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Nanoparticle-assisted biohydrogen production from pretreated food industry wastewater sludge: Microbial community shifts in batch and continuous processes

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Abstract

Biohydrogen production from industrial waste has gained a significant attention as a sustainable energy source. In this study, the enrichment of biohydrogen production from pretreated dissolved air flotation (DAF) sludge, generated from food industry wastewater treatment plants, was investigated using SiO 2 @Cu-Ag dendrites core shell nanostructure (NS). The effect of NS on the changes of the microbial community and biohydrogen yield was evaluated through batch and continuous tests. In batch mode, various nanomaterial doses were investigated with several concentrations ranging from 20 to 50 mg/L for hydrogen production using glucose as a substrate. The optimum core-shell NS amount was 40 mg/L, achieving a maximum H 2 yield of 163 mL/g volatile solids (VS) compared to the control's 79 mL/g VS. However, 50 mg/L NS inhibited most bacteria in the sludge. The continuous experiment used a continuous stirring tank reactor (CSTR) with 40 mg/L SiO 2 @Cu-Ag core-shell NS and pretreated industrial sludge as substrate. The H 2 yield increased to 115 L/kg VS compared to the control reactor's 89 L/kg VS. The gas analysis showed compositional proportions of 83 % H 2 , 7 % CO 2 , and 4.5 % methane, while the microbial community analysis indicated the development of hydrogen-producing species such as Clostridium. In conclusion, SiO 2 @Cu-Ag core-shell NS addition enhanced anaerobic degradation of organic matter and its conversion to biohydrogen. The selected nanomaterial can be used for an effective continuous treatment system for industrial sludge while promoting dark fermentation.

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Anaerobic digestion (AD) is one of the most energy-efficient waste treatment technologies for biodegradable wastes. Owing to the increasing trend of metallic nanoparticle applications in industry, they are ubiquitous to the waste streams, which may lead to remarkable impacts on the performance of the AD process. This review addresses the knowledge gaps and summarises the findings from the academic articles published from 2010 to 2019 focusing on the influences on both AD processes of biochemical hydrogen-generation and methane-production from selected metallic nano-materials. Both qualitative and quantitative analyses were conducted with selected indicators to evaluate the metallic nanoparticles' influences on the AD process. The selected metallic nanoparticles were grouped in the view of their chemical formulations aiming to point out the possible mechanisms behind their effects on AD processes. In summary, most metallic nanoparticles with trace-element-base (e.g. iron, cobalt, nickel) have positive effects on both AD hydrogen-generation and methane-production processes in terms of gas production, effluent quality, as well as process optimisation. Within an optimum concentration, they serve as key nutrients providers, aid key enzymes and co-enzymes synthesis, and thus stimulate anaerobic microorganism activities. As for the nano-additives without trace-element base, their positive influences are relied on providing active sites for the microorganism, as well as absorbing inhibitory factors. Moreover, comparisons of these nano-additives’ impacts on the two gas-production phases were conducted, while methane-production phases are found to be more sensitive to additions of these nanoparticles then hydrogen-production phase. Research perspectives and research gaps in this area are discussed.
Article
Hydrogen is considered the energy of the future. In order to meet the requirements of a green production, many technological advances were achieved in the last 20 years. Reviewing these advances allows the understanding the constraints of the sector and the identification of the paths for future research. In this work three routes for renewable hydrogen production from renewable sources were reviewed with focus on patented technologies: dissociation of the H2O molecule, microbial production and thermochemical processes. Three patent databases were accessed, covering documents written in English, Spanish and Portuguese. Water dissociation is the only commercial technology and most efforts were identified in new materials for electrodes, new catalysts and reagent recycling. Microbial production is thermodynamic limited but strategies to maximize the production and overcome economic barriers are mostly related to the use of wastewaters, improving microbial communities' composition and genetic manipulation. Most patents of thermochemical production patents brought contributions to the efficient use of energy especially by the combination with other energy producing technologies. The establishment of a green hydrogen society is strongly dependent of future developments on new materials, recycle of chemical catalysts and efficient use of energy in the short-term.
Article
Hydrogen applicability in the power, chemical and petrochemical industries is constantly growing. Efficient methods of hydrogen generation from renewable sources, including waste products, are currently being developed, even though hydrogen is mainly produced through steam reforming or thermal cracking of natural gas or petroleum fractions. In paper alternative methods of hydrogen production with a particular emphasis on dark fermentation are discussed. The review compiles essential information on strains of bacteria used in the production of hydrogen from waste products in the agroindustry and from lignocellulosic biomass. The effect of such parameters as kind of raw material, method of processing, temperature, pH, substrate concentration, partial pressure of hydrogen, hydraulic retention time, method of inoculum preparation and the type and operating parameters of a reactor on the yield of dark fermentation is discussed. The review aims at presentation of current state of knowledge on the dark fermentation process utilizing waste materials as substrates. The results of investigations with emphasis on the most important issues regarding operating parameters of dark fermentation are also included.
Article
Anaerobic digestion (AD) of sewage sludge is one of the most efficient, effective, and environmentally sustainable remediation techniques; however, the presence of complex floc structures, hard cell walls, and large amounts of molecular organic matter in the sludge hinder AD hydrolysis. Consequently, sewage sludge pretreatment is a prerequisite to accelerate hydrolysis and improve AD efficiency. This review focuses on pretreatment techniques for improving sewage sludge AD, which include mechanical, chemical, thermal, and biological processes. The various pretreatment process effects are discussed in terms of advantages and disadvantages, including their effectiveness, and recent achievements are reviewed for improved biogas production.
Article
This paper illustrates the method to predict the production of biohydrogen and biogas from the horizontal and vertical continuous mixed tank reactor using a numerical approach. Utilization of computational fluid dynamics on the estimation of bioreactor performance is very crucial owing to the uncertainty in the numerical results. Since there has been little work on CFD to determine the influence of hydraulic retention time, impeller speeds, vortex growth, and pH on biohydrogen yield rate the effort had been made. A series of simulations are done with optimal boundary conditions to ensure maximum hydrogen and biogas production rate. Two types of reactors HCSTR and VCSTR are operated at different impeller speed from 40 rpm to 120 rpm. Further, the rate of HRT and organic loading are varied. As the rpm of the impeller increase the rate of hydrogen and biomass production increases not later than 80 rpm. Meanwhile, the optimal range of HRT and pH are 4–8 h and 6.0–8.0. Running the impeller at optimized rate with derived conditions leads to high hydrogen and biogas production of 6 LH2/Ld and 30 L/d. The obtained results are validated with the experimental findings to compare the uncertainty formed due to the numerical simulations. The optimum boundary condition obtained from the study is expected to provide the essential knowledge in establishing the full-scaled reactors.
Article
The efficiency of microbial electron transfer is fundamental for determining the performance of fermentative hydrogen/methane production. To facilitate microbial electron transfer, conductive magnetite nanoparticles (MNPs) were added into a cascading dark fermentation and anaerobic digestion system that was inoculated with Enterobacter aerogenes ZJU1 and methanogenic activated sludge (MAS), respectively. During the hydrogen-producing stage, the ratio of NADH/NAD⁺ and the activities of hydrogenase and electron transport system (ETS) of E. aerogenes ZJU1 were all increased by dosing 200 mg/L MNPs, which was conducive to hydrogen production through the NADH-dependent pathway. In the presence of 200 mg/L MNPs, hydrogen production increased by 21.1%, while subsequent methane production improved by 22.9%. Electrochemical analysis demonstrated the improvement in extracellular electron transfer capacity of MAS after adding MNPs, which can be ascribed to the contribution of MNPs and electrochemically active extracellular polymeric substances (EPS) induced by MNPs, such as humic acid-like and fulvic acid-like substances. Bacteria Syntrophomonas and Archaea Methanosarcina were the dominating enriched syntrophic partners, and the expression of functional genes involved in CO2 reduction to methane pathway was found to increase. Therefore, a more efficient fermentative hydrogen and methane co-production system was established by improving microbial electron transfer with the addition of MNPs.
Article
Photo-fermentation seems to be an attractive hydrogen production pathway. However, the light conversion efficiency and photo-hydrogen production of purple non-sulphur bacteria (PNSB) are very low, and hence, various biotechnological approaches are investigated to improve biohydrogen production. This article presents an overview of the advanced biotechnological approaches to enhance the photo-fermentative biohydrogen production. The advancements reviewed include optimisation of the medium, abiotic factors, the lighting regime, immobilisation techniques, application of photoluminating nanomaterials, genetic engineering, and other strategies. These approaches show positive results in the enhancement of photo-hydrogen production by PNSB. Some recommendations are suggested for further studies in the enhancement of photo-hydrogen production, such as green nanomaterials application, integrated dark- and photo-fermentation, genetic manipulation, and the application of the non-technological analysis approaches.
Article
In this study, the effects of alkaline (pH 10) and acidic (pH 2–5) chemical pretreatment on dissolution of organic matters and biochemical methane potential (BMP) at waste activated sludge (WAS). For each pretreatment methods at different temperature (25, 40, 50 and 60 °C) and operating time (5, 15, 30, 45 min) are the two factors. In the first step, the feasibility of chemical pretreatment in anaerobic digestion was investigated. Increases in soluble chemical oxygen demand (sCOD)/total chemical oxygen demand (tCOD) were determined in all chemical pretreatments. In the second step, the sCOD/tCOD ratio was used to determine the effects on the pretreatment and BMP assay was used to examine the enhanced anaerobic digestion. The pretreatment study conditions were determined due to the highest sCOD/tCOD ratios. These highest ratios were obtained at different pH values, operational times and temperatures. The highest cumulative BMP values were taken at pH 10, 10 min, 60 °C and pH 5, 15 min, 40 °C. Under these pretreatment conditions, the cumulative BMP values were 47.7 mL CH4/g VSS and 12.3 mL CH4/g VSS at conditions pH 10, 10 min, 60 °C and pH 5, 15 min, 40 °C (the control BMP value was extracted). The methane yield values were 43.61% and 12.34% at alkaline acidic conditions (pH 10 and 5). In the pH 2 study results indicated that the cumulative BMP values were 105.1 and 90.5 mL CH4/g VSS for 50–60 °C. These values were exactly the same or lower than the control BMP value.
Article
Dark fermentative hydrogen production from organic wastes can achieve dual benefits of clean energy generation and waste utilization, which offers the best prospects for a biohydrogen production process with high environmental benefits. Biohydrogen production system is a complex biological process, which is affected by many factors, including operational conditions (e.g. temperature, pH), substrate type, reactor design etc., and depends on the microbial type, retention time, activity, productivity and end products. Among these influencing factors the hydrogen-producing microorganisms play a vital role. Great efforts have been made to enhance the hydrogen production efficiency from the perspective of microbiology. In this review, the microbiology, biochemistry and enzymology for biological hydrogen production were briefly summarized and analyzed. The recent progress in microbiology for hydrogen production through dark fermentation was reviewed, including microorganisms, biochemistry, enzymology, microbial modification and the identification of the microbial community structure. Metabolic pathways can be modified by metabolic engineering, thus enhancing the biological hydrogen production through overcoming limiting factors for hydrogen production in various systems by increasing the flow of electrons to hydrogen-producing pathways, increasing substrate utilization, and engineering more efficient and/or oxygen-resistant hydrogen-evolving enzymes. Finally, concluding remarks and perspectives are given.
Article
Ultrasonic treatment has become a modern method for removal of micropollutants and refractory compounds from water/wastewater and to improve biodegradation efficiency of biological activated sludge from wastewater treatment plants, in order to produce biogas. This paper is referring to the ultrasonic pretreatment of biological activated sludge, before anaerobic fermentation phase, to increase the amount of biogas generation. The pretreatment of biological sludge is based on two steps: alkaline digestion and ultrasonication. Ten minutes of alkaline condition (pH 9.5 - 10.5) followed by 10 minutes ultrasonication (20 kHz frequency) were the general operating condition of sludge pretreatment phase. Parallel tests (with and without ultrasonic pretreatment step) were performed in order to assess the effect of ultrasonic pretreatment on biogas generation. Ultrasonication in alkaline condition of biological sludge heave led to doubling the amount of biogas generated in anaerobic fermentation phase.
Article
Pretreatment of waste activated sludge (WAS) results in an improved efficiency of the subsequent anaerobic biotransformation of the organic matter to volatile fatty acids. The pretreatment process has been carried out using alkaline treatment, ultrasonic treatment (20 KHz, 120 W) and different combination of these two methods: alkaline followed by ultrasonic, as well as the combining method in which ultrasonic treatment is applied to WAS samples dosed with alkaline. The hydrolysis efficiency was evaluated based on the quantity of soluble COD (SCOD) and organic nitrogen in the pretreated WAS as well as the production of total volatile fatty acids (TVFA) in the following biochemical acid potential (BAP) test. For WAS samples with described pretreatments, the released SCOD varied from 36% to 89% of the total COD (TCOD) and soluble organic nitrogen from 34% to 42%. The TVFA/TCOD ratio of the raw WAS used in this study was less than 10%. For the alkaline pretreated WAS, the TVFA/TCOD ratio increased to 30%, and the following ultrasonic treatment enhanced the ratio 66%. Further, WAS samples pretreated using simultaneous ultrasound and alkaline treatment in which ultrasonic was applied to WAS samples dosed with 40 meq/L NaOH for 14.4 sec/mL could achieve a maximum TVFA/TCOD ratio of 84% in 21 hours. Therefore, the combination of simultaneous alkaline and ultrasound pretreatment is efficient in enhancing the production of volatile acids in WAS in order to achieve recovery of volatile fatty acids from the WAS.
Article
Biohydrogen production is considered as one of the most promising alternative processes to produce hydrogen due to its effectiveness, renewability, and environmental friendliness compared to the conventional way, such as thermochemical and electrochemical methods. Biohydrogen production via photofermentation produces hydrogen by photo-decomposing organic matters through the nitrogenase of photosynthetic bacteria. Despite its advantages, high energy requirement during nitrogenase-catalyzed reaction and low biohydrogen production efficiencies in the reality have become the foremost concern in a large scale application of photofermentation. Thus, an improvement of biohydrogen yield and light conversion efficiency is necessary to increase the feasibility of photofermentation. One of the simplest ways to improve photofermentation is by adding suitable chemical enhancer. Various studies have shown that an addition of some chemicals, such as iron, molybdenum, ethylenediaminetetraacetic acid (EDTA), vitamins, buffer solution, and others chemicals could increase the biohydrogen production rates and yields by a significant value. However, an addition of other chemicals, such as nickel ions, diphenylene iodonium, dimethylsulphoxide, and copper ions, might cause an adverse effect on the process. Addition of EDTA, molybdenum, ethanol or yeast may inhibit the photofermentation process, depending on the type of bacteria and substrates used during photofermentation process, as well as the concentration of the added chemicals. Hence, the importance and effects of chemicals addition on photofermentative biohydrogen production were discussed in this review paper.
Article
ZVI was reported to enrich H2-utilizing methanogens that enhanced interspecies H2 transfer, while Fe(III) oxide served as a conductive material to promote direct interspecies electron transfer (DIET). However, the interaction of these two modes in anaerobic digestion has not been clarified yet. In this study, when adding Fe3O4 and ZVI simultaneously into an anaerobic digester, the abundance of hydrogenotrophic methanogens decreased drastically compared to ZVI-added digester and Fe-free digester. However, the methane production of ZVI + Fe3O4 added digester were 68.9% higher than Fe-free digester and 20.0% higher than ZVI-added digester, respectively. Sludge reduction rate of these three digesters also showed similar results. These indicated that hydrogenotrophic methanogenesis was not the main reason for methanogenesis in Fe3O4-added digester. Instead, Syntrophomonas and Methanosaeta were specially enriched in Fe3O4-added digesters, which implied that the potential DIET between Syntrophomonas and Methanosaeta was likely a crucial reason for accelerating anaerobic digestion of waste sludge.
Article
Hydrogen production from organic wastes by dark fermentation is promising. Among a variety of organic wastes, sewage sludge has drawn extensive attention due to its huge amount, high organic content and stable source. This paper reviewed the characterization of sludge and the principles and potential of sludge hydrogen fermentation. Poor hydrolysis and low C/N ratio of sludge were two main limitations for sludge hydrogen fermentation. To improve hydrogen production, some pretreatment methods (heat, ultrasound, microwave, alkaline, acid, oxidation, enzyme and bacteria) and the addition of co-fermentation substrates have been applied for enhancing hydrogen production from sludge fermentation. The effect of key factors (temperature, pH, retention time and organic loading rate, agitation intensity, nutrients, inhibitors and inoculum) on hydrogen production and process stability was introduced and discussed. Furthermore, the kinetic models were briefly discussed. After sludge hydrogen fermentation, some end products, including acetate, propionate, butyrate and ethanol, could be used for deducing the fermentation type, and applied as substrates for second stage process (e.g. anaerobic digestion and photo fermentation) for further energy recovery. The development of these two-stage processes was illustrated. Concluding remarks and perspectives for this process were also evaluated.
Chapter
The phenol-sulfuric acid method is a simple and rapid colorimetric method to determine total carbohydrates in a sample. While the method detects virtually all classes of carbohydrates (mono-, di-, oligo-, and polysaccharides), the absorptivity of the different carbohydrates varies. Thus, unless a sample is known to contain only one carbohydrate, the results must be expressed arbitrarily in terms of one carbohydrate. In this laboratory exercise, the total carbohydrate content of soft drinks and beers is determined with the phenol-sulfuric acid method, using a glucose standard curve. Data generated are used to calculate the caloric content of those beverages.
Article
Sewage sludge management is now becoming a serious issue all over the world. Anaerobic digestion is a simple and well-studied process capable of biologically converting the chemical energy of sewage sludge into methane-rich biogas, as a carbon-neutral alternative to fossil fuels whilst destroying pathogens and removing odors. Hydrolysis is the rate-limiting step because of the sewage sludge complex floc structure (such as extracellular polymeric substances) and hard cell wall. To accelerate the rate-limiting hydrolysis and improve the efficiency of anaerobic digestion, various pretreatment technologies have been developed. This paper presents an up-to-date review of recent research achievements in the pretreatment technologies used for improving biogas production including mechanical (ultrasonic, microwave, electrokinetic and high-pressure homogenization), thermal, chemical (acidic, alkali, ozonation, Fenton and Fe(II)-activated persulfate oxidation), and biological options (temperature-phased anaerobic digestion and microbial electrolysis cell). The effectiveness and relative worth of each of the studied technologies are summarized and compared in terms of the resulting sludge properties, the digester performance, the environmental benefits and the current state of real-world application. The challenge and technical issues encountered during sludge cotreatment are discussed, and the future research needs in promoting full-scale implementations of those approaches are proposed.
Article
Biohydrogen production from waste bread in a continuous stirred tank reactor (CSTR) was techno-economically assessed. The treating capacity of the H2-producing plant was assumed to be 2 ton waste bread per day with lifetime of 10 years. Aspen Plus was used to simulate the mass and energy balance of the plant. The total capital investment (TCI), total annual production cost (TAPC) and annual revenue of the plant were USD931020, USD299746/year and USD639920/year, respectively. The unit hydrogen production cost was USD1.34/m³ H2 (or USD14.89/kg H2). The payback period and net present value (NPV) of the plant were 4.8 years and USD1266654, respectively. Hydrogen price and operators cost were the most important variables on the NPV. It was concluded that biohydrogen production from waste bread in the CSTR was feasible for practical application.
Article
Silver nanoparticles were added into anaerobic batch reactors to enhance acidogenesis and fermentative hydrogen production simultaneously. The effects of silver nanoparticles concentration (0-200nmolL(-1)) and inorganic nitrogen concentration (0-4.125gL(-1)) on cell growth and hydrogen production were investigated using glucose-fed mixed bacteria dominated by Clostridium butyricum. The tests with silver nanoparticles exhibited much higher H2 yields than the blank, and the maximum hydrogen yield (2.48mol/molglucose) was obtained at the silver concentration of 20nmolL(-1). Presence of silver nanoparticles reduced the yield of ethanol, but increased the yield of acetic acid. The high silver nanoparticles had higher cell biomass production rate. Further study using the alkaline pretreated culture as inoculum was carried out to verify the positive effect of silver nanoparticles on H2 production. Results demonstrated that silver nanoparticles could not only increase the hydrogen yield, but reduce the lag phase for hydrogen production simultaneously.
Article
The influence of self-immobilization of enriched acidogenic mixed consortia on fermentative hydrogen (H2) production was studied on different supporting materials [SBA-15 (mesoporous) and activated carbon (granular; GAC and powder; PAC)] using chemical wastewater as substrate. Batch fermentation experiments were performed with same substrate at different organic loading rates (OLRs) under acidophilic microenvironment (pH 5.5) and room temperature (28 ± 2 °C). Experimental data evidenced the effectiveness of attached growth on both the H2 yields and substrate degradation efficiency, particularly at higher loading rates. Among the three materials evaluated, immobilization on SBA-15 material showed comparatively effective performance in enhancing both H2 yield and substrate degradation. Suspended growth (SG-control) culture showed inhibition in terms of both H2 production and substrate degradation especially at applied higher loading rates. Immobilization on SBA-15 resulted in nine times higher H2 production (7.29 mol/kg CODR-day at OLR of 0.83 kg COD/m3-day) than the lowest yield observed (suspended growth at OLR of 2.55 kg COD/m3-day). Maximum substrate degradation rate (SDR) of 0.96 kg COD/m3-day (OLR 2.55 kg COD/m3-day) was also observed with SBA-15 immobilization, which is 1.62 times higher than the lowest substrate degradation observed with SG-control experiments with the same OLR. Attached growth on GAC and PAC also showed remarkable improvement in the process performance at higher OLRs compared to SG-control.
Article
Pretreatment of waste activated sludge (WAS) results in an improved efficiency of the subsequent anaerobic biotransformation of the organic matter to volatile fatty acids. The pretreatment process has been carried out using alkaline treatment, ultrasonic treatment (20 KHz, 120 W) and different combination of these two methods: alkaline followed by ultrasonic, as well as the combining method in which ultrasonic treatment is applied to WAS samples dosed with alkaline. The hydrolysis efficiency was evaluated based on the quantity of soluble COD (SCOD) and organic nitrogen in the pretreated WAS as well as the production of total volatile fatty acids (TVFA) in the following biochemical acid potential (BAP) test For WAS samples with described pretreatments, the released SCOD varied from 36% to 89°/a of the total COD (TCOD) and soluble organic nitrogen from 34% to 42%. The TVFA/TCOD ratio of the raw WAS used in this study was less than 10%. For the alkaline pretreated WAS, the TVFA/TCOD ratio increased to 30%, and the following ultrasonic treatment enhanced the ratio 66%. Further, WAS samples pretreated using simultaneous ultrasound and alkaline treatment in which ultrasonic was applied to WAS samples dosed with 40 meq/L NaOH for 14.4 sec/mL could achieve a maximum TVFA/TCOD ratio of 84% in 21 hours. Therefore, the combination of simultaneous alkaline and ultrasound pretreatment is efficient in enhancing the production of volatile acids in WAS in order to achieve recovery of volatile fatty acids from the WAS.