Current advances of chlorinated organics degradation by bioelectrochemical systems: a review.

Chlorinated organic compounds (COCs) are typical refractory organic compounds, having high biological toxicity. These compounds are a type of pervasive pollutants that can be present in polluted soil, air, and various types of waterways, such as groundwater, rivers, and lakes, posing a significant threat to the ecological environment and human health. Bioelectrochemical systems (BESs) are an effective strategy for the degradation of bio-refractory compounds. BESs improve the waste treatment efficiency through the application of weak electrical stimulation. This review discusses the processes of BESs configurations and degradation performances in different environmental media including wastewater, soil, waste gas and groundwater. In addition, the degradation mechanisms and performance-enhancing additives are summarized. The future challenges and perspectives on the development of BES for COCs removal are briefly discussed.

Effect of ozone injection on the long-term performance and microbial community structure of a VOCs biofilter.

For biofilters treating waste gases containing volatile organic compounds (VOCs), biomass accumulation is a common problem which will induce bed clogging and significant decrease in VOCs removal efficiency during long-term operation. In this study, ozone injection was developed as a biomass control strategy, and its effects on the biofilter performance and the microbial community structure were investigated in long-term operation. Two biofilters, identified as BF1 and BF2, were operated continuously for 160 days treating gaseous toluene under the same conditions, except that 200 mg/m3 ozone was continuously injected into BF1 during days 45-160. During the operation period, ozone injection did not change the toluene removal efficiency, while the pressure drop of BF1 with ozone injection was significantly lowered compared with BF2. The wet biomass accumulation rate of BF1 was 11 g/m3/hr, which was only 46% of that in BF2. According to the carbon balance result, ozone injection also increased the toluene mineralization rate from 83% to 91%, which could be an important reason for the low biomass accumulation. The PMA-qPCR result indicated that ozone injection increased the microbial viability of the biofilm. The high-throughput sequencing result also revealed that the dominant phyla and genera were not changed significantly by ozone injection, but some ozone-tolerant genera such as Rhodanobacter, Dokdonella and Rhodococcus were enhanced by ozone exposure. All the results verified that ozone injection is capable of sustaining the long-term performance of biofilters by lowering the biomass accumulation, increasing the microbial viability and changing the microbial community structure.

Investigation of the characteristics of biofilms grown in gas-phase biofilters with and without ozone injection by CLSM technique.

Recently, ozone injection technique was developed as a novel biomass control method to reduce bed clogging in biofilters treating volatile organic compounds (VOCs). However, the effects of ozone on the characteristics of biofilms are still unknown. In this study, two identical lab-scale biofilters treating gaseous toluene were operated in parallel except that one was continuously injected with 200 mg/m(3) ozone. Four glass slides were placed inside each biofilter on day 57 and then were taken out sequentially after 1, 2, 4, and 6 weeks of cultivation. The biofilms grown on the glass slides were stained by the ViaGram™ Red + Bacterial Gram Stain and Viability Kit and observed through the confocal laser scanning microscopy (CLSM). According to the CLSM images of 1, 2, and 4 weeks, the ozonated biofilm was significantly thinner than the control biofilm, which demonstrated that ozone could effectively control the biomass in the biofilter. For the biofilter without ozone injection, the ratios of viable cells (0.51~0.89) and the ratios of Gram-positive bacteria (0.22~0.57) both decreased within 4 weeks of cultivation. The CLSM image analysis results also demonstrated that a continuous injection of 200 mg/m(3) ozone was able to significantly enhance the ratio of viable cells to 0.77~0.97 and allow the dominance of Gram-positive bacteria in the biofilms with the ratio 0.46~0.88 instead of Gram-negative bacteria. For the 6-week samples, the biofilm thickness of the control system was reduced significantly which indicated the detachment of accumulated biofilms might occur in the samples without ozone.

Shifts of live bacterial community in secondary effluent by chlorine disinfection revealed by Miseq high-throughput sequencing combined with propidium monoazide treatment.

Chlorine disinfection is a commonly used disinfection process in wastewater treatment, but its effects on the indigenous bacterial community in treated wastewater have not been fully elucidated. In this study, secondary effluent samples collected in four wastewater treatment plants (WWTPs) were selected for chlorine disinfection. Shifts in the bacterial community compositions in secondary effluent samples upon chlorine disinfection, both immediately and after 24 h of storage, were investigated using Illumina MiSeq sequencing combined with propidium monoazide (PMA) treatment. The results showed that the phylum Proteobacteria was sensitive to chlorine, with the relative proportions of Proteobacteria decreased from 39.2 to 75.9 % in secondary effluent samples to 7.5 to 62.2 % immediately after chlorine disinfection. The phylogenetic analysis indicated that the most dominant genera belonging to Proteobacteria were sensitive to chlorine. In contrast, the phyla Firmicutes and Planctomycetes showed a certain resistance to chlorine, with their relative proportions increasing from 5.1 to 23.1 % and 0.8 to 9.3 % to 11.3 to 44.6 % and 1.5 to 13.3 %, respectively. Most dominant genera belonging to Firmicutes showed resistance to chlorine. A significant reduction in the richness and diversity of the bacterial community was observed after 24 h of storage of chlorinated secondary effluent. During the 24-h storage process, the relative proportions of most dominant phyla shifted in reverse from the changes induced by chlorine disinfection. Overall, chlorine disinfection not only changes the bacterial community compositions immediately after the disinfection process but also exerts further impacts over a longer period (24 h).

UV light tolerance and reactivation potential of tetracycline-resistant bacteria from secondary effluents of a wastewater treatment plant.

Tetracycline-resistant bacteria (TRB) are of concern as emerging microbial contaminants in reclaimed water. To understand the effects of UV disinfection on TRB, both inactivation and reactivation profiles of TRB, as well as 16 tetracycline-resistant isolates from secondary effluent, were characterized in this study. The inactivation ratio of TRB was significantly lower (3.0-log) than that of heterotrophic bacteria (>4.0-log) in the secondary effluent. Additionally, the proportion of TRB significantly increased from 1.65% to 15.51% under 20mJ/cm(2) ultraviolet (UV) exposure. The inactivation rates of tetracycline-resistant isolates ranged from 0.57/s to 1.04/s, of which tetracycline-resistant Enterobacter-1 was the most tolerant to UV light. The reactivation of TRB, tetracycline-resistant isolated strains, as well as heterotrophic bacteria commonly occurred in the secondary effluent even after 20mJ/cm(2) UV exposure. The colony forming ability of TRB and heterotrophic bacteria reached 3.2-log and 3.0-log under 20mJ/cm(2) UV exposure after 22hr incubation. The final inactivation ratio of tetracycline-resistant Enterobacter-1 was 1.18-log under 20mJ/cm(2) UV exposure after 22hr incubation, which is similar to those of TRB (1.18-log) and heterotrophic bacteria (1.19-log). The increased proportion of TRB and the reactivation of tetracycline-resistant enterobacteria in reclaimed water could induce a microbial health risk during wastewater reuse.

Effect of continuous ozone injection on performance and biomass accumulation of biofilters treating gaseous toluene.

Biofilters treating high-concentration gaseous volatile organic compounds (VOC) can be subject to bed clogging induced by excess biomass accumulation. In this study, O3 was continuously injected into biofilters to control biomass. Its effects on the performance of the biofilters and on biomass accumulation were investigated. Four identical biofilters designed to treat gaseous toluene were operated for 70 days, and three of them were continuously injected with O3 at different concentrations (from 80 to 320 mg/m(3)). The results showed that continuous O3 injection could effectively keep the bed pressure drop stable and had no adverse effect on toluene removal when O3 concentrations were 180-220 mg/m(3). The maximum toluene elimination capacity of the four biofilters was 140 g-toluene/m(3)/h, and the bed pressure drop of the biofilter fed with 180-220 mg/m(3) O3 remained below 3 mmH2O/m throughout the operation period. The biomass accumulation rates of the three biofilters with O3 at 80-320 mg/m(3) were lowered by 0.15-0.25 g/L/day compared with the biofilter without O3. The decreases in biomass accumulation resulted in higher void fractions of the filter beds with O3 injection. Carbon balance analysis indicated that CO2 production had increased while biomass accumulation and leachate waste production decreased in response to O3 injection. Based on the experimental results, it was concluded here that continuous O3 injection can reduce increases in bed pressure effectively, preserve VOC removal capacity, and prevent production of extra leachate waste.

Effect of continuous ozone injection on performance and biomass accumulation of biofilters treating gaseous toluene.

Biofilters treating high-concentration gaseous volatile organic compounds (VOC) can be subject to bed clogging induced by excess biomass accumulation. In this study, O3 was continuously injected into biofilters to control biomass. Its effects on the performance of the biofilters and on biomass accumulation were investigated. Four identical biofilters designed to treat gaseous toluene were operated for 70 days, and three of them were continuously injected with O3 at different concentrations (from 80 to 320 mg/m(3)). The results showed that continuous O3 injection could effectively keep the bed pressure drop stable and had no adverse effect on toluene removal when O3 concentrations were 180-220 mg/m(3). The maximum toluene elimination capacity of the four biofilters was 140 g-toluene/m(3)/h, and the bed pressure drop of the biofilter fed with 180-220 mg/m(3) O3 remained below 3 mmH2O/m throughout the operation period. The biomass accumulation rates of the three biofilters with O3 at 80-320 mg/m(3) were lowered by 0.15-0.25 g/L/day compared with the biofilter without O3. The decreases in biomass accumulation resulted in higher void fractions of the filter beds with O3 injection. Carbon balance analysis indicated that CO2 production had increased while biomass accumulation and leachate waste production decreased in response to O3 injection. Based on the experimental results, it was concluded here that continuous O3 injection can reduce increases in bed pressure effectively, preserve VOC removal capacity, and prevent production of extra leachate waste.

Electrochemical biofilter enhances performance of volatile organic compounds abatement.

An electrochemical biofilter (EBF) was developed for enhancing the removal of volatile organic compounds (VOCs) through current. The removal efficiency (RE) of toluene exhibited a notable increase of 15% while the biomass growth rate exhibited a corresponding decline of 46% under an optimal current intensity of 50 mA. Meanwhile, the efficacy of the EBF system was markedly enhanced upon the removal of n-hexane, styrene, dichloromethane, and diisobutylene. The results indicated that there was an 11% to 49% increase in RE and a 0% to 64% reduction in biomass growth rates under the influence of the current. The current stimulation inhibited the accumulation of microorganisms, thereby alleviating biofilm clogging. The relative abundance of gram-positive phyla, including Firmicutes and Actinobacteria, increased by 15% and 23%, respectively, while the traditionally dominant genera within the Proteobacteria phylum, such as Rhodococcus and Dokdonella, exhibited a decline. In addition, the presence of hydrogen peroxide, free chlorine, and superoxides in the leachate indicated that the oxidative reaction increased in EBF system. This study provides an attractive pathway for current stimulation to enhance degradation of VOCs and alleviate biofilm clogging.

Experimental evaluation of a full-scale in-duct UV germicidal irradiation system for bioaerosols inactivation.

Bioaerosols control techniques, especially ultraviolet germicidal irradiation (UVGI) are gaining attention due to increasing needs for controlling of health risk caused by airborne biocontaminants. The effectiveness of a full-scale in-duct UVGI air disinfection system was investigated. One bacterium, a wild type Escherichia coli, and three fungal spores, Penicillium aragonense, Rhodotorula glutinis, and Cladosporium sp., were selected as test organisms and their inactivation under different conditions representative of a real application in HVAC systems were investigated. The results demonstrated that inactivation of airborne E. coli by the UVGI system was extremely effective, with >99.5 % of the input E. coli inactivated at a residence time lower than 0.36 s in the disinfection section. Airborne fungal spores were less susceptible to UV irradiation than E. coli. Under same conditions, viable counts reduction of P. aragonense, R. glutinis, and Cladosporium sp. spores were 53 %, 63 % and 73 %, respectively. The effect of UV light intensity, air flowrate and relative humidity were analyzed separately. A simplified model based on redefinition of the parameters in the classical inactivation kinetic equation was used to simulate the inactivation of airborne contaminants in the in-duct system under different conditions. The results showed that the simplified model was adequate to estimate disinfection efficacy of different bioaerosols by the UVGI system which could be useful for system design. Overall, this study shows that such in-duct UVGI systems can provide significant control of bioaerosols.

Enhancing biological conversion of NO to N2O by utilizing thermophiles instead of mesophiles.

The production of nitrous oxide (N2O) through the biological denitrification of nitric oxide (NO) from flue gases has recently been achieved. Although the temperature of flue gas after desulphurization is usually 45-70 °C, all previous studies conducted microbial denitrification of NO under mesophilic conditions (22-35 °C). This study investigated the biological conversion of NO to N2O in both mesophilic (35-45 °C) and thermophilic conditions (45-50 °C). The results showed that temperature has a great impact on N2O production, with a maximum conversion efficiency (from NO to N2O) of 82% achieved at 45 °C, which is obviously higher than the reported conversion efficiencies (24-71%) under mesophilic conditions. Additionally, high-throughput sequencing result showed that the genera Enterococcus, Clostridium, Romboutsia, and Streptococcus were closely related to NO denitrification and N2O production. Microbial communities at 40 and 45 °C had greater metabolizing capacities for polymeric carbon sources. This study suggests that thermophilic condition (45 °C) is more suitable for biological production of N2O from NO.

Development of a CFD model indicating the quantitative relationship among reactor dimension, bed flow unevenness, and performance for VOCs biofilters.

This study presents a Computational Fluid Dynamics (CFD) based biofiltration model to investigate the airflow distribution and the impact of bed flow unevenness (BFU) on the removal of Volatile Organic Compounds (VOCs) in biofilters. The biofiltration model consists of a gas flow sub-model and a VOCs removal sub-model, which were validated by pilot-scale experiments. The model was used to examine the quantitative relationship among reactor dimensions, including the width to height ratio of the filter bed and empty bed residence time (EBRT), BFU, and performance for VOCs biofilters. Simulation results demonstrate that the flow unevenness index (FUI) of the packing layer changes from 0.06 to 0.48 m2‧s-1 with reactor dimension changes. With an increase in the width to height ratio at a constant EBRT, FUI increases, BFU changes, and flow velocity fluctuation on the cross-section becomes larger, leading to a reduction of about 10% in VOCs removal efficiency. Concentration distribution of VOCs becomes uneven in the horizontal direction. At a constant width to height ratio of the filter bed, an increase in EBRT causes an increase in FUI, leading to a decrease in VOCs removal efficiency. When the width to height ratio is 0.5, velocity fluctuation of filter bed cross-section is small, the concentration of VOCs decreases evenly across the filter bed layer, and FUI is at a low level (0.06-0.11 m2‧s-1).Implication: In this manuscript, a biofiltration model of VOCs biofilter based on CFD has constructed and validated. And the manuscript gave the quantitative relationship among reactor dimension, bed flow unevenness and performance for VOCs biofilters for the first time. This study can lead to enhanced VOCs removal efficiency and improved overall performance of biofilters in practical engineering applications.

Effect of weak electrical stimulation on m-dichlorobenzene biodegradation in biotrickling filters: Insights from performance and microbial community analysis.

The microbial electrolysis cell coupled with the biotrickling filters (MEC-BTF) was developed for enhancing the biodegradation of gaseous m-dichlorobenzene (m-DCB) through weak electrical stimulation. The maximum removal efficiency and elimination capacity in MEC-BTF were 1.48 and 1.65 times higher than those in open-circuit BTF (OC-BTF), respectively. Weak electrical stimulation had a positive impact on the characteristics of the biofilm. Additionally, microbial community analysis revealed that weak electrical stimulation increased the abundance of key functional genera (e.g., Rhodanobacter and Bacillus) and genes (e.g., catA/E and E1.3.1.32), thereby accelerating reductive dechlorination and ring-opening of m-DCB. Macrogenomic sequencing further revealed that electron transfer pathway in MEC-BTF might be mediated through extracellular electroactive mediators and cytochromes.

Simulation of Biomass Accumulation Pattern in Vapor-Phase Biofilters.

Existence of inert biomass and its impact on biomass accumulation patterns and biofilter performance were investigated. Four biofilters were set up in parallel to treat gaseous toluene. Each biofilter operated under different inlet toluene loadings for 100 days. Two microbial growth models, one with an inert biomass assumption and the other without, were established and compared. Results from the model with the inert biomass assumption showed better agreement with the experimental data than those based on the model without the inert biomass assumption thus verifying that inert biomass accumulation cannot be ignored in the long-term operation of biofilters. According to the model with an inert biomass assumption, the ratio of active biomass to total biomass will decrease and the inert biomass will become dominant in total biomass after a period of time. Filter bed structure simulation results showed that the void fraction is more sensitive to biomass accumulation than the specific surface area. The final void fraction of the biofilters with the highest inlet toluene loading is only 67% of its initial level while the final specific surface area is 82%. Identification and quantification of inert biomass will give a better understanding of biomass accumulation in biofilters and will result in a more exact simulation of biomass change during long-term operations. Results also indicate that an ideal biomass control technique should be able to remove most inert biomass while simultaneously preserving as much active biomass as possible.

Two quorum sensing enhancement methods optimized the biofilm of biofilters treating gaseous chlorobenzene.

In this study, effects of two quorum sensing (QS) enhancement methods on the performance and biofilm of biofilters treating chlorobenzene were investigated. Three biofilters were set up with BF1 as a control, BF2 added exogenous N-acyl-homoserine lactones (AHLs) and BF3 inoculated AHLs-producing bacterium identified as Acinetobacter. The average chlorobenzene elimination capacities were 73 and 77 g/m3/h for BF2 and BF3 respectively, which were significantly higher than 50 g/m3/h for BF1. The wet biomass of BF2 and BF3 with QS enhancement eventually increased to 60 and 39 kg/m3 respectively, and it was 29 kg/m3 for BF1. Analysis on biofilms in three biofilters showed that distribution uniformity, extracellular polymeric substances production, adhesive strengths, viability, and metabolic capacity of biofilms were all prompted by the two QS enhancement methods. Comparisons between the two QS enhancement methods showed that adding exogenous AHLs had more significant enhancing effect on biofilm due to its higher AHLs level in start-up period, while AHLs-producing bacteria had an advantage in enhancing bacterial community diversity. These results demonstrate that QS enhancement methods have the potential to optimize the biofilm and thus improve the performance of biofilters treating recalcitrant VOCs.

Quorum sensing improved the low-temperature performance of biofilters treating gaseous toluene.

Biofilters usually have poor VOC removal performance at temperatures lower than 20 °C. In this study, two quorum sensing (QS) enhancement methods, which are addition of exogenous N-acyl-homoserine lactones (AHLs) and inoculation of AHL-producing bacteria, were applied in biofilters treating gaseous toluene at a low temperature of 12 °C. Their effects on biofilter performance and biofilm characteristics were investigated. The results showed that adding exogenous AHLs and AHL-producing bacteria in biofilters raised the average toluene elimination capacity by 39% and 26% respectively, and raised the average mineralization efficiency by 25% and 47% respectively in first 24 days. In addition, the two QS enhancement methods could increase the attached biomass by 48% and 87% respectively and made the biofilm distribute more uniform by increasing its extracellular polymeric substances content and microbial adhesive strength. The two QS enhancement methods resulted in more mesopores in biofilm, lower O/C and (O+N)/C of organic elements in biofilm, and increased the solubility of toluene in liquid phase, which all benefit VOCs mass transfer in biofilters. These results demonstrate that QS enhancement methods have the potential to optimize the biofilm and thus improve the performance of biofilters treating VOCs at a low temperature. This work provides us a new choice to improve industrial-scale biofilters treating VOCs at high latitude regions or in winter.

Sustaining low pressure drop and homogeneous flow by adopting a fluidized bed biofilter treating gaseous toluene.

A biofilter treating gaseous VOCs is usually a packed bed system which will encounter bed clogging problems with increased pressure drop and uneven gas flow in the filter bed. In this study, a lab-scale fluidized bed reactor (FBR) was set up treating gaseous toluene and compared with a packed bed reactor (PBR) with the same bed height of 150 cm. During 45 days of operation, the average elimination capacity of the FBR was 242 g m-3∙h-1, similar to that in the PBR (228 g m-3∙h-1) under an inlet toluene concentration of 100-300 mg m-3 and an empty bed residence time (EBRT) of 0.60 s. A better mass transfer was also confirmed in the FBR by molecular residence time distribution measurement. The pressure drop of the PBR increased dramatically and exceeded 8000 Pa m-1 while that of the FBR maintained approximately 200 Pa m-1. On the 40th day, the air flow distribution in the FBR was more homogeneous than that in the PBR. The differences in pressure drop and air flow distribution were due to a much lower and more uniform distribution of biomass in the FBR than that in the PBR. The detached biomass collected from the off-gas of the FBR was almost 13 times of that from the PBR. Similar microbial community structures were observed in both systems, with the dominant bacterial genus Stenotrophomonas and the fungal genera Meyerozyma, Aspergillus. The results in this study demonstrated that the FBR could achieve a more stable performance than a PBR in long-term operation.

Modeling of a combined ultraviolet-biofilter system to treat gaseous chlorobenzene I: model development and parametric sensitivity.

A new type of a combined ultraviolet (UV)-biofilter system for air pollution control is developed. In this paper, two conceptual mathematical submodels of the UV reactor and standalone biofilter are developed. All model parameters have been determined by independent experiments or have been taken from literature. Results from UV and the standalone biofilter submodels are in a good agreement with experimental data. However, the performance of the combined system has significantly deviated from those of the UV or standalone submodels because of the stimulating effects of UV irradiation products on the subsequent biofilter performance. A modified model that considers the stimulating effects has agreed well with experimental data over a wide range of operating conditions. Further analysis of the primary parametric sensitivity of the model has shown that inlet chlorobenzene concentrations, gas empty-bed residence time in the UV reactor, and light intensity are important operating conditions.

Low-dosage ozonation in gas-phase biofilter promotes community diversity and robustness.

BACKGROUND: The ozonation of biofilters is known to alleviate clogging and pressure drop issues while maintaining removal performances in biofiltration systems treating gaseous volatile organic compounds (VOCs). The effects of ozone on the biofilter microbiome in terms of biodiversity, community structure, metabolic abilities, and dominant taxa correlated with performance remain largely unknown. METHODS: This study investigated two biofilters treating high-concentration toluene operating in parallel, with one acting as control and the other exposed to low-dosage (200 mg/m3) ozonation. The microbial community diversity, metabolic rates of different carbon sources, functional predictions, and microbial co-occurrence networks of both communities were examined. RESULTS: Consistently higher biodiversity of over 30% was observed in the microbiome after ozonation, with increased overall metabolic abilities for amino acids and carboxylic acids. The relative abundance of species with reported stress-tolerant and biofilm-forming abilities significantly increased, with a consortium of changes in predicted biological pathways, including shifts in degradation pathways of intermediate compounds, while the correlation of top ASVs and genus with performance indicators showed diversifications in microbiota responsible for toluene degradation. A co-occurrence network of the community showed a decrease in average path distance and average betweenness with ozonation. CONCLUSION: Major degrading species highly correlated with performance shifted after ozonation. Increases in microbial biodiversity, coupled with improvements in metabolizing performances of multiple carbon sources including organic acids could explain the consistent performance commonly seen in the ozonation of biofilters despite the decrease in biomass, while avoiding acid buildup in long-term operation. The increased presence of stress-tolerant microbes in the microbiome coupled with the decentralization of the co-occurrence network suggest that ozonation could not only ameliorate clogging issues but also provide a microbiome more robust to loading shock seen in full-scale biofilters. Video abstract.