CN114908126A - Process for coproducing high-quality gas carbon clean recycling product by anaerobic fermentation-pyrolysis coupling - Google Patents
Process for coproducing high-quality gas carbon clean recycling product by anaerobic fermentation-pyrolysis coupling Download PDFInfo
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Abstract
The invention discloses a process for coproducing high-quality gas carbon clean recycling products by anaerobic fermentation-pyrolysis coupling. The process comprises the following steps: (1) carrying out anaerobic fermentation reaction on the biomass raw material to obtain a solid-liquid mixture of biogas, biogas residues and biogas slurry, and carrying out solid-liquid separation on the solid-liquid mixture to obtain biogas residues and biogas slurry; (2) drying the biogas residues, performing pyrolysis reaction to generate pyrolysis gas and biogas residue biochar, physically activating a part of biogas residue biochar, then allowing the activated biogas residue biochar to enter an anaerobic fermentation system for reaction, and chemically activating the other part of biogas residue biochar to serve as a cathode catalyst of the microbial fuel cell; (3) the biogas slurry is purified by a microbial fuel cell system, and the obtained clean water is circularly supplemented to an anaerobic fermentation system for reuse. The anaerobic-pyrolysis coupling process provided by the invention effectively improves the energy gas yield on the whole, the byproduct biogas residue biochar can purify biogas slurry, and the obtained clean water can be circularly supplemented to an anaerobic fermentation system for reuse.
Description
Technical Field
The invention relates to the technical field of biomass energy resource utilization and biomass pyrolysis, in particular to a process for coproducing high-quality gas carbon clean recycling products by anaerobic fermentation-pyrolysis coupling.
Background
The biomass energy is used as the only green renewable clean energy containing carbon resources, the raw materials are various and widely distributed, and the biomass energy is an ideal energy source choice, can solve the increasingly prominent environmental problem, can realize the diversification of energy supply, and can obtain high value-added chemicals. Currently, biomass-based energy conversion technologies mainly include physical conversion technologies, biological conversion technologies, and thermochemical conversion technologies. The single conversion utilization technology has certain defects, such as the biotransformation mode has mild reaction conditions but long conversion time; while the thermochemical conversion is rapid in reaction, the product components are complex, the energy consumption is high, secondary environmental pollution is possibly caused, and the like. In addition, a single conversion mode is low in energy recovery efficiency, resource waste and pollution phenomena exist, and how to convert and utilize the green energy becomes a research hotspot in the field of renewable energy sources.
Disclosure of Invention
The invention solves the problems in the prior art, and aims to provide a process for producing a high-quality gas-carbon clean recycling product by anaerobic fermentation-pyrolysis coupling.
In order to achieve the purpose, the invention adopts the technical scheme that: a process for producing high-quality gas-carbon clean recycling products by anaerobic fermentation-pyrolysis coupling comprises the following steps:
(1) carrying out anaerobic fermentation reaction on a biomass raw material to obtain biogas and a solid-liquid mixture containing biogas residues and biogas slurry, carrying out solid-liquid separation on the solid-liquid mixture to obtain biogas residues and biogas slurry, and treating for further treatment;
(2) drying the biogas residues obtained in the step (1), performing pyrolysis reaction to generate pyrolysis gas and biogas residue biochar, further utilizing the pyrolysis gas and the biogas as biogas, enabling one part of the biogas residue biochar to enter the anaerobic fermentation system in the step (1) for reacting after physical activation, and enabling the other part of the biogas residue biochar to serve as a cathode catalyst of a microbial fuel cell after chemical activation;
(3) and (2) purifying the biogas slurry obtained in the step (1) by using a microbial fuel cell system to obtain clean water, and circularly replenishing the clean water to an anaerobic fermentation system for reuse. The biogas slurry can be purified by a microbial fuel cell to degrade toxic substances in the biogas slurry.
The biogas residue after the anaerobic fermentation of the biomass waste is used as a raw material for a pyrolysis reaction, biogas residue biochar prepared by pyrolysis through different regulation and control methods can be respectively used as an additive for the anaerobic fermentation and a cathode catalyst of a microbial fuel cell, and generated biogas and pyrolysis gas can be used as biogas. The zero-emission cleaning process for realizing the efficient recycling of biomass resources by an anaerobic-pyrolysis coupling technology.
Preferably, the biomass raw material is crushed in the step (1), the anaerobic fermentation reaction is carried out, the biomass raw material is crushed, the crushed biomass raw material and the cow dung inoculum are placed in an anaerobic reactor for fermentation, and the VS ratio of the biomass raw material to the cow dung inoculum is 1:1-2: 1.
In the step (2), the marsh gas is mainly CH 4 And CO 2 The main component of the pyrolysis gas is H 2 、CO、CO 2 And CH 4 。
Preferably, the temperature of the anaerobic fermentation reaction in the step (1) is 37 +/-1 ℃ or 55 +/-1 ℃ at high temperature, and the hydraulic retention time is 0-15 days.
Further preferably, the temperature of the anaerobic fermentation reaction in the step (1) is 37 +/-1 ℃, and the hydraulic retention time is 3-15 days.
Preferably, the inert carrier gas for the pyrolysis reaction in the step (2) is argon or nitrogen, the reaction temperature is 500-1000 ℃, and the residence time is 10-120 min.
Preferably, the chemical activation in the step (2) is to mix and stir the biogas residue biochar and a sulfuric acid solution according to a mass-volume ratio of 1:15-1:25g/mL, and then wash and dry the mixture to obtain sulfuric acid activated biogas residue biochar which is used as a cathode catalyst of the microbial fuel cell.
Preferably, the physically activated activating agent in the step (2) is oxygen, the oxygen with the volume concentration of 5% and the nitrogen with the volume concentration of 95% are uniformly mixed through a gas mixing device, the biogas residue biochar is physically activated under the mixed atmosphere, the reaction temperature is 900 ℃, the residence time is 120min, the biogas residue biochar activated by the oxygen is obtained after natural cooling, and the biogas residue biochar is added into the anaerobic fermentation system in the step (1) to participate in the reaction.
Preferably, the biomass raw material in the step (1) is pennisetum hydridum.
Compared with the prior art, the invention has the beneficial effects that:
(1) the anaerobic-pyrolysis coupling process can be used for integrally and efficiently utilizing biomass resources, and when the hydraulic retention time is 3 days, 9 days and 15 days respectively, the energy conversion utilization rate is respectively as high as 41.64%, 49.44% and 48.79%.
(2) The anaerobic-pyrolysis coupling process effectively improves the yield of energy gas on the whole, the byproduct biogas residue biochar can purify biogas slurry, and the obtained cleaning water can be circularly supplemented to an anaerobic fermentation system for reuse.
(3) The anaerobic-pyrolysis coupling process realizes energy cleaning by water recharging, and achieves zero emission and no pollution of the system.
(4) After the biochar is added in the anaerobic fermentation reaction, enrichment of DIET functional microorganisms can be promoted, the gas production efficiency is improved, the removal rate of the refractory compounds is obviously improved, and the method has important significance and value for improving the recovery efficiency of hydrothermal liquefied water phase energy.
Drawings
FIG. 1 is a schematic view of a process flow proposed by the present invention;
FIG. 2 is a diagram showing the composition of pyrolysis gas in example 1 of the process of the present invention;
FIG. 3 is a scanning electron micrograph of biogas residue biochar before and after chemical activation in example 2; wherein a is before activation and b is after activation;
FIG. 4 is a graph showing the variation of output voltage of the microbial fuel cell of example 3 loaded with 1000 Ω resistance at different pH values when the microbial fuel cell is used for treating 1.0g/L sodium propionate;
FIG. 5 is a graph of the cumulative gas production after strengthening with biochar in example 4.
Detailed Description
The following examples are further illustrative of the present invention and are not intended to be limiting thereof. Experimental procedures without specific conditions noted in the following examples, generally according to conditions conventional in the art or as recommended by the manufacturer; the raw materials, reagents and the like used are, unless otherwise specified, regarded as raw materials and reagents that are commercially available through conventional markets and the like. Any insubstantial changes and substitutions made by those skilled in the art based on the present invention are intended to be covered by the claims.
Example 1
As shown in fig. 1, a process for co-producing high-quality gas-carbon clean recycling products by anaerobic fermentation-pyrolysis coupling comprises the following steps:
taking an energy plant pennisetum hydridum as a raw material for anaerobic fermentation, crushing pennisetum hydridum, taking 150g of crushed pennisetum hydridum raw material and 1600mL of cow dung inoculum, putting the crushed pennisetum hydridum raw material and 1600mL of cow dung inoculum into a 2L anaerobic reactor for fermentation, wherein the pH value of the anaerobic fermentation reaction is 7.8, the fermentation temperature is 37 +/-1 ℃, the different hydraulic retention times are respectively 3d, 9d and 15d, collecting biogas by using a 5L air bag, and collecting the biogasMeasuring gas components and contents thereof, wherein CH with different hydraulic retention times of 3d, 9d and 15d 4 And CO 2 The cumulative yields reached 55.18mL/gVS and 86.31mL/gVS, 189.36mL/gVS and 162.02mL/gVS, 241.89mL/gVS and 185.73mL/gVS, respectively. And after each hydraulic retention time fermentation is finished, performing solid-liquid separation, drying the biogas residues, wherein the pyrolysis temperature is 800 ℃, the retention time is 30min, the heating rate is 5 ℃/min, the flow rate is 150mL/min, the hot carrier gas is nitrogen, so as to obtain biogas residue biochar, and calculating that the yield of biogas residue pyrolysis gas with different degradation degrees reaches more than 45%, wherein a pyrolysis gas composition diagram is shown in fig. 2.
Example 2
As shown in fig. 1, a process for co-producing high-quality gas-carbon clean recycling products by anaerobic fermentation-pyrolysis coupling comprises the following steps:
(1) taking an energy plant pennisetum hydridum as a raw material for anaerobic fermentation, crushing pennisetum hydridum, taking 150g of crushed pennisetum hydridum raw material and 1600mL of cow dung inoculum, putting the crushed pennisetum hydridum raw material and 1600mL of cow dung inoculum into a 2L anaerobic reactor for fermentation, wherein the pH value of the anaerobic fermentation reaction is 7.8, the fermentation temperature is 37 +/-1 ℃, the hydraulic retention time is 9d, collecting biogas by using a 5L air bag, after the hydraulic retention time fermentation is finished, carrying out solid-liquid separation, drying biogas residues, the pyrolysis temperature is 800 ℃, the retention time is 30min, and the hot carrier gas is argon gas to obtain biogas residue biochar.
(2) The method for preparing biogas residue biochar for strengthening anaerobic fermentation and purifying biogas slurry through activation regulation comprises the following specific operations: mixing a part of biogas residue biochar with a sulfuric acid solution with the mass concentration of 10% according to the mass-volume ratio of 1: mixing 20g/mL, stirring on a magnetic stirrer at the rotating speed of 600r/min for 24h, washing the activated biochar to be neutral by using deionized water, and drying in a 60 ℃ drying oven to obtain the sulfuric acid activated biogas residue biochar. As shown in fig. 3, which is a scanning electron microscope image of activated biogas residue biochar, it can be seen that the activated biogas residue biochar has a rougher surface and richer pore structures, and provides more adsorption sites for removing toxic substances.
The other part of the biogas residue biochar is subjected to physical activation, and the specific steps are as follows: selecting a physical activating agent as oxygen, uniformly mixing oxygen with the volume concentration of 5% and nitrogen with the volume concentration of 95% through a gas mixing device, carrying out physical activation on the biogas residue biochar under the mixed atmosphere, wherein the reaction temperature is 900 ℃, the retention time is 120min, and naturally cooling to obtain the oxygen activated biogas residue biochar.
Example 3
The microbial fuel cell in which 1.0g/L of sodium propionate was used as a substrate and the biogas residue biochar obtained in example 2 was used as a cathode catalyst was operated for one cycle under the condition of pH 6.5, and the COD concentration of the anolyte influent and effluent water and the removal rate of the substrate COD were measured. After being purified by the microbial fuel cell, the COD of the inlet water is lowered from 1190mg/L to 120mg/L, and the removal rate of the COD is up to 89.9 percent. Meanwhile, in order to further study the operation conditions of the microbial fuel cell under different pH conditions, the COD concentration of the inlet water and the outlet water of the anolyte, the removal rate of the substrate COD and the like, tests of the microbial fuel cell at pH 6.0 and 5.5 are respectively carried out. The result shows that when the pH is 6.0, after the wastewater is purified by the microbial fuel cell, the COD of the influent water is reduced from 1310mg/L to 210mg/L, and the removal rate of the COD reaches 83.9 percent; when the pH value is 5.5, after the wastewater is purified by the microbial fuel cell, the COD of the inlet water is reduced from 1140mg/L to 250mg/L, and the removal rate of the COD reaches 78.1 percent. Under different pH values, the microbial fuel cell processes 1.0g/L sodium propionate, the output voltage change diagram of the load 1000 omega resistor is shown in FIG. 4, along with the continuous reduction of the pH value, the power generation period of the MFC processing 1.0g/L sodium propionate is continuously prolonged, and the generated maximum output voltage is also continuously reduced. Therefore, the activity of the electrogenesis bacteria can be influenced by the reduction of the pH value, so that the output voltage of the MFC is reduced, and the electrogenesis performance is poor; at the same time, the time required for MFC to degrade the same concentration of sodium propionate becomes longer.
Example 4
Adding the biogas residue biochar after physical activation in the embodiment 2 into an anaerobic fermentation system to participate in reaction, and the specific steps are as follows:
the actual microalgae hydrothermal liquefied water phase is used as an anaerobic digestion raw material, and the physically activated biogas residue biochar is added to strengthen the promotion effect on the hydrothermal liquefied water phase anaerobic digestion. The working volume of a batch type reaction bottle (250mL) for anaerobic digestion is 200mL, anaerobic digestion reaction is carried out in a constant-temperature water bath kettle, the temperature is set to be 37 +/-1 ℃, and a 10mL injector and a 200mL air bag are used for respectively extracting biogas slurry and collecting biogas in the anaerobic digestion reaction process. In a hydrothermal liquefaction water phase anaerobic digestion experiment without adding biochar, the accumulated gas production is 125 mL/gCOD; after the biochar is added, the accumulated gas production reaches 135mL/gCOD, the accumulated gas production is improved by 7.6 percent compared with a control group, and the accumulated gas production is shown in figure 5. After the biochar is added, enrichment of DIET functional microorganisms can be promoted, gas production efficiency is improved, the removal rate of refractory compounds is obviously improved, and the method has important significance and value for improving the recovery efficiency of hydrothermal liquefied water phase energy.
The above is only a preferred embodiment of the present invention, and it should be noted that the above preferred embodiment should not be considered as limiting the present invention, and the protection scope of the present invention should be subject to the scope defined by the claims. It will be apparent to those skilled in the art that various modifications and adaptations can be made without departing from the spirit and scope of the invention, and should be considered to be within the scope of the invention.
Claims (8)
1. A process for producing high-quality gas-carbon clean recycling products by anaerobic fermentation-pyrolysis coupling is characterized by comprising the following steps:
(1) carrying out anaerobic fermentation reaction on a biomass raw material to obtain biogas and a solid-liquid mixture containing biogas residues and biogas slurry, carrying out solid-liquid separation on the solid-liquid mixture to obtain biogas residues and biogas slurry, and treating for further treatment;
(2) drying the biogas residues obtained in the step (1), performing pyrolysis reaction to generate pyrolysis gas and biogas residue biochar, further utilizing the pyrolysis gas and the biogas as biogas, enabling one part of the biogas residue biochar to enter the anaerobic fermentation system in the step (1) for reacting after physical activation, and enabling the other part of the biogas residue biochar to serve as a cathode catalyst of a microbial fuel cell after chemical activation;
(3) and (2) purifying the biogas slurry obtained in the step (1) by using a microbial fuel cell system to obtain clean water, and circularly replenishing the clean water to an anaerobic fermentation system for reuse.
2. The process of claim 1, wherein the biomass raw material crushing and anaerobic fermentation reaction in the step (1) comprises the following specific steps: crushing a biomass raw material, putting the crushed biomass raw material and a cow dung inoculum into an anaerobic reactor for fermentation, wherein the VS ratio of the biomass raw material to the cow dung inoculum is 1:1-2: 1.
3. The process according to claim 1 or 2, wherein the temperature of the anaerobic fermentation reaction in the step (1) is 37 plus or minus 1 ℃ or the high temperature is 55 plus or minus 1 ℃, and the hydraulic retention time is 0 to 15 days.
4. The process of claim 3, wherein the anaerobic fermentation reaction in step (1) is carried out at a temperature of 37 ± 1 ℃ and a hydraulic retention time of 3-15 days.
5. The process of claim 1, wherein the inert carrier gas for the pyrolysis reaction in step (2) is argon or nitrogen, the reaction temperature is 500-1000 ℃, and the residence time is 10-120 min.
6. The process according to claim 1, wherein the chemical activation in the step (2) is to mix and stir the biogas residue biochar and a sulfuric acid solution according to the mass-to-volume ratio of 1:15-1:25g/mL, and then wash and dry the mixture to obtain the sulfuric acid activated biogas residue biochar.
7. The process according to claim 1, wherein the activating agent for physical activation in the step (2) is oxygen, the oxygen with the volume concentration of 5% and the nitrogen with the volume concentration of 95% are uniformly mixed, the biogas residue biochar is physically activated in a mixed atmosphere, the reaction temperature is 900 ℃, the retention time is 120min, the biogas residue biochar activated by the oxygen is obtained after natural cooling, and the biogas residue biochar is added into the anaerobic fermentation system in the step (1) to participate in the reaction.
8. The process according to claim 1, wherein the biomass raw material in step (1) is pennisetum hydridum.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN115818898A (en) * | 2023-01-03 | 2023-03-21 | 华南农业大学 | Biogas slurry desalting system |
| CN115975656A (en) * | 2023-01-18 | 2023-04-18 | 中国电建集团西北勘测设计研究院有限公司 | System and method for preparing monocyclic aromatic hydrocarbon and co-producing nitrogen-containing pyrolytic carbon by catalytic pyrolysis of biogas residues |
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| CN101914572A (en) * | 2010-07-20 | 2010-12-15 | 中国科学院广州能源研究所 | Energy utilization method of carbon dioxide zero-emission type organic waste |
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