CN110643403A - Chemical absorption combined biological removal hydrogen sulfide and sulfur resource technology in methane - Google Patents

Chemical absorption combined biological removal hydrogen sulfide and sulfur resource technology in methane Download PDF

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CN110643403A
CN110643403A CN201810677308.8A CN201810677308A CN110643403A CN 110643403 A CN110643403 A CN 110643403A CN 201810677308 A CN201810677308 A CN 201810677308A CN 110643403 A CN110643403 A CN 110643403A
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王晓伟
张婷婷
党康飞
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Zhengzhou University
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Abstract

The invention discloses a process for removing hydrogen sulfide and sulfur resource in biogas by combining chemical absorption with biology, which is to absorb H in flue gas by using alkaline absorption liquid in an absorption tower2S produces sodium sulfide, sodium hydrosulfide, carbonate. Containing absorbed H2S, the solution of sodium sulfide, sodium hydrosulfide and carbonate enters a micro-aerobic bioreactor; the method utilizes microorganisms to convert sulfides into elemental sulfur, does not need to add a carbon source, and utilizes methane to absorbThe collected carbon dioxide is used as a carbon source, the operation cost is saved, the mixed liquid containing elemental sulfur generated by the aerobic bioreactor is treated by a sulfur recovery system to obtain sulfur with higher content for recycling, and the alkaline solution obtained by the sulfur recovery system is returned to the absorption tower for recycling. The method has reasonable process, low energy consumption, low investment and operation cost and small secondary pollution, can achieve the aims of desulfurizing the methane and recovering elemental sulfur, and is an ideal methane desulfurization process.

Description

Chemical absorption combined biological removal hydrogen sulfide and sulfur resource technology in methane
Technical Field
The invention belongs to the technical field of waste gas purification in environmental protection engineering, and relates to a process for removing hydrogen sulfide from biogas by combining chemical absorption with biology and recycling sulfur.
Background
With the wide application of the anaerobic biological treatment technology of industrial and agricultural wastes, biogas is a renewable energy source and is increasingly concerned and valued by people under the condition of increasingly deficient fossil energy sources. The biogas energy is fully utilized, and the pressure caused by the shortage of energy in China can be relieved. Generally, the main components of biogas are methane and carbon dioxide, and the biogas contains a small amount of carbon monoxide, ammonia gas, hydrogen gas, oxygen gas, nitrogen gas and the like, and biogas prepared from different raw materials often contains hydrogen sulfide with different contents. The over-high concentration of hydrogen sulfide is one of the biggest limiting factors for using the methane as fuel gas, because the hydrogen sulfide is a highly toxic harmful gas and has strong corrosion action on pipelines, instruments and equipment; after the biogas is combusted, hydrogen sulfide is converted into sulfur oxides and released into the air, so that atmospheric pollution is caused and the human health is harmed. Therefore, in order to protect human health and prolong the service life of equipment, effective measures must be taken for methane desulfurization. The national environmental protection standard strictly stipulates that the content of the biogas gas cannot exceed 20 mg/L when the biogas energy is utilized. The mass concentration of the marsh gas is generally 5000-. Therefore, the removal of hydrogen sulfide becomes an essential link in the use process of the methane.
The methane desulfurization method comprises a chemical method, a physical and chemical method and a biological method. The physical and chemical methods commonly used can be generally classified into direct desulfurization and indirect desulfurization. The principle of the direct desulfurization method of methane can be divided into a wet method and a dry method. Wet desulfurization is a method of removing sulfur from a gas by countercurrent contact of a specific solvent with the gas, and is a method of oxidizing the gas to sulfur or sulfur oxides by regenerating the solvent and then absorbing the gas again, and may be referred to as a dry oxidation method. At present, domestic desulfurization technology is mature, and a plurality of desulfurization methods and desulfurization processes exist, but generally, the defects that dry desulfurization efficiency is low, a desulfurizer is difficult to regenerate, sulfur capacity is relatively low, the method is mainly suitable for fine desulfurization and wet desulfurization, the treatment capacity is large, the desulfurization efficiency is high, continuous operation can be realized, the investment and operation cost is high, and common users using biogas cannot bear the method. With the strictness of environmental regulations, the development of technologies with high efficiency, low investment, resource utilization and no secondary pollution becomes the mainstream of the development of the desulfurization technology. In order to solve some defects of the physical and chemical desulphurization, a more efficient and low-consumption desulphurization technology is sought, and a biological desulphurization method is produced. The biological desulfurization is a research hotspot gradually because of the advantages of simple equipment, easy control, convenient maintenance, low construction cost, no waste discharge in the purification process, no secondary pollution and the like.
Biological desulfurization is to convert hydrogen sulfide in biogas into elemental sulfur or sulfate by utilizing the metabolism of microorganisms. The reaction formula is respectively
Figure 599920DEST_PATH_IMAGE001
（1）
Figure 929270DEST_PATH_IMAGE002
（2）
At present, biological desulfurization has been popularized and applied to a certain extent, but a plurality of problems still exist to be solved. As shown in the equation, in the case of excess oxygen, the sulfide is oxidized into sulfate to affect the desulfurization efficiency. This is undesirable during desulfurization. How to control reasonable aeration quantity and ensure that if the oxygen content in the biogas exceeds the oxygen content in the biogas with biological desulfurization safety, explosion can occur in case of naked fire, and simultaneously, the control of the final product after biological desulfurization to be elemental sulfur is the key point of the biogas biological desulfurization technology. In addition, how to ensure the efficient operation of the desulfurization bacteria in the biological desulfurization device is a difficult point of the biogas biological desulfurization technology. However, the defects of the two aspects are not effectively solved at present, and further the popularization and the application of the biogas biological desulfurization technology are hindered.
The study of microbial desulfurization began with the study of microbial beneficiation. In 1947, Colmer and Hinkle discovered and demonstrated that chemoautotrophic bacteria are able to promote oxidation and dissolution of pyrite present in coal, which is considered to be the beginning of a bio-hydrometallurgical study. Leathan and Temple, etc. respectively find some chemoautotrophic microorganisms and FeS in coal2And separating thiobacillus ferrooxidans from the coal mine wastewaterThiobacillus ferroxidans). Another organism, DeH, developed by Paques corporation2The S process has been industrialized in a paper mill in the Netherlands, and a sulfur production plant with a capacity of 0.20 t/d has been put into operation, which can carry out the H production in the gas stream2The S content is reduced from 12000 mu g/g to 40 mu g/g. In the Bio-SR process developed by Tokyo NKK company by applying thioether bacilliform bacteria and iron-oxidizing bacteria, a ferric sulfate solution adsorbs H from gas flow2S and generating elemental sulfur and ferrous sulfate solution, filtering the sulfur, and regenerating the solution into ferric iron compound solution by using a thioether iron oxidant.
An energy-saving method for biological desulfurization of marsh gas (CN 201010591471.6) invented by Hanhongjun, Haerbin Industrial university, comprises adding thiobacillus denitrificans and nitrobacteria during biological desulfurization, and metabolizing in gas phase to generate H2S and NH3The sulfur and nitrogen are converted, the thiobacillus denitrificans and the nitrobacteria are a symbiotic system, air (oxygen) is not required to be added in the reaction, and the microorganisms in the system can be completely self-sufficient by utilizing the oxygen and the ammonia in the methane, so that the operation cost is saved.
The biological marsh gas desulfurizing apparatus and desulfurizing process (CN 201020289228.4) applied in 2016 of Dingjinling et al propose that only 0.5 m is needed by three sections of desulfurizing tower, biological oxidizer and sulfur separator3air/kgS will biologically oxidize the hydrogen sulfide to elemental sulfur and separate it.
Yan Shiying et al, applied in 2017, a strain of Paracoccus Bengal and an application patent (CN 201711112005.3) propose to screen out a sulfur oxidizing bacterium using nitrate as an electron acceptor under anoxic conditions by enrichment culture, (Paracoccus Bengal strain: (CN 201711112005.3)Paracoccus bengalensis). When the bacteria are used for treating the methane, the concentration of hydrogen sulfide is 4000ppm, the highest removal rate can reach 97.2 percent; under the condition of coexistence of sulfide and nitric acid, the removal rate of sulfide reaches 94% and the removal rate of nitrate reaches 70%, and the catalyst can be used alone or immobilized for biogas desulfurization treatment and is widely applied.
An integrated biogas desulfurization device patent (CN 201020289228.4) applied in 2010 by Hubaolan and the like proposes biological removal of sulfides in biogas; in addition, the biological method for methane desulfurization is provided in Chinese patents with application numbers of CN201020513151.4, CN201710939414.4, CN201510513117.4 and CN 201620408548.4.
In the process of biological desulfurization of the biogas, hydrogen sulfide in the biogas is absorbed by an absorption tower, the hydrogen sulfide is converted into sodium sulfide and sodium hydrosulfide through alkaline absorption liquid, and then the solution containing the sodium sulfide and the sodium hydrosulfide is sent into a micro-aerobic bioreactor, so that Sulfur is converted into elemental Sulfur by Sulfur-oxidizing bacteria (SOB), and harmlessness, Sulfur recycling and regeneration of the alkaline absorption liquid in the biogas are realized.
The process is characterized in that only one bioreactor is added on the basis of chemical absorption desulphurization, hydrogen sulfide is removed from methane, elemental sulfur is recovered, a certain amount of dissolved oxygen is added into the reactor, the toxicity of sulfide to organisms in the reactor is solved, the reactor operates stably, and the problem of water pollution caused by wet desulphurization is solved.
Disclosure of Invention
The invention aims to provide a process for removing hydrogen sulfide from biogas by combining chemical absorption with biology and recycling sulfur, which can remove sulfide in the biogas and convert the sulfide into elemental sulfur by utilizing the combined action of a chemical absorbent and microorganisms under the combined process of chemical absorption and biology, so that pollutants can be removed and the elemental sulfur can be recycled, and the purpose of recycling the sulfur pollutants is achieved.
The technical scheme of the invention is as follows:
a process for removing hydrogen sulfide from biogas by combining chemical absorption and biology and recycling sulfur is characterized in that:
(1) absorbing hydrogen sulfide in the biogas by using an absorption tower, and absorbing the hydrogen sulfide in the biogas by using alkaline absorption liquid in the absorption tower to generate a solution of sodium sulfide and sodium hydrosulfide;
(2) the solution containing sodium sulfide and sodium hydrosulfide generated by absorbing hydrogen sulfide enters a micro-aerobic bioreactor, the microorganisms are utilized to convert sulfide into elemental sulfur, and simultaneously, carbonate generated by absorbing carbon dioxide in the biogas provides a carbon source for sulfur oxidizing bacteria;
(3) the mixed liquid containing elemental sulfur generated by the micro-aerobic bioreactor is treated by a sulfur recovery system to obtain sulfur with higher content for recycling, and the alkaline solution generated by the sulfur recovery system returns to the desulfurization absorption tower for recycling.
The absorption tower is a packed tower or a spray tower, the micro-aerobic bioreactor adopts a micro-aerobic activated sludge reactor, and the sulfur recovery system comprises a sedimentation tank and a solid-liquid separation device.
The alkaline absorption liquid in the desulfurization absorption process is NaOH and NaHCO3、Na2CO3One or more than two of the sulfur recovery systems and alkaline supernatant in a sedimentation tank of the sulfur recovery system.
The pH value in the micro-aerobic bioreactor is controlled to be 8.5-10, and the temperature is controlled to be 25-38oC, the retention time is controlled to be 3-24 h, C: N: P =500:5: 1, and the dissolved oxygen is controlled to be 0.01-0.3 mg/L.
The nitrogen source used by the microorganism in the micro-aerobic reactor is sludge fermentation to generate ammonia nitrogen recovery liquid, and the phosphorus source is dihydric phosphate or dibasic phosphate.
The invention has the advantages that:
a process for removing hydrogen sulfide from marsh gas by chemical absorption and biological removal and recycling sulfur is characterized in that on the basis of marsh gas desulfurization by a chemical absorption method, only one bioreactor is needed to be added, sulfur oxidizing bacteria in a micro-aerobic bioreactor are utilized to convert generated sulfide into elemental sulfur, a carbon source is not needed to be added, carbon dioxide absorbed from marsh gas is used as the carbon source, the operation cost is saved, and the elemental sulfur is recovered in the process of realizing marsh gas desulfurization. The method has reasonable process, low energy consumption, low investment and operation cost, and no secondary pollution.
Drawings
The attached figure is a flow chart of a process for removing hydrogen sulfide in biogas and recycling sulfur by combining chemical absorption with organisms.
In the figure: 1. a biogas inlet; 2. a biogas pressure stabilizing cabinet; 3. an absorption tower; 4. an absorption liquid circulating pump; 5. adding an alkaline solution to prepare a system; 6. adding alkali liquor; 7. adding a nutrient solution to prepare a system; 8. adding a nutrient solution pump; 9. a biogas outlet; 10. an air compressor; 11. a micro-aerobic bioreactor (SOB); 12. a sulfur recovery system; 13. and a reflux pump, wherein a circulating liquid outlet refluxes to 2.
Detailed Description
The following detailed description of the present invention will be made in conjunction with the accompanying drawings and the technical solutions, but the present invention is not limited to the following examples.
The biogas is sent to the lower part of an absorption tower 2 through a biogas pressure stabilizing cabinet 1 arranged in the process, the initial absorption liquid is a mixed solution added with sodium carbonate and sodium bicarbonate, the biogas in the tower is in countercurrent contact with the absorption liquid flowing from the upper part of the tower, and H in the biogas2S is absorbed by alkaline solution to convert hydrogen sulfide into sodium sulfide and sodium hydrosulfide, and the absorption solution passes through a circulating pump to saturate H2Pumping the S absorption liquid into a micro-aerobic tank; the sulfide is oxidized into elemental sulfur by sulfur oxidizing bacteria in the micro-aerobic biological tank, so that the aim of methane desulfurization can be fulfilled, the elemental sulfur can be recycled, and the aims of environmental protection and waste recycling are fulfilled.
The treated liquid after aerobic microbial conversion treatment enters a sulfur recovery system 14, and the alkaline solution is returned to the absorption tower circulation system by a circulation liquid conveying pump and is recycled as the desulfurization and denitrification absorption liquid.
Example 1
One anaerobic IC reactor for treating 1000 m3Per d landfill leachate, the amount of generated biogas is 10000 Nm3/d，H2The S content is 30000 mg/Nm3The temperature of the biogas is 30oC, according to the process of the invention, on leaving the absorption column, H2S content of 80 mg/Nm3The biogas desulfurization efficiency is 99.7 percent, and the recovery of the elemental sulfur is 2299.1 kg/d. SO (SO)2The absorption tower is a spray tower with diameter of 1.0 m and height of 12 m, and liquid-gas ratio of 3L/Nm3The denitration absorption liquid in the absorption process is NaOH and NaHCO3、Na2CO3One or more than two of the sulfur recovery systems and alkaline solution of the sulfur recovery system. The micro-aerobic bioreactor adopts an activated sludge method, the pH value is controlled to be 8.5 +/-0.3, and the temperature is controlled to be 30oC, the retention time is controlled to be 3 h, C: N: P =500:5: 1,the dissolved oxygen is controlled to be 0.01-0.3 mg/L. The sulfur recovery system consists of a coagulating sedimentation system, a sulfur sludge drying system and a sulfur sludge purification system.
Example 2
10000 m processed by anaerobic IC reactor3D papermaking wastewater with the generated biogas amount of 140000 Nm3/d，H2The S content is 25000 mg/Nm3The temperature of the biogas is 30oC, according to the process of the invention, on leaving the absorption column, H2The S content is 70 mg/Nm3The biogas desulfurization efficiency is 99.7 percent, and the recovery of the elemental sulfur is 3489.5 kg/d. SO (SO)2The absorption tower is a spray tower with a diameter of 1.5 m and a height of 16 m, and has a liquid-gas ratio of 3.5L/Nm3The denitration absorption liquid in the absorption process is NaOH and NaHCO3、Na2CO3One or more than two of the sulfur recovery systems and alkaline solution of the sulfur recovery system. The micro-aerobic bioreactor adopts an activated sludge method, the pH value is controlled to be 8.5 +/-0.3, and the temperature is controlled to be 30oC, the retention time is controlled to be 3 h, C: N: P =500:5: 1, and the dissolved oxygen is controlled to be 0.01-0.3 mg/L. The sulfur recovery system consists of a coagulating sedimentation system, a sulfur sludge drying system and a sulfur sludge purification system.

Claims (5)

1. A process for removing hydrogen sulfide from biogas by combining chemical absorption with biology and recycling sulfur is characterized by comprising the following process steps:
(1) absorbing hydrogen sulfide in the biogas by using an absorption tower, and absorbing the hydrogen sulfide in the biogas by using alkaline absorption liquid in the absorption tower to generate a solution of sodium sulfide and sodium hydrosulfide;
(2) the solution containing sodium sulfide and sodium hydrosulfide generated by absorbing hydrogen sulfide enters a micro-aerobic bioreactor, the microorganisms are utilized to convert sulfide into elemental sulfur, and simultaneously, carbonate generated by absorbing carbon dioxide in the biogas provides a carbon source for sulfur oxidizing bacteria;
(3) the mixed liquid containing elemental sulfur generated by the micro-aerobic bioreactor is treated by a sulfur recovery system to obtain sulfur with higher content for recycling, and the alkaline solution generated by the sulfur recovery system returns to the desulfurization absorption tower for recycling;
the absorption tower is a packed tower or a spray tower, the micro-aerobic bioreactor adopts a micro-aerobic activated sludge reactor, and the sulfur recovery system comprises a sedimentation tank and a solid-liquid separation device.
2. The process of claim 1, wherein the absorption tower is a packed tower or a spray tower, the micro-aerobic bioreactor is a micro-aerobic activated sludge reactor, and the sulfur recovery system comprises a sedimentation tank and a solid-liquid separation device.
3. The process of claim 1, wherein the alkaline absorption solution is NaOH or NaHCO in the desulfurization absorption process3、Na2CO3One or more than two of the sulfur recovery systems and alkaline supernatant in a sedimentation tank of the sulfur recovery system.
4. The process for removing hydrogen sulfide from biogas and recycling sulfur through chemical absorption and biology as claimed in claim 1, wherein the pH value of the micro-aerobic bioreactor is controlled to be 8.5-10, and the temperature is controlled to be 25-38oC, the retention time is controlled to be 3-24 h, C: N: P =500:5: 1, and the dissolved oxygen is controlled to be 0.01-0.3 mg/L.
5. The process of claim 1, wherein the nitrogen source used by the microorganisms in the micro-aerobic reactor is sludge fermentation to produce ammonia nitrogen recovery liquid, and the phosphorus source is dihydrogen phosphate or dihydrogen phosphate.
CN201810677308.8A 2018-06-27 2018-06-27 Chemical absorption combined biological removal hydrogen sulfide and sulfur resource technology in methane Pending CN110643403A (en)

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CN113072989A (en) * 2020-10-15 2021-07-06 辽宁省能源研究所有限公司 Semi-continuous two-stage biogas autotrophic biological desulfurization method and system
CN114053850A (en) * 2021-08-18 2022-02-18 中国水电建设集团十五工程局有限公司 Biogas biological desulfurization process in sludge digestion gas thermoelectric cogeneration application
CN114506982A (en) * 2020-10-28 2022-05-17 中国石油化工股份有限公司 Device and method for treating sulfur-containing sludge in high-sulfur-containing gas field
CN114774175A (en) * 2022-04-19 2022-07-22 宁夏滨泽新能源科技有限公司 System and method for resource utilization of sulfur-containing methane

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CN104607029A (en) * 2015-01-23 2015-05-13 大连理工大学 Synchronous flue gas desulfurization and denitrification process combining chemical absorption with anaerobic-aerobic conversion
CN106381183A (en) * 2016-11-30 2017-02-08 唐山绿源环保科技有限公司 Biological desulfurization device and desulfurization process for biogas

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CN113072989A (en) * 2020-10-15 2021-07-06 辽宁省能源研究所有限公司 Semi-continuous two-stage biogas autotrophic biological desulfurization method and system
CN114506982A (en) * 2020-10-28 2022-05-17 中国石油化工股份有限公司 Device and method for treating sulfur-containing sludge in high-sulfur-containing gas field
CN114506982B (en) * 2020-10-28 2024-04-26 中国石油化工股份有限公司 Sulfur-containing sludge treatment device and method for high-sulfur-content gas field
CN114053850A (en) * 2021-08-18 2022-02-18 中国水电建设集团十五工程局有限公司 Biogas biological desulfurization process in sludge digestion gas thermoelectric cogeneration application
CN114774175A (en) * 2022-04-19 2022-07-22 宁夏滨泽新能源科技有限公司 System and method for resource utilization of sulfur-containing methane

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