CN104591083B - A kind of hydrogen production process - Google Patents
A kind of hydrogen production process Download PDFInfo
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- CN104591083B CN104591083B CN201510047475.0A CN201510047475A CN104591083B CN 104591083 B CN104591083 B CN 104591083B CN 201510047475 A CN201510047475 A CN 201510047475A CN 104591083 B CN104591083 B CN 104591083B
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E50/00—Technologies for the production of fuel of non-fossil origin
- Y02E50/30—Fuel from waste, e.g. synthetic alcohol or diesel
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Abstract
The invention provides a kind of hydrogen production process, belong to hydrogen preparation field.The method includes：1), biological waste is carried out with anaerobic fermentation, produces biogas；2), 34 MPas will be forced into after described marsh gas purifying, and carry out hydrocarbon conversion reaction, obtain the mixed gas containing CO, CO2, H2 and vapor；3), by described mixed gas under the conditions of 2.2 2.6 MPas, 300 350 DEG C, and after carrying out CO transformationreation under the effect of ferrum cobalt series catalyst, the temperature of mixed gas will be down to 35 45 DEG C after reaction, and carry out pressure-variable adsorption, obtain hydrogen.The technique effect that this hydrogen production process has low cost, economizes on resources；Improve the present situation obtaining undue dependence oil and natural gas of hydrogen in prior art；A kind of new preparation method that offer is provided for plant hydrogen；While having ensured that hydrogen is produced, also greatly promote the development of biogas industry.
Description
Technical field
The present invention relates to hydrogen preparation field, in particular to a kind of hydrogen production process.
Background technology
Hydrogen is the gas of known density minimum in the world, is the minimum material of relative molecular mass, the quality of hydrogen
Only air 1/14, when 0 DEG C, the pressure of standard atmosphere, the density of hydrogen is 0.0899g/L.Hydrogen be one kind easily
The gas of combustion, aerial volume fraction is can to burn when 4% to 75%.
As most important industrial gases and special gas, hydrogen is in petrochemical industry, electronics industry, metallurgical industry, food
The aspects such as processing, float glass, Minute Organic Synthesis, Aero-Space have a wide range of applications.Meanwhile, hydrogen is also a kind of preferable
Secondary energy sources (secondary energy sources refer to must be by a kind of primary energy energy that for example solar energy, coal etc. to be produced).
Generally, hydrogen is easily combined with oxygen.This characteristic becomes natural reducing agent and is used in and prevents
In the production of oxidation.In the high temperature working processes of glass manufacture and the manufacture of electronic microchip, add in nitrogen shielding gas
Hydrogen is to remove the oxygen of remnants.In petrochemical industry, need to be hydrogenated with and be refined crude oil by desulfuration and hydrogenation cracking.Hydrogen another
Important purposes is the fatty hydrogen preventing in margarine, edible oil, shampoo, lubricant, household cleaning agent and other products
Change.Further, since the height of hydrogen is fuel, aerospace industry is used liquid hydrogen as fuel.
In correlation technique, hydrogen feedstock is mainly oil and natural gas, and that is, oil and natural gas are (containing Petroleum, heavy oil, refining
Factory's gas and oven gas etc.) pass through producing hydrogen from steam conversion.But utilize oil and natural gas hydrogen manufacturing one side complex operation, cost
High；On the other hand, under petroleum resources trend increasingly in short supply, also there is the technical problem of the wasting of resources in this hydrogen production process.Cause
This, provide a kind of new hydrogen preparation method and improve producing of plant hydrogen in prior art and undue rely on showing of fossil energy
Shape is a problem of people's urgent need to resolve.
In view of this, the special proposition present invention.
Content of the invention
It is an object of the invention to provide a kind of hydrogen production process, described hydrogen production process is originated with biogas for hydrogen manufacturing, has
Low cost, the technique effect economizing on resources.
In order to realize the above-mentioned purpose of the present invention, spy employs the following technical solutions：
The invention provides a kind of hydrogen production process, comprise the following steps：
1), biological waste is carried out with anaerobic fermentation, produces biogas；
2), it is forced into 3-4 MPa by after described marsh gas purifying, and carries out hydrocarbon conversion reaction, obtain containing CO, CO2、H2
And the mixed gas of vapor；
3), by described mixed gas under the conditions of 2.2-2.6 MPa, 300-350 DEG C, and in ferrum-cobalt series catalyst effect
Under carry out CO transformationreation after, the temperature of mixed gas will be down to 35-45 DEG C after reaction, and carry out pressure-variable adsorption, obtain hydrogen.
In this hydrogen production process that the present invention provides, carry out anaerobic fermentation with biological waste for initial feed and produce natural pond
Gas, the biogas of generation passes through purified treatment, is risen using compressor after removing contained sulfur (hydrogen sulfide) and part moisture
Press so as to pressure reaches 3-4 MPa, further to remove moisture removal.
During carrying out hydrocarbon conversion reaction (predominantly steam conversion reaction and methane reforming with carbon dioxide),
A large amount of methane in biogas carry out reaction with the rear vapor adding and produce hydrogen and carbon monoxide, and part carbon monoxide is steamed with water
Solid/liquid/gas reactions liquid generates hydrogen and carbon dioxide.In addition, methane also can generate carbon monoxide and hydrogen with carbon dioxide reaction.Cause
This, by hydrocarbon conversion reaction, can obtain containing CO, CO2、H2And the mixed gas of vapor；This mixed gas is in 2.2-
2.6 MPas, under the conditions of 300-350 DEG C, and carry out CO transformationreation under ferrum-cobalt series catalyst effect so that carbon monoxide and
Water reacts, and generates hydrogen and carbon dioxide again；Reacted mixed gas are cooled to 35-45 DEG C, carry out pressure-variable adsorption (main
It is the gases such as the carbon monoxide, the carbon dioxide that remove and do not participate in reaction), thus obtaining highly purified hydrogen.
The preparation method of the hydrogen that the present invention provides, it achieves the effect of biogas hydrogen manufacturing, and biogas can pass through fermenting organism
Fertilizer is obtained in a large number, and (, compared with oil and natural gas, its preparation cost is cheap, therefore substantially reduces for biogas for its wide material sources
The preparation cost of hydrogen, also a saving the fossil energy of increasingly depleted simultaneously), biogas is passed through a series of to purify and turn
Highly purified hydrogen can be produced after changing reaction.Therefore, the preparation method of this hydrogen that the present invention provides, it has cost
Technique effect that is low, economizing on resources；Improve the present situation obtaining undue dependence oil and natural gas of hydrogen in prior art；For
A kind of new preparation method that offer is provided of plant hydrogen；While having ensured that hydrogen is produced, also greatly promote biogas
The development of industry.
Optionally, in step 2) in, described purification specifically includes：Biogas utilization sulfur bacteria is carried out desulfurization process.
Optionally, in step 2) in, specifically include：
After marsh gas purifying, it is forced into 3-4 MPa, and carries out pressure-variable adsorption and take off CO2, then at 800-900 DEG C, the catalysis of nickel system
Carry out steam conversion reaction under agent effect, obtain containing CO, CO2、H2And the mixed gas of vapor.
Optionally, in described steam conversion reaction, steam/hydrocarbons ratio is 2.5～3.
Optionally, described steam conversion reaction is carried out in reburner.
Optionally, in step 2) in, specifically include：
3-4 MPa will be forced into after marsh gas purifying, and in 600-800 DEG C, with Ni-Al2O3/SiO2Carry out as catalyst
Methane reforming with carbon dioxide, obtains containing CO, CO2、H2And the mixed gas of vapor.
Optionally, after obtaining mixed gas, in step 3) before, also include：
Mixed gas are cooled to after 35-45 DEG C and carry out the de- H of pressure-variable adsorption2.
Optionally, in step 3) in：In described CO transformationreation, CO used is anti-by described methane carbon dioxide reformation
The mixed gas that should produce are heated to 300-350 DEG C.
Optionally, described sulfur bacteria includes thiobacillus thiooxidans or thiobacillus ferrooxidant.
Optionally, described biological waste includes：Straw, excrement of animals, rubbish landfill gas, productive life organic sewage
One or more of.
Compared with prior art, beneficial effects of the present invention are：
(1), originated for hydrogen manufacturing with biogas, there is low cost, the effect economizing on resources.
(2), biogas can be obtained in a large number by carrying out anaerobic fermentation to bio-feritlizer, and bio-feritlizer wide material sources,
Fermentation also achieves the re-using of bio-feritlizer while producing biogas, and then makes the preparation method environmental protection section of whole hydrogen
Learn.
(3), during using biogas hydrogen manufacturing, the further purified treatment achieving biogas, it is stripped of in biogas
The compositions such as contained sulfur, carbon；With directly biogas is carried out using compared with, more environmentally-friendly.
(4), the method will be changed into hydrogen by biogas, and then for biogas using providing a kind of new approach.
Brief description
In order to be illustrated more clearly that the embodiment of the present invention or technical scheme of the prior art, below will be to embodiment or existing
The accompanying drawing having required use in technology description is briefly described.
Fig. 1 provides the preparation flow figure of hydrogen production process for the present invention.
Specific embodiment
Below in conjunction with embodiment, embodiment of the present invention is described in detail, but those skilled in the art will
Understand, the following example is merely to illustrate the present invention, and be not construed as limiting the scope of the present invention.Unreceipted concrete in embodiment
Condition person, the condition according to normal condition or manufacturer's suggestion is carried out.Agents useful for same or the unreceipted production firm person of instrument, are
Can be by the commercially available conventional products bought and obtain.
Refer to Fig. 1, the hydrogen production process that the present invention provides, comprise the following steps：
Step 101：Biological waste is carried out with anaerobic fermentation, produces biogas；
Step 102：Be forced into 3-4 MPa by after described marsh gas purifying, and carry out hydrocarbon conversion reaction, obtain containing CO,
CO2、H2And the mixed gas of vapor；
Specifically, in this step, in purification process, main purpose is contained sulfur and part moisture in removing biogas；
After purification, biogas is forced into 3-4 MPa, its principle is the saturated steam removing using cold partition method in biogas；Hydrocarbon
During conversion reaction, following steam conversion reaction can occur：
CH4+H2O=CO+3H2-Q；
Wherein, there is following reaction in the carbon monoxide that part generates again：
CO+H2O (g)=CO2+H2+Q.
Or, during hydrocarbon conversion reaction, by controlling response path and condition, following methane dioxy can occur
Change carbon reforming reaction：
CH4+CO2=2CO+2H2.
After entirely hydrocarbon conversion reaction terminates, you can produce and contain CO, CO2、H2And the mixed gas of vapor, wherein,
H2With the content highest of CO, other two kinds of gas content very littles.
Step 103：By described mixed gas under the conditions of 2.2-2.6 MPa, 300-350 DEG C, and in ferrum-cobalt series catalyst
After carrying out CO transformationreation under effect, the temperature of mixed gas after reaction is down to 35-45 DEG C, and carries out pressure-variable adsorption, obtain
Hydrogen.
After CO transformationreation, carbon monoxide and additional vapor is made to be reacted, i.e. CO+H2O (g)=CO2+H2+
Q.
Obtain after reaction in mixed gas, containing the carbon dioxide that substantial amounts of hydrogen and part generate, its temperature is reduced
Carry out pressure swing adsorption decarbonization (carbon dioxide) to after 35-45 DEG C, and then obtain highly purified hydrogen.
Preferably, on the basis of said method, can be combined with the next item down or whole restriction：
Described purification specifically includes and for biogas utilization sulfur bacteria to carry out desulfurization process.
Sulfur content in biogas too high then can etching apparatus and pipeline, reduce its service life it is therefore desirable to carry out to it
Desulfurization (hydrogen sulfide) is processed.Specifically, in the present invention, biological desulfurization can be adopted, this method is using colorless sulfur bacteria (preferably
Thiobacillus thiooxidans or thiobacillus ferrooxidant), under conditions of certain temperature, humidity and micro- oxygen, this antibacterial can be by H2S oxygen
Chemical conversion simple substance S or H2SO3.
Desulphurization mechanism is：
①、H2S gas dissolves, and is liquid phase by gas phase conversion；
2. the H after, dissolving2S is absorbed by the micro-organisms, and is transferred in microbial body；
3., enter the H in microbial cell2S is decomposed by the microorganisms as nutrient, trans-utilization, thus reaching removal
H2The purpose of S.Its reaction equation is as follows：
2H2S+3O2→2H2SO3；
2H2S+O2→2S+2H2O.
Most sulfur-oxidizing bacteria broadly falls into Thiobacillus.Due to Thiobacillus wide material sources, therefore remove H2During S, institute
Bacterium need not inoculate.In addition, most Thiobacillus is autotrophic microbe, the surface of anaerobic digestion thing can be supplied to they one
The required microcosmic aerobic environment of growth and necessary nutrition.So, with bioanalysises desulfurization, directly toward anaerobic digestor or gas storage
It is passed through a certain amount of O in tank2Or air keeping certain time, method is fairly simple.When adjusting suitable temperature, reaction
Between and air capacity, the H in biogas can be made2S content reduces to 50ppm.
Further, since removing CH in biogas4Outer other components mostly are harmful composition or impurity, therefore, need to be taken off respectively
Remove.Wherein in addition to hydrogen sulfide, CO2It is also a kind of major impurity, CO2Higher, then gas heating value is lower, according to China's natural gas
Standard《GB17820-1999》In a class gas and two class gas technical requirements, less than 3.0% need to be removed to.In the present invention
In, for CO2, removed using pressure swing adsorption method.
Preferably, in step 2) in, specifically include：After marsh gas purifying, it is forced into 3-4 MPa, and carry out transformation suction
Attached de- CO2, carry out steam conversion reaction under 800-900 DEG C, nickel catalyst, obtain containing CO, CO2、H2And vapor
Mixed gas；Further, during steam conversion reaction, steam/hydrocarbons ratio is 2.5～3 (mol ratios)；And, in order to just
In realizing steam conversion reaction, this process is carried out preferably in reburner.
In aforesaid operations, part vapor can be deviate from after biogas pressurization, and can deviate from certain during pressure-variable adsorption
The carbon dioxide of amount, the biogas after purification and vapor carries out steam conversion reaction, and in 800-900 DEG C, nickel catalyst
Under the conditions of generate contain CO, CO2、H2And the mixed gas of vapor.By exploration discovery, in the process of steam conversion reaction
In, steam/hydrocarbons ratio (mole) is set as that 2.5～3 are beneficial to a large amount of acquisition hydrogen.
As another preferred technical scheme, in step 2) in, specifically include：
3-4 MPa will be forced into after marsh gas purifying, and in 600-800 DEG C, with Ni-Al2O3/SiO2Carry out as catalyst
Methane reforming with carbon dioxide, obtains containing CO, CO2、H2And the mixed gas of vapor.
This process achieves methane reforming with carbon dioxide so that methane and carbon dioxide carry out reaction generation containing big
Amount hydrogen and the mixed gas of part carbon monoxide, contain substantial amounts of hydrogen in this mixed gas, for the ease of collecting product, excellent
It is selected in after this mixed gas is cooled to 35-45 DEG C and carry out the de- H of pressure-variable adsorption2Carry out step 3 afterwards again.Meanwhile, convert in described CO
In reaction, CO used is heated to 300-350 DEG C by the mixed gas that described methane reforming with carbon dioxide produces, in methane
The temperature of the mixed gas that CO 2 reforming reaction produces can reach 600-800 DEG C, and CO transformationreation needs 300-350 DEG C
Reaction temperature, and during removing hydrogen, the mixed gas of generation need to be lowered the temperature, therefore, in order to realize heat
The CO needing to participate in CO transformationreation, before not removing hydrogen (cooling), is carried out by making full use of of amount using mixed gas
Heat exchange, is heated to 300-350 DEG C.
Further, bio-feritlizer may include straw, excrement of animals, rubbish landfill gas, productive life organic sewage
One or more of.
To sum up, this hydrogen production process that the present invention provides, carries out anaerobic fermentation with biological waste for initial feed and produces
Biogas, the biogas of generation passes through purified treatment, is carried out using compressor after removing contained sulfur (hydrogen sulfide) and part moisture
Boost so as to pressure reaches 3-4 MPa, further to remove moisture removal.
During carrying out hydrocarbon conversion reaction (predominantly steam conversion reaction and methane reforming with carbon dioxide),
A large amount of methane in biogas carry out reaction with the rear vapor adding and produce hydrogen and carbon monoxide, and part carbon monoxide is steamed with water
Solid/liquid/gas reactions liquid generates hydrogen and carbon dioxide.In addition, methane also can generate carbon monoxide and hydrogen with carbon dioxide reaction.Cause
This, by hydrocarbon conversion reaction, can obtain containing CO, CO2、H2And the mixed gas of vapor；This mixed gas is in 2.2-
2.6 MPas, under the conditions of 300-350 DEG C, and carry out CO transformationreation in the presence of ferrum-cobalt series catalyst so that carbon monoxide
With water reaction, generate hydrogen and carbon dioxide again；Reacted mixed gas are cooled to 35-45 DEG C, carry out pressure-variable adsorption (main
If removing and not participating in the gases such as carbon monoxide, the carbon dioxide of reaction), thus obtaining highly purified hydrogen.
The preparation method of the hydrogen that the present invention provides, it achieves the effect of biogas hydrogen manufacturing, and biogas can pass through fermenting organism
Fertilizer is obtained in a large number, its wide material sources, and biogas can be produced high-purity after a series of purification and conversion reaction
Hydrogen.Therefore, the preparation method of this hydrogen that the present invention provides, its technique effect that there is low cost, economize on resources；Change
It has been apt to the present situation obtaining undue dependence oil and natural gas of hydrogen in prior art；One kind that offer is provided for plant hydrogen
New preparation method；While having ensured that hydrogen is produced, also greatly promote the development of biogas industry.
Next, combining above content, the hydrogen production process and its preparation method of the present invention is enumerated in detail below
Embodiment：
Embodiment 1
S11：Biological waste is carried out with anaerobic fermentation, produces biogas；
Biological waste includes：Straw, excrement of animals, rubbish landfill gas and productive life organic sewage.
S12：Biogas is carried out after desulfurization process, using compressor, biogas is boosted to 3.5 million using thiobacillus thiooxidans
Handkerchief；
S13：Biogas after boosting is carried out pressure-variable adsorption under room temperature and takes off CO2, under 850 DEG C, nickel catalyst
Carry out steam conversion reaction in reburner, obtain containing CO, CO2、H2And the mixed gas of vapor；
Wherein, during steam conversion reaction, steam/hydrocarbons ratio is 2.5～3 (moles).
In this step, generation chemical reaction is：
CH4+H2O=CO+3H2- Q, or CO+H2O (g)=CO2+H2+Q.
S14：By described mixed gas under the conditions of 2.4 MPas, 320 DEG C, and carry out CO under ferrum-cobalt series catalyst effect
After transformationreation, the temperature of mixed gas after reaction is down to 40 DEG C, and carries out pressure-variable adsorption, obtain purity and be more than 99.9%
Hydrogen.
In this step, generation chemical reaction is：CO+H2O (g)=CO2+H2+Q.
In the present embodiment, the main emergence work of first paragraph pressure-variable adsorption (in S13), to improve fire damp purity；Second
Section pressure-variable adsorption (in S14) main purpose is by trace amounts of CO, CO in mixed gas2Deng impurity removal, to realize hydrogen purification effect.
Embodiment 2
S21：Biological waste is carried out with anaerobic fermentation, produces biogas；
Biological waste includes：Straw, excrement of animals, rubbish landfill gas and productive life organic sewage.
S22：Biogas is carried out after desulfurization process, using compressor, biogas is boosted to 3.5 million using thiobacillus thiooxidans
Handkerchief；
S23：By the biogas after boosting in 700 DEG C, with Ni-Al2O3/SiO2Carry out methane and carbon dioxide weight as catalyst
Whole reaction, obtains containing CO, CO2、H2And the mixed gas of vapor；
In this step, the chemical reaction of generation is：CH4+CO2=2CO+2H2.
S24：By described mixed gas under the conditions of 2.4 MPas, 320 DEG C, and carry out CO under ferrum-cobalt series catalyst effect
After transformationreation, the temperature of mixed gas after reaction is down to 40 DEG C, and carries out pressure-variable adsorption, obtain purity and be more than 99.9%
Hydrogen.
The chemical reaction occurring in this step is consistent with the chemical reaction implemented in step S14 in 1.
Although illustrate and describing the present invention with specific embodiment, but it will be appreciated that without departing substantially from the present invention's
Many other changes can be made in the case of spirit and scope and change.It is, therefore, intended that in the following claims
Including all such changes and modifications belonging in the scope of the invention.
Claims (9)
1. a kind of hydrogen production process is it is characterised in that comprise the following steps：
1), biological waste is carried out with anaerobic fermentation, produces biogas；
2), it is forced into 3-4 MPa by after described marsh gas purifying, and carries out hydrocarbon conversion reaction, obtain containing CO, CO2、H2And
The mixed gas of vapor；
3), by described mixed gas under the conditions of 2.2-2.6 MPa, 300-350 DEG C, and enter under ferrum-cobalt series catalyst effect
After row CO transformationreation, the temperature of mixed gas after reaction is down to 35-45 DEG C, and carries out pressure-variable adsorption, obtain hydrogen；
In step 2) in, described purification specifically includes：
Biogas utilization sulfur bacteria is carried out desulfurization process；
Described hydrocarbon conversion reaction includes following reaction：
CH4+H2O=CO+3H2-Q、CO+H2O (g)=CO2+H2+ Q and CH4+CO2=2CO+2H2.
2. hydrogen production process according to claim 1 is it is characterised in that in step 2) in, specifically include：
After marsh gas purifying, it is forced into 3-4 MPa, and carries out pressure-variable adsorption and take off CO2, then at 800-900 DEG C, nickel catalyst work
With under carry out steam conversion reaction, obtain containing CO, CO2、H2And the mixed gas of vapor.
3. hydrogen production process according to claim 2 is it is characterised in that in described steam conversion reaction, and steam/hydrocarbons ratio is 2.5～
3.
4. hydrogen production process according to claim 2 is it is characterised in that described steam conversion reaction is carried out in reburner.
5. hydrogen production process according to claim 1 is it is characterised in that in step 2) in, specifically include：
3-4 MPa will be forced into after marsh gas purifying, and in 600-800 DEG C, with Ni-Al2O3/SiO2Carry out methane as catalyst
CO 2 reforming reaction, obtains containing CO, CO2、H2And the mixed gas of vapor.
6. hydrogen production process according to claim 5 is it is characterised in that after obtaining mixed gas, in step 3) before,
Also include：
Mixed gas are cooled to after 35-45 DEG C and carry out the de- H of pressure-variable adsorption2.
7. hydrogen production process according to claim 6 is it is characterised in that in step 3) in：
In described CO transformationreation, CO used is heated to by the mixed gas that described methane reforming with carbon dioxide produces
300-350℃.
8. hydrogen production process according to claim 7 is it is characterised in that described sulfur bacteria includes thiobacillus thiooxidans or oxidation
Ferrous Thiobacillus.
9. the hydrogen production process according to any one of claim 1-8 is it is characterised in that described biological waste includes：Plant straw
One or more of stalk, excrement of animals, rubbish landfill gas, productive life organic sewage.
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| RU2781559C1 (en) * | 2022-06-10 | 2022-10-13 | Общество с ограниченной ответственностью "Чистая энергия" | Method for hydrogen production by landfill gas conversion method |
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| CN105861083B (en) * | 2016-04-26 | 2018-09-04 | 碧城（上海）新能源科技有限公司 | Synthesize hydrogen fuel and preparation method thereof |
| CN107758617B (en) * | 2016-08-22 | 2020-10-23 | 四川天采科技有限责任公司 | Method for producing hydrogen by using biogas biomass |
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