Nitrate increases the capacity of an aerobic moving-bed biofilm reactor (MBBR) for winery wastewater treatment.

We used bench-scale tests and mathematical modeling to explore chemical oxygen demand (COD) removal rates in a moving-bed biofilm reactor (MBBR) for winery wastewater treatment, using either urea or nitrate as a nitrogen source. With urea addition, the COD removal fluxes ranged from 34 to 45 gCOD/m2-d. However, when nitrate was added, fluxes increased up to 65 gCOD/m2-d, twice the amount reported for aerobic biofilms for winery wastewater treatment. A one-dimensional biofilm model, calibrated with data from respirometric tests, accurately captured the experimental results. Both experimental and modelling results suggest that nitrate significantly increased MBBR capacity by stimulating COD oxidation in the deeper, oxygen-limited regions of the biofilm. Our research suggests that the addition of nitrate, or other energetic and broadly used electron acceptors, may provide a cost-effective means of covering peak COD loads in biofilm processes for winery or another industrial wastewater treatment.

Quantitative Microbial Risk Assessment Framework Incorporating Water Ages with Legionella pneumophila Growth Rates.

Water age in drinking water systems is often used as a proxy for water quality but is rarely used as a direct input in assessing microbial risk. This study directly linked water ages in a premise plumbing system to concentrations of Legionella pneumophila via a growth model. In turn, the L. pneumophila concentrations were used for a quantitative microbial risk assessment to calculate the associated probabilities of infection (Pinf) and clinically severe illness (Pcsi) due to showering. Risk reductions achieved by purging devices, which reduce water age, were also quantified. The median annual Pinf exceeded the commonly used 1 in 10,000 (10-4) risk benchmark in all scenarios, but the median annual Pcsi was always 1-3 orders of magnitude below 10-4. The median annual Pcsi was lower in homes with two occupants (4.7 × 10-7) than with one occupant (7.5 × 10-7) due to more frequent use of water fixtures, which reduced water ages. The median annual Pcsi for homes with one occupant was reduced by 39-43% with scheduled purging 1-2 times per day. Smart purging devices, which purge only after a certain period of nonuse, maintained these lower annual Pcsi values while reducing additional water consumption by 45-62%.

Effects of temperature on nitrifying membrane-aerated biofilms: An experimental and modeling study.

Temperature is known to have an important effect on the morphology and removal fluxes of conventional, co-diffusional biofilms. However, much less is known about the effects of temperature on membrane-aerated biofilm reactors (MABRs). Experiments and modeling were used to determine the effects of temperature on the removal fluxes, biofilm thickness and morphology, and biofilm microbial community structure of nitrifying MABRs. Steady state tests were carried out at 10 °C and 30 °C. MABRs grown at 30 °C had higher ammonium removal fluxes (5.5 ± 0.9 g-N/m2/day at 20 mgN/L) than those grown at 10 °C (3.4 ± 0.2 g-N/m2/day at 20 mgN/L). The 30 °C biofilms were thinner and rougher, with a lower protein to polysaccharides ratio (PN/PS) in their extracellular polymeric substance (EPS) matrix and greater amounts of biofilm detachment. Based on fluorescent in-situ hybridization (FISH), there was a higher relative abundance of nitrifying bacteria at 30 °C than at 10 °C, and the ratio of AOB to total nitrifiers (AOB + NOB) was higher at 30 °C (95.1 ± 2.3%) than at 10 °C (77.2 ± 8.6 %). Anammox bacteria were more abundant at 30 °C (16.6 ± 3.7 %) than at 10 °C (6.5 ± 2.4 %). Modeling suggested that higher temperatures increase ammonium oxidation fluxes when the biofilm is limited by ammonium. However, fluxes decrease when oxygen becomes limited, i.e., when the bulk ammonium concentrations are high, due to decreased oxygen solubility. Consistent with the experimental results, the model predicted that the percentage of AOB to total nitrifiers at 30 °C was higher than at 10 °C. To investigate the effects of temperature on biofilm diffusivity and O2 solubility, without longer-term changes in the microbial community, MABR biofilms were grown to steady state at 20 °C, then the temperature changed to 10 °C or 30 °C overnight. Higher ammonium oxidation fluxes were obtained at higher temperatures: 1.91 ± 0.24 g-N/m2/day at 10 °C and 3.19 ± 0.40 g-N/m2/day at 30 °C. Overall, this work provides detailed insights into the effect of temperature on nitrifying MABRs, which can be used to better understand MABR behavior and manage MABR reactors.

Impact of fixture purging on water age and excess water usage, considering stochastic water demands.

Higher water ages are linked with water quality decline as chlorine dissipates, temperatures become more favorable for microbial growth, and metals and organic matter leach from the pipes. Water fixtures with automated purging devices can limit water age in premise plumbing systems, but also increase water use. To develop purging strategies that lower age while also minimizing water use, the stochastic nature of water demands must be considered. In this research, a hydraulic plumbing network model, with stochastic demands at fixtures, was used to compare water age and water use for five purging conditions: purging at regular intervals, "smart" purging (considering the time of last use), purging with different volumes of water, purging at different fixtures, and the purging with different levels of home occupancy. Higher purging frequency and volume resulted in lower water ages, but higher water use. Purging greatly reduced the variability in water ages, avoiding extreme ages entirely. Water age was minimized by scheduling the purging around occupancy behavior, such as before the occupants wake up or return from work. Scheduled purging used more water than smart purging. Purging after 12 h of nonuse used only 55% of the additional water required for purging every 12 h. Purging after 24 h of nonuse at the kitchen tap and shower used only 38% of the additional water required for purging every 24 h, while maintaining lower water ages and removing the variability in water ages. While larger purging volumes had a greater impact on water age, there were diminishing returns. Purging has a larger impact on low-occupancy homes because fixtures have less frequent use. Overall, this research provides a methodology to compare purging strategies that minimize both water age and water use. While the numerical results presented here are only valid for the specific layout and usage habits, they provide insights and trends applicable to other cases.

Perchlorate and chlorate assessment in drinking water in northern Chilean cities.

Perchlorate and chlorate are endocrine disruptors considered emerging contaminants (ECs). Both oxyanions are commonly associated with anthropogenic contamination from fertilizers, pesticides, explosives, and disinfection byproducts. However, the soils of the Atacama Desert are the most extensive natural reservoirs of perchlorate in the world, compromising drinking water sources in northern Chile. Field campaigns were carried (2014-2018) to assess the presence of these ECs in the water supply networks of twelve Chilean cities. Additionally, the occurrence of perchlorate, chlorate and other anions typically observed in drinking water matrices of the Atacama Desert (i.e., nitrate, chloride, sulfate) was evaluated using a Spearman correlation analysis to determine predictors for perchlorate and chlorate. High concentrations of perchlorate (up to 114.48 µg L-1) and chlorate (up to 9650 µg L-1) were found in three northern cities. Spatial heterogeneities were observed in the physicochemical properties and anion concentrations of the water supply network. Spearman correlation analysis indicated that nitrate, chloride, and sulfate were not useful predictors for the presence of perchlorate and chlorate in drinking water in Chile. Hence, this study highlights the need to establish systematic monitoring, regulation, and treatment for these EC of drinking water sources in northern Chilean cities for public health protection.

Unique stratification of biofilm density in heterotrophic membrane-aerated biofilms: An experimental and modeling study.

We consistently find a band of high cell density develop within heterotrophic membrane-aerated biofilms. This study reports and attempts to explain this unique behavior. Biofilm density affects volumetric reaction rates, biofilm growth rates, substrate diffusion, and mechanical behavior. Yet the mechanisms and dynamics of biofilm density development are poorly understood. In this study, a membrane-aerated biofilm, where O2 was supplied from the base of the biofilm and acetate from the bulk liquid, was used to explore spatial and temporal patterns of density development. Biofilm density was assessed by optical coherence tomography. After inoculation, the biofilm quickly increased in thickness, with a low density throughout. However, as the biofilm reached a stable thickness of around 1000 µm, a high-density layer developed in the biofilm interior. The layer slowly expanded over time. Oxygen microprofiles in the biofilm showed this layer coincided with the most metabolically active zone, resulting from counter-diffusing O2 and acetate. The formation of this dense layer appeared to be related to changes in growth rates. Initially, high growth rates throughout the biofilm presumably led to fast-growing, low-density biofilms. As the biofilm became thicker, and as substrates became limiting in the biofilm interior, growth rates decreased, resulting in new growth at a higher density. A 1-D mathematical model with variable biofilm density was developed by linking the rates of extracellular polymeric substances (EPS) production to the growth rate. The model captured the initial fast growth at a low density, followed by a slower, substrate-limited growth in the biofilm interior, producing a dense band within the biofilm. Together, these results suggest that low growth rates can lead to high-density zones within the interior of counter-diffusional biofilms. These findings should also be relevant to conventional, co-diffusional biofilms, although differences in density may be less obvious.

Unique biofilm structure and mass transfer mechanisms in the foam aerated biofilm reactor (FABR).

The foam-aerated biofilm reactor (FABR) is a novel biofilm process that can simultaneously remove carbon and nitrogen from wastewater. A porous polyurethane foam sheet forms an interface between wastewater and aerated water, making it a counter-diffusional biofilm process similar to the membrane-aerated biofilm reactor (MABR). However, it is not clear how biofilm develops the foam interior, and how this impacts mass transfer and performance. This research explored biofilm development within the foam sheet and determined whether advective transport within the sheet played a significant role. Foam sheets with 2-, 4.5- and 9-mm thicknesses were explored. Oxygen, nitrate, nitrite and ammonia profiles in the sheet were measured using microsensors, and biofilm imaging studies were carried out using optical coherence tomography (OCT). On the foam's aerated side, a dense nitrifying biofilm formed. Beyond the aerobic zone, much less biomass was observed, with a high porosity foam-biofilm layer. The higher effective diffusivity within the foam for the 4- and 9-mm sheets suggested advective transport within the foam channel structures. Using an effective diffusivity factor in conventional 1-D biofilm models reproduced the measured substrate concentration profiles within the foam. Four different practical conditions were modelled. The maximum TN removal efficiency was about 70% and a nitrogen removal flux of 1.25 gN.m-2.d-1. We conclude that mass transfer resistance occurred primarily in the dense, nitrifying layer near the aerated side. The rest of the foam sheet was porous, allowing the advective mass transfer.

Effects of biofilm heterogeneity on the apparent mechanical properties obtained by shear rheometry.

Rheometry is an experimental technique widely used to determine the mechanical properties of biofilms. However, it characterizes the bulk mechanical behavior of the whole biofilm. The effects of biofilm mechanical heterogeneity on rheometry measurements are not known. We used laboratory experiments and computer modeling to explore the effects of biofilm mechanical heterogeneity on the results obtained by rheometry. A synthetic biofilm with layered mechanical properties was studied, and a viscoelastic biofilm theory was employed using the Kelvin-Voigt model. Agar gels with different concentrations were used to prepare the layered, heterogeneous biofilm, which was characterized for mechanical properties in shear mode with a rheometer. Both experiments and simulations indicated that the biofilm properties from rheometry were strongly biased by the weakest portion of the biofilm. The simulation results using linearly stratified mechanical properties from a previous study also showed that the weaker portions of the biofilm dominated the mechanical properties in creep tests. We note that the model can be used as a predictive tool to explore the mechanical behavior of complex biofilm structures beyond those accessible to experiments. Since most biofilms display some degree of mechanical heterogeneity, our results suggest caution should be used in the interpretation of rheometry data. It does not necessarily provide the "average" mechanical properties of the entire biofilm if the mechanical properties are stratified.

Effect of membrane type on the behavior of nitrifying membrane aerated biofilms: silicone membranes vs. micromembrane cords.

There is increasing interest in membrane-aerated biofilm reactors (MABRs), due to their energy efficiency and ability to intensify wastewater treatment. While MABR membranes play a key role, supporting biofilms and transferring O2, little research has addressed how membrane types impact MABR performance. This research compared two types of membranes used in commercial MABRs: a silicone hollow-fibre membrane and a 'micromembrane cord,' consisting of an inert cord surrounded by fine proprietary polymeric membranes. We used single-membrane MABRs to determine the oxygen mass transfer coefficient, Km, and explore biofilm development. The silicone membrane had a measured Km of 2.6 m/d, and the micromembrane cord had an apparent Km of 1 m/d. Pure MABR bundles (only biofilm) were operated with synthetic wastewater, and hybrid MABRs (suspended biomass and biofilm) with real wastewater, to explore behaviour for a wide range of conditions. The maximum ammonium oxidation fluxes with synthetic wastewater were 7.8 gN/m2d for the silicone membrane and 4.3 gN/m2d for the micromembrane cord. However, at bulk NH4+ concentrations below 5 mgN/L, the ammonium oxidation fluxes were similar. A previously published MABR model effectively captured the behaviour of each membrane. Nitrification fluxes with real wastewater were lower than synthetic wastewater, likely because of the presence of chemical oxygen demand (COD). Although the ammonium oxidation fluxes were higher for the silicone membranes for a given air supply pressure, the fluxes for the micromembrane cord could be increased using higher intramembrane air pressures. Overall, this research helped understand the impact of membrane types on nitrification fluxes.

Assessing Intermediate Formation and Electron Competition during Thiosulfate-Driven Denitrification: An Experimental and Modeling Study.

There is increasing interest in thiosulfate-driven denitrification for low C/N wastewater treatment, but the denitrification performance varies with the thiosulfate oxidation pathways. Models have been developed to predict the products of denitrification, but few consider thiosulfate reduction to elemental sulfur (S0), an undesirable reaction that can intensify electron competition with denitrifying enzymes. In this study, the model using indirect coupling of electrons (ICE) was developed to predict S0 formation and electron competition during thiosulfate-driven denitrification. Kinetic data were obtained from sulfur-oxidizing bacteria (SOB) dominated by the branched pathway and were used to calibrate and validate the model. Electron competition was investigated under different operating conditions. Modeling results reveal that electrons produced in the first step of thiosulfate oxidation typically prioritize thiosulfate reduction, then nitrate reduction, and finally nitrite reduction. However, the electron consumption rate for S0 formation decreases sharply with the decline of thiosulfate concentration. Thus, a continuous feeding strategy was effective in alleviating the competition between thiosulfate reduction and denitrifying enzymes. Electron competition leads to nitrite accumulation, which could be a reliable substrate for anammox. The model was further evaluated with anammox integration. Results suggested that the branched pathway and continuous supply of thiosulfate are favorable to create a symbiotic relationship between SOB and anammox.

Chlorate addition enhances perchlorate reduction in denitrifying membrane-biofilm reactors.

Perchlorate is a widespread drinking water contaminant with regulatory standards ranging from 2 to 18 µg/L. The hydrogen-based membrane-biofilm reactor (MBfR) can effectively reduce perchlorate, but it is challenging to achieve low-µg/L levels. We explored chlorate addition to increase the abundance of perchlorate-reducing bacteria (PRB) and improve removals. MBfR reactors were operated with and without chlorate addition. Results show that chlorate doubled the abundance of putative PRB (e.g., Rhodocyclales) and improved perchlorate reduction to 23 ± 17 µg/L, compared to 53 ± 37 µg/L in the control. Sulfate reduction was substantially inhibited during chlorate addition, but quickly recovered once suspended. Our results suggest that chlorate addition can enhance perchlorate reduction by providing a selective pressure for PRB. It also decreases net sulfate reduction. KEY POINTS: • Chlorate increased the abundance of perchlorate-reducing bacteria • Chlorate addition improved perchlorate removal • Chlorate appeared to suppress sulfate reduction.

Extracellular DNA plays a key role in the structural stability of sulfide-based denitrifying biofilms.

Sulfide-based biofilm processes are increasingly used for wastewater denitrification, yet little is known about the extracellular polymeric substance (EPS) composition of sulfide-oxidizing biofilms. This can have an important impact on biofilm mechanical strength and stability. In this research, the properties and roles of EPS components in biofilm stability were investigated. Weak biofilm stability characterized by high roughness and numerous "needle" structures was visualized by optical coherence tomography (OCT) and microscopy. A high abundance of extracellular DNA (eDNA) and a low protein to polysaccharide ratio were found in the biofilm. The roles of eDNA, protein and polysaccharide in biofilm cohesion and adhesion were identified through enzyme treatment and atomic force microscopy (AFM). The enzymatic hydrolysis of eDNA increased the elastic modulus of biofilms by 57 times and reduced the adhesion energy by 96%. The hydrolysis of proteins led to an increase of elastic modulus by 27 times and a loss of adhesion energy by 95.5%. The enzymatic hydrolysis of polysaccharides caused minimal changes in elastic modulus and adhesion energy. These results suggest that eDNA was the key EPS component for biofilm cohesion and adhesion, possibly because it provided special binding sites and can form strong cross-linking with magnesium or other multivalent cations. This study provided new insights into the role of eDNA in biofilm stability and shed light on the development of sulfide-based denitrifying biofilms.

Data-driven modeling of heterogeneous viscoelastic biofilms.

Biofilms are typically heterogeneous in morphology, structure, and composition, resulting in nonuniform mechanical properties. The distribution of mechanical properties, in turn, determines the biofilm behavior, such as deformation and detachment. Most biofilm models neglect biofilm heterogeneity, especially at the microscale. In this study, an image-based modeling approach was developed to transform two-dimensional optical coherence tomography (OCT) biofilm images to a pixel-scale non-Newtonian viscosity map of the biofilm. The map was calibrated using the bulk viscosity data from rheometer tests, based on assumed maximum and minimum viscosities and a relationship between OCT image intensity signals and non-Newtonian viscosity. While not quantitatively measuring biofilm viscosity for each pixel, it allows a rational spatial allocation of viscosities within the biofilm: areas with lower cell density, for example, voids, are assigned lower viscosities, and areas with high cell densities are assigned higher viscosities. The spatial distribution of non-Newtonian viscosity was applied in an established Oldroyd-B constitutive model and implemented using the phase-field continuum approach for the deformation and stress analysis. The heterogeneous model was able to predict deformations more accurately than a homogenous one. Stress distribution in the heterogeneous biofilm displayed better characteristics than that in the homogeneous one, because it is highly dependent on the viscosity distribution. This study, using a pixel-scale, image-based approach to map the mechanical heterogeneity of biofilms for computational deformation and stress analysis, provides a novel modeling approach that allows the consideration of biofilm structural and mechanical heterogeneity. Future research should better characterize the relationship between OCT signal and viscosity, and consider other constitutive models for biofilm mechanical behavior.

Unraveling encapsulated growth of Nitrosomonas europaea in alginate: An experimental and modeling study.

Encapsulation is a promising technology to retain and protect autotrophs for biological nitrogen removal. One-dimensional biofilm models have been used to describe encapsulated systems; they do not, however, incorporate chemical sorption to the encapsulant nor do they adequately describe cell growth and distribution within the encapsulant. In this research we developed a new model to describe encapsulated growth and activity of Nitrosomonas europaea, incorporating ammonium sorption to the alginate encapsulant. Batch and continuous flow reactors were used to verify the simulation results. Quantitative PCR and cross-section fluorescence in situ hybridization were used to analyze the growth and spatial distribution of the encapsulated cells within alginate. Preferential growth of Nitrosomonas near the surface of the encapsulant was predicted by the model and confirmed by experiments. The modeling and experimental results also suggested that smaller encapsulants with a larger surface area to volume ratio would improve ammonia oxidation. Excessive aeration caused the breakage of the encapsulant, resulting in unpredicted microbial release and washout. Overall, our modeling approach is flexible and can be used to engineer and optimize encapsulated systems for enhanced biological nitrogen removal. Similar modeling approaches can be used to incorporate sorption of additional species within an encapsulant, additional nitrogen-converting microorganisms, and the use of other encapsulation materials.

Biofilm formation of Ancylobacter sp. TS-1 on different granular materials and its ability for chemolithoautotrophic As(III)-oxidation at high concentrations.

The oxidation of arsenic (As) is a key step in its removal from water, and biological oxidation may provide a cost-effective and sustainable method. The biofilm-formation ability of Ancylobacter sp. TS-1, a novel chemolithoautotrophic As oxidizer, was studied for four materials: polypropylene, graphite, sand, and zeolite. After seven days under batch mixotrophic conditions, with high concentrations of As(III) (225 mg·L-1), biofilm formation was detected on all materials except for polypropylene. The results demonstrate As(III)-oxidation of TS-1 biofilms and suggest that the number of active cells was similar for graphite, sand, and zeolite. However, the biofilm biomass follows the specific surface area of each material: 7.0, 2.4, and 0.4 mg VSS·cm-3 for zeolite, sand, and graphite, respectively. Therefore, the observed biofilm-biomass differences were probably associated with different amounts of EPS and inert biomass. Lastly, As(III)-oxidation kinetics were assessed for the biofilms formed on graphite and zeolite under chemolithoautotrophic conditions. The normalized oxidation rate for biofilms formed on these materials was 3.6 and 1.0 mg·L-1·h-1·cm-3, resulting among the highest reported values for As(III)-oxidizing biofilms operated at high-As(III) concentrations. Our findings suggest that biofilm reactors based on Ancylobacter sp. TS-1 are highly promising for their utilization in As(III)-oxidation pre-treatment of high-As(III) polluted waters.

Spatial distribution of mechanical properties in Pseudomonas aeruginosa biofilms, and their potential impacts on biofilm deformation.

The mechanical properties of biofilms can be used to predict biofilm deformation under external forces, for example, under fluid flow. We used magnetic tweezers to spatially map the compliance of Pseudomonas aeruginosa biofilms at the microscale, then applied modeling to assess its effects on biofilm deformation. Biofilms were grown in capillary flow cells with Reynolds numbers (Re) ranging from 0.28 to 13.9, bulk dissolved oxygen (DO) concentrations from 1 mg/L to 8 mg/L, and bulk calcium ion (Ca2+ ) concentrations of 0 and 100 mg CaCl2 /L. Higher Re numbers resulted in more uniform biofilm morphologies. The biofilm was stiffer at the center of the flow cell than near the walls. Lower bulk DO led to more stratified biofilms. Higher Ca2+ concentrations led to increased stiffness and more uniform mechanical properties. Using the experimental mechanical properties, fluid-structure interaction models predicted up to 64% greater deformation for heterogeneous biofilms, compared with a homogeneous biofilms with the same average properties. However, the deviation depended on the biofilm morphology and flow regime. Our results show significant spatial mechanical variability exists at the microscale, and that this variability can potentially affect biofilm deformation. The average biofilm mechanical properties, provided in many studies, should be used with caution when predicting biofilm deformation.

Predicting biofilm deformation with a viscoelastic phase-field model: Modeling and experimental studies.

Biofilms commonly develop in flowing aqueous environments, where the flow causes the biofilm to deform. Because biofilm deformation affects the flow regime, and because biofilms behave as complex heterogeneous viscoelastic materials, few models are able to predict biofilm deformation. In this study, a phase-field (PF) continuum model coupled with the Oldroyd-B constitutive equation was developed and used to simulate biofilm deformation. The accuracy of the model was evaluated using two types of biofilms: a synthetic biofilm, made from alginate mixed with bacterial cells, and a Pseudomonas aeruginosa biofilm. Shear rheometry was used to experimentally determine the mechanical parameters for each biofilm, used as inputs for the model. Biofilm deformation under fluid flow was monitored experimentally using optical coherence tomography. The comparison between the experimental and modeling geometries, for selected horizontal cross sections, after fluid-driven deformation was good. The relative errors ranged from 3.2 to 21.1% for the synthetic biofilm and from 9.1 to 11.1% for the P. aeruginosa biofilm. This is the first demonstration of the effectiveness of a viscoelastic PF biofilm model. This model provides an important tool for predicting biofilm viscoelastic deformation. It also can benefit the design and control of biofilms in engineering systems.

A computational model for the catalytic hydrogel membrane reactor.

The catalytic hydrogel membrane reactor (CHMR) is a promising new technology for hydrogenation of aqueous contaminants in drinking water. It offers numerous benefits over conventional three-phase reactors, including immobilization of nano-catalysts, high reactivity, and control over the hydrogen (H2) supply concentration. In this study, a computational model of the CHMR was developed using AQUASIM and calibrated with 32 experimental datasets for a nitrite (NO2-)-reducing CHMR using palladium (Pd) nano-catalysts (~4.6 nm). The model was then used to identify key factors impacting the behavior of the CHMR, including hydrogel catalyst density, H2 supply pressure, influent and bulk NO2- concentrations, and hydrogel thickness. Based on the model calibration, the reaction rate constants for the NO2- steady-state adsorption Hinshelwood reaction equation, k1 and k2, were 0.0039 m3 mole-Pd-1 s-1 and 0.027 (mole-H2 m3)1/2 mole-Pd-1 s-1, respectively. The reactant flux, which is the overall NO2- removal rate for the CHMR, is affected by the NO2- reduction rate at each catalyst site, which is in turn controlled by the available NO2- and H2 concentrations that are regulated by their mass transport behavior. Reactant transport in the CHMR is counter-diffusional. So for thick hydrogels, the concurrent concentrations of NO2- and H2 are limiting in the middle region along the x-y plane of the hydrogel, which results in a low overall NO2- removal rate (i.e., flux). Thinner hydrogels provide higher concurrent reactant concentrations throughout the hydrogel, resulting in higher fluxes. However, if the hydrogel is too thin, the flux becomes limited by the amount of Pd that can be loaded, and unused H2 can diffuse into the bulk and promote biofilm growth. The hydrogel thickness that maximized the NO2- flux ranged between 30 and 150 µm for the conditions tested. The computational model is the first to describe CHMR behavior, and it is an important tool for the further development of the CHMR. It also can be adapted to assess CHMR behavior for other contaminants or catalysts or used for other types of interfacial catalytic membrane reactors.

New insight into CO2-mediated denitrification process in H2-based membrane biofilm reactor: An experimental and modeling study.

The H2-based membrane biofilm reactor (H2-MBfR) is an emerging technology for removal of nitrate (NO3-) in water supplies. In this research, a lab-scale H2-MBfR equipped with a separated CO2 providing system and a microsensor measuring unit was developed for NO3- removal from synthetic groundwater. Experimental results show that efficient NO3- reduction with a flux of 1.46 g/(m2⋅d) was achieved at the optimal operating conditions of hydraulic retention time (HRT) 80 min, influent NO3- concentration 20 mg N/L, H2 pressure 5 psig and CO2 addition 50 mg/L. Given the complex counter-diffusion of substrates in the H2-MBfR, mathematical modeling is a key tool to both understand its behavior and optimize its performance. A sophisticated model was successfully established, calibrated and validated via comparing the measured and simulated system performance and/or substrate gradients within biofilm. Model results indicate that i) even under the optimal operating conditions, denitrifying bacteria (DNB) in the interior and exterior of biofilm suffered low growth rate, attributed to CO2 and H2 limitation, respectively; ii) appropriate operating parameters are essential to maintaining high activity of DNB in the biofilm; iii) CO2 concentration was the decisive factor which matters its dominant role in mediating hydrogenotrophic denitrification process; iv) the predicted optimum biofilm thickness was 650 µm that can maximize the denitrification flux and prevent loss of H2.

Hydrophobic Gas Transfer Membranes for Wastewater Treatment and Resource Recovery.

Gaseous compounds, such as CH4, H2, and O2, are commonly produced or consumed during wastewater treatment. Traditionally, these gases need to be removed or delivered using gas sparging or liquid heating, which can be energy intensive with low efficiency. Hydrophobic membranes are being increasingly investigated in wastewater treatment and resource recovery. This is because these semipermeable barriers repel water and create a three-phase interface that enhances mass transfer and chemical conversions. This Critical Review provides a first comprehensive analysis of different hydrophobic membranes and processes, and identifies the challenges and potential for future system development. The discussions and analyses were grouped based on mechanisms and applications, including membrane gas extraction, membrane gas delivery, and hybrid processes. Major challenges, such as membrane fouling, wetting, and limited selectivity and functionality, are identified, and potential solutions articulated. New opportunities, such as electrochemical coating, integrated membrane electrodes, and membrane functionalization, are also discussed to provide insights for further development of more efficient and low-cost membranes and processes.