CN104591083A - Hydrogen preparation method - Google Patents
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- CN104591083A CN104591083A CN201510047475.0A CN201510047475A CN104591083A CN 104591083 A CN104591083 A CN 104591083A CN 201510047475 A CN201510047475 A CN 201510047475A CN 104591083 A CN104591083 A CN 104591083A
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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
Abstract
The invention provides a hydrogen preparation method and belongs to the field of preparation of hydrogen. The method comprises the following steps: (1) carrying out anaerobic fermentation on biological wastes to produce biogas; (2), purifying the biogas, pressurizing to 3-4 MPa and carrying out hydrocarbon conversion reaction to obtain a mixed gas containing CO, CO2, H2 and steam; and (3), carrying out CO conversion reaction on the mixed gas under the conditions of 2.2-2.6 MPa and 300-350 DEG C in the presence of an iron-cobalt catalyst, cooling the temperature of the reacted mixed gas to 35-45 DEG C and carrying out pressure swing adsorption to obtain hydrogen. The hydrogen preparation method has the technical effects of low cost and energy resource conservation; the current situation that the preparation of hydrogen in the prior art is too dependent on petroleum and natural gas is improved; the hydrogen preparation method provides a novel preparation method of industrial hydrogen; while the hydrogen preparation is ensured, the development of the biogas industry is also greatly promoted.
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 minimum gas of known in the world density, and be the minimum material of relative molecular mass, the quality of hydrogen only has 1/14 of air, and 0 DEG C time, a standard atmosphere pressure, the density of hydrogen is 0.0899g/L.Hydrogen is a kind of gas very easily fired, and can burn when aerial volume fraction is 4% to 75%.
As most important industrial gasses and special gas, hydrogen has a wide range of applications in petrochemical complex, electronic industry, metallurgical industry, food-processing, float glass, Minute Organic Synthesis, aerospace etc.Meanwhile, hydrogen is also a kind of desirable secondary energy (secondary energy refer to the energy must produced as sun power, coal etc. by a kind of primary energy).
Generally, hydrogen is very easily combined with oxygen.This characteristic becomes natural reductive 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, in nitrogen protection gas, add hydrogen to remove remaining oxygen.In petrochemical industry, hydrogenation is needed to be refined crude oil by desulfuration and hydrocracking.Another important purposes of hydrogen is the fatty hydrogenation prevented in oleomargarine, edible oil, shampoo, lubricant, household cleaning agent and other products.In addition, because the height of hydrogen is fuel, space industry uses liquid hydrogen as fuel.
In correlation technique, hydrogen feedstock is mainly oil and natural gas, and namely oil and natural gas (containing petroleum naphtha, heavy oil, refinery gas and coke(oven)gas etc.) passes through producing hydrogen from steam conversion.But utilizing oil and natural gas hydrogen manufacturing complicated operation on the one hand, cost is high; On the other hand, under the trend that petroleum resources are day by day in short supply, also there is the technical problem of the wasting of resources in this hydrogen production process.Therefore, providing a kind of new hydrogen preparation method and improve the present situation producing undue dependence fossil energy of plant hydrogen in prior art is the problem that people need solution badly.
In view of this, special proposition the present invention.
Summary of the invention
The object of the present invention is to provide a kind of hydrogen production process, described hydrogen production process is that hydrogen manufacturing is originated with biogas, has the technique effect that cost is low, economize on resources.
In order to realize above-mentioned purpose of the present invention, spy by the following technical solutions:
The invention provides a kind of hydrogen production process, comprise the following steps:
1), to biological waste carry out anaerobically fermenting, produce biogas;
2), by after described marsh gas purifying be forced into 3-4 MPa, and carry out hydrocarbon conversion reaction, obtain containing CO, CO
2, H
2and the mixed gas of water vapour;
3), by described mixed gas under 2.2-2.6 MPa, 300-350 DEG C condition, and carry out CO transformationreation under iron-cobalt series catalyst effect after, the temperature of mixed gas after reaction is down to 35-45 DEG C, and carries out pressure-variable adsorption, obtain hydrogen.
In this hydrogen production process provided by the invention, be that initial feed is carried out anaerobically fermenting and produces biogas with biological waste, the biogas produced passes through purifying treatment, compressor is utilized to boost after sulphur (hydrogen sulfide) contained by removing and portion of water, its pressure is made to reach 3-4 MPa, further to remove moisture.
(steam conversion reaction and methane reforming with carbon dioxide is mainly) in the process of carrying out hydrocarbon conversion reaction, a large amount of methane in biogas with after the water vapour that adds carry out reaction and produce hydrogen and carbon monoxide, and part carbon monoxide and water vapour reaction solution generate hydrogen and carbonic acid gas.In addition, methane also can with carbon dioxide reaction, generate carbon monoxide and hydrogen.Therefore, by hydrocarbon conversion reaction, can obtain containing CO, CO
2, H
2and the mixed gas of water vapour; This mixed gas under 2.2-2.6 MPa, 300-350 DEG C condition, and carries out CO transformationreation under iron-cobalt series catalyst effect, makes carbon monoxide and water reaction, again generates hydrogen and carbonic acid gas; Reacted mixed gas is cooled to 35-45 DEG C, carries out pressure-variable adsorption (mainly removing the gas such as carbon monoxide, carbonic acid gas not participating in reaction), thus obtains highly purified hydrogen.
The preparation method of hydrogen provided by the invention, it achieves the effect of biogas hydrogen manufacturing, biogas is obtained in a large number by fermenting organism fertilizer, (biogas is compared with oil and natural gas for its wide material sources, its preparation cost is cheap, therefore greatly reduce the preparation cost of hydrogen, also a saving day by day exhausted fossil energy simultaneously), by biogas by highly purified hydrogen can be produced after a series of purification and conversion reaction.Therefore, the preparation method of this hydrogen provided by the invention, it has the technique effect that cost is low, economize on resources; The acquisition improving hydrogen in prior art too relies on the present situation of oil and natural gas; A kind of new preparation method provided is produced for plant hydrogen; While having ensured that hydrogen is produced, also greatly promote the development of biogas industry.
Optionally, in step 2) in, described purification specifically comprises: biogas utilization thiobacterium is carried out desulfurization process.
Optionally, in step 2) in, specifically comprise:
After marsh gas purifying, be forced into 3-4 MPa, and carry out pressure-variable adsorption and take off CO2, then in 800-900 DEG C, carry out steam conversion reaction under nickel catalyst effect, obtain containing CO, CO
2, H
2and the mixed gas of water vapour.
Optionally, in described steam conversion reaction, steam/hydrocarbons ratio is 2.5 ~ 3.
Optionally, described steam conversion reaction carries out in converter.
Optionally, in step 2) in, specifically comprise:
3-4 MPa will be forced into after marsh gas purifying, and in 600-800 DEG C, with Ni-Al
2o
3/ SiO
2carry out methane reforming with carbon dioxide as catalyzer, obtain containing CO, CO
2, H
2and the mixed gas of water vapour.
Optionally, after obtaining mixed gas, in step 3) before, also comprise:
Carry out pressure-variable adsorption after mixed gas being cooled to 35-45 DEG C and take off H
2.
Optionally, in step 3) in: in described CO transformationreation, the mixed gas that CO used is produced by described methane reforming with carbon dioxide is heated to 300-350 DEG C.
Optionally, described thiobacterium comprises thiobacillus thiooxidans or thiobacillus ferrooxidant.
Optionally, described biological waste comprises: one or more in straw, excrement of animals, refuse embedded gas, productive life organic sewage.
Compared with prior art, beneficial effect of the present invention is:
(1), with biogas be that hydrogen manufacturing is originated, there is cost low, the effect economized on resources.
(2), biogas obtains in a large number by carrying out anaerobically fermenting to bio-feritlizer, and bio-feritlizer wide material sources, while fermentation produces biogas, also achieve the re-using of bio-feritlizer, and then make the preparation method environmental protection science of whole hydrogen.
(3), in the process utilizing biogas hydrogen manufacturing, the further purifying treatment achieving biogas, is stripped of the composition such as sulphur, carbon contained in biogas; With directly biogas is carried out compared with utilization, environmental protection more.
(4), the method will change hydrogen into by biogas, and then provides a kind of new approach for the utilization of biogas.
Accompanying drawing explanation
In order to be illustrated more clearly in the embodiment of the present invention or technical scheme of the prior art, be briefly described to the accompanying drawing used required in embodiment or description of the prior art below.
Fig. 1 is the preparation flow figure that the invention provides hydrogen production process.
Embodiment
Below in conjunction with embodiment, embodiment of the present invention are described in detail, but it will be understood to those of skill in the art that the following example only for illustration of the present invention, and should not be considered as limiting the scope of the invention.Unreceipted actual conditions person in embodiment, the condition of conveniently conditioned disjunction manufacturers suggestion is carried out.Agents useful for same or the unreceipted production firm person of instrument, be and can buy by commercially available the conventional products obtained.
Please refer to Fig. 1, hydrogen production process provided by the invention, comprises the following steps:
Step 101: carry out anaerobically fermenting to biological waste, 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, CO
2, H
2and the mixed gas of water vapour;
Concrete, in this step, in scavenging process, main purpose removes sulphur contained in biogas and portion of water; After purification, biogas is forced into 3-4 MPa, its principle adopts the saturated steam in cold partition method removing biogas; In the process of hydrocarbon conversion reaction, can following steam conversion reaction be there is:
CH
4+H
2O=CO+3H
2-Q;
Wherein, there is again following reaction in the carbon monoxide that part generates:
CO+H
2O(g)=CO
2+H
2+Q。
Or, in the process of hydrocarbon conversion reaction, by controlling response path and condition, following methane reforming with carbon dioxide can be there is:
CH
4+CO
2=2CO+2H
2。
After whole hydrocarbon conversion reaction terminates, can produce containing CO, CO
2, H
2and the mixed gas of water vapour, wherein, H
2the highest with the content of CO, other two kinds of gas contents are very little.
Step 103: by described mixed gas under 2.2-2.6 MPa, 300-350 DEG C condition, and carry out CO transformationreation under iron-cobalt series catalyst effect after, is down to 35-45 DEG C by the temperature of mixed gas after reaction, and carries out pressure-variable adsorption, obtain hydrogen.
After CO transformationreation, carbon monoxide and additional water vapour are reacted, i.e. CO+H
2o (g)=CO
2+ H
2+ Q.
Obtain the carbonic acid gas containing a large amount of hydrogen and part generation in mixed gas after reaction, carry out pressure swing adsorption decarbonization (carbonic acid gas) after its temperature is reduced to 35-45 DEG C, and then obtain highly purified hydrogen.
As preferably, on the basis of aforesaid method, can also in conjunction with the next item down or all limit:
Described purification specifically comprises carries out desulfurization process by biogas utilization thiobacterium.
Sulphur content in biogas is too high then can etching apparatus and pipeline, reduces its work-ing life, therefore needs to carry out desulfurization (hydrogen sulfide) process to it.Concrete, in the present invention, can adopt biological desulfurization, this method utilizes colorless sulfur bacteria (preferential oxidation sulphur thiobacillus or thiobacillus ferrooxidant), and under the condition of certain temperature, humidity and micro-oxygen, this bacterium can by H
2s is oxidized to simple substance S or H
2sO
3.
Desulphurization mechanism is:
1., H
2namely S gas dissolving is liquid phase by gas phase conversion;
2. the H after, dissolving
2s, by antimicrobial absorbent, is transferred in microbe;
3. the H in microorganism cells, is entered
2s is decomposed by the microorganisms as nutrition, trans-utilization, thus reaches removal H
2the object of S.Its reaction equation is as follows:
2H
2S+3O
2→2H
2SO
3;
2H
2S+O
2→2S+2H
2O。
Most sulfur-oxidizing bacteria all belongs to Thiobacillus.Due to thiobacillus wide material sources, therefore remove H
2during S, bacterium used is without the need to inoculation.In addition, most thiobacillus is autotrophic microorganism, and the surface of anaerobic digestion thing can be supplied to their microcosmic aerobic environments needed for a growth and required nutrition.So, use biological process desulfurization, directly in anaerobic digestor or gas-holder, pass into a certain amount of O
2or air keep certain hour, Measures compare is simple.Adjust suitable temperature, reaction times and air capacity, the H in biogas can be made
2s content is reduced to 50ppm.
In addition, owing to removing CH in biogas
4other outer component mostly is harmful composition or impurity, therefore, need remove respectively.Wherein except hydrogen sulfide, CO
2also be a kind of major impurity, CO
2higher, then gas heating value is lower, according to a class gas in China's natural gas standard " GB17820-1999 " and two class gas technical requirements, need be removed to less than 3.0%.In the present invention, for CO
2, adopt pressure swing adsorption process to remove.
As preferably, in step 2) in, specifically comprise: after marsh gas purifying, be forced into 3-4 MPa, and carry out pressure-variable adsorption and take off CO
2, then in 800-900 DEG C, carry out steam conversion reaction under nickel catalyst, obtain containing CO, CO
2, H
2and the mixed gas of water vapour; Further, in the process of steam conversion reaction, steam/hydrocarbons ratio is 2.5 ~ 3 (mol ratios); And for the ease of realizing steam conversion reaction, this process is preferably carried out in converter.
In aforesaid operations, part water vapour can be deviate from after biogas pressurization, and a certain amount of carbonic acid gas can be deviate from the process of pressure-variable adsorption, the biogas after purification and water vapour carry out steam conversion reaction, and in 800-900 DEG C, generate containing CO, CO under the condition of nickel catalyst
2, H
2and the mixed gas of water vapour.By exploration discovery, in the process of steam conversion reaction, steam/hydrocarbons ratio (mole) is set as that 2.5 ~ 3 are beneficial to and obtain hydrogen in a large number.
As another preferred technical scheme, in step 2) in, specifically comprise:
3-4 MPa will be forced into after marsh gas purifying, and in 600-800 DEG C, with Ni-Al
2o
3/ SiO
2carry out methane reforming with carbon dioxide as catalyzer, obtain containing CO, CO
2, H
2and the mixed gas of water vapour.
This process implementation methane reforming with carbon dioxide, methane and carbonic acid gas is made to carry out reacting the mixed gas produced containing a large amount of hydrogen and part carbon monoxide, containing a large amount of hydrogen in this mixed gas, for the ease of collecting product, after this mixed gas is cooled to 35-45 DEG C, preferably carries out pressure-variable adsorption takes off H
2after carry out step 3 again.Simultaneously, in described CO transformationreation, the mixed gas that CO used is produced by described methane reforming with carbon dioxide is heated to 300-350 DEG C, 600-800 DEG C can be reached in the temperature of the mixed gas of methane reforming with carbon dioxide generation, and CO transformationreation needs the temperature of reaction of 300-350 DEG C, and in the process removing hydrogen, the mixed gas generated needs to lower the temperature, therefore, in order to realize making full use of of heat, before not removing hydrogen (cooling), mixed gas is utilized to carry out heat exchange by needing the CO participating in CO transformationreation, be heated to 300-350 DEG C.
Further, bio-feritlizer can comprise one or more in straw, excrement of animals, refuse embedded gas, productive life organic sewage.
To sum up, this hydrogen production process provided by the invention, be that initial feed is carried out anaerobically fermenting and produces biogas with biological waste, the biogas produced passes through purifying treatment, compressor is utilized to boost after sulphur (hydrogen sulfide) contained by removing and portion of water, its pressure is made to reach 3-4 MPa, further to remove moisture.
(steam conversion reaction and methane reforming with carbon dioxide is mainly) in the process of carrying out hydrocarbon conversion reaction, a large amount of methane in biogas with after the water vapour that adds carry out reaction and produce hydrogen and carbon monoxide, and part carbon monoxide and water vapour reaction solution generate hydrogen and carbonic acid gas.In addition, methane also can with carbon dioxide reaction, generate carbon monoxide and hydrogen.Therefore, by hydrocarbon conversion reaction, can obtain containing CO, CO
2, H
2and the mixed gas of water vapour; This mixed gas under 2.2-2.6 MPa, 300-350 DEG C condition, and carries out CO transformationreation under the effect of iron-cobalt series catalyst, makes carbon monoxide and water reaction, again generates hydrogen and carbonic acid gas; Reacted mixed gas is cooled to 35-45 DEG C, carries out pressure-variable adsorption (mainly removing the gas such as carbon monoxide, carbonic acid gas not participating in reaction), thus obtains highly purified hydrogen.
The preparation method of hydrogen provided by the invention, it achieves the effect of biogas hydrogen manufacturing, and biogas is obtained in a large number by fermenting organism fertilizer, its wide material sources, by biogas by producing highly purified hydrogen after a series of purification and conversion reaction.Therefore, the preparation method of this hydrogen provided by the invention, it has the technique effect that cost is low, economize on resources; The acquisition improving hydrogen in prior art too relies on the present situation of oil and natural gas; A kind of new preparation method provided is produced for plant hydrogen; While having ensured that hydrogen is produced, also greatly promote the development of biogas industry.
Next, in conjunction with above content, following specific embodiment has been enumerated to hydrogen production process of the present invention and its preparation method:
Embodiment 1
S11: carry out anaerobically fermenting to biological waste, produces biogas;
Biological waste comprises: straw, excrement of animals, refuse embedded gas and productive life organic sewage.
S12: utilize compressor that biogas is boosted to 3.5 MPas after adopting thiobacillus thiooxidans to carry out desulfurization process to biogas;
S13: the biogas after boosting is carried out pressure-variable adsorption under normal temperature and takes off CO
2, then in 850 DEG C, in converter, carry out steam conversion reaction under nickel catalyst, obtain containing CO, CO
2, H
2and the mixed gas of water vapour;
Wherein, in the process of steam conversion reaction, steam/hydrocarbons ratio is 2.5 ~ 3 (moles).
Chemical reaction occurs in this step is:
CH
4+ H
2o=CO+3H
2-Q, or CO+H
2o (g)=CO
2+ H
2+ Q.
S14: by described mixed gas under 2.4 MPas, 320 DEG C of conditions, and carry out CO transformationreation under iron-cobalt series catalyst effect after, is down to 40 DEG C by the temperature of mixed gas after reaction, and carries out pressure-variable adsorption, obtain the hydrogen that purity is greater than 99.9%.
Chemical reaction occurs in this step is: CO+H
2o (g)=CO
2+ H
2+ Q.
In the present embodiment, the main emergence work of first paragraph pressure-variable adsorption (in S13), to improve fire damp purity; Second segment pressure-variable adsorption (in S14) main purpose is by trace amounts of CO, CO in mixed gas
2deng impurity removal, to realize hydrogen purification effect.
Embodiment 2
S21: carry out anaerobically fermenting to biological waste, produces biogas;
Biological waste comprises: straw, excrement of animals, refuse embedded gas and productive life organic sewage.
S22: utilize compressor that biogas is boosted to 3.5 MPas after adopting thiobacillus thiooxidans to carry out desulfurization process to biogas;
S23: by boosting after biogas in 700 DEG C, with Ni-Al
2o
3/ SiO
2carry out methane reforming with carbon dioxide as catalyzer, obtain containing CO, CO
2, H
2and the mixed gas of water vapour;
The chemical reaction occurred in this step is: CH
4+ CO
2=2CO+2H
2.
S24: by described mixed gas under 2.4 MPas, 320 DEG C of conditions, and carry out CO transformationreation under iron-cobalt series catalyst effect after, is down to 40 DEG C by the temperature of mixed gas after reaction, and carries out pressure-variable adsorption, obtain the hydrogen that purity is greater than 99.9%.
The chemical reaction occurred in this step is consistent with the chemical reaction implemented in 1 in step S14.
Although illustrate and describe the present invention with specific embodiment, however it will be appreciated that can to make when not deviating from the spirit and scope of the present invention many other change and amendment.Therefore, this means to comprise all such changes and modifications belonged in the scope of the invention in the following claims.
Claims (10)
1. a hydrogen production process, is characterized in that, comprises the following steps:
1), to biological waste carry out anaerobically fermenting, produce biogas;
2), by after described marsh gas purifying be forced into 3-4 MPa, and carry out hydrocarbon conversion reaction, obtain containing CO, CO
2, H
2and the mixed gas of water vapour;
3), by described mixed gas under 2.2-2.6 MPa, 300-350 DEG C condition, and carry out CO transformationreation under iron-cobalt series catalyst effect after, the temperature of mixed gas after reaction is down to 35-45 DEG C, and carries out pressure-variable adsorption, obtain hydrogen.
2. hydrogen production process according to claim 1, is characterized in that, in step 2) in, described purification specifically comprises:
Biogas utilization thiobacterium is carried out desulfurization process.
3. hydrogen production process according to claim 1, is characterized in that, in step 2) in, specifically comprise:
After marsh gas purifying, be forced into 3-4 MPa, and carry out pressure-variable adsorption and take off CO
2, then in 800-900 DEG C, carry out steam conversion reaction under nickel catalyst effect, obtain containing CO, CO
2, H
2and the mixed gas of water vapour.
4. hydrogen production process according to claim 3, is characterized in that, in described steam conversion reaction, steam/hydrocarbons ratio is 2.5 ~ 3.
5. hydrogen production process according to claim 3, is characterized in that, described steam conversion reaction carries out in converter.
6. hydrogen production process according to claim 1, is characterized in that, in step 2) in, specifically comprise:
3-4 MPa will be forced into after marsh gas purifying, and in 600-800 DEG C, with Ni-Al
2o
3/ SiO
2carry out methane reforming with carbon dioxide as catalyzer, obtain containing CO, CO
2, H
2and the mixed gas of water vapour.
7. hydrogen production process according to claim 6, is characterized in that, after obtaining mixed gas, in step 3) before, also comprise:
Carry out pressure-variable adsorption after mixed gas being cooled to 35-45 DEG C and take off H
2.
8. hydrogen production process according to claim 7, is characterized in that, in step 3) in:
In described CO transformationreation, the mixed gas that CO used is produced by described methane reforming with carbon dioxide is heated to 300-350 DEG C.
9. hydrogen production process according to claim 2, is characterized in that, described thiobacterium comprises thiobacillus thiooxidans or thiobacillus ferrooxidant.
10. the hydrogen production process according to any one of claim 1-8, is characterized in that, described biological waste comprises: one or more in straw, excrement of animals, refuse embedded gas, productive life organic sewage.
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CN112922740A (en) * | 2021-02-08 | 2021-06-08 | 山东大学 | Cold, heat, electricity and hydrogen combined supply system driven by waste heat of engine and working method |
CN112922740B (en) * | 2021-02-08 | 2022-06-28 | 山东大学 | Engine waste heat driven cold-heat electricity-hydrogen combined supply system and working method |
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