Enhanced methane production using pretreated sludge in MEC-AD system: Performance,microbial activity,and implications at different applied voltages

Although various pretreatment methods are employed to promote sludge hydrolysis and thereby promoting methane production in the subsequent microbial electrolysis cell assisted anaerobic digestion (MEC-AD) system, the questions arise are, “which pretreatment method on waste activated sludge (WAS) maximises the sludge hydrolysis and what is the optimal applied voltage on anaerobic digestion (AD) to stimulates the direct interspecies electron transfer (DIET) performance and thereby accelerating the methane production fed with pretreated WAS?” was still unanswered. Herein, firstly, a series of pretreatment methods to hydrolyse and mineralise the organic matter of WAS was performed to evaluate solubilization efficiency and thereafter, the influence of different applied voltages (0.3 V, 0.6 V, and 0.9 V) on coupled MEC-AD reactors fed with pretreated WAS was investigated to apprehend the DIET promotion for methane production. The results indicated that in MEC-AD reactors, the methane yield increased by 27.2%, 44.8%, and 37.3% when the applied voltages were 0.3 V, 0.6 V, and 0.9 V, respectively. Therefore, the alkaline-thermal pretreatment (ATP) enhanced the sludge hydrolysis in WAS, followed by an applied voltage of 0.6 V in the MEC-AD reactor fed with pretreated WAS, enhanced methane production under DIET stimulation induced by the increased abundance of electroactive microorganisms (EAM) and the advanced electron transfer. Besides, the energy balance estimation validates that with an applied voltage of 0.6 V in MEC-AD could achieve higher net energy input.     

Integration of submersible microbial fuel cell in anaerobic digestion for enhanced production of methane and current at varying glucose levels

A submersible microbial fuel cell (SMFC) was coupled with anaerobic digestion (AD) system to establish synergy for enhancing the electricity and methane production at different glucose concentration of 2, 4 and 10 g/l. High amount of stable current generation of 0.35 mA was obtained at 4 g/l, which was about 1.5 times higher than the SMFC-AD operated at 10 g/l glucose. Methane production and yield were enhanced by 69% and 28%, respectively in SMFC-AD in comparison with AD operation at 2 g/l. Maximum methane yield of 0.32 l-CH₄/g COD was observed in SMFC-AD operation at 2 g/l, followed by 4 g/l (0.28 l-CH₄/g COD) and 10 g/l (0.18 l-CH₄/g COD). Furthermore, the SMFC-AD process increased COD removal and maintained proper pH of around 6.8–7.3 for efficient methane production. This study suggests that the SMFC-AD can achieve enhanced methane production compared to stand-alone AD with additional electricity generation.     

Source of methane and methods to control its formation in single chamber microbial electrolysis cells

Methane production occurs during hydrogen gas generation in microbial electrolysis cells (MECs), particularly when single chamber systems are used which do not keep gases, generated at the cathode, separate from the anode. Few studies have examined the factors contributing to methane gas generation or the main pathway in MECs. It is shown here that methane generation is primarily associated with current generation and hydrogenotrophic methanogenesis and not substrate (acetate). Little methane gas was generated in the initial reaction time (<12 h) in a fed batch MEC when acetate concentrations were high. Most methane was produced at the end of a batch cycle when hydrogen and carbon dioxide gases were present at the greatest concentrations. Increasing the cycle time from 24 to 72 h resulted in complete consumption of hydrogen gas in the headspace (applied voltage of 0.7 V) with methane production. High applied voltages reduced methane production. Little methane (<4%) accumulated in the gas phase at an applied voltage of 0.6–0.9 V over a typical 24 h cycle. However, when the applied voltage was decreased to 0.4 V, there was a greater production of methane than hydrogen gas due to low current densities and long cycle times. The lack of significant hydrogen production from acetate was also supported by Coulombic efficiencies that were all around 90%, indicating electron flow was not altered by changes in methane production. These results demonstrate that methane production in single chamber MECs is primarily associated with current generation and hydrogen gas production, and not acetoclastic methanogenesis. Methane generation will therefore be difficult to control in mixed culture MECs that produce high concentrations of hydrogen gas. By keeping cycle times short, and using higher applied voltages (≥0.6 V), it is possible to reduce methane gas concentrations (<4%) but not eliminate methanogenesis in MECs.     

Bioelectrochemical enhancement of methane production in anaerobic digestion of food waste

This study was conducted to optimize microbial electrolysis cells (MECs) + anaerobic digestion (AD) using integrated Taguchi method and response surface methodology (RSM). The MECSs were applied to enhance the efficiency of AD using food waste as substrate. Using Taguchi method and RSM, the optimum conditions of the MEC + AD were applied voltage (1.2 V), substrate (2.4 g COD/L) and ratio of reactor volume and electrode area (0.33 m3/m2), respectively. The results of the modified Gompertz and dual-pool 1st order showed that the maximum methane yield, maximum methane production rate, and rate constant for rapidly degradable substrate were 1.2, 1.3 and 1.5 fold higher than those of the AD, respectively. Microbial communities analyses indicated that acetoclastic methanogens were initially floating in MEC + AD reactor, but they became attached onto electrodes over time.     

Enhanced hydrogen production in a UASB reactor by retaining microbial consortium onto carbon nanotubes (CNTs)

Biohydrogen and subsequent biomethane generation from biomass is a promising strategy for renewable energy supply, because this combination can lead to higher energy recovery efficiency and faster fermentation than single methane fermentation. Microbial consortium control by retaining hydrogen-producers through the addition of microbial carriers is an alternative to constructing hydrogen-producing reactors. Here we report the use of carbon nanotubes (CNTs) as microbial carriers to enhance microbial retention and the production of biohydrogen. Laboratory-scale upflow anaerobic sludge blanket (UASB) reactors with CNTs at 100 mg/L achieved a maximal hydrogen production rate of 5.55 L/L/d and a maximal hydrogen yield of 2.45 mol/mol glucose. Compared to frequently used activated carbon (AC) particles, CNTs resulted in quicker startup and better performance of hydrogen fermentation in UASB reactors. Scanning electron microscopy (SEM) and pyrosequencing results revealed that the reactor with CNTs led to a high proportion of hydrogen-producing bacteria among the microbial consortium, which endowed the microbes with strong flocculation capacity and hydrogen productivity.     

Promoting direct interspecies electron transfer for methane production in bioelectrochemical anaerobic digestion: Impact of electrode surface area and switching circuit

The bioelectrochemical enhancement of direct interspecies electron transfer (DIET) for methane production was investigated in a UASB reactor under different electrode surface areas. The specific methane production rate is stabilized at 316.7 mL/g COD in the bioelectrochemical UASB (BUASB) reactor with an electrode surface area of 10 m²/m³, which is significantly higher than the 216.8 mL/g COD of the UASB reactor. The electroactive bacteria, involved in the DIET for methane production, is signifianctly increased in the BUASB reactor. When the electrode surface area is expanded to (20 and 30) m²/m³, the specific methane production rates in the BUASB reactor are further increased to (358.4 and 361.0) mL/g COD, respectively (p-value > 0.05). The theoretical methane production from the electrode surface is approximate 3.1% of the total methane production in all BUASB reactors, and the bioelectrochemical methane production is mainly attributed to the biological DIET pathway (54%) in the bulk solution. The BUASB reactor at the electrode surface area of 20 m²/m³ showes better performance according to the methane production, process stability, and enrichment of electroactive microorganisms. The bioelectrochemical system provides a new platform that can dramatically improve the performance of UASB process for treating brewery wastewater.     

Enhanced methane fermentation of municipal sewage sludge by microbial electrochemical systems integrated with anaerobic digestion

Sewage sludge from a municipal wastewater treatment plant was fed into a microbial electrochemical system, combined with an anaerobic digester (MES-AD), for enhanced methane production and sludge stabilization. The effect of thermally pretreating the sewage sludge on MES-AD performance was investigated. These results were compared to those obtained from control operations, in which the sludge was not pretreated or MES integration was absent. The soluble chemical oxygen demand (SCOD) in the raw sewage sludge after pretreatment was 31% higher than the SCOD in untreated sludge (5804.85 mg/L vs. 4441.46 mg/mL). The methane yield and proportion of methane in biogas generated by the MES-AD were higher than those of the control systems, regardless of the pretreatment process. The maximum methane yield (0.28 L CH₄/g COD) and methane production (1139 mL) were obtained with the MES inoculated with pretreated sewage sludge. Methane yield and production with this system using pretreated sewage were 47% and 56% higher, respectively, than those of the control (0.19 L CH₄/g COD, 730 mL). Additionally, the maximum SCOD removal (89%) and current generation were obtained with the MES inoculated with a pretreated substrate. These results suggested that sewage sludge could be efficiently stabilized with enhanced methane production by synergistic combination of MES-AD system with pretreatment process.     

Thermodynamic analysis of hydrogen production from methane via autothermal reforming and partial oxidation followed by water gas shift reaction

Reaction characteristics of hydrogen production from a one-stage reaction and a two-stage reaction are studied and compared with each other in the present study, by means of thermodynamic analyses. In the one-stage reaction, the autothermal reforming (ATR) of methane is considered. In the two-stage reaction, it is featured by the partial oxidation of methane (POM) followed by a water gas shift reaction (WGSR) where the temperatures of POM and WGSR are individually controlled. The results indicate that the reaction temperature of ATR plays an important role in determining H₂ yield. Meanwhile, the conditions of higher steam/methane (S/C) ratio and lower oxygen/methane (O/C) ratio in association with a higher reaction temperature have a trend to increase H₂ yield. When O/C ≤ 0.125, the coking behavior may be exhibited. In regard to the two-stage reaction, it is found that the methane conversion is always high in POM, regardless of what the reaction temperature is. When the O/C ratio is smaller than 0.5, H₂ is generated from the partial oxidation and thermal decomposition of methane, causing solid carbon deposition. Following the performance of WGSR, it suggests that the H₂ yield of the two-stage reaction is significantly affected by the reaction temperature of WGSR. This reflects that the temperature of WGSR is the key factor in producing H₂. When methane, oxygen and steam are in the stoichiometric ratio (i.e. 1:0.5:1), the maximum H₂ yield from ATR is 2.25 which occurs at 800 °C. In contrast, the maximum H₂ yield of the two-stage reaction is 2.89 with the WGSR temperature of 200 °C. Accordingly, it reveals that the two-stage reaction is a recommended fuel processing method for hydrogen production because of its higher H₂ yield and flexible operation.     

In situ integration of microbial electrochemical systems into anaerobic digestion to improve methane fermentation at different substrate concentrations

Microbial electrochemical system (MES) was integrated into anaerobic digestion (AD) to improve the overall process efficiency by enhancing methane (CH₄) production. CH₄ fermentation at various glucose concentrations (2, 4, 8 and 10 g/l) was evaluated along with corresponding control (without electrodes) operations. The maximum CH₄ yield of 0.34 l- CH₄/g COD was obtained with both 2 and 4 g/l glucose concentrations (MES), which was about 1.4 and 2.4 times, respectively, higher than the values obtained with corresponding control operations. However, at 10 g/l, similar performance (∼0.07 l- CH₄/g COD) was observed with both control and MES operations, which might be due to pH drop occurred by volatile fatty acids (VFAs) buildup in the process. Substrate removal was amplified in the presence of MES with faster degradation of VFAs at all substrate concentrations except 10 g/l. This enhanced utilization of VFAs in the MES process is an important aspect to recover from initial pH drops, especially at higher substrate concentration to maintain the optimum pH for methane fermentation. The current generation and cyclic voltammetric profiles suggest that the enhanced CH₄ production in MES was attributed to the bioelectrochemical reactions on the electrodes.     

Relationship of methane and electricity production in two-chamber microbial fuel cell using sewage sludge as substrate

The relationship of methane and electricity production from sewage sludge in a two-chamber microbial fuel cell (MFC) was studied. The results showed that methane production in the anode chamber could enhance the electricity production from sewage sludge, and the output voltage of the MFC with methane production (0.505–0.600 V) was higher than that of the MFC without it (0.506–0.576 V) in the stable electricity-producing stage. The polarization curves analysis of the two MFCs suggested that methane production could improve the performance characteristics of the MFC. Simultaneous methane and electricity production from sludge in the two-chamber MFC could maintain the mixed sludge in a suitable pH range in the anode chamber for electricity production. Meanwhile, simultaneous methane and electricity production could enhance the hydrolysis of sludge, which increased the reduction of sludge concentration (about 8.31% VSS) and offered more substrates to alleviate the competition between methane and electricity production. Additionally, the addition of 2-Bromoethanesulfonate (BES) could substantially affect the dominant archaea but had little effect on the dominant bacteria in the anode chamber.     

High efficient biohydrogen production from palm oil mill effluent by two-stage dark fermentation and microbial electrolysis under thermophilic condition

Biohydrogen production from palm oil mill effluent by two-stage dark fermentation and microbial electrolysis was investigated under thermophilic condition. The optimum chemical oxygen demand (COD) concentration and pH for dark fermentation were 66 g·L⁻¹ and 6.5 with a hydrogen yield of 73 mL-H₂·gCOD⁻¹. The dark fermentation effluent consisted of mainly acetate and butyrate. The optimum voltage for microbial electrolysis was 0.7 V with a hydrogen yield of 163 mL-H₂·gCOD⁻¹. The hydrogen yield of continuous two-stage dark fermentation and microbial electrolysis was 236 mL-H₂·gCOD⁻¹ with a hydrogen production rate of 7.81 L·L⁻¹·d⁻¹. The hydrogen yield was 3 times increased when compared with dark fermentation alone. Thermoanaerobacterium sp. was dominated in the dark fermentation stage while Geobacter sp. and Desulfovibrio sp. dominated in the microbial electrolysis cell stage. Two-stage dark fermentation and microbial electrolysis under thermophilic condition is a highly promising option to maximize the conversion of palm oil mill effluent into biohydrogen.     

Hydrogen gas production from waste anaerobic sludge by electrohydrolysis: Effects of applied DC voltage

Waste anaerobic sludge was subjected to different DC voltages (0.5-5 V) for hydrogen gas production by using aluminum electrodes and a DC power supply. Effects of applied DC voltage on the rate and extent of hydrogen gas production were investigated. The highest cumulative hydrogen production (2775 ml), daily hydrogen gas formation (686.7 ml d⁻¹), hydrogen yield (96 ml H₂ g⁻¹ COD) and percent hydrogen (94.3%) in the gas phase were obtained with 2 V DC voltage. Energy conversion efficiency (H₂ energy/electrical energy) also reached the highest level (74%) with 2 V DC voltage application. Control experiments with no voltage application to the sludge yielded almost the same level of COD removal, but no hydrogen gas production. Voltage application to water resulted in much lower hydrogen gas production as compared to sludge indicating negligible electrolysis of water. The results indicated that the sludge was naturally decomposed by the active cells removing COD and releasing hydrogen ions to the medium which reacted with the electrons provided by DC current to produce hydrogen gas. Hydrogen gas production from electrohydrolysis of waste sludge was found to be a fast and effective method with high energy efficiency.     

Maximizing performance of microbial electrolysis cell fed with dark fermentation effluent from water hyacinth

The performance of microbial electrolysis cell (MEC) fed with dark fermentation effluent (DEF) from water hyacinth (WH) was enhanced in this study. First, the single effects of the auxiliary processes, including centrifugation, dilution, buffering, and external power input, were investigated. Then, the interaction of these processes was further evaluated using response surface methodology (RSM) and a combination of artificial neural network (ANN) and particle swarm optimization (PSO). Statistical analysis results revealed that ANN-PSO outperformed RSM in predictability. Consequently, the ANN-PSO approach determined that a 2.2-fold dilution of centrifuged-DFE (～1.64 g of soluble metabolite products per L), buffer concentration of 75 mM, and an applied voltage of 0.7 V were the optimal conditions for simultaneously maximizing H₂ production yield and energy efficiency of DFE@WH-fed MEC. Under co-optimized conditions, H₂ yield (560.8 ± 10.8 mL/g-VS) and electrical energy recovery (162.2 ± 4.7%) significantly improved compared to unoptimized conditions.     

Enhanced H2 production from corn stalk by integrating dark fermentation and single chamber microbial electrolysis cells with double anode arrangement

The low conversion efficiency of substrate is one of the main bottlenecks in dark fermentation for bio-H₂ production. Herein, an enhanced H₂ yield from corn stalk was achieved by integrating dark fermentation and single chamber microbial electrolysis cells (MECs). In the dark fermentation stage, a H₂ yield of 129.8 mL H₂/g-corn stalk and an average H₂ production rate of 1.73 m³/m³ d were recorded at 20 g/L of corn stalk and initial pH 7.0. The effluent from dark fermentation was diluted and further employed as feedstock to generate H₂ by MECs. A H₂ yield of 257.3 mL H₂/g-corn stalk, an HPR of 3.43 ± 0.12 m³/m³ d and an energy efficiency of 166 ± 10% were obtained with the effluent COD of 3995.5 mg/L under 0.8 V applied voltage. During MECs operation stage, about 90 ± 2% of acetate was converted to H₂ and the corresponding COD removal reached 44 ± 2% in MECs. Overall, the H₂ yield can reach 387.1 mL H₂/g-corn stalk by integrating dark fermentation and MECs, which had nearly tripled as against that of dark fermentation.     

Bioproduction of hydrogen from food waste by pilot-scale combined hydrogen/methane fermentation

A pilot-scale two-phase hydrogen/methane fermentation system generated 3.9 L biogas per unit time and reactor volume from food waste, of which the fraction of H₂ was approximately 60% at a hydraulic retention time (HRT) of 21 h. As substrate, 90% of the carbohydrates in the organic compounds were consumed, based on COD removal efficiency, and the hydrogen yield was approximately 1.82 (H₂-mol/glucose-mol). The maximum decomposition rate coefficient of hydrogen fermentation was observed at an HRT of 21 h, indicating that reducing HRTs improves hydrogen production. Over 80% of the methane was produced in the methane fermentation tank and the predominant fraction of organic acids after methane fermentation comprised acetic acid. Based on our economic evaluation, two-phase hydrogen/methane fermentation has greater potential for recovering energy than methane-only fermentation.     

Production of methane from ozonated palm oil mill effluent

Methane (CH₄) production from palm oil mill effluent (POME) pre-treated by ozonation was conducted under mesophilic (37 °C) condition. The results demonstrated that methane can be produced from both non-ozonated and ozonated POME at a concentration range of 3,000 to 15,000 mg COD L⁻¹. Methane yield rised 54% when POME was pre-treated by ozonation at POME concentration of 15,000 mg COD L⁻¹. The methane yield increased the POME concentration was increased. At POME above 15,000 mg COD L⁻¹, the methane yield was dropped dramatically. The methane production rates (R_max) and yields exerted similar trend regarding the POME concentration. Accumulation of volatile fatty acids in the reactor posed the drop of methane production. Ozonation pretreatment process of POME can improve the biodegradability of the complex organic matter in POME and enhanced methane yield and rate at POME concentration range of 3,000–15,000 mg COD L⁻¹.     

Hydrogen production from methane under the interaction of catalytic partial oxidation,water gas shift reaction and heat recovery

Hydrogen production from the combination of catalytic partial oxidation of methane (CPOM) and water gas shift reaction (WGSR), viz. the two-stage reaction, in a Swiss-roll reactor is investigated numerically. Particular emphasis is placed on the interaction among the reaction of CPOM, the cooling effect due to steam injection and the excess enthalpy recovery with heat recirculation. A rhodium (Rh) catalyst bed sitting at the center of the reactor is used to trigger CPOM, and two different WGSRs, with the aids of a high-temperature (Fe–Cr-based) shift catalyst and a low-temperature (Cu–Zn-based) shift catalyst, are excited. Two important parameters, including the oxygen/methane (O/C) ratio and the steam/methane (S/C) ratio, affecting the efficiencies of methane conversion and hydrogen production are taken into account. The predictions indicate that the O/C ratio of 1.2 provides the best production of H₂ from the two-stage reaction. For a fixed O/C ratio, the H₂ yield is relatively low at a lower S/C ratio, stemming from the lower performance of WGSR, even though the cooling effect of steam is lower. On the contrary, the cooling effect becomes pronounced as the S/C ratio is high to a certain extent and the lessened CPOM leads to a lower H₂ yield. As a result, with the condition of gas hourly space velocity (GHSV) of 10,000 h⁻¹, the optimal operation for hydrogen production in the Swiss-roll reactor is suggested at O/C = 1.2 and S/C = 4–6.     

Application of an electric field for pretreatment of a feedstock (Laminaria japonica) for dark fermentative hydrogen production

When using cellulosic biomass as feedstock for dark fermentative hydrogen production (DFHP), feedstock preparation is essential step for enhancement of biodegradability. In the present work, electric field was newly applied as a novel pretreatment technique to Laminaria japonica, a marine brown algae, as an alternative method for feedstock preparation. A feasibility test was first conducted (20–100 V for 30 min). The highest H₂ yield (93.6 mL H₂ g⁻¹ dry cell weight (dcw)) was achieved at applied voltage of 60 V, while the performance was decreased from applied voltage of 80–100 V due to increasing formation of hydroxymethylfurfural. Subsequently, electric pretreatment conditions (applied voltage and reaction time) were statistically optimized, and a H₂ yield of 102.7 mL g⁻¹ dcw was recorded with applied voltage 58.5 V and reaction time 30 min. This was 96.1% of the predicted value. These findings clearly revealed that the application of electric field as pretreatment method has enormous potential as an alternative method for feedstock preparation in DFHP.     

Bioelectrochemical enhancement of hydrogen and methane production from the anaerobic digestion of sewage sludge in single-chamber membrane-free microbial electrolysis cells

Batch tests were carried out to investigate the bioelectrochemical enhancement of hydrogen and methane production from the anaerobic digestion of sewage sludge in single-chamber membrane-free microbial electrolysis cells (MEC) and non-MECs. Hydrogen and methane were produced from the anaerobic digestion of sewage sludge in all reactors. Compared with controls, hydrogen production was enhanced 1.7–5.2-fold, and methane production 11.4–13.6-fold with Ti/Ru electrodes at applied voltages of 1.4 and 1.8 V, respectively. Most of hydrogen was produced in the first 5 days of digestion and most of methane was generated after 5 days. No oxygen was detected in the biogas and no hydrogen production was detected in the control test with water. The applied voltages can enhance the removal of suspended and volatile suspended solids, increase the transformation of soluble chemical oxygen demand, accelerate the conversion of volatile fatty acids and maintain an optimal pH range for methanogen growth.     

Impact of applied cell voltage on the performance of a microbial electrolysis cell fully catalysed by microorganisms

The effect of the operating voltage on the performance of a microbial electrolysis cell (MEC) equipped with both a bioanode and a biocathode for hydrogen production is reported. Chronoamperometry tests ranged between 0.3 and 2.0 V were carried out after both bioelectrodes were developed. A maximum current density up to 1.6 A m⁻² was recorded at 1.0 V with hydrogen production rate of nearly 6.0 ± 1.5 L m⁻² cathode day⁻¹. Trace amounts of methane, acetone and formate were detected in cathode's headspace and catholyte which followed the same trend as hydrogen production rate. Meanwhile substrate consumption in anolyte also followed the trend of hydrogen production and current density changes. The bioanode could utilise up to 95% of acetate in the tested voltage ranges, however, at a cell voltage of 2.0 V the bioanode's activity stopped due to oxygen evolution from water hydrolysis. Cyclic voltammograms revealed that the bioanode activity was vital to maintain the functionality of the whole system. The biocathode relied on the bioanode to maintain its potential during the hydrogen evolution. The overall energy efficiency recovered from both bioanode and external power in terms of hydrogen production at the cathode was determined as 29.4 ± 9.0%, within which substrate oxidation contributed up to nearly 1/3 of the total energy marking the importance of bioanode recovering energy from wastewater to reduce the external power supply.