CN102225744B - Method and device for preparing hydrogen and separating CO2 based on Fe2O3-NiO mixture - Google Patents

Method and device for preparing hydrogen and separating CO2 based on Fe2O3-NiO mixture Download PDF

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CN102225744B
CN102225744B CN2011100838119A CN201110083811A CN102225744B CN 102225744 B CN102225744 B CN 102225744B CN 2011100838119 A CN2011100838119 A CN 2011100838119A CN 201110083811 A CN201110083811 A CN 201110083811A CN 102225744 B CN102225744 B CN 102225744B
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reactor
air
fuel
nio
water vapour
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CN102225744A (en
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向文国
陈时熠
王东
薛志鹏
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Southeast University
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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
    • Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
    • Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
    • Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
    • 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
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis

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Abstract

The invention discloses a method and a device for preparing hydrogen and separating CO2 based on Fe2O3-NiO mixture. The method comprises the following steps that: Fe2O3 and NiO are introduced to a fuel reactor and reduced by fuel gases to obtain gas products of CO2 and steam, and the gas products are condensed to separate water and obtain pure CO2, wherein the solid products in the fuel reactor are FeO, Fe and Ni; FeO, Fe and Ni are introduced into a steam reactor fluidized bed through an overflowing tank; FeO and Fe react with steam to generate hydrogen and Fe3O4, Ni does not react with steam, gas-solid product is separated by a cyclone separator, and the gas product is condensed to separate water and obtain pure hydrogen; and unreacted Ni and the solid product Fe3O4 in the steam reactor fluidized bed are introduced into an air reactor fluidized bed, oxidation reaction is carried out on Fe3O4 and Ni and air to generate Fe2O3 and NiO, simultaneously heat is released, and Fe2O3 and NiO are returned to the fuel reactor for recycling.

Description

A kind of based on Fe 2O 3-NiO mixture hydrogen making and separation of C O 2Method and device thereof
Technical field
The present invention relates to a kind of method and apparatus that utilizes the fuel hydrogen making, particularly relate to a kind of based on Fe 2O 3-NiO mixture hydrogen making and separation of C O 2Method and apparatus.
Background technology
The high efficiency of energy clean utilization is to realize one of sustainable development strategies of the energy.Hydrogen is as clean energy, and in the conversion process of energy, following product is water, can really realize zero release of pollutant.Hydrogen is combustion power generation, heat supply directly, perhaps is converted into electric energy by fuel cell.Along with the whole world " Oil Safety ", " Greenhouse effect " and " environment protection " problem are increasingly serious; in order to reduce the interdependency to oil; strengthen the capture of carbonic acid gas and seal up for safekeeping; reduce greenhouse gases to the impact of environment; in the sustainable energy system in future, hydrogen is expected to become important energy carrier.But regrettably the hydrogen of occurring in nature is to exist with the chemical combination attitude mostly, must be obtained by the conversion of the carbon containing primary energy source such as other primary energy source such as Sweet natural gas, coal, biomass as secondary energy.China be one take coal as main energy consumption big country, in the selection of the energy, will play the part of very important role take coal as main fossil oil.Fossil energy can give off a large amount of CO in the process of Hydrogen Energy conversion 2, the Greenhouse effect that cause thus cause serious destruction to ecotope.Because the CO of the hydrogen production process discharging take fossil oil as the basis 2Amount quite huge, hydrogen will disappear as the advantage of eco-friendly clean energy.Therefore, in the fossil oil hydrogen production process, effective separation also captures CO 2Become one of key that realizes the hydrogen manufacturing of fossil oil cleaning.
Summary of the invention
The invention provides a kind of based on Fe 2O 3-NiO mixture hydrogen making and separation of C O 2Method and device thereof, the present invention can effective separation when utilizing the fuel hydrogen making CO 2, have the advantage that reduces greenhouse gas emission.
Technical scheme of the present invention is as follows:
A kind of based on Fe 2O 3-NiO mixture hydrogen making and separation of C O 2Method, simple substance Fe and Ni are placed in the air reactor fluidized-bed, the temperature of air reactor fluidized-bed is controlled at 950 ~ 1000 ℃, passes into air in air reactor fluidized-bed lower end, the air reactor bottom compartment is in bubbling fluidization; Simple substance Fe and Ni oxidation by air are Fe 2O 3With NiO; Fe 2O 3Enter the air reactor riser tube with NiO through the air reactor transition section, to the air cyclonic separator, the gas-solid two-phase is separated through the air cyclonic separator by air-lift unit; Gas after the separation is oxygen debt air, and oxygen debt air is overflowed from the outlet of air cyclonic separator; Solid after the separation is Fe 2O 3With NiO, Fe 2O 3Enter fuel reactor with NiO through tremie pipe and the second overflow groove, the temperature of fuel reactor is controlled at 900 ~ 950 ℃; The fuel reactor lower end passes into fuel gas, and the fuel reactor main body is in the moving-bed state; Fe 2O 3Fall Fe from the fuel reactor top with NiO 2O 3The reductibility fuel gas that is risen is reduced to FeO and Fe; NiO is reduced to Ni; The gas of fuel reactor top exit only is CO 2With water vapour, behind water wherein, obtain pure CO 2The FeO of reduction-state, Fe and Ni enter the fuel reactor bottom compartment through the fuel reactor transition section; Fuel reactor bottom compartment sectional area is less than the fuel reactor main body and be in bubbling fluidization; The FeO of reduction-state, Fe and Ni enter water vapour reactor fluidisation bed in the fuel reactor bottom compartment through the first overflow groove; Pass into water vapour in water vapour reactor fluidisation bed lower end, water vapour reactor bottom compartment is in bubbling fluidization, and the temperature of water vapour reactor fluidisation bed is controlled at 750 ~ 850 ℃; FeO, Fe and water vapour reaction generate hydrogen, and solid product is Fe 3O 4Ni and water vapour can not react, Ni and solid product Fe 3O 4Be promoted to the hydrogen cyclonic separator through water vapour reactor transition section and water vapour reactor riser by water vapour and hydrogen, gas-solid separates through the hydrogen cyclonic separator, hydrogen and water vapour are overflowed from the outlet of hydrogen cyclonic separator, behind water wherein, obtain pure hydrogen; Solid Fe after the separation 3O 4Enter the air reactor fluidized-bed with Ni through tremie pipe and the 3rd overflow groove, again be oxidized to Fe by air 2O 3With NiO, the while releases heat; Fe 2O 3Realize recycle with NiO.
Device technique scheme of the present invention is as follows:
A kind of for above-mentioned Fe 2O 3-NiO mixture hydrogen making and separation of C O 2The device of method, formed by water vapour reactor fluidisation bed, fuel reactor and air reactor fluidized-bed; Water vapour reactor fluidisation bed is comprised of water vapour reactor bottom compartment, water vapour reactor transition section and water vapour reactor riser; The water vapour reactor riser links to each other with water vapour reactor bottom compartment by water vapour reactor transition section, the upper end of water vapour reactor riser is connected with the hydrogen cyclonic separator, the hydrogen cyclonic separator links to each other with the 3rd overflow groove by tremie pipe, and the 3rd overflow groove is connected with the air reactor fluidized-bed; The air reactor fluidized-bed is comprised of air reactor bottom compartment, air reactor transition section, air reactor riser tube, air cyclonic separator and tremie pipe, the air reactor bottom compartment links to each other with the air reactor riser tube by the air reactor transition section, the top of air reactor riser tube links to each other with the air cyclonic separator, described the 3rd overflow groove is connected with air reactor bottom compartment in the air reactor fluidized-bed, and the air cyclonic separator is connected with fuel reactor by tremie pipe and the second overflow groove; Fuel reactor is comprised of fuel reactor main body, fuel reactor transition section, fuel reactor bottom compartment and the first overflow groove, the fuel reactor main body links to each other with the fuel reactor bottom compartment by the fuel reactor transition section, the fuel reactor bottom compartment links to each other with the first overflow groove, the first overflow groove links to each other with water vapour reactor bottom compartment, and described air cyclonic separator is connected with the top of the fuel reactor main body of fuel reactor by tremie pipe and the second overflow groove.
Compared with prior art, the present invention has following advantage:
(1) before understanding apparatus of the present invention, at first relates to Fe 2O 3Reduction process with NiO:
Fe 2O 3The reduction order be:
Fe 2O 3→ Fe 3O 4→ FeO → Fe is higher than 570 ℃
Fe 2O 3→ FeO → Fe is lower than 570 ℃
The reduction order of NiO only is:
NiO→Ni
Fe 2O 3Be converted into Fe 3O 4Process as follows:
3Fe 2O 3+H 2→2Fe 3O 4+H 2O
3Fe 2O 3+CO→2Fe 3O 4+CO 2
12Fe 2O 3+CH 4→8Fe 3O 4+CO 2+2H 2
The process that NiO is converted into Ni is as follows:
NiO+H 2→Ni+H 2O
NiO+CO→Ni+CO 2
4NiO+CH 4→4Ni+CO 2+2H 2O
According to chemical reaction thermodynamic principles, Fe 2O 3Be converted into Fe 3O 4Be converted into the process of Ni with NiO, be non-reversible process, i.e. fuel gas H 2, CO and CH 4Can be converted into CO fully 2And water vapour, so when reacting beinthebalancestate, there is not unreacted H in the exit gas 2, CO and CH 4On the driven mechanics, the reactive behavior of NiO is higher than Fe 2O 3Reactive behavior.
Secondly, Fe 3O 4The process that is converted into FeO and Fe is as follows:
Fe 3O 4+CO→3FeO+CO 2
Fe 3O 4+H 2→3FeO+H 2O
4Fe 3O 4+CH 4→12FeO+CO 2+2H 2O
FeO+CO→Fe+CO 2
FeO+H 2→Fe+H 2O
4FeO+CH 4→4Fe+CO 2+2H 2O
According to chemical thermodynamics equilibrium principle, Fe 3O 4Be reversible reaction in the reaction that is converted into FeO and Fe.Reach in reaction in the situation of equilibrium state, still have part CO, H 2And CH 4Do not participate in reaction.
If hydrogen making, ferric oxide Fe 2O 3Must be reduced to FeO or Fe than lower valency, and react with water vapour, namely must relate to Fe in the hydrogen production process 3O 4Be reduced to the reaction of FeO and Fe.According to above-mentioned thermomechanical analysis, Fe 3O 4The reaction process that is converted into FeO and Fe is reversible reaction, contains the H that does not transform fully in the gas of discharging 2, CO and CH 4, behind water wherein, can't obtain pure CO 2, and present method has been utilized non-reversibility that NiO reduces and the high reactivity of NiO and fuel reactant gas in fuel gas, utilize NiO to react unconverted residual fuel gas, realizes the fully conversion of fuel gas.
In fuel reactor, Fe 2O 3Enter from the top of fuel reactor with NiO, then from the bottom overflow of fuel reactor to the water vapour reactor, fuel gas then enters from the fuel reactor bottom.The cross-sectional area of fuel reactor main body is greater than the fuel reactor bottom compartment, and gas-solid mixture is in the moving-bed state in the fuel reactor main body, fuel gas and Fe 2O 3With the NiO inverse motion.The fuel reactor bottom compartment is because bed body cross-sectional area dwindles, and gas flow rate is high, and the gas-solid two-phase is in bubbling fluidization.In the fuel reactor main body, Fe 2O 3Move downward with NiO, gas moves upward.Newly enter the Fe of fuel reactor 2O 3Be reduced to Fe on top by the fuel gas that does not transform fully from the bottom with NiO 3O 4And Ni, this reaction is non-reversible process, gaseous product only is CO 2And water vapour, behind water wherein, obtain pure CO 2Fe after the reduction 3O 4Continue with Ni, in the fuel reactor bottom because the fuel gas concentration of newly advancing is high, Fe 3O 4Further be reduced to FeO and Fe.In the fuel reactor bottom compartment, because cross-sectional reactor area reduces, gas flow rate is high, and the gas-solid two-phase is in bubbling fluidization, and the FeO of reduction-state, Fe and Ni overflow to water vapour reactor carries out hydrogen production reaction.The fuel gas of complete reaction is not along with the CO that generates 2Rise together with water vapour, and the Fe that is newly entered by fuel reactor top 2O 3React completely with NiO and to be converted into CO 2And H 2O.Utilize Aspen Plus chemical engineering software simulation, consider existing producing hydrogen by using chemical chain and device from the chemical reaction equilibrium angle, when fuel reaction actuator temperature during at 900 ℃, the fuel reactor inlet gas is synthetic gas, CO and H 2Mol ratio be 1:1, if only utilize Fe 2O 3During as oxygen carrier, exit gas is CO, H 2, CO 2And H 2The mixture of O, its mol ratio are 0.2:0.8:0.17:0.83, and 20% CO and 17% H are namely arranged in the fuel gas 2Fail to transform, behind the water condensation and separation of the fuel reactor outlet, can not obtain pure CO 2Utilize hydrogen production process of the present invention, because the non-reversibility of NiO reduction, when inlet gas is synthetic gas, and CO and H 2Mol ratio be 1:1, in the exit gas except CO 2With H 2O, CO and H 2Concentration sum less than 1%, behind water wherein, CO 2The purity of discharging is up to more than 99%.
(2) with traditional ferriferous oxide three beds reaction hydrogen manufacturing separation of C O 2Technology is compared, the fuel gas that this law has used the NiO absorption reaction not transform fully because of the ferriferous oxide drastic reduction.On kinetics, the reactive behavior of NiO is higher than Fe 2O 3, guaranteed the fully conversion of fuel gas.Simultaneously, adopted moving-bed in the design of fuel reactor, NiO has reacted the fuel gas that does not transform fully on fuel reactor top, and the Ni of generation enters the fuel reactor bottom, and Ni no longer participates in reaction, so it does not affect the drastic reduction of ferriferous oxide.At the FeO and the Fe that have realized having obtained when fuel transforms fully reduction-state.On thermodynamics, the Ni of reduction-state reacts with water vapour hardly, enters air reactor behind the Ni process water vapour reactor, and the oxidizing reaction of Ni is strong exothermic process, and the heat of release can be secondary use.Simultaneously, NiO takes a large amount of heats to fuel reactor with the form of solid sensible heat from air reactor as a kind of solid carrier, in order to keep thermo-negative reaction in the fuel reactor.
(3) traditional gas water vapour reforming hydrogen producing be obtain after will reforming first with H 2And CO 2Be the gaseous product of main component, then process and the product hydrogen of acquisition certain purity through purification, CO conversion and PSA separating-purifying etc.Compare with traditional gas water vapour reforming hydrogen producing, the present invention need not to relate to CO 2And H 2Separation equipment, reduce to realize the related energy consumption of above technique.By water vapour and FeO and Fe reaction generation hydrogen, resultant is pure hydrogen through cooling.
Description of drawings
Fig. 1 is for the present invention is based on Fe 2O 3-NiO mixture hydrogen making and separation of C O 2Setting drawing.
Embodiment
Embodiment 1
A kind of based on Fe 2O 3-NiO mixture hydrogen making and separation of C O 2Method, it is characterized in that: simple substance Fe and Ni are placed in the air reactor fluidized-bed, and the temperature of air reactor fluidized-bed is controlled at 1000 ℃, passes into air in air reactor fluidized-bed lower end, and the air reactor bottom compartment is in bubbling fluidization; Simple substance Fe and Ni oxidation by air are Fe 2O 3With NiO; Fe 2O 3Enter the air reactor riser tube with NiO through the air reactor transition section, to the air cyclonic separator, the gas-solid two-phase is separated through the air cyclonic separator by air-lift unit; Gas after the separation is oxygen debt air, and oxygen debt air is overflowed from the outlet of air cyclonic separator; Solid after the separation is Fe 2O 3With NiO, pass into water vapour in the bottom of the second overflow groove as loosening wind, Fe 2O 3Enter fuel reactor with NiO through tremie pipe and the second overflow groove, the temperature of fuel reactor is controlled at 900 ℃; The fuel reactor lower end passes into fuel gas, and the fuel reactor main body is in the moving-bed state; Fe 2O 3Fall Fe from the fuel reactor top with NiO 2O 3The reductibility fuel gas that is risen is reduced to FeO and Fe; NiO is reduced to Ni; The gas of fuel reactor top exit only is CO 2With water vapour, behind water wherein, obtain pure CO 2The FeO of reduction-state, Fe and Ni enter the fuel reactor bottom compartment through the fuel reactor transition section; Fuel reactor bottom compartment sectional area is less than the fuel reactor main body and be in bubbling fluidization; Pass into water vapour in the bottom of the first overflow groove as loosening wind, the FeO of reduction-state, Fe and Ni enter water vapour reactor fluidisation bed in the fuel reactor bottom compartment through the first overflow groove; Pass into water vapour in water vapour reactor fluidisation bed lower end, water vapour reactor bottom compartment is in bubbling fluidization, and the temperature of water vapour reactor fluidisation bed is controlled at 850 ℃; FeO, Fe and water vapour reaction generate hydrogen, and solid product is Fe 3O 4Ni and water vapour can not react, Ni and solid product Fe 3O 4Be promoted to the hydrogen cyclonic separator through water vapour reactor transition section and water vapour reactor riser by water vapour and hydrogen, gas-solid separates through the hydrogen cyclonic separator, hydrogen and water vapour are overflowed from the outlet of hydrogen cyclonic separator, behind water wherein, obtain pure hydrogen; Pass into air in the bottom of the 3rd overflow groove as loosening wind, the solid Fe after the separation 3O 4Enter the air reactor fluidized-bed with Ni through tremie pipe and the 3rd overflow groove, again be oxidized to Fe by air 2O 3With NiO, the while releases heat; Fe 2O 3Realize recycle with NiO; Such as accompanying drawing 1.
Embodiment 2
A kind of realization is claimed in claim 1 based on Fe 2O 3-NiO mixture hydrogen making and separation of C O 2Device, it is characterized in that: formed by water vapour reactor fluidisation bed, fuel reactor and air reactor fluidized-bed; Water vapour reactor fluidisation bed is comprised of water vapour reactor bottom compartment, water vapour reactor transition section and water vapour reactor riser; The water vapour reactor riser links to each other with water vapour reactor bottom compartment by water vapour reactor transition section, the upper end of water vapour reactor riser is connected with the hydrogen cyclonic separator, the hydrogen cyclonic separator links to each other with the 3rd overflow groove by tremie pipe, and the 3rd overflow groove is connected with the air reactor fluidized-bed; The air reactor fluidized-bed is comprised of air reactor bottom compartment, air reactor transition section, air reactor riser tube, air cyclonic separator and tremie pipe, the air reactor bottom compartment links to each other with the air reactor riser tube by the air reactor transition section, the top of air reactor riser tube links to each other with the air cyclonic separator, described the 3rd overflow groove is connected with air reactor bottom compartment in the air reactor fluidized-bed, and the air cyclonic separator is connected with fuel reactor by tremie pipe and the second overflow groove; Fuel reactor is comprised of fuel reactor main body, fuel reactor transition section, fuel reactor bottom compartment and the first overflow groove, the fuel reactor main body links to each other with the fuel reactor bottom compartment by the fuel reactor transition section, and the cross-sectional area of fuel reactor main body is greater than the cross-sectional area of fuel reactor bottom compartment; The fuel reactor bottom compartment links to each other with the first overflow groove, and the first overflow groove links to each other with water vapour reactor bottom compartment, and described air cyclonic separator is connected with the top of the fuel reactor main body of fuel reactor by tremie pipe and the second overflow groove; Such as accompanying drawing 1.

Claims (1)

1. one kind based on Fe 2O 3-NiO mixture hydrogen making and separation of C O 2Method, it is characterized in that: simple substance Fe and Ni are placed in the air reactor fluidized-bed (3), the temperature of air reactor fluidized-bed (3) is controlled at 950 ~ 1000 ℃, passes into air in air reactor fluidized-bed lower end (E), and air reactor bottom compartment (3-1) is in bubbling fluidization; Simple substance Fe and Ni oxidation by air are Fe 2O 3With NiO; Fe 2O 3Enter air reactor riser tube (3-3) with NiO through air reactor transition section (3-2), to air cyclonic separator (3-4), the gas-solid two-phase is separated through air cyclonic separator (3-4) by air-lift unit; Gas after the separation is oxygen debt air, and oxygen debt air is overflowed from air cyclonic separator outlet (C); Solid after the separation is Fe 2O 3With NiO, Fe 2O 3Enter fuel reactor (2) with NiO through tremie pipe (3-5) and the second overflow groove (2-5), the temperature of fuel reactor (2) is controlled at 900 ~ 950 ℃; Fuel reactor lower end (G) passes into fuel gas, and fuel reactor main body (2-4) is in the moving-bed state; Fe 2O 3Fall Fe from the fuel reactor top with NiO 2O 3The reductibility fuel gas that is risen is reduced to FeO and Fe; NiO is reduced to Ni; The gas of fuel reactor top exit (I) only is CO 2With water vapour, behind water wherein, obtain pure CO 2The FeO of reduction-state, Fe and Ni enter fuel reactor bottom compartment (2-2) through fuel reactor transition section (2-3); Fuel reactor bottom compartment (2-2) sectional area is less than fuel reactor main body (2-4) and be in bubbling fluidization; The FeO of reduction-state, Fe and Ni enter water vapour reactor fluidisation bed (1) at fuel reactor bottom compartment (2-2) through the first overflow groove (2-1); Pass into water vapour in water vapour reactor fluidisation bed lower end (A), water vapour reactor bottom compartment (1-1) is in bubbling fluidization, and the temperature of water vapour reactor fluidisation bed (1) is controlled at 750 ~ 850 ℃; FeO, Fe and water vapour reaction generate hydrogen, and solid product is Fe 3O 4Ni and water vapour can not react, Ni and solid product Fe 3O 4Be promoted to hydrogen cyclonic separator (1-4) through water vapour reactor transition section (1-2) and water vapour reactor riser (1-3) by water vapour and hydrogen, gas-solid separates through hydrogen cyclonic separator (1-4), hydrogen and water vapour are overflowed from hydrogen cyclonic separator outlet (B), behind water wherein, obtain pure hydrogen; Solid Fe after the separation 3O 4Enter air reactor fluidized-bed (3) with Ni through tremie pipe (5) and the 3rd overflow groove (4), again be oxidized to Fe by air 2O 3With NiO, the while releases heat; Fe 2O 3Realize recycle with NiO.
CN2011100838119A 2011-04-02 2011-04-02 Method and device for preparing hydrogen and separating CO2 based on Fe2O3-NiO mixture Expired - Fee Related CN102225744B (en)

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CN101746721A (en) * 2009-08-12 2010-06-23 东南大学 Method and device for producing hydrogen and separating CO2 based on iron or iron oxide

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CN101746721A (en) * 2009-08-12 2010-06-23 东南大学 Method and device for producing hydrogen and separating CO2 based on iron or iron oxide

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