CN101705126B - In-situ biogas coupling type long-acting desulfurizer - Google Patents
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- CN101705126B CN101705126B CN2009100127317A CN200910012731A CN101705126B CN 101705126 B CN101705126 B CN 101705126B CN 2009100127317 A CN2009100127317 A CN 2009100127317A CN 200910012731 A CN200910012731 A CN 200910012731A CN 101705126 B CN101705126 B CN 101705126B
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Abstract
The invention discloses an in-situ biogas coupling type long-acting desulfurizer, which is added into a biogas fermentation device to make desulfurization and raw material fermentation carried out synchronously, and solves the problems of short service cycle, frequent and inconvenient replacement and the like of the conventional biogas desulfurizer. The in-situ biogas coupling type long-acting desulfurizer adopts the technical key points that: the desulfurizer comprises a sulfate reducing bacteria inhibitor and a sulfureted hydrogen removing agent of which the mass ratio is (1-4): (19-16); and the mass ratio of the desulfurizer to the dried raw materials is (1-35): 1,000. The in-situ biogas coupling type long-acting desulfurizer directly added into the biogas fermentation device to desulfurize the in-situ biogas, and has the outstanding advantages of abundant raw materials, obvious improvement on desulfurization efficiency, simple process, convenient operation, economy and the like which cannot be matched by other desulfurizers; and through a process of coupling the biology with chemistry, the in-situ biogas coupling type long-acting desulfurizer comprehensively treats and removes the sulfureted hydrogen in the in-situ biogas in a biogas pool, and is a new trend of desulfurizing the biogas.
Description
Technical field:
Patent of the present invention relates to the in-situ biogas coupling type long-acting desulfurizer that carries out desulfurization in a kind of direct adding biogas fermentation device, can be used for the in-situ biogas desulfurization of large, medium and small anaerobic fermentation tank and domestic methane tank.
Technical background:
Hydrogen sulfide is a kind of hypertoxic gas, the serious harm person poultry safety.Because popularizing of rat chow, sulphur content constantly increases in the feces of livestock and poultry, causes the hydrogen sulfide content in the biogas also general by 1 original～2g/m
3Rise to 3～4g/m
3, biogas desulfurization is more urgent.In China, no matter be big-and-middle-sized biogas engineering or rural area household biogas, biogas desulfurization is main with traditional dry desulfurization (sweetening agent is a red oxide of iron) still at present; There is the part biogas engineering to adopt biological desulphurization abroad.The red oxide of iron method is with a long history, technology maturation, relatively be suitable for hydrogen sulfide in methane content lower (≤1g/L); And desulfurization when biogas makings is relatively drier; The initial stage desulfuration efficiency all can reach more than 95%, but along with the reduction of Sulfur capacity, the later stage sweetening effectiveness is decay rapidly; Because of Sulfur capacity restriction cause life cycle short, change frequently and inconvenient, running cost is high, in actual use, many users feel trouble and sweetening agent are not regenerated or changes that desulfurizer performs practically no function, and causes high sulfur-bearing biogas by directly use.
In order to overcome the drawback of red oxide of iron desulfurization, some units are through improving the chemical desulfurization agent, add means such as catalyzer and improve sweetening agent both at home and abroad, with the cost that reduces sweetening agent, improve desulfuration efficiency, extend working time.Biogas desulfurization efficient etc. improves through adding flocculation agent in cu-zsm catalyzer, vannadate oxygenant, Germany like the Maria of U.S. development, and Hebaiyi Ecological Energy Sci., & Tech. Development Co., Ltd., Beijing has developed the multi-functional devulcanizer that peasant household uses.These measures can partly improve the deficiency of iron processes, but still can not effectively overcome the drawback of dry desulfurization.
In view of some drawbacks of materialization desulfurization, scientific research personnel both domestic and external is successively with the biological removal technology introduction biogas desulfurization of hydrogen sulfide.Because biological desulphurization has working pressure and temperature is low, running cost is low, level of automation is high, do not have advantage such as secondary pollution, thereby has obtained certain achievement, has market outlook preferably.
In recent years, utilize both at home and abroad the desulfurization mikrobe that from different habitats, is separated to carry out biogas desulfurization, and comprised photosynthetic sulfur bacteria, thiobacillus etc., the most sophisticated to represent bacterium be T.f bacterium (thiobacillus ferrooxidant).Carried out the mechanism research of microbial desulfurization simultaneously.Verified the metabolism principle of some bacterial strains at present, found out the gene of coding desulphurase, made up engineering strain, to improve desulfuration efficiency and range of application.It is reported that the dsz gene cluster successfully is cloned in many strains pseudomonas.Recombinant bacterial strain is than more effectively desulfurization of original strain.And the engineering bacteria of structure has wide industrial application and environment protection prospect.States such as Holland, Germany, Japan, the U.S. have obtained some successes aspect biological desulphurization.According to the reported in literature of some biological desulphurization aspects, as 1) German patent is in " biogas biochemical doctor treatment " of DE102005025040, disclose with biogas with derive from photosynthetic oxygen rich gas and in biochemical desulfurizer, mix biochemical desulfurization afterwards; 2) the Japanese Patent patent No. is in " the methane bio-desulfurization system " of JP2004135579, discloses through nitrification liquid to contact with biogas is reverse hydrogen sulfide in absorption, the oxidation biogas; 3) Japanese Patent No. is in " sulfur method and the desulfurizer " of JP2003113386, disclose natural pond liquid is imported in the biological desulphurization tower, thereby and put into the hydrogen sulfide that carrier fixing sulfur bacterium is removed biogas; 4) Japanese Patent No. is in " bio-desulfurization device " of JP2003062421, discloses aerobic aeration mud is sprayed in the thionizer and the reverse contact desulfuriation of sulfurous gas, and desulfurization mud passes back into and carries out regeneration activating in the aeration tank; 5) at " ACTA Scientiae Circumstantiae " (2008; Vol.28; No.8:1542-1548) in " startup of piggery wastewater denitrogenation and marsh gas desulfurization coupling reactor drum " literary composition, the biogas desulfurization that Ministry of Agriculture's biogas studied and the contents such as linked reaction of denitrogenation of waste water are disclosed; 6) the Chinese patent notification number is in " a kind of methane bio-desulfurization equipment " of CN 2870960Y, discloses a kind of biological process sweetener of inventor's exploitation, promptly utilizes the immobilization thiobacterium to remove the bio-desulfurization device of the hydrogen sulfide in the biogas; 7) at " Harbin Institute of Technology's journal " (2005; Vol.37, " low-temperature biological is handled sulfur-bearing nitrogenous gas usefulness and mechanism research " No.2:167-197) is at " Techniques and Equipment for Environmental Pollution Control " (2006; Vol.7, " modified version bio-trickling filter processing H No.2:45-49)
2The righttest processing condition research of S foul smell " 8) inventor once delivered in " use with environmental organism journal " (2004, Vol.10, No.2:215～217) and had been entitled as that " the wood chip microbial film is handled H
2The S gas studies ", from different environment seed selection several plant heights imitate the desulfurization mikrobes, at H
2The S inlet gas concentration is 1107mg/m
3The time desulfurization degree reach 94%.This method successfully is applied to (daily output biogas 1500m in Tanzania's sisal hemp waste residue biogas engineering
3), desulfurization degree can reach more than 95%.
But biological desulfurizing technology is relatively more responsive to temperature, if will reach the clearance more than 90%, its temperature of reaction must be controlled at more than 25 ℃, is only limited to the biogas engineering desulfurization at present, and the stability of its desulfurization receives the influence of envrionment temperature bigger.And after running to certain phase, because of the desulfurization particle accumulates in the device, latch up phenomenon appears, need change filler to certain phase.
Existing sulfur method all is outside the pond or Chi Ding sets up a desulfurizer; Utilize chemical substance or mikrobe to deviate from the hydrogen sulfide in the biogas; Because of it all is after hydrogen sulfide produces, to carry out desulfurization again; Belong to desulfurization afterwards, thus exist investment higher, change complicated, need drawback such as extra occupation of land.The report that in biogas fermentation device, carries out in-situ biogas comprehensive treating process desulfurization is not seen in the home and abroad at present.
Summary of the invention:
The purpose of this invention is to provide a kind of in-situ biogas coupling type long-acting desulfurizer that desulfurization and fermenting raw materials are carried out synchronously that adds, it has solved the life cycle of existing biogas desulfurizer existence and has lacked, changed problems such as frequent and inconvenience.Through in-situ biogas coupling type long-acting desulfurizer being added directly in the biogas fermentation device in-situ biogas desulfurization, it is abundant to have raw material sources, significantly improves desulfuration efficiency, easy to operate, save advantages such as sweetener expense, working cost are low.
The technical scheme that the present invention adopted is: the in-situ biogas coupling type long-acting desulfurizer that in this adding biogas fermentation device desulfurization and fermenting raw materials is carried out synchronously; Its technical essential is: said sweetening agent comprises sulfate reduction bacteria inhibitor and hydrogen sulfide scavengers, and both mass ratioes are (1～4): (19～16); The consumption mass ratio of desulfurizer therefor and biogas fermentation raw material dry product is (1～35): 1000.
Said sulphate reducing bacteria suppressor factor comprises Sodium orthomolybdate, formaldehyde and qingfengmeisu qiong, and three's mass ratio is (10～88): (10～88): (1～2).
Said hydrogen sulfide scavengers is a molysite, comprises in Ferrox, iron protochloride, ferrous sulfate, Iron nitrate, iron protocarbonate, iron(ic)chloride, ferric sulfate, iron nitrate, all molysite of ironic citrate one or more.
Said in-situ biogas coupling type long-acting desulfurizer adopts solid or liquid, is used for the biogas fermentation device of TS≤35%.
Advantage and positively effect that the present invention has are: produce the active sulfate reduction bacteria inhibitor of bacterium owing to contain the hydrogen sulfide that can suppress in the biogas fermentation device in the component of sweetening agent of the present invention; Utilize biochemical technology in biogas fermentation device, a large amount of ions that can produce hydrogen sulfide to be restrained; So can in the biogas generative process, just carry out desulfurization first; Reduce the generation of hydrogen sulfide in the in-situ biogas significantly, also just reduced the workload of follow-up desulfurization in a large number.In addition; Because of also containing hydrogen sulfide scavengers in this sweetening agent component, can make its hydrogen sulfide that is produced with fermenting process in position that the reaction of on-gaseous sulfide takes place irreversibly to be converted into, so desulfurization again in biogas fermentation device; Generate water-fast sulfide, discharge with discharging.Therefore, the present invention is readily embodied in the interior twice comprehensive treating process desulfurization to in-situ biogas of biogas fermentation device, stablizes to remove the hydrogen sulfide in the biogas, thereby need not to be provided with extraly desulfurizer.This both can directly export the biogas that produces; Carry out the high-value-use of biogas, can reduce the cost of high-value-use of volume and the biogas of necessary refining desulfurization device again significantly, fundamentally solved the problem of environmental pollution that hydrogen sulfide brings; The real construction investment that realizes that biogas desulfurization had economizes; Advantages such as technical process is simple, and is easy to operate, and running cost is low.In addition, also can reduce the corrosion of hydrogen sulfide, the work-ing life of significant prolongation export pipeline and biogas fermentation device, improve desulfuration efficiency and reduce cost output channel through in-situ biogas desulfurization.Prove through actual survey, directly in biogas fermentation device, add coupling type long-acting desulfurizer, in-situ biogas is carried out hydrogen sulfide stripping, clearance reaches as high as 99%.In sum; The incomparable advantages of other sweetening agent such as the technology that in-situ biogas coupling type long-acting desulfurizer has is simple, economical and practical; Adopt biological and chemical coupled technology through it; In methane-generating pit, the hydrogen sulfide in the in-situ biogas is carried out comprehensive treating process and remove, will become the new trend of biogas desulfurization.
Embodiment:
Below in conjunction with embodiment the present invention is elaborated.The in-situ biogas coupling type long-acting desulfurizer that in this adding biogas fermentation device desulfurization and fermenting raw materials is carried out synchronously; The sweetening agent that is adopted comprises sulfate reduction bacteria inhibitor and hydrogen sulfide scavengers, and both mass ratioes can be in (1～4): select as required in the scope of (19～16).The consumption mass ratio of used sulfate reduction bacteria inhibitor and hydrogen sulfide scavengers and the biogas fermentation raw material dry product that adopts is (1～35): 1000.The sulfate reduction bacteria inhibitor has adopted Sodium orthomolybdate, formaldehyde and qingfengmeisu qiong in the present embodiment, and make this triangular mass ratio according to actual materials amount in (10～88): (10～88): in (1～2) scope the apolegamy.Hydrogen sulfide scavengers mainly adopts molysite; Can select a kind of in all molysite of Ferrox, iron protochloride, ferrous sulfate, Iron nitrate, iron protocarbonate, iron(ic)chloride, ferric sulfate, iron nitrate, ironic citrate for use, can select also that wherein two or more are used in combination for use.Dosing method can adopt dosing pump quantitatively coupling type long-acting desulfurizer to be pumped into the biogas fermentation device from medicine storage device according to actual needs and (generally be applicable to various biogas engineering), also can adopt artificial with in an amount of coupling type long-acting desulfurizer input methane-generating pit (generally being applicable to methane-generating pit for farm household).Coupling type long-acting desulfurizer both can add by liquid form, can add by solid-state form again.But be more evenly distributed with the liquid form adding.The biogas fermentation raw material comprises one or more in feces of livestock and poultry, stalk, high density industrial or agricultural organic waste water and the various organic waste.
Embodiment one
The biogas engineering application example
First the 300kg sweetening agent is dissolved in the water, from opening for feed, add 450m
3Fermentor tank in (contain 13～25 tons of dry-matteies approximately, fermentation raw material is feces of livestock and poultry such as cow dung, chicken manure), stirred then 5 minutes, make sweetening agent uniform distribution in fermentor tank, make the H that produces in the fermentor tank
2S and reactive desulfurizing agent generate indissoluble FeS deposition, get rid of with the discharge of biogas residue and biogas liquid, thereby realize in-situ biogas desulfurization.After adding sweetening agent first, add sweetening agent 1～10kg/T raw material with raw material when adding raw material later at every turn, add when the biogas sulphur content is high, add less after a little while.
The sweetening agent prescription is: Sodium orthomolybdate 17.6g, formaldehyde 2g, qingfengmeisu qiong 0.4g, ferrous sulfate 80g.
Through a month desulfurization test, make H in the biogas
2S concentration is from 1200mg/m
3Drop to about 15mg/m
3, clearance reaches more than 98%.
Embodiment two
The domestic methane tank application example
At different rural area 8m
3The disposable input 2Kg of (fermentation raw material is organic mixtures such as pig manure, stalk, dish leaf, contains about 0.20～0.48 ton of dry-matter) difference, 4kg, 8kg sweetening agent stir in the domestic methane tank.
The sweetening agent prescription is: Sodium orthomolybdate 0.5g, formaldehyde 4.4g, qingfengmeisu qiong 0.1g, Ferrox 30g, iron(ic)chloride 25g, ferrous sulfate 25g, iron protocarbonate 15g.
Each group test shows, in methane-generating pit, drops into 2～8Kg sweetening agent respectively, all can make methane-generating pit continue desulfurization 3～6 months.Make H in the biogas
2S concentration is from 2000～3000mg/m
3Drop to 100～1000mg/m
3, clearance reaches as high as more than 95%.
The family is better at the interpolation initial stage with the sweetening effectiveness in pond, and the later stage desulfuration efficiency has certain decline, and then can promote desulfuration efficiency as carrying out suitably replenishing sweetening agent in the above described manner this moment.
Embodiment three
Application example in batches ferments
In ten groups of 1.5L upper and lower opening filter flasks, add the 1L high concentrated organic wastewater respectively and carry out biogas fermentation; The methane inoculum is 20%; About 1～3% (TS=1～3%) of fermentation total solids, the disposable coupling type long-acting desulfurizer 0.5～2g that adds respectively when charging feedstock shakes up back 30 ℃ of fermentations.Blank fermentation group with not adding sweetening agent compares.
First group of coupling type long-acting desulfurizer prescription is: Sodium orthomolybdate 2.9g, formaldehyde 7g, qingfengmeisu qiong 0.1g, iron nitrate 90g.
Second group of coupling type long-acting desulfurizer prescription is: Sodium orthomolybdate 2.9g, formaldehyde 7g, qingfengmeisu qiong 0.1g, ironic citrate 90g.
The 3rd group of coupling type long-acting desulfurizer prescription is: Sodium orthomolybdate 2.9g, formaldehyde 7g, qingfengmeisu qiong 0.1g, iron protochloride 90g.
The 4th group of coupling type long-acting desulfurizer prescription is: Sodium orthomolybdate 2.9g, formaldehyde 7g, qingfengmeisu qiong 0.1g, ferric sulfate 90g.
The 5th group of coupling type long-acting desulfurizer prescription is: Sodium orthomolybdate 2.9g, formaldehyde 7g, qingfengmeisu qiong 0.1g, iron(ic)chloride 90g.
The 6th group of coupling type long-acting desulfurizer prescription is: Sodium orthomolybdate 2.9g, formaldehyde 7g, qingfengmeisu qiong 0.1g, Ferrox 90g.
The 7th group of coupling type long-acting desulfurizer prescription is: Sodium orthomolybdate 2.9g, formaldehyde 7g, qingfengmeisu qiong 0.1g, Iron nitrate 90g.
The 8th group of coupling type long-acting desulfurizer prescription is: Sodium orthomolybdate 2.9g, formaldehyde 7g, qingfengmeisu qiong 0.1g, iron protocarbonate 90g.
The 9th group of coupling type long-acting desulfurizer prescription is: Sodium orthomolybdate 2.9g, formaldehyde 7g, qingfengmeisu qiong 0.1g, ferric sulfate 20g, iron protochloride 20g, ironic citrate 20g, iron nitrate 20g, iron protocarbonate 10g.
The tenth group is blank, does not add sweetening agent.
Test group continues about 2 months of desulfurization, all can not remove hydrogen sulfide on the same group, but clearance becomes downtrending as time passes.Each is organized the hydrogen sulfide removal rate and all drops to 70%～80% of february gradually from initial about 95%.
Embodiment four
Do the fermentation application example
In big mouthful of vial of 2.5L, add the 200g stalk; Add an amount of inoculum and water; Make in the fermentation flask total solid concentration about 35%, about 20%, the 30 ℃ of fermentation of biogas inoculum; Disposable adding original position coupling type long-acting desulfurizer 2～6g when charging feedstock, original position coupling type long-acting desulfurizer prescription is: Sodium orthomolybdate 1.82g, qingfengmeisu qiong 0.18g, formaldehyde 16g, Iron nitrate 20g, iron protochloride 20g, ferric sulfate 17g, iron nitrate 15g, ironic citrate 10g.Add and fashionable compound coupling type long-acting desulfurizer and fermentation raw material etc. are mixed.
Test shows, the sustainable desulfurization of original position coupling type long-acting desulfurizer 4～6 months.Make stalk fermentation produce hydrogen sulfide in methane concentration by 500～800mg/m
3Drop to 10～50mg/m
3
Embodiment five
The preparation of solid desulfurating agent
At first Sodium orthomolybdate, qingfengmeisu qiong, formaldehyde etc. are mixed by a certain percentage, be configured to the sulfate reduction bacteria inhibitor.Three's mass ratio is (10～88): (10～88): (1～2), concrete ratio are according to hydrogen sulfide in methane concentration, market price of raw material and different.Add an amount of molysite then; Molysite is one or more in the molysite such as Ferrox, iron protochloride, ferrous sulfate, Iron nitrate, iron protocarbonate, iron(ic)chloride, ferric sulfate, iron nitrate, ironic citrate, the mass ratio (16～19) of molysite and sulfate reduction bacteria inhibitor: (1～4).Mix the back with aluminum plastic film, plastics film equal vacuum sealing pack.
Embodiment six
The preparation of liquid sweetening agent
At first Sodium orthomolybdate, qingfengmeisu qiong, formaldehyde are dissolved in respectively in the water, three's mass ratio is (10～88): (10～88): (1～2), containing three's total amount in every 1L water is 50～200g, is configured to the sulphate reducing bacteria inhibitor solution.Molysite with 950～800g adds in the vitriol inhibitor solution then; Molysite is one or more in the molysite such as Ferrox, iron protochloride, ferrous sulfate, Iron nitrate, iron protocarbonate, iron(ic)chloride, ferric sulfate, iron nitrate, ironic citrate, and the back that stirs is with brown container encloses such as Plastic Bottles.Shady and cool dry place preserves.
Claims (1)
1. in-situ biogas coupling type long-acting desulfurizer; It is characterized in that: said sweetening agent is by sulfate reduction bacteria inhibitor and hydrogen sulfide scavengers; Both mass ratioes are (1 ~ 4): (19 ~ 16) are formed; The consumption mass ratio of desulfurizer therefor and biogas fermentation raw material dry product is (1 ~ 35) : 1000; Said sulfate reduction bacteria inhibitor is made up of Sodium orthomolybdate, formaldehyde and qingfengmeisu qiong; Three's mass ratio is (10 ~ 88): (10 ~ 88): (1 ~ 2), said hydrogen sulfide scavengers is a molysite, comprises in Ferrox, iron protochloride, ferrous sulfate, Iron nitrate, iron protocarbonate, iron(ic)chloride, ferric sulfate, iron nitrate, all molysite of ironic citrate one or more.
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| CN104762588B (en) * | 2015-03-19 | 2018-03-13 | 中国石油化工股份有限公司青岛安全工程研究院 | A kind of method for assessing sulphur iron compound passivation effect |
| CN105969717A (en) * | 2016-05-30 | 2016-09-28 | 青岛理工大学 | Method for preparing efficient ecological restoration floras for Hg contaminated site from biogas residues |
| CN106554837B (en) * | 2016-11-17 | 2019-10-22 | 南京工业大学 | A kind of method of iron containing compounds and Acidithiobacillus caldus combined removal hydrogen sulfide in methane |
| CN107699593A (en) * | 2017-12-01 | 2018-02-16 | 江苏中科重工股份有限公司 | A kind of batch (-type) dry method marsh gas fermentation process |
| CN108326031A (en) * | 2018-01-16 | 2018-07-27 | 航天凯天环保科技股份有限公司 | A kind of method of sulphide staining soil stabilization processing |
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| CN1089579A (en) * | 1993-01-11 | 1994-07-20 | 农业部成都沼气科学研究所 | The iron processes pre-treatment of marsh gas fermentation of molasses containing waste water |
| CN1121950A (en) * | 1994-10-25 | 1996-05-08 | 上海市煤气公司研究所 | Dry shaping desulfurizing agent, its preparation and use |
| CN101143290A (en) * | 2006-09-13 | 2008-03-19 | 宝山钢铁股份有限公司 | Normal temperature iron oxide desulfurizing agent, preparation method and application thereof |
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Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1089579A (en) * | 1993-01-11 | 1994-07-20 | 农业部成都沼气科学研究所 | The iron processes pre-treatment of marsh gas fermentation of molasses containing waste water |
| CN1121950A (en) * | 1994-10-25 | 1996-05-08 | 上海市煤气公司研究所 | Dry shaping desulfurizing agent, its preparation and use |
| CN101143290A (en) * | 2006-09-13 | 2008-03-19 | 宝山钢铁股份有限公司 | Normal temperature iron oxide desulfurizing agent, preparation method and application thereof |
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