Boosting o-xylene removal and power generation in an airlift microbial fuel cell system.

Microbial fuel cells (MFCs) are widely acknowledged to be a promising eco-friendly abatement technology of pollutants, and are capable of generating electricity. However, the poor mass transfer and reaction rate in MFCs significantly decrease their treatment capacity for contaminants, especially hydrophobic substances. The present work developed a novel MFC integrated with an airlift (ALR) reactor using a polypyrrole modified anode to promote the bioaccessibility of gaseous o-xylene and attachment of microorganisms. The results indicated that the established ALR-MFC system showed excellent elimination capability, with removal efficiency exceeding 84% even at high o-xylene concentration (1600 mg m-3). The maximum output voltage of 0.549 V and power density of 13.16 mW m-2 obtained by the Monod-type model were approximately twice and sixfold higher than that of a conventional MFC, respectively. According to the microbial community analysis, the superior performances of the ALR-MFC in terms of o-xylene removal and power generation were mainly ascribed to the enrichment of degrader (i.e. Shinella) and electrochemical active bacteria (i.e. Proteiniphilum). Moreover, the electricity generation of the ALR-MFC did not decrease at a high O2 concentration, as O2 was conducive to o-xylene degradation and electron release. The supplication of an external carbon source such as sodium acetate (NaAc) was conducive to increasing output voltage and coulombic efficiency. The electrochemical analysis revealed that released electrons can be transmitted with the action of NADH dehydrogenase to OmcZ, OmcS, and OmcA outer membrane proteins via a direct or indirect pathway, and ended up transferring to the anode directly.

BiOI-SnO2 Heterojunction Design to Boost Visible-Light-Driven Photocatalytic NO Purification.

The efficient, stable, and selective photocatalytic conversion of nitric oxide (NO) into harmless products such as nitrate (NO3-) is greatly desired but remains an enormous challenge. In this work, a series of BiOI/SnO2 heterojunctions (denoted as X%B-S, where X% is the mass portion of BiOI compared with the mass of SnO2) were synthesized for the efficient transformation of NO into harmless NO3-. The best performance was achieved by the 30%B-S catalyst, whose NO removal efficiency was 96.3% and 47.2% higher than that of 15%B-S and 75%B-S, respectively. Moreover, 30%B-S also exhibited good stability and recyclability. This enhanced performance was mainly caused by the heterojunction structure, which facilitated charge transport and electron-hole separation. Under visible light irradiation, the electrons gathered in SnO2 transformed O2 to ·O2- and ·OH, while the holes generated in BiOI oxidized H2O to produce ·OH. The abundantly generated ·OH, ·O2-, and 1O2 species effectively converted NO to NO- and NO2-, thus promoting the oxidation of NO to NO3-. Overall, the heterojunction formation between p-type BiOI and n-type SnO2 significantly reduced the recombination of photo-induced electron-hole pairs and promoted the photocatalytic activity. This work reveals the critical role of heterojunctions during photocatalytic degradation and provides some insight into NO removal.

Dibenzothiophene Removal from Fuel Oil by Metal-Organic Frameworks: Performance and Kinetics.

Desulfurization of organic sulfur in the fuel oil is essential to cut down the emission of sulfur dioxide, which is a major precursor of the acid rain and PM2.5. Currently, hydrodesulfurization is regarded as a state-of-art technology for the desulfurization of fuel oil. However, due to the stringent legislation of the fuel oil, the deep desulfurization technology is urgent to be developed. Adsorptive desulfurization method is promising due to the high selectivity and easy operation. The development of efficient adsorbent is important to advance this technology into industrial application. In this work, the five types of metal-organic frameworks (MOFs), including Cu-BTC, UMCM-150, MIL-101(Cr), UIO-66, and Cu-ABTC were synthesized for the adsorption of dibenzothiophene (DBT), a typical organic sulfur compound in the fuel oil. The experimental results revealed that the adsorption capacity of the five MOFs followed the order of Cu-ABTC, UMCM-150, Cu-BTC, MIL-101(Cr), and UIO-66, which adsorption capacities were 46.2, 34.2, 28.3, 26.3, and 22.0 mgS/g, respectively. The three types of Cu-based MOFs such as Cu-ABTC, UMCM-150, and Cu-BTC outperformed the Cr-based MOFs, MIL-101, and Zr-based MOFs, UIO-66. Since the surface area and pore volumes of the Cu-based MOFs were not the greatest among the tested five MOFs, the physical properties of the MOFs were not the only limited factor for the DBT adsorption. The π-complexation between DBT and linkers/metal in the MOFs was also important. Kinetic analysis showed that the DBT adsorption onto the five tested MOFs follows the pseudo-second-order kinetics, confirming that the chemical π-complexation was also contributed to the DBT adsorption. Furthermore, the operation parameters such as oil-adsorbent ratio, initial sulfur concentration and adsorption temperature for the DBT adsorption onto Cu-ABTC were optimized to be 100:1 g/g, 1000 mgS/L and 30 °C, respectively. This work can provide some insights into the development of efficient adsorbent for the organic sulfur adsorption.

Simulation of suspended sediment transport in a floating canopy channel based on random displacement model.

In conventional research, the suspended sediment distribution in a channel under the action of floating canopy has been rarely studied. In this study, experiments on sediment transport in flume with fixed suspended vegetation were carried out under different velocity conditions. It was performed to examine the suspended sediment transport and distribution law as impacted by the floating canopy. The vertical distribution formula of velocity impacted by the floating canopy was derived based on improved two-layer theory. Combined with the random displacement model (RDM), a Lagrangian method was developed to simulate the suspended sediment transport under the action of the floating canopy. Compared with the experimental data, the R2 of vertical velocity simulation was higher than 0.96, and the vertical distribution of suspended sediment concentration varied significantly (4.64 to 19.83 g/L) following the vertical coordinate. Subsequently, the numerical model of sandy flow with the floating canopy was established by complying with the stratified sediment turbulence diffusion coefficient to predict the suspended sediment transport. Besides, the established numerical model can lay a theory basis for sediment transport in such channels (floating canopy channels).

The bacterial community structure in epiphytic biofilm on submerged macrophyte Potamogetom crispus L. and its contribution to heavy metal accumulation in an urban industrial area in Hangzhou.

Submerged macrophytes and their epiphytic biofilms are important media for metal transport/transformation in aquatic environment. However, the bacterial community structure and the contribution of the epiphytic biofilm to the heavy metal accumulation remain unclear. Therefore, in this study, water, sediment, submerged macrophyte (Potamogeton crispus L.) and its epiphytic biofilm samples in three sites of the moat in the industrial area of Hangzhou were collected for analyzing. The bacterial community structure was significantly impacted by the TN concentrations, and Genus Aeromonas (24.5-41.8%), Acinetobacter (16.2-29.8%) and Pseudomonas (12.6-23.6%) dominated in all epiphytic biofilm samples, which had the heavy metal pollutant resistibility. The contents of Cr in biofilms (7.4-8.3 mg/kg, DW) were significantly higher than those in leaves (1.0-2.4 mg/kg, DW), while the contents of Cu (11.0-13.9 mg/kg, DW) in leaves were significantly higher than those in biofilms (0.7-3.9 mg/kg, DW) in all the three sites. The BCF values of metals in the biofilm were followed the order of YF < IC < ETS. The results indicated that the epiphytic biofilm had positive effects on the metal bioaccumulation, and the metal accumulation ability increased with the hydrodynamic forces. Bioaccumulation by the epiphytic biofilm may be an effective way for metal (especially Cr) remediation.

Removal of nitrate from agricultural runoff in biochar electrode based biofilm reactor: Performance and enhancement mechanisms.

A biochar electrode based biofilm reactor was developed for advanced removal of nitrate from agricultural runoff. The corn-straw (Zea mays L.) biochar formed at 500 °C has an adsorption capacity of NO3--N up to 2.659 mg g-1. After 45-day start-up phase, the removal efficiency of nitrate reached 93.4% when impressed current was 20 mA, hydraulic retention time was 12 h and chemical oxygen demand/total nitrogen (C/N) ratio was 0.56 without additional carbon source. In comparison, neither electrochemical reduction alone nor microbial denitrification alone could obtain the ideal nitrate removal efficiency. The results implied that bio-electrochemical reduction was the main way of nitrate removal in the biofilm electrode reactor (BER). The denitrification efficiency of 88.9% could still be obtained when C/N = 0. It is because biochar can significantly promote the utilization efficiency of cathode electrons by microorganisms. Thus, biochar is a promising electrode material, which provides a new idea for the optimization of BER.

Nitrogen transformation in slightly polluted surface water by a novel biofilm reactor: Long-term performance and microbial population characteristics.

This study proposes a modular floating biofilm reactor (MFBR) for in situ nitrogen removal from slightly polluted water in rivers using enriched indigenous microorganisms. Its main structure is a 60 cm × 60 cm × 90 cm rectangular reactor filled with hackettens. After a 96-day startup, the removal efficiencies of ammonia-N and total N (TN) reached 80% and 25%, respectively, with a hydraulic retention time (HRT) of 10 h, whereas those in a control reactor (without biofilm) were only 4.9% and 0.2%, respectively. The influences of HRT and dissolved oxygen (DO) were also investigated. As a key factor, HRT significantly affected the removal efficiencies of ammonia-N and TN. When HRT was close to the actual value for a river studied (2.4 min), the removal efficiencies of ammonia-N and TN were only 8.7% and 3.1%, respectively. Aeration increased the concentration of DO in water, which enhanced nitrification but inhibited denitrification. When HRT was 2.4 min, aeration intensity was 20 L/min; the ammonia-N and TN removal rates were 9.5 g/(m2·d) and 11.3 g/(m2·d), respectively. The results of microbial community analysis indicated that the microorganisms forming the biofilm were indigenous bacteria. The findings demonstrated a concept-proof of MFBR, which may be evaluated in scaling up investigation for developing a new methodology for nitrogen removal from slightly polluted surface water in plain river networks.

Recent advances in mitigating membrane biofouling using carbon-based materials.

Biofouling is the Achilles Heel of membrane processes. The accumulation of organic foulants and growth of microorganisms on the membrane surface reduce the permeability, shorten the membrane life, and increase the energy consumption. Advancements in novel carbon-based materials (CBMs) present significant opportunities in mitigating biofouling of membrane processes. This article provides a comprehensive review of the recent progress in the application of CBMs in antibiofouling membrane. It starts with a detailed summary of the different antibiofouling mechanisms of CBM-containing membrane systems. Next, developments in membrane modification using CBMs, especially carbon nanotubes and graphene family materials, are critically reviewed. Further, the antibiofouling potential of next-generation carbon-based membranes is surveyed. Finally, the current problems and future opportunities of applying CBMs for antibiofouling membranes are discussed.

Bioaccumulation of potentially toxic elements by submerged plants and biofilms: A critical review.

The accumulation of potentially toxic elements (PTEs) in aquatic ecosystems has become a global concern, as PTEs may exert a wide range of toxicological impacts on aquatic organisms. Submerged plants and the microorganisms attached to their surfaces, however, have displayed great potential as a means of coping with such pollution. Therefore, it is crucial to understand the transport pathways of PTEs across sediment and organisms as well as their accumulation mechanisms in the presence of submerged plants and their biofilms. The majority of previous studies have demonstrated that submerged plants and their biofilms are indicators of PTE pollution in the aquatic environment, yet relatively little is known about PTE accumulation in epiphytic biofilms. In this review, we describe the transport pathways of PTEs in the aquatic environment in order to offer remarkable insights into bioaccumulation mechanisms in submerged plants and their biofilms. Based on the literature cited in this review, the roles of epiphytic biofilms in bioaccumulation and as an indicator of ecosystem health are discussed.

Microbial compositions and metabolic interactions in one- and two-phase partitioning airlift bioreactors treating a complex VOC mixture.

Engineered microbial ecosystems in bioscrubbers for the treatment of volatile organic compounds (VOCs) have been complicated by complex VOC mixtures from various industrial emissions. Microbial associations with VOC removal performance of the bioscrubbers are still not definitive. Here, one- and two-phase partitioning airlift bioreactors were used for the treatment of a complex VOC mixture. Microbial characteristics in both bioreactors were uncovered by high-throughput metagenomics sequencing. Results showed that dominant species with specialized VOC biodegradability were mainly responsible for high removal efficiency of relative individual VOC. Competitive enzyme inhibitions among the VOC mixture were closely related to the deterioration of removal performance for individual VOC. Relative to the mass transfer resistance, the specialized biodegrading functions of microbial inoculations and enzymatic interactions among individual VOC biodegradation also must be carefully evaluated to optimize the treatment of complex VOC mixtures in bioreactors.

A Biophysicochemical Model for NO Removal by the Chemical Absorption-Biological Reduction Integrated Process.

The chemical absorption-biological reduction (CABR) integrated process is regarded as a promising technology for NOx removal from flue gas. To advance the scale-up of the CABR process, a mathematic model based on mass transfer with reaction in the gas, liquid, and biofilm was developed to simulate and predict the NOx removal by the CABR system in a biotrickling filter. The developed model was validated by the experimental results and subsequently was used to predict the system performance under different operating conditions, such as NO and O2 concentration and gas and liquid flow rate. NO distribution in the gas phase along the biotrickling filter was also modeled and predicted. On the basis of the modeling results, the liquid flow rate and total iron concentration were optimized to achieve >90% NO removal efficiency. Furthermore, sensitivity analysis of the model revealed that the performance of the CABR process was controlled by the bioreduction activity of Fe(III)EDTA. This work will provide the guideline for the design and operation of the CABR process in the industrial application.

Bioelectrochemical Reduction of Fe(II)EDTA-NO in a Biofilm Electrode Reactor: Performance, Mechanism, and Kinetics.

A biofilm electrode reactor (BER) is proposed to effectively regenerate Fe(II)EDTA, a solvent for NOx removal from flue gas, from Fe(II)EDTA-NO, a spent solution. In this study, the performance, mechanism, and kinetics of the bioelectrochemical reduction of Fe(II)EDTA-NO were investigated. The pathways of Fe(II)EDTA-NO reduction were investigated via determination of nitrogen element balance in the BER and an abiotic electrode reactor. The experimental results indicate that the chelated NO (Fe(II)EDTA-NO) is reduced to N2 with N2O as an intermediate. However, the oxidation of NO occurred in the absence of Fe(II)EDTA in abiotic reactors. Furthermore, the accumulation of N2O was suppressed with the help of electricity. The preponderant electron donor for reduction of Fe(II)EDTA-NO was also confirmed via analysis of the electron conservation. About 87% of Fe(II)EDTA-NO was reduced using Fe(II)EDTA as the electron donor in the presence of both glucose and cathode electrons while the cathode electrons were utilized for the reduction of Fe(III)EDTA to Fe(II)EDTA. Michaelis-Menten kinetic constants of bioelectrochemical reduction of Fe(II)EDTA-NO were also calculated. The maximum reduction rate of Fe(II)EDTA-NO was 13.04 mol m(-3) h(-1), which is 50% higher than that in a conventional biofilter.

Pathway of FeEDTA transformation and its impact on performance of NOx removal in a chemical absorption-biological reduction integrated process.

A novel chemical absorption-biological reduction (CABR) integrated process, employing ferrous ethylenediaminetetraacetate (Fe(II)EDTA) as a solvent, is deemed as a potential option for NOx removal from the flue gas. Previous work showed that the Fe(II)EDTA concentration was critical for the NOx removal in the CABR process. In this work, the pathway of FeEDTA (Fe(III)/Fe(II)-EDTA) transformation was investigated to assess its impact on the NOx removal in a biofilter. Experimental results revealed that the FeEDTA transformation involved iron precipitation and EDTA degradation. X-ray photoelectron spectroscopy analysis confirmed the iron was precipitated in the form of Fe(OH)3. The iron mass balance analysis showed 44.2% of the added iron was precipitated. The EDTA degradation facilitated the iron precipitation. Besides chemical oxidation, EDTA biodegradation occurred in the biofilter. The addition of extra EDTA helped recover the iron from the precipitation. The transformation of FeEDTA did not retard the NO removal. In addition, EDTA rather than the iron concentration determined the NO removal efficiency.

Re-acclimation performance and microbial characteristics of a thermophilic biofilter for NOx removal from flue gas.

Currently, a novel chemical absorption-biological reduction (CABR) integrated process, employing Fe(II)EDTA as a solvent, is being under development to reduce the cost of NOx removal from flue gas. In this work, the NO removal profile, re-acclimation performance, and microbial characteristics in a thermophilic biofilter were investigated at the conditions typical to CABR process. The biofilter comprised of four layers of packing material with a surface area of 1200 m(2) m(-3). Experimental results revealed that the biofilter could remove 95 % of the fed NO at typical flue gas conditions. As the gas residence time varied from 90 to 15 s, the NO removal efficiency decreased from 100 to 56.5 % due to the NO mass transfer limitation. The longer period of the biofilter shutdown required more time for its re-acclimation. For example, after 8-day shutdown, the biofilter was re-acclimated in 32 h. Denaturing gradient gel electrophoresis analysis of PCR-amplified product showed that Pseudomonas, a group of denitrifier, was dominant in the biofilter. Because the Pseudomonas was abundant at the bottom layer of packed-bed, the bottom layer contributed to 60-70 % of the total NO removal. In addition, Pseudomonas gradually faded away along the gas flow path from the bottom to the top of biofilter, resulting in a significant decrease in NO removal at the other three packed-bed layers. These observed results will provide the process engineering and scale-up data with respect to the biofilter operations to help advance the CABR process to pilot-scale testing.

Generation, utilization, and transformation of cathode electrons for bioreduction of Fe(III)EDTA in a biofilm electrode reactor related to NOx removal from flue gas.

A chemical absorption-biological reduction (CABR) integrated system, which employs iron chelate as a solvent, is under development for NOx removal from flue gas. Biofilm electrode reactor (BER) is deemed as a promising bioreactor to regenerate the iron chelate. Although it has been proved that BER can significantly enhance the bioreduction of Fe(III)EDTA, the bioelectrochemistry mechanism involved in the bioreduction of Fe(III)EDTA remains unknown. This work aims to explore this mechanism via the analysis of the generation, utilization, and transformation of cathode electrons in the BER. The results indicate that the generation of cathode electrons follows Faraday's law. The generated cathode electrons were used to produce H2 and directly reduce Fe(III)EDTA in the BER. Meanwhile, the produced H2 served as an electron donor for bioreduction of Fe(III)EDTA. The excess H2 product was transformed to simple organics, e.g., methanol by the hydrogen autotrophy of Pseudomonas under the inorganic and anaerobic conditions. Overall, this work revealed that the reduction of Fe(III)EDTA in the BER was enhanced by both direct electrochemical reduction and indirect bioreduction using H2 as an intermediate. It is also interesting that the excess H2 product was transformed to methanol for microbial metabolism and energy storage in the BER.

Current advances of integrated processes combining chemical absorption and biological reduction for NO x removal from flue gas.

Anthropogenic nitrogen oxides (NO x ) emitted from the fossil-fuel-fired power plants cause adverse environmental issues such as acid rain, urban ozone smoke, and photochemical smog. A novel chemical absorption-biological reduction (CABR) integrated process under development is regarded as a promising alternative to the conventional selective catalytic reduction processes for NO x removal from the flue gas because it is economic and environmentally friendly. CABR process employs ferrous ethylenediaminetetraacetate [Fe(II)EDTA] as a solvent to absorb the NO x following microbial denitrification of NO x to harmless nitrogen gas. Meanwhile, the absorbent Fe(II)EDTA is biologically regenerated to sustain the adequate NO x removal. Compared with conventional denitrification process, CABR not only enhances the mass transfer of NO from gas to liquid phase but also minimize the impact of oxygen on the microorganisms. This review provides the current advances of the development of the CABR process for NO x removal from the flue gas.

NOx removal in chemical absorption-biological reduction integrated system: process rate and rate-limiting step.

Biological reduction of Fe(III)EDTA is considered as the key step that limits the removal efficiency of the chemical absorption-biological reduction integrated system. In this study, the process rates of each reaction step under typical conditions (T=50°C, C FeII(EDTA)=1-5 mmol/L, CNO=0-500 ppm, CO2=1-10%, pH=7) were determined. Relevant kinetic constants including rate constants of absorption part and Michaelis-Menten kinetic constants of regeneration part were also obtained. On this basis, the theoretical process rates of each reaction step were predicted and compared in a steady state. The results confirmed that the removal rate of NO in this system is limited by the biological reduction of Fe(III)EDTA. Moreover, it indicated that increasing the concentration of total iron appropriately could enhance the bioreduction of Fe(III)EDTA.

Enhanced reduction of Fe(II)EDTA-NO/Fe(III)EDTA in NO(x) scrubber solution using a three-dimensional biofilm-electrode reactor.

A promising technique called chemical absorption-biological reduction (CABR) integrated approach has been developed recently for the nitrogen oxides (NO(x)) removal from flue gases. The major challenge for this approach is how to enhance the rate of the biological reduction step. To tackle the challenge, a three-dimensional biofilm-electrode reactor (3D-BER) was utilized. This reactor provides not only considerable amount of sites for biofilm, but also many electron donors for bioreduction. Factors affecting the performance of 3D-BER were optimized, including material of the third electrode (graphite), glucose concentration (1000 mg·L(-1)), and volume current density (30.53 A·m(-3) NCC). Experimental results clearly demonstrated that this method significantly promotes the bioreduction rate of Fe(II)EDTA-NO (0.313 mmol·L(-1)·h(-1)) and Fe(III)EDTA (0.564 mmol·L(-1)·h(-1)) simultaneously. Experiments on the mechanism showed that Fe(II)EDTA serves as the primary electron donor in the reduction of Fe(II)EDTA-NO, whereas the reduction of Fe(III)EDTA took advantage of both glucose and electrolysis-generated H(2) as electron donors. High concentration of Fe(II)EDTA-NO or Fe(III)EDTA interferes the bioreduction of the other one. The proposed methodology shows a promising prospect for NO(x) removal from flue gas.