CN107539949A - The process unit and process of a kind of hydrogen production of chemical chain - Google Patents
The process unit and process of a kind of hydrogen production of chemical chain Download PDFInfo
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- CN107539949A CN107539949A CN201610457306.9A CN201610457306A CN107539949A CN 107539949 A CN107539949 A CN 107539949A CN 201610457306 A CN201610457306 A CN 201610457306A CN 107539949 A CN107539949 A CN 107539949A
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Abstract
The present invention provides a kind of process unit and method of hydrogen production of chemical chain, the process unit includes two fuel reactors, vapour reactor and air reactor, the gas outlet of fuel reactor I is connected with the air inlet of fuel reactor II, the oxygen carrier import of the oxygen carrier outlet connection vapour reactor of two fuel reactors, vapour reactor are connected with air reactor.Using above-mentioned process unit, it is 750 ~ 800 DEG C to control the reaction temperature in fuel reactor I, and the reaction temperature in fuel reactor II is 650 ~ 750 DEG C, reaction of the fuel gas in fuel reactor is divided into two sections, compared with the reaction temperature of general technology condition（850~950℃）Substantially reduce, reduce energy expenditure, and make conversion of the fuel gas to carbon dioxide more thorough, improve CH4Conversion ratio and CO2Selectivity.
Description
Technical field
The present invention relates to a kind of new device of hydrogen production of chemical chain, belong to the technology in hydrogen production of chemical chain field.
Background technology
The domestic annual hydrogen usages of the t of hydrogen about 50,000,000 that the whole world consumes every year at present occupy world head more than 10,000,000 t
Position, wherein more than 90% is used to synthesize ammonia, synthesizing methanol and petroleum refining hydrogenation.Hydrogen is the important process raw material of refinery, extensively
Applied to processes such as gasoline, diesel oil, residual hydrogenations, for adjusting product hydrogen-carbon ratio and desulfurization, denitrogenation.In the world,
Crude oil heaviness, in poor quality are increasingly severe, for large-scale refinery, be hydrocracked in terms of heavy, crude oil with poor quality processing and
Hydroprocessing technique route is advantageous to raw material " eating dry bleed ", benefit being better than coking route, with oil quality upgrading not
Disconnected to accelerate, refinery hydrogen demand quickly increases.
Natural gas hydrogen preparation pollutes less, American-European advanced oil refinery company is mostly using natural gas as waste hydrogen.Production
1000m3Hydrogen, the comprehensive energy consumption of its state-of-the-art technology is 11.30GJ ~ 12.56GJ, and the design objective of domestic new equipment has also dropped
To 13.66GJ.It is mainly industrially vapor reforming SRM, partial oxidation POM and self-heating by the technology of natural gas hydrogen making
Reform tri- kinds of ATR.Possessing the company of natural gas hydrogen preparation technology in the world at present mainly has De Xinibu Technip of France, moral
The strange Lurgi in Shandong, Lin De Linde of state and Wood Uhde, the Foster Wheeler Foster Wheeler of Britain and the Top of Denmark
Rope Tops e.Vapor reforming method refers to make the hydro carbons such as methane react with vapor under catalyst presence and hot conditions
Synthesis gas is generated, to prevent catalyst poisoning, raw natural gas need to carry out desulfurization pretreatment to the mass fraction of sulphur and be less than 10-7,
Then synthesis gas synthesis gas is prepared by reforming reaction, then CO is further converted to hydrogen and CO through water gas shift reaction2,
Finally by CO2Hydrogen is obtained by pressure-variable adsorption (PSA) removing.
Hydrogen production of chemical chain is the hydrogen producing technology of most industrial prospect, and it is that a kind of hydrogen manufacturing takes into account collecting carbonic anhydride
New technology.Natural gas steam reforming reaction is divided into three steps and carried out by it, obtains hydrogen and titanium dioxide in two reactors respectively
Carbon, it is not necessary to which gas separates, and has the advantages of hydrogen production efficiency is high, hydrogen purity is high, carbon dioxide zero discharge, meets very much now
And the demand for development of following hydrogen producing technology.By the research and development of more than ten years, the U.S. has built up first industrialization demonstration plant of the whole world, from
Industrial applications are more and more nearer.Consider the energy, resource and the aspect of environment three, natural gas is as the fuel of hydrogen production of chemical chain
Optimal selection, but need to be improved in economy.
Hydrogen production of chemical chain includes fuel reactor, vapour reactor and air reactor.Domestic Chinese Academy of Sciences Guangzhou energy institute
Research was carried out to chemical chain biomass preparing synthetic gas with Southeast China University, they use fluidized-bed reactor at fuel reactor.Stream
There is the problem of methane can not be completely converted into carbon dioxide in fluidized bed reactor, that is, have substantial amounts of carbon monoxide to produce.External Russia
The fuel reactor and vapour reactor of the hydrogen production of chemical chain of Hai E state universities Fan Liangshi professors all use moving bed, and air is anti-
Device is answered to use riser, three reactors are together in series.All it is high temperature because hydrogen production of chemical chain includes three cascade reactions altogether
850 ~ 950 DEG C of reaction, high temperature can accelerate reaction rate, but high temperature can propose harshness to reactor material, pipeline and valve
It is required that if reducing reaction temperature, methane cannot be completely converted into carbon dioxide, urgently to be resolved hurrily be asked so this is one
Topic.
The content of the invention
To solve the problem of reaction temperature is higher in hydrogen production of chemical chain technique in the prior art, higher to reactor requirement,
The present invention intends providing a kind of new hydrogen production of chemical chain process unit and method, and by increasing a fuel reactor, fuel is existed
Reaction in fuel reactor is divided into two-part, in the hope of reducing reaction temperature, reaches reaction and requires.
The technical purpose of the present invention is achieved through the following technical solutions：
A kind of process unit of hydrogen production of chemical chain, it is anti-that the process unit includes fuel reactor I, fuel reactor II, steam
Answer device and air reactor；The lower end of fuel reactor I and fuel reactor II is respectively provided with oxygen carrier outlet, with vapour reactor
Oxygen carrier import connection, vapour reactor oxygen carrier outlet is connected with the oxygen carrier import of air reactor, air reaction
The oxygen carrier import of device connects the oxygen carrier import of fuel reactor I and fuel reactor II respectively；It is each in the process unit
Reactor is respectively provided with gas feed and gas vent, and the gas vent of fuel reactor I connects with the air inlet of fuel reactor II
Connect.
Further, the fuel reactor I, fuel reactor II and vapour reactor are counter-flow moving bed reaction
Device, air reactor are riser reactor.
Further, when the size of all reactors can be according to air speed, gas flow rate and contact in device of the invention
Between calculated, preferably 0.2 ~ 5m3, more preferably 0.5 ~ 3m3。
Further, for each reactor using the stainless steel material for being adapted to pyroreaction, temperature resistant range is room temperature ~ 1000
℃。
Another technical purpose of the present invention is to provide the process using process unit progress hydrogen production of chemical chain,
Carried out using following steps：Fuel gas is passed through fuel reactor I by air inlet, the reaction temperature in fuel reactor I is 750
~ 800 DEG C, fuel gas and oxygen carrier precursor reactant generate the incoming fuel reactor II of gas I, and the reaction temperature in fuel reactor II is
650 ~ 750 DEG C, generation gas I produces generation gas II with oxygen carrier precursor reactant, and generation gas II is carried out into condensation collection；Fuel reactor I
With the oxygen carrier outflow reactor in fuel reactor II, the air inlet for passing through vapour reactor into vapour reactor, vapor
Mouth enters, and produces generation gas III with oxygen carrier precursor reactant, is collected in outlet, reacted oxygen carrier air inlet reactor,
Air is entered by the import of air reactor, and with oxygen carrier precursor reactant, generation gas IV is discharged by outlet, the oxygen carrier after being oxidized
Separately flow into fuel reactor I and fuel reactor II, circular response.
Further, the reaction temperature in the vapour reactor is 600 ~ 850 DEG C, the reaction temperature in air reactor
For 600 ~ 800 DEG C.
Further, the fuel gas is methane.
Further, it will be apparent to a skilled person that heretofore described oxygen carrier can use chemical chain system
The oxygen carrier commonly used in hydrogen field, wherein it is preferred that active component is Fe2O3, carrier Al2O3Or MgO oxygen carrier, can be ball
Type, powder or graininess, preferably ball-type.
In the process unit and process of the present invention, reaction of the fuel gas in fuel reactor is divided into two sections
Formula, wherein in fuel reactor I, fuel gas reaction temperature is 750 ~ 800 DEG C, and at a temperature of this, fuel gas does not have complete oxidation,
Generation gas I includes fuel gas, carbon monoxide, carbon dioxide.In fuel reactor II, reaction temperature is down to 650 ~ 750 DEG C,
Generate gas I can complete oxidation generation generation gas II, generation gas II includes carbon dioxide and water vapour, then condensed dehydration can richness
Collect carbon dioxide.
Compared with prior art, the invention has the advantages that：
1st, process unit of the invention sets two fuel reactors, and the reaction that fuel gas is generated to carbon dioxide is divided into two-part
Reaction, two-stage reaction can use 750 ~ 800 DEG C and 650 ~ 750 DEG C of relatively low reaction temperatures, compared with the reaction temperature of general technology condition
Degree（850~950℃）Substantially reduce, reduce energy expenditure, and reactor and pipe material range of choice are also wider.
2nd, the two-part reaction of fuel reactor of the present invention makes conversion of the fuel gas to carbon dioxide more thorough, effectively solution
Determine fuel（Such as methane）The problem of carbon dioxide can not be fully converted into.
3rd, formed counter-flow moving bed in fuel reactor, fuel gas enters oxygen carrier bed at reactor lower ending opening
In, walk from the bottom up, oxygen carrier is walked from top to bottom, can so be made oxygen carrier and methane time of contact longer, is advantageous to improve
Methane conversion and carbon dioxide selectivity.
4th, the cost of device is reduced, improves economy.
5th, the level of integrated system it is high, it is simple in construction, be easily achieved industrialization.
Brief description of the drawings
The schematic device of the hydrogen production of chemical chain of Fig. 1 present invention；
Wherein 11. fuel reactors I, 12. fuel reactors II, 2. vapour reactor, 3. air reactors.
Embodiment
Following non-limiting examples can make one of ordinary skill in the art be more fully understood the present invention, but not with
Any mode limits the present invention.
Embodiment 1
As shown in figure 1, the process unit of the hydrogen production of chemical chain for the present invention, including fuel reactor I 11, fuel reactor II
12nd, vapour reactor 2 and air reactor 3；The lower end of fuel reactor I 11 and fuel reactor II 12 is respectively provided with oxygen carrier and gone out
Mouthful, it is connected with the oxygen carrier import of vapour reactor 2, the oxygen carrier outlet of vapour reactor 2 and the oxygen carrier of air reactor 3
Import connects, and the oxygen carrier import of air reactor 3 connects the oxygen carrier of fuel reactor I 11 and fuel reactor II 12 respectively
Import；Each reactor is respectively provided with gas feed and gas vent in the process unit, the gas vent of fuel reactor I 11 with
The air inlet connection of fuel reactor II 12.The fuel reactor I 11, fuel reactor II 12 and vapour reactor 2 are
Counter-flow moving bed reactor, air reactor 3 are riser reactor.
Embodiment 2
The method for carrying out hydrogen production of chemical chain using the process unit of embodiment 1, wherein oxygen carrier is Fe2O3/Al2O3, take 20g points
Not Zhuan Ru fuel reactor I 11 and fuel reactor II 12, fuel gas is methane.Concretely comprise the following steps：
（1）Methane is passed through with 10mL/min flow velocity from the lower end of fuel reactor I 11, it is anti-to enter fuel by air distribution plate
Answer in device I 11, it is 800 DEG C to control its reaction temperature, normal pressure, and methane produces generation gas I with oxygen carrier precursor reactant, and generation gas I includes
Methane, carbon monoxide, carbon dioxide.
（2）Generation gas I flows out from upper left-hand perforate, enters from perforate on the right side of the lower end of fuel reactor II 12, control
Reaction temperature processed is 750 DEG C, normal pressure, and generation gas I and oxygen carrier precursor reactant produce generation gas II, generation gas II include carbon dioxide and
Water vapour, flowed out in being open from upper end left side, then condensed dehydration can carbon dioxide-enriched.
（3）After completion of the reaction, the oxygen carrier of fuel reactor I 11 and fuel reactor II 12 flows out two reactors, passes through
Inclined tube converges, and is flowed into from the upper end of vapour reactor 2, and vapor enters from lower end side opening, steam rates 150mL/
Min, it is 800 DEG C to control its reaction temperature, and with oxygen carrier precursor reactant, oxygen carrier is carried out into preliminary oxidation, produces generation gas III（Hydrogen
Gas）, it is collected in upper side outlet.
（4）Oxygen carrier in vapour reactor 2 outflow reactor under gravity, is entered by the bottom of air reactor 3
Enter, it is 800 DEG C to control reactor temperature, and air is passed through from bottom sides entrance, flow velocity 10mL/min, in air push
Under, oxygen carrier moves up, and and air reaction, by exhaustive oxidation, oxygen carrier flows out from upper end outlet, and it is anti-to be further separated into fuel
Answer in device I 11 and fuel reactor II 12 and carry out circular response, tail gas caused by reaction is discharged into air.
Embodiment 3
Other steps with embodiment 2, unlike by step（1）The reaction temperature control of fuel reactor I 11 is 750 DEG C.
Embodiment 4
Other steps with embodiment 2, unlike by step（2）The reaction temperature control of fuel reactor II 12 is 700 DEG C.
Embodiment 5
Other steps with embodiment 2, unlike by step（2）The reaction temperature control of fuel reactor II 12 is 650 DEG C.
Embodiment 6
Other steps with embodiment 2, unlike by step（1）The reaction temperature control of fuel reactor I 11 is 750 DEG C,
By step（2）The reaction temperature control of fuel reactor II 12 is 700 DEG C.
Embodiment 7
Other steps with embodiment 2, unlike by step（1）The reaction temperature control of fuel reactor I 11 is 750 DEG C,
By step（2）The reaction temperature control of fuel reactor II 12 is 650 DEG C.
Comparative example 1
Reacted on fixed fluidized-bed reactor, with Fe2O3/Al2O3For oxygen carrier, methane is fuel gas.Take 50g
Fe2O3/Al2O3It is fitted into fuel reactor, methane is entered in fuel reactor with 50mL/min flow velocity, fuel reactor
Temperature is 800 DEG C, normal pressure, after reacting 10min, stops methane feed, leads to nitrogen purging 10min.Then water flowing steam, flow are
50mL/min, temperature is 800 DEG C, after reacting 10min, leads to nitrogen purging 10min.Then blowing air, flow 50mL/min, temperature
Spend for 800 DEG C, after reacting 10min, lead to nitrogen purging 10min.
Using Agilent 7820A type gas-chromatography on-line analyses, 5A molecular sieve columns and Porapak Q posts, TCD detections.Respectively
CH in embodiment and comparative example4Conversion ratio and CO2Selectivity is shown in Table 1.
Table 1.
* methane conversion and carbon dioxide selectivity are all the average value after circulating 100 times.
Claims (8)
1. a kind of process unit of hydrogen production of chemical chain, the process unit includes fuel reactor I（11）, fuel reactor II
（12）, vapour reactor（2）And air reactor（3）；Fuel reactor I（11）With fuel reactor II（12）Lower end be all provided with
Oxygen carrier outlet is put, with vapour reactor（2）Oxygen carrier import connection, vapour reactor（2）Oxygen carrier outlet and air
Reactor（3）Oxygen carrier import connection, air reactor（3）Oxygen carrier import connect fuel reactor I respectively（11）With
Fuel reactor II（12）Oxygen carrier import；Each reactor is respectively provided with gas feed and gas vent in the process unit,
Fuel reactor I（11）Gas vent and fuel reactor II（12）Air inlet connection.
2. process unit according to claim 1, it is characterised in that the fuel reactor I（11）, fuel reactor II
（12）And vapour reactor（2）It is counter-flow moving bed reactor, air reactor（3）For riser reactor.
3. process unit according to claim 1, it is characterised in that the volume of each reactor is 0.2 ~ 5m3, preferably 0.5
~3m3。
4. process unit according to claim 1, it is characterised in that each reactor is stainless steel material, and temperature resistant range is
Room temperature ~ 1000 DEG C.
5. the process of hydrogen production of chemical chain is carried out using process unit described in claim 1 ~ 4 any one, it is characterised in that
Carried out using following steps：Fuel gas is passed through fuel reactor I by air inlet（11）, fuel reactor I（11）Interior reaction
Temperature is 750 ~ 800 DEG C, fuel gas and oxygen carrier precursor reactant, generates the incoming fuel reactor II of gas I（12）, fuel reactor II
（12）Interior reaction temperature is 650 ~ 750 DEG C, and generation gas I produces generation gas II with oxygen carrier precursor reactant, generation gas II is carried out cold
It is solidifying to collect；Fuel reactor I（11）With fuel reactor II（12）Interior oxygen carrier outflow reactor, into vapour reactor
（2）, vapor passes through vapour reactor（2）Air inlet enter, with oxygen carrier precursor reactant produce generation gas III, received in outlet
Collection, reacted oxygen carrier air inlet reactor（3）, air passes through air reactor（3）Import enter, it is anti-with oxygen carrier
Should, generation gas IV is discharged by outlet, and the oxygen carrier after being oxidized separately flows into fuel reactor I（11）With fuel reactor II
（12）, carry out circular response.
6. process according to claim 5, it is characterised in that the vapour reactor（2）Interior reaction temperature is
600 ~ 850 DEG C, air reactor（3）Interior reaction temperature is 600 ~ 800 DEG C.
7. process according to claim 5, it is characterised in that the active component of the oxygen carrier is Fe2O3, carrier
For Al2O3Or MgO.
8. process according to claim 5, it is characterised in that the fuel gas is methane.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
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| CN201610457306.9A CN107539949B (en) | 2016-06-23 | 2016-06-23 | Process device and process method for chemical looping hydrogen production |
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| CN201610457306.9A CN107539949B (en) | 2016-06-23 | 2016-06-23 | Process device and process method for chemical looping hydrogen production |
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| CN107539949B CN107539949B (en) | 2020-10-16 |
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| CN111217380A (en) * | 2018-11-26 | 2020-06-02 | 中国科学院大连化学物理研究所 | Method for synthesizing ammonia |
| CN111655609A (en) * | 2018-02-24 | 2020-09-11 | 北京联力源科技有限公司 | Fuel chemical looping hydrogen production system and method |
| CN114702332A (en) * | 2022-03-23 | 2022-07-05 | 山东科技大学 | Red mud ceramic ball oxygen carrier and preparation method and application thereof |
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Cited By (4)
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| CN114702332A (en) * | 2022-03-23 | 2022-07-05 | 山东科技大学 | Red mud ceramic ball oxygen carrier and preparation method and application thereof |
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| Publication number | Publication date |
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| CN107539949B (en) | 2020-10-16 |
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