and investigate the potential nitrobenzene degraders among indigenous microorganisms in sediments. The abundance of inoculated strain JS45 and indigenous bacteria in sediments was quantified using real-time polymerase chain reaction. Furthermore, community structure of the indigenous bacteria was analyzed through high throughput sequencing based on Illumina MiSeq platform. The results showed that indigenous bacteria in native sediments were abundant, approximately 1014 CFU/g dry weight, which is about six orders of magnitude higher than that in fertile soils. In addition, the levels of indigenous Proteobacteria (Acinetobacter, Comamonadaceae_ uncultured, Pseudomonas, and Thauera) and Firmicutes (Clostridium, Sporacetigenium, Fusibacter, Youngiibacter, and Trichococcus) increased significantly during nitrobenzene removal. Their quantities sharply decreased after nitrobenzene was removed completely, except for Pseudomonas and Thauera. Based on the results, it can be concluded that indigenous microorganisms including Proteobacteria and Firmicutes can have great potential for removing nitrobenzene from sediments. Although P. australis - JS45 system was set up in an attempt to eliminate nitrobenzene from sediments, and the system did not meet the expectation. The findings still provide valuable information on enhancing nitrobenzene removal by optimizing the sediment conditions for better growth of indigenous Proteobacteria and Firmicutes.
Methane production from low-strength wastewater (LSWW) is generally difficult because of the low metabolism rate of methanogens. Here, an up-flow biofilm reactor equipped with conductive granular graphite (GG) as fillers was developed to enhance direct interspecies electron transfer (DIET) between syntrophic electroactive bacteria and methanogens to stimulate methanogenesis process. Compared to quartz sand fillers, using conductive fillers significantly enhanced methane production and accelerated the start-up stage of biofilm reactor. At HRT of 6 h, the average methane production rate and methane yield of reactor with GG were 0.106 m3/(m3·d) and 74.5 L/kg COD, which increased by 34.3 times and 22.4 times respectively compared with the reactor with common quartz sand fillers. The microbial community analysis revealed that methanogens structure was significantly altered and the archaea that are involved in DIET (such as Methanobacterium) were enriched in GG filler. The beneficial effects of conductive fillers on methane production implied a practical strategy for efficient methane recovery from LSWW.
Polycyclic aromatic hydrocarbons (PAHs) often occur in oil-contaminated soil, coke wastewater and domestic sludge; however, associated PAH degraders in these environments are not clear. Here we evaluated phenanthrene degradation potential in the mixed samples of above environments, and obtained a methanogenic community with different microbial profile compared to those from sediments. Phenanthrene was efficiently degraded (1.26 mg/L/d) and nonstoichiometric amount of methane was produced simultaneously. 16S rRNA gene sequencing demonstrated that bacterial populations were mainly associated with Comamonadaceae Nocardiaceae and Thermodesulfobiaceae, and that methanogenic archaea groups were dominated by Methanobacterium and Methanothermobacter. Substances such as hexane, hexadecane, benzene and glucose showed the most positive effects on phenanthrene degradation. Substrate utilization tests indicated that this culture could not utilize other PAHs. These analyses could offer us some suggestions on the putative phenanthrene-degrading microbes in such environments, and might help us develop strategies for the removal of PAHs from contaminated soil and sludge.
A sampling campaign including summer, autumn and winter of 2014 and spring of 2015 was accomplished to obtain the characteristic of chemical components in PM2.5 at three sites of Kunming, a plateau city in South-west China. Nine kinds of water-soluble inorganic ions (WSI), organic and element carbon (OC and EC) in PM2.5 were analyzed by ion chromatography and thermal optical reflectance method, respectively. Results showed that the average concentrations of total WSI, OC and EC were 22.85±10.95 µg·m-3, 17.83±9.57 µg·m-3 and 5.11±4.29 µg·m-3, respectively. They totally accounted for 53.0% of PM2.5. Secondary organic and inorganic aerosols (SOA and SIA) were also assessed by the minimum ratio of OC/EC, nitrogen and sulfur oxidation ratios. The annual average concentrations of SOA and SIA totally accounted for 28.3% of the PM2.5 concentration. The low proportion suggested the primary emission was the main source of PM2.5 in Kunming. However, secondary pollution in the plateau city should also not be ignorable, due to the appropriate temperature and strong solar radiation, which can promote the atmospheric photochemical reactions.
Various pretreatments methods including sonication and grinding were performed on red seaweed Gelidium amansii for the subsequent extraction of agarose. The agarose products are usually extracted from agar powder products from seaweeds. In this study, the agarose was extracted using a direct polyethylene glycol (PEG) method without the need to first process the agar from seaweed. The agar extract was frozen then thawed and mixed directly with PEG solution to precipitate the agarose. The quality of agarose obtained was evaluated through physico-chemical properties analysis which includes spectral technique (FTIR), melting and boiling point, gel strength and sulfate content. These properties were compared with a non-pretreated sample and it was found that the addition of pretreatment steps improved the quality of agarose but gave a slightly lower yield. The gel strength of pretreated samples was much higher and the sulfate content was lower compared to non-pretreated samples. The best pretreatment method was sonication which gave gel strength of 742 g cm-2 and sulfate content of 0.63%. The extraction of agarose can be further improved with the use of different neutralizing agents. Pretreating the seaweed shows potential in improving the quality of agarose from seaweed and can be applied for future extraction of the agarose.
