CN112680481A - Method for producing methane by strengthening organic wastes through microbial electrocatalysis - Google Patents
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Abstract
A method for producing methane by kitchen waste through synergistic enhancement of anaerobic fermentation and microbial electrocatalysis comprises the following steps: (1) anaerobic fermentation: crushing organic garbage into slurry, and adding the slurry into an anaerobic fermentation reactor in an intermittent feeding mode to perform acid-production and hydrogen-production fermentation; (2) starting a methanogenic phase reactor: taking granular sludge as an inoculum, mixed acid as a culture solution and a single-chamber microbial electrolytic cell as a methanogenic phase reactor, and carrying out enrichment of electroactive microorganisms and starting of the methanogenic phase reactor; (3) and (2) after solid-liquid separation is carried out on the fermentation liquor obtained in the step (1), the pH value of the supernatant is adjusted to 6.0-8.0, the supernatant is pumped into the methane-producing phase reactor which is successfully started in the step (2), the biogas generated by fermentation in the step (1) is injected into the methane-producing phase reactor, the hydrogen partial pressure in the headspace of the reactor is kept lower than 1.0bar, hydrogen and carbon dioxide in the biogas are converted into methane at the cathode, and the methane-producing phase reactor is operated in an internal reflux mode.
Description
Technical Field
The invention relates to an organic waste energy regeneration method, in particular to a method for producing methane by strengthening organic waste through microbial electrocatalysis.
Background
Anaerobic methanation is one of effective methods for realizing green energy regeneration of organic wastes, but the existing anaerobic fermentation process generally has the problems of low methane conversion efficiency, difficult stable operation (acidification feedback inhibition, high ammonia nitrogen inhibition and the like), long and tedious process period and the like. The two-phase anaerobic fermentation technology separates the biological phase in the fermentation process, so that the complex anaerobic process is easy to regulate and control physiologically and ecologically, the substrate conversion efficiency and the gas yield are effectively improved, and the two-phase anaerobic fermentation technology is widely applied. However, due to the limitation of the traditional methanation metabolic rate, high-concentration organic wastewater produced by the anaerobic acidification phase cannot be rapidly converted into methane, and the low pH value of the acidogenic phase causes impact on the microenvironment of the methanogenic phase, so that the organic waste anaerobic fermentation process still has the problems of poor stability and robustness and the like.
The microbial electrocatalysis process is to utilize the high-efficiency biological electrocatalysis performance of the surface of an electrode, oxidize organic matters through a biological anode to release protons and electrons, and transfer the generated electrons to the anode; under the drive of an external electric field, electrons are transferred from the anode to the cathode, and are combined with protons diffused to the surface of the cathode to be reduced, and carbon dioxide is reduced to generate methane under the action of methanogen on the surface of the cathode. Therefore, the coupling of the acid and hydrogen production stage in the initial stage of anaerobic fermentation and the microbial electrocatalytic methane production shortens the period of anaerobic fermentation, and the generated micromolecular acid, hydrogen and carbon dioxide are further degraded and converted into methane, so that the method is a novel method for enhancing the methane production by organic wastes.
Disclosure of Invention
The invention aims to provide a method for strengthening the methane production of organic wastes by microbial electrocatalysis, which improves the anaerobic fermentation performance of the existing organic wastes, improves the methane production rate and enhances the acid resistance of the methane production process.
In order to achieve the purpose, the invention provides a method for producing methane by strengthening organic wastes through microbial electrocatalysis, which comprises the following steps:
(1) anaerobic fermentation: crushing organic wastes into slurry, and adding the slurry into an anaerobic fermentation reactor in an intermittent feeding mode to perform acid-production and hydrogen-production fermentation;
(2) starting a methanogenic phase reactor: taking granular sludge as an inoculum, mixed acid as a culture solution and a single-chamber microbial electrolytic cell as a methanogenic phase reactor, and carrying out enrichment of electroactive microorganisms and starting of the methanogenic phase reactor;
(3) after the fermentation liquor obtained in the step 1 is subjected to solid-liquid separation, the pH value of the supernatant is adjusted to 6.0-8.0, the supernatant is pumped into a methane-producing phase reactor which is successfully started in the step 2, biogas generated by fermentation in the step 1 is injected into the methane-producing phase reactor, the hydrogen partial pressure of the headspace of the reactor is kept lower than 1.0bar, hydrogen and carbon dioxide in the biogas are converted into methane at a cathode, the methane-producing phase reactor operates in an internal reflux mode, the reflux ratio is 20-80%, the hydraulic retention time is 1-7d, and the organic load of inlet water is 2-10kg/(m & lt/m & gt) & lt/103D), the voltage applied to the reactor is 0.2-1.0V, and the operating temperature is 20-40 ℃.
In the method, the anaerobic fermentation reactor in the step 1 is controlled at the temperature of 55 +/-1 ℃, the pH value of 6-6.5 and the organic load of 6-8 kgVS/(m)3D), hydraulic retention times of 2 to 4 d.
In the method, the anode of the methane-producing phase reactor in the step 2 is made of carbon-based materials such as carbon brushes, graphite felts and the like, the cathode is made of carbon brushes, graphite felts or Magnesli phase titanium suboxide conductive ceramic materials, the starting external voltage is 0.2-1.0V, and the operating temperature is 20-40 ℃.
In the method, the granular sludge and the mixed acid in the step 2 are added into a methanogenesis phase reactor according to the volume ratio of 1:1-1:10, the solid content is 6-10%, the applied voltage is 0.2-1.0V, the cathode potential is controlled to be-0.6-0.8V, and the anode potential is controlled to be-0.2-0.1V.
In the method, the mixed acid in the step 2 consists of sodium acetate, sodium propionate, sodium butyrate, phosphoric acid buffer solution and trace element liquid.
In the method, the methane-producing phase reactor which is successfully started in the step 3 is continuously kept stable for more than 3 periods of maximum current and methane yield in the starting process of the step 2, which indicates that the methane-producing phase reactor is successfully started.
Compared with the prior art, the invention has the following advantages:
1. the invention couples the microorganism anaerobic fermentation with the microorganism electrocatalysis, the microorganism electrolytic cell is arranged at the rear end of the anaerobic fermentation reactor for producing acid and hydrogen, and the two phases form an organic waste biological strengthening methane production system with substrate gradient utilization by optimizing and regulating, thereby solving the problems of insufficient electron donor of the anaerobic fermentation system and low methane production efficiency by direct electron transfer, and improving the degradation and methanation efficiency of the organic waste.
2. The invention utilizes the microbial electrocatalysis principle to introduce biogas which is rich in hydrogen and carbon dioxide in an anaerobic fermentation acid-producing hydrogen phase into a microbial electrolytic cell to produce a methane phase, and the biogas is converted into methane under the synergistic effect of hydrogen nutrition type methanogens and direct electron transfer type methane-producing electroactive microorganisms, so that the biogas (hydrogen, carbon dioxide and the like) of the acid-producing hydrogen phase is recycled, the carbon emission is reduced, the thermodynamic limit of further degradation of propionic acid and butyric acid caused by overhigh hydrogen partial pressure is overcome, the acetic acid conversion efficiency in the anaerobic fermentation phase is promoted, and high-purity biogas with the methane content of more than 90 percent can be obtained from fermentation liquor taking acetic acid as a main component in a methane phase reactor, thereby being beneficial to commercialization of the biogas.
3. According to the invention, the microbial electro-catalysis methane-producing phase can realize the advanced treatment and energy utilization of anaerobic fermentation liquid by regulating and controlling the process parameters such as voltage, hydraulic retention time and the like according to the fermentation liquid component change of the anaerobic fermentation acid-producing and hydrogen-producing phase, and the high-efficiency and stable operation of the whole enhanced methane-producing process is ensured, and the feedback inhibition effect brought by acid accumulation is avoided.
4. The electrode material of the methane-producing phase reactor adopts a carbon-based material and a Magneli-phase titanium suboxide conductive ceramic coupling material. Magnesli phase titanium suboxide periodic TiO2Stacking and staggering the structure with TiO to ensure that the material has abnormal chemical resistance; the magneli phase titanium suboxide has an oxygen-deficient TiO shearing surface, has excellent electronic conductivity, has the conductivity of about 1000S/cm and is similar to a metal material; high mechanical abrasion resistance, liquid scouring resistance and long service life; the method is safe, nontoxic, environment-friendly, good in biocompatibility and beneficial to enrichment of methane-producing electroactive microorganisms, so that the method is high in methane production efficiency, stable in operation, low in operation and maintenance cost and high in added value of products.
Drawings
FIG. 1 is a flow chart of the process for producing methane by the kitchen waste reinforced by the cooperation of anaerobic fermentation and microbial electrocatalysis.
FIG. 2 is a flow diagram of a conventional two-stage anaerobic digestion process for producing methane according to comparative example.
FIG. 3 is a flow chart of a process for producing methane by enhancing anaerobic digestion in a conventional microbial cell according to a second comparative example.
Detailed Description
The invention discloses a method for producing methane by microorganism electrocatalysis reinforcement anaerobic, which uses an anaerobic fermentation and microorganism electrolytic cell methane production two-phase reactor, kitchen waste is subjected to anaerobic fermentation and rapid hydrolysis acidification in the anaerobic fermentation phase reactor to realize acid production and hydrogen production, and fermentation liquor enters the microorganism electrolytic cell to be coupled with anaerobic digestion sludge for co-fermentation to efficiently produce methane. The process comprises the following steps: pulping the kitchen waste and adding the kitchen waste into an anaerobic fermentation acid and hydrogen production phase to realize the directional fermentation of the kitchen waste to produce acid and hydrogen; the anaerobic fermentation phase fermentation liquid directly enters a microbial electrolytic cell to produce a methane phase, biogas rich in hydrogen and carbon dioxide is introduced into the microbial electrolytic cell to produce the methane phase, and the purpose of bioelectrochemical catalysis and enhanced methane production of the kitchen waste is realized under the synergistic effects of hydrogenotrophic methanogens, direct electron transfer methanogenic electroactive microorganisms and the like.
The technical scheme of the invention is as follows:
(1) the organic garbage is crushed and sieved to prepare slurry, the slurry is added into an anaerobic fermentation reactor in an intermittent feeding mode, and the organic garbage is subjected to high temperature of 55 +/-1 ℃, pH of 6-6.5 and organic load of 6-8 kgVS/(m)3D) performing acid-production and hydrogen-production fermentation under the operation condition of hydraulic retention time of 2-4d, wherein acetic acid and butyric acid in the fermentation broth account for more than 70% of total volatile organic acid, and the gas yield is 150L/(kgVS d), wherein the hydrogen accounts for 50-60%;
(2) the method comprises the following steps of (1) taking granular sludge as an inoculum, mixed acid as a culture solution, a single-chamber microbial electrolytic cell as a methanogenic phase reactor, wherein the anode of the reactor is made of carbon-based materials (carbon brushes, graphite felts and the like), the cathode of the reactor is made of carbon-based materials (carbon brushes, graphite felts and the like) or conductive ceramic materials (Magneli phase titanium suboxide), and the enrichment of electroactive microorganisms and the start of the methanogenic phase reactor are carried out under the conditions that the applied voltage is 0.2-1.0V and the operating temperature is 20-40 ℃;
(3) centrifuging the fermentation liquor obtained in the step (1) to obtain supernatant rich in volatile fatty acid, adjusting the pH value of the supernatant to 6.5-7.5, pumping the supernatant into a methane-producing phase reactor which is successfully started in the step (2), and fermenting the fermentation liquor in the step (1) to generate gas with the volume of 1.0-2.0m3/(m3D) injecting the load into the reactor, maintaining the headspace hydrogen partial pressure of the anaerobic fermentation reactor to be lower than 1.0bar, converting hydrogen and carbon dioxide in the gas into methane at the cathode, operating the reactor in an internal reflux mode, wherein the reflux ratio is 20-50%, the hydraulic retention time is 1-3d, and the organic load of the inlet water is 2-10 kg/(m) and3d), the voltage applied to the reactor is 0.6-1.0V, and the operating temperature is 20-40 ℃.
Adding the granular sludge and the mixed acid culture solution into a methane-producing phase reactor according to the volume ratio of 1:1-1:10, wherein the solid content is 6-10%, the applied voltage is 0.2-1.0V, the cathode potential is controlled to be-0.6-0.8V, and the anode potential is controlled to be-0.2-0.1V.
The mixed acid culture solution in the step (2) consists of sodium acetate, sodium propionate, sodium butyrate, phosphoric acid buffer solution and trace element solution.
The successful start-up of the methanogenic phase reactor in the step (3) is to keep stable when the maximum current and the methane yield are continuously maintained for more than 3 cycles in the start-up process in the step (2), which indicates that the methanogenic phase reactor is successfully started up, the anode has the capacity of quickly oxidizing the mixed acid substrate to generate electricity, and the cathode has the capacity of directly generating methane through electron transfer.
In the invention, the anaerobic fermentation phase provides a carbon source mainly comprising volatile fatty acid and hydrogen required for methane conversion for methane production of a Microbial Electrolysis Cell (MEC), and the MEC methane production phase further degrades the volatile fatty acid under the synergistic action of an acid degradation flora and an electroactive flora and promotes the hydrolytic acidification process of the front-end anaerobic fermentation phase; hydrogen from an anaerobic fermentation phase is utilized by hydrogenotrophic methanogen enriched on the surface of a cathode in the MEC, so that the accumulation of propionic acid and butyric acid caused by overhigh hydrogen partial pressure in the anaerobic fermentation process is avoided, and the methane production efficiency of the kitchen waste can be improved, the period is shortened, and the running stability of a system is maintained by the combined use of the anaerobic fermentation and the methane production of the MEC.
The technical solution of the present invention is further described below with reference to the accompanying drawings and examples.
The first embodiment is as follows:
as shown in figure 1, the kitchen waste crushing and screening unit removes large substances such as bones, fishbones and the like, the large substances enter a damp and hot pretreatment unit, enter an anaerobic fermentation phase reactor through damp and hot hydrolysis, and the organic load is 3-6 kgVS/(m)3And d) operating the pH value to be 5.5-6.5, performing acid-production and hydrogen-production fermentation at the high temperature of 45-55 ℃, wherein the content of hydrogen in the generated biogas is more than 50 percent, the hydrogen yield is 100-1500 mg/L (butyric acid is the main organic acid component), and the content of ethanol and volatile fatty acid in the fermentation broth is 1000-1500 mg/L.
The methanogenic MEC reactor needs to be started and debugged in advance. Anaerobic granular sludge required for starting is taken from a citric acid wastewater anaerobic digestion tank, and is subjected to methanation activation treatment after glucose and ethanol solution are mixed with the anaerobic granular sludge. Wherein a small amount of ethanol promotes the proliferation of electroactive flora in the anaerobic granular sludge. The activation temperature is 30-40 ℃, and the activation time is not less than 14 d; adding the activated anaerobic granular sludge and a culture solution into a microbial electrolytic cell reactor according to the volume ratio of 1:1, operating under the conditions of an external voltage of 0.2-0.8V and a temperature of 30-40 ℃, and when the maximum current value of the methanogenic phase reactor is kept consistent for more than three continuous periods, and the daily average methane yield is considered as successful start-up.
Fermentation liquor generated by the kitchen waste anaerobic fermentation unit is centrifugally filtered and input into a methane production MEC reactor which is successfully started, and biogas containing hydrogen is conveyed to the reactor through an air pump and is uniformly distributed in the reactor through a bottom gas diffuser. The process conditions are that the applied voltage is 0.2-0.8V, the hydraulic retention time is 24-48h, the operating temperature is 30-40 ℃, the fermentation liquor rich in volatile fatty acid is used as a substrate of electroactive microorganism, electrons and carbon dioxide are released by anode biodegradation, methane-producing bacteria at the cathode are quickly reduced into methane by a direct electron transfer way, and the hydrogen conveyed by an anaerobic fermentation phase generates methane under the action of hydrogenotrophic methane-producing bacteria, wherein the methane content is 80-90%.
Example two:
the kitchen waste is subjected to crushing, screening and damp-heat pretreatment and then enters an anaerobic fermentation reactorReactor, at an organic load of 9 kgVS/(m)3D) performing acid-production and hydrogen-production fermentation at the operating pH of 6 and the high temperature of 35 +/-1 ℃, wherein the hydrogen yield is 60-100L/(kgVS d), the ethanol and volatile organic acid content in the fermentation broth is 13000-16000mg/L, and the acetic acid is 6000-8000mg/L, the propionic acid is 1000-1200mg/L, and the butyric acid is 5600-6000 mg/L.
The methanogenic phase MEC reactor was started up as in example one.
And (3) centrifugally filtering fermentation liquor generated by anaerobic fermentation of the kitchen waste, inputting the fermentation liquor into a methane-producing phase MEC reactor which is successfully started, conveying generated biogas containing hydrogen to the reactor through an air pump, and uniformly distributing the biogas in the methane-producing phase MEC reactor through a bottom gas diffuser. The MEC process conditions are that the applied voltage is 0.6-0.8V, the hydraulic retention time is 12-48h, the operation temperature is 35-40 ℃, and the internal circulation reflux of the methanogenic MEC reactor is needed due to higher water inlet concentration, and the reflux ratio is 50%. The methane content in the treated biogas is up to more than 90 percent, and the carbon dioxide emission reduction and the advanced treatment of high-concentration organic waste liquid are realized simultaneously.
Comparative example one:
the known two-stage anaerobic digestion methanogenesis process is shown in fig. 2, wherein the kitchen waste crushing and screening and the wet-heat pretreatment are the same as in the first and second embodiments. In the two-stage anaerobic digestion process shown in fig. 2, the kitchen waste is crushed, screened, subjected to wet heat pretreatment, enters an anaerobic reactor for hydrolytic acidification, the hydraulic retention time is 24-48h, the pH value is 5.0-6.0, the content of generated acetic acid, propionic acid and butyric acid is 50:20:30-40:40:20, the fermentation liquor after hydrolytic acidification enters the anaerobic digestion reactor, the hydraulic retention time is 8-10 days, the pH value is 6.0-8.0, and the methane content is 50-60%.
Comparative example two:
the flow chart of the prior art microbial electrolytic cell enhanced anaerobic digestion methanogenesis process is shown in figure 3. In the known microorganism electrolytic tank intensified anaerobic digestion process, after kitchen waste is subjected to crushing and screening and wet-heat pretreatment, an anaerobic reactor is subjected to anaerobic fermentation, the hydraulic retention time is 24-4h, the pH value is 5.0-6.0, the content ratio of generated acetic acid, propionic acid and butyric acid is 60:20:20-50:20:30, fermentation liquor after the anaerobic fermentation enters an MEC reactor to carry out methanogenesis reaction, and the collection and utilization of anaerobic fermentation phase biogas and the backflow of an MEC unit are not generated in the process flow. The voltage applied to the MEC is 0.6-0.8V, the hydraulic retention time is 2-6d, the pH is controlled to be 6.0-8.0, and the methane content is 70-80%; the content ratio of the generated acetic acid, propionic acid and butyric acid is 70:10:20-60:10: 30.
Through comparative analysis of the first and second embodiments and the first and second comparative examples, the hydraulic retention time of the anaerobic fermentation phase in the method is shortened to 1d, the hydraulic retention time of the methane-producing phase MEC reactor is 0.5-2d, the methane content can reach more than 90%, the operation period of the whole process is shortened, and the substrate utilization rate and the methane yield are obviously improved.
Claims (7)
1. A method for producing methane by kitchen waste through synergistic enhancement of anaerobic fermentation and microbial electrocatalysis comprises the following steps:
(1) anaerobic fermentation: crushing organic garbage into slurry, and adding the slurry into an anaerobic fermentation reactor in an intermittent feeding mode to perform acid-production and hydrogen-production fermentation;
(2) starting a methanogenic phase reactor: taking granular sludge as an inoculum, mixed acid as a culture solution and a single-chamber microbial electrolytic cell as a methanogenic phase reactor, and carrying out enrichment of electroactive microorganisms and starting of the methanogenic phase reactor;
(3) after solid-liquid separation is carried out on the fermentation liquor obtained in the step 1, the pH value of the supernatant is adjusted to 6.0-8.0, the supernatant is pumped into a methane-producing phase reactor which is successfully started in the step 2, biogas generated by fermentation in the step 1 is injected into the methane-producing phase reactor, the hydrogen partial pressure of the headspace of the reactor is kept lower than 1.0bar, hydrogen and carbon dioxide in the biogas are converted into methane under the action of methanogens at the cathode, the methane-producing phase reactor operates in an internal reflux mode, the reflux ratio is 20-80%, the hydraulic retention time is 1-7d, and the organic load of inlet water is 2-10kg/(m & lt/m & gt/(3D), the voltage applied to the reactor is 0.2-1.0V, and the operating temperature is 20-40 ℃.
2. The method of claim 1, wherein the anaerobic fermentation reactor in step 1 is controlled at 55 ± 1 ℃, pH6-6.5, organic load 6-8 kgVS/(m)3D), hydraulic retention times of 2 to 4 d.
3. The method of claim 1, wherein the anode of the methanogenic phase reactor in step 2 is a carbon-based material, the cathode is a carbon-based material or a conductive ceramic material, the applied voltage for starting is 0.2-1.0V, and the operating temperature is 20-40 ℃.
4. The method of claim 3, wherein the carbon-based material of the electrode of the methanogenic phase reactor in the step 2 is carbon brush or graphite felt, and the cathode conductive ceramic material is Magneli phase titanium suboxide.
5. The method according to claim 1, wherein the granular sludge and the mixed acid in the step 2 are added into a methanogenic phase reactor according to the volume ratio of 1:1-1:10, the solid content is 6-10%, the applied voltage is 0.2-1.0V, the cathode potential is controlled to be-0.6-0.8V, and the anode potential is controlled to be-0.2-0.1V.
6. The method according to claim 1, wherein the mixed acid in the step 2 consists of sodium acetate, sodium propionate, sodium butyrate, phosphoric acid buffer solution and trace element liquid.
7. The method of claim 1, wherein the successful start-up of the methanogenic phase reactor in step 3 is indicated by the successful start-up of the methanogenic phase reactor when the maximum current and methane production during the start-up of step 2 are maintained for more than 3 consecutive cycles.
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| CN115404088A (en) * | 2022-07-14 | 2022-11-29 | 广州市金宝生态农业有限公司 | Method for preparing hydrothermal carbon and improving quality of in-situ biogas |
| CN116177829A (en) * | 2022-12-08 | 2023-05-30 | 同济大学 | Lateral flow micro-aeration coupled main flow electric drive anaerobic digestion method |
| CN116216924A (en) * | 2022-12-08 | 2023-06-06 | 同济大学 | Lateral flow micro-aeration coupling main flow electric drive anaerobic digestion system |
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