CN1917263A - System and method for circulating gas from biomass in fuel bank of soild oxide - Google Patents

System and method for circulating gas from biomass in fuel bank of soild oxide Download PDF

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Publication number
CN1917263A
CN1917263A CNA200610011051XA CN200610011051A CN1917263A CN 1917263 A CN1917263 A CN 1917263A CN A200610011051X A CNA200610011051X A CN A200610011051XA CN 200610011051 A CN200610011051 A CN 200610011051A CN 1917263 A CN1917263 A CN 1917263A
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solid oxide
oxide fuel
heap
anode
biomass gas
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CN100553020C (en
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马文会
王�华
杨斌
戴永年
刘荣辉
刘大春
于洁
阳书文
李伟宏
徐宝强
刘永成
杨部正
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Kunming University of Science and Technology
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Kunming University of Science and Technology
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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
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells

Abstract

The system includes fused salt pond, fuel cell pile of solid oxide in intermediate temperature, and gas delivery and collection device. First, basis methane in biomass gas is oxidized to H2 and CO by lattice oxygen dispersed in fused salt. Impurity S and heavy metals etc in biomass gas are absorbed by fused salt. H2 and CO at anode of SOFCs is electrochemical-oxidized as CO2 and H2O. Most of energy released by reaction is converted to electrical energy. Being absorbed and desorbed by renewable material Li4SiO4, most of CO2 is purified and recovered at specific temperature. Being circulated to fused salt pond, a small quantity of CO2 and H2O takes reforming reaction with methane. Quantity of heat needed by reaction is supplied by quantity of heat released from partial oxidation of methane. Features are: good performance of SOFCs for anti carbon deposition, and good tolerance for fuel of containing impurities S and N, high use ratio for energy, and zero discharge of CO2.

Description

A kind of solid oxide fuel heap biogas systemic circulatory system and method
Technical field: the present invention relates to a kind of solid oxide fuel heap biogas systemic circulatory system and method, belong to energy technology field.
Technical background: China is vast in territory, and there is abundant biogas (main component is a methane) resource particularly vast rural area.These gases are potential Solid Oxide Fuel Cell (SOFC) fuel.When SOFC used biogas as fuel, because the methane stable performance, electro-chemical activity was obviously not as H2, so generally need earlier with steam with methane reforming gases such as preparation CO and H2.When using outside the reformation, because reforming reaction is a strong endothermic reaction, and institute's calorific requirement can not directly be supplied with by the electric reaction heat of fuel, needs extra heater and energy consumption, increased the complexity and the production cost of technology.When using the inside reforming mode, because catalyst defective, operating condition are improper, be easy to form the carbon distribution phenomenon, and the S in the biomass gas and heavy metal also can make anode catalyst poison at anode, these phenomenons can cause battery performance to be decayed rapidly.In addition, the strong endothermic effect of steam inside reforming reaction also can cause the anode interior temperature difference bigger, increases temperature controlled difficulty in the operating process.
Summary of the invention: the deficiency that the objective of the invention is to overcome prior art, a kind of solid oxide fuel heap biogas systemic circulatory system is provided, do not use the external heat device, problems such as the temperature difference when avoiding inside reforming in anode carbon distribution phenomenon and the anode chamber is bigger, simplify technology, reduce production costs, realize making full use of of resource.
Technical scheme of the present invention is: this solid oxide fuel heap biogas systemic circulatory system comprises the fusion salt pond, intermediate temperature solid oxide fuel cell heap, CO 2(sorbing material is Li to adsorbent equipment 4SiO 4), and gas delivery and gathering-device (pipeline, blower fan and the caisson that are connected fusion salt pond and battery pile); The fusion salt pond is circulating fluidized bed or the fixed bed reactors that the carbonate fuse salt is housed, and its working temperature is 700～900 ℃; Carbonate in the fusion salt pond can be one or both mixture (as Na 2CO 3And K 2CO 3), its concrete kind or ratio are determined according to actual needs (if when adopting two kinds, mass ratio generally can be 1: 1～1: 3), also be dispersed with proper amount of oxidant and catalyst in the fusion salt pond, these oxidants and catalyst can be that the variable valency metal oxide of high valence state is (as Fe 2O 3, CeO 2, Ce 1-xGd xO 2Deng) or perovskite (ABO 3, as La 1-xSr xCr 1-yMn yO 3-δ, LaFeO 3Deng) the type catalysis material, the ratio of oxidant and catalyst and fuse salt is determined (the run-of-the-mill ratio can be 10～20%) according to actual needs.
This solid oxide fuel heap biomass gas round-robin method is: put into fuse salt earlier in circulating fluidized bed or fixed bed reactors and be heated to 700～900 ℃ and form the fusion salt ponds (fuse salt is a carbonate, can adopt one or both mixture, as: Na 2CO 3K 2CO 3Deng, its concrete kind or ratio can determine according to actual needs, if when adopting two kinds, mass ratio generally can be 1: 1～1: 3), then proper amount of oxidant and catalyst are disperseed to put into fuse salt or load on honeycomb support (as Al 2O 3) on be placed in the fuse salt, oxidant and catalyst can be that the variable valency metal oxide of high valence state is (as Fe 2O 3, CeO 2, Ce 1-xGd xO 2Deng) or perovskite (ABO 3, as La 1-xSr xCr 1-yMn yO 3-δ, LaFeO 3Deng) the type catalysis material, its addition is determined (mass ratio general and fuse salt can be 10～20%) according to actual needs; By air supply plant biogas is sent in the molten bath, made impurity S in the biogas and heavy metal etc. be melted salt and absorb, methane wherein then generates CO and H with Lattice Oxygen generation partial oxidation reaction 2Forming gas; This forming gas is transported to anode chamber and the carrier of oxygen effect that intermediate temperature solid oxide fuel cell is piled, makes it be turned to CO by electrochemistry oxygen 2And H 2O, most of energy that reaction discharges is converted into electric energy, the Lattice Oxygen that consumes when blasting simultaneously compressed air with the recovery methane portion oxidation in the molten bath; By gas delivery and gathering-device, the battery pile anode is not participated in the CO and the H of reaction 2Recycling, carry small part reaction product of anode CO simultaneously 2And H 2O in the fuse salt device with CH 4Reforming reaction takes place, and obtains CO and H 2And send into the anode of solid oxide fuel cell chamber; Most of reaction product of anode CO 2Through CO 2Adsorbent equipment is by renewable sorbing material (Li 4SiO 4) after absorption-desorption purifies, be used to prepare products such as plastics and diamond.
Electrolyte, anode, the cathode material of intermediate temperature solid oxide fuel cell heap of the present invention can be respectively LaGaO 3Sill, LaCrO 3Sill, LaFeO 3Sill, also can add doped chemical (as Sr, Ca, Mg, Mn, Co etc.) as required, battery components material coefficient of thermal expansion coefficient is adjusted, making simultaneously has good chemical compatibility (the concrete addition of doped chemical is adjusted according to actual needs, guarantees to have between electrolyte and the electrode material good heat coupling and chemical compatibility to get final product) between electrolyte and the electrode material.
The Lattice Oxygen that utilization of the present invention is dispersed in the fuse salt is CO and H with the methane portion oxidation in the biogas 2Synthesis gas is turned to CO at the anode of SOFCs by electrochemistry oxygen 2And H 2O, most of Conversion of energy that reaction discharges is a utilization of power; And heat and SOFCs generating waste-heat that the methane portion oxidation that stores in the fuse salt discharges also are used to united heat or generating, SOFCs anode residual air CO 2Then be collected, purification and the utilization of resources.Therefore, compared with prior art, present technique has following characteristics:
1, because of methane portion oxidation is gentle exothermic reaction, the heater when having saved the outside reforming methane of steam, problem such as the anode carbon distribution phenomenon when having avoided inside reforming, the temperature difference in the anode chamber are bigger;
2, in biogas such as biogas, contain SO 2Or during heavy metal, impurity such as S element and heavy metal are enriched in the fuse salt, have avoided the poison deactivation of the anode of SOFC;
3, fused carbonate has higher thermal capacitance and chemical stability, and the reaction heat that the methane portion oxidation synthesis gas course of reaction is emitted is stored in the fuse salt, and CH 4And CO 2, H 2The reforming reaction that takes place between the O is the endothermic reaction, so the methane portion oxidation liberated heat will be at CH 4And CO 2, H 2Reforming reaction or catalyst take place between the O to be recovered to be utilized again in the Lattice Oxygen course of reaction;
4, utilize fuse salt partial oxidation methane preparing synthetic gas, intermediate temperature solid oxide fuel cell and Li 4SiO 4CO absorption 2Working temperature (being about 800 ℃) close, whole system configuration and UTILIZATION OF VESIDUAL HEAT IN are convenient, integral energy utilization ratio height;
5, realize carbon dioxide zero discharge.The generating residual air CO of solid-oxide fuel cell stack 2Through renewable sorbing material (Li 4SiO 4) after absorption-desorption purifies, directly as industrial chemicals.Preparation plastics and diamond etc. are beneficial to the environmental protection and the utilization of resources.
Description of drawings: the present invention is further elaborated below in conjunction with drawings and Examples.
Fig. 1 is a work system schematic diagram of the present invention.
Fig. 2 is a process chart of the present invention.
Fig. 3 is the renewable sorbing material (Li of the present invention 4SiO 4) the operation principle schematic diagram.
Embodiment: embodiment 1: as Figure 1-3, this solid oxide fuel heap biogas systemic circulatory system comprises the fusion salt pond, intermediate temperature solid oxide fuel cell heap, CO 2(sorbing material is Li to adsorbent equipment 4SiO 4), and gas delivery and gathering-device (pipeline, blower fan and the caisson that are connected fusion salt pond and battery pile); The fusion salt pond is that Na is housed 2CO 3And K 2CO 3The stainless steel fixed bed reactors of fuse salt, its working temperature are 750 ℃, Na 2CO 3With K 2CO 3Mass ratio be 1: 1, also contain the oxidant and the catalyst Fe of 15% (mass ratio) in the fusion salt pond 2O 3
This solid oxide fuel heap biomass gas round-robin method is: in the stainless steel fixed bed reactors, put into Na by 1: 1 mass ratio earlier 2CO 3And K 2CO 3Form the fusion salt pond, press the amount of 15% mass ratio then, oxidant and catalyst Fe 2O 3Disperse to put in the fuse salt; The fuse salt device is heated to 850 ℃ of stable 1h, reducing to 750 ℃ of reaction temperatures, pass through air supply plant again, feed biomass gas from the stainless steel reactor bottom that is full of fuse salt, gas flow rate is 20ml/min, make impurity S in the biogas and heavy metal etc. be melted salt and absorb, methane wherein then generates CO and H with Lattice Oxygen generation partial oxidation reaction 2(collect gas on reactor assembly top, with gas chromatograph the component of mist is carried out on-line analysis, mixing gas component is forming gas: H 263%, CO21%, CO 27%, CH 49%).Anode chamber and the carrier of oxygen effect of warm SOFCs made it be turned to CO by electrochemistry oxygen during this forming gas was transported to 2And H 2O, most of energy that reaction discharges is converted into electric energy, the Lattice Oxygen that consumes when blasting simultaneously compressed air with the recovery methane portion oxidation in the molten bath; By gas delivery and gathering-device, anode is not participated in the CO and the H of reaction 2Recycling, while transport portion reaction product of anode CO 2And H 2O in the fuse salt device with CH 4Reforming reaction takes place, and obtains CO and H 2And send into the anode of solid oxide fuel cell chamber; Most of reaction product of anode CO 2Through renewable sorbing material Li 4SiO 4(with Li 2CO 3And SiO 2Be raw material, adopt the solid phase method synthetic) after absorption-desorption purifies, be used to prepare products such as plastics and diamond.
In this System and method for, electrolyte, anode, the cathode material of intermediate temperature solid oxide fuel cell heap are respectively La 1-xSr xGa 1-yMg yO 3-δ, La 1-xSr xCr 1-yMn yO 3-δ, La 1-xSr xFe 1-yCo yO 3-δSolid-oxide fuel cell stack.
Honeycomb ceramics shape Li 4SiO 4The material compacting sintering is that diameter is that 13mm, thickness are the 10mm sheet, carries out carbon dioxide absorption in tube furnace, under 750 ℃, and the flow of carbon dioxide is 2L/min, at 750 ℃ of insulations after two hours down, Li 4SiO 4The weight of material increases by 24%; Carry out the carbon dioxide of material then and resolve under 850 ℃, 2h is interior with adsorbed CO 2Resolve fully.
Embodiment 2: as Figure 1-3, this solid oxide fuel heap biogas systemic circulatory system comprises the fusion salt pond, intermediate temperature solid oxide fuel cell heap, CO 2(sorbing material is Li to adsorbent equipment 4SiO 4), and gas delivery and gathering-device (pipeline, blower fan and the caisson that are connected fusion salt pond and battery pile); The fusion salt pond is that Na is housed 2CO 3And K 2CO 3The circulating fluid bed reactor of fuse salt, its working temperature are 700 ℃, Na 2CO 3And K 2CO 3Mass ratio be 1: 2, also contain the oxidant and the catalyst Ce of 20% (mass ratio) in the fusion salt pond 0.8Gd 0.2O 1.85
This solid oxide fuel heap biomass gas round-robin method is: in fluidized-bed reactor, put into Na by 1: 2 mass ratio earlier 2CO 3And K 2CO 3Form the fusion salt pond, press the amount of 20% mass ratio then, oxidant and catalyst Ce 0.8Gd 0.2O 1.85Disperse to put in the fuse salt; The fuse salt device is heated to 800 ℃ of stable 1h, reducing to 700 ℃ of reaction temperatures, pass through air supply plant again, feed biomass gas from the fluidized-bed reactor bottom that is full of fuse salt, gas flow rate is 15ml/min, make impurity S in the biogas and heavy metal etc. be melted salt and absorb, methane wherein then generates CO and H with Lattice Oxygen generation partial oxidation reaction 2(collect gas on reactor assembly top, with gas chromatograph the component of mist is carried out on-line analysis, mixing gas component is forming gas: H 258%, CO26%, CO 26%, CH 45%).This forming gas is transported to anode chamber and the carrier of oxygen effect that intermediate temperature solid oxide fuel cell is piled, makes it be turned to CO by electrochemistry oxygen 2And H 2O, most of energy that reaction discharges is converted into electric energy; The Lattice Oxygen that consumes when blasting simultaneously compressed air with the recovery methane portion oxidation in the molten bath is not participated in anode the CO and the H of reaction by gas delivery and gathering-device 2Recycling, while transport portion reaction product of anode CO 2And H 2O in the fuse salt device with CH 4Reforming reaction takes place, and obtains CO and H 2And send into the anode chamber of solid-oxide fuel cell stack; Most of reaction product of anode CO 2Through CO 2Adsorbent equipment is by renewable sorbing material Li 4SiO 4Absorption-desorption is used to prepare products such as plastics and diamond after purifying.
Li 4SiO 4Material compacting sintering honeycomb ceramics carries out carbon dioxide absorption under 725 ℃, and the flow of carbon dioxide is 2L/min, be incubated after two hours the weight of material increase by 36% (reaching the theoretical adsorptive value of material substantially); Carry out the carbon dioxide of material again and resolve under 850 ℃, 1.5h is interior with adsorbed CO 2Resolve fully.
In this System and method for, electrolyte, anode, the cathode material of intermediate temperature solid oxide fuel cell heap are respectively La 1-xSr xGa 1-y-zMg yCo zO 3-δ, La 1-xCa xCr 1-yMn yO 3-δ, La 1-x-ySr xCa yFe 1-zCo zO 3-δMaterial.
Embodiment 3: as Figure 1-3, this solid oxide fuel heap biogas systemic circulatory system comprises the fusion salt pond, intermediate temperature solid oxide fuel cell heap, CO 2(sorbing material is Li to adsorbent equipment 4SiO 4), and gas delivery and gathering-device (pipeline, blower fan and the caisson that are connected fusion salt pond and battery pile); The fusion salt pond is the K that was equipped with 1: 3 2CO 3And Li 2CO 3The circulating fluid bed reactor of fuse salt, its working temperature are 900 ℃; Also contain 10% oxidant and catalyst La in the fusion salt pond 1-xSr xFe 1-yCo yO 3-δ
This solid oxide fuel heap biomass gas round-robin method is: in fixed bed reactors, put into 1: 3 K earlier 2CO 3And Li 2CO 3Form the fusion salt pond, press the amount of 10% mass ratio then, oxidant and catalyst La 1-xSr xFe 1-yCo yO 3-δLoad on honeycomb support Al 2O 3On be placed in the fuse salt; The fuse salt device is heated to 950 ℃ of stable 1h, reducing to 900 ℃ of reaction temperatures, pass through air supply plant again, feed biomass gas from the fluidized-bed reactor bottom that is full of fuse salt, gas flow rate is 15ml/min, make impurity S in the biogas and heavy metal etc. be melted salt and absorb, methane wherein then generates CO and H with Lattice Oxygen generation partial oxidation reaction 2(collect gas on reactor assembly top, with gas chromatograph the component of mist is carried out on-line analysis, mixing gas component is forming gas: H 270%, CO26%, CO 24%).This forming gas is transported to anode chamber and the carrier of oxygen effect that intermediate temperature solid oxide fuel cell is piled, makes it be turned to CO by electrochemistry oxygen 2And H 2O, the Lattice Oxygen that consumes when in the molten bath, blasting simultaneously compressed air with the recovery methane portion oxidation, most of energy that reaction discharges is converted into electric energy; By gas delivery and gathering-device, anode is not participated in the CO and the H of reaction 2Recycling, while transport portion reaction product of anode CO 2And H 2O in the fuse salt device with CH 4Reforming reaction takes place, and obtains CO and H 2And send into the anode of solid oxide fuel cell chamber; Most of reaction product of anode CO 2Through renewable sorbing material Li 4SiO 4Absorption-desorption is used to prepare products such as plastics and diamond after purifying.
In this System and method for, electrolyte, anode, the cathode material of intermediate temperature solid oxide fuel cell heap are respectively La 1-xSr xGa 1-y-zMg yFe zO 3-δ, La 1-xSr xCr 1-yCo yO 3-δ, La 1-xSr xFe 1-yMn yO 3-δMaterial.
With Li 4SiO 4Material compacting sintering honeycomb ceramics carries out carbon dioxide absorption under 700 ℃, and the flow of carbon dioxide is 2I/min, be incubated after two hours the weight of material increase by 32% (reaching the theoretical adsorptive value of material substantially); Carry out the carbon dioxide of material again and resolve under 800 ℃, 2h is interior with adsorbed CO 2Resolve fully.

Claims (10)

1, a kind of circulatory system of solid oxide fuel heap biomass gas is characterized in that it comprises the fusion salt pond, intermediate temperature solid oxide fuel cell heap, CO 2Adsorbent equipment, and the gas delivery and the gathering-device that connect them.
2, the circulatory system of solid oxide fuel heap biomass gas according to claim 1 is characterized in that electrolyte, anode, the cathode material of intermediate temperature solid oxide fuel cell heap can be respectively LaGaO 3Sill, LaCrO 3Sill, LaFeO 3Sill, fusion salt pond are that fuse salt, working temperature are housed is 700～900 ℃ circulating fluidized bed or fixed bed reactors, CO 2The sorbing material of adsorbent equipment is Li 4SiO 4
3, the circulatory system of solid oxide fuel according to claim 2 heap biomass gas is characterized in that the oxidant and the catalyst that are dispersed with in the fusion salt pond, and the fuse salt in the fusion salt pond is a carbonate.
4, the circulatory system of solid oxide fuel heap biomass gas according to claim 3 is characterized in that the carbonate in the fusion salt pond can be one or both mixture.
5,, it is characterized in that variable valency metal oxide or Ca-Ti ore type catalysis material that oxidant in the fusion salt pond and catalyst can be high valence state according to the circulatory system of claim 3 or 4 described solid oxide fuels heap biomass gas.
6, a kind of round-robin method of solid oxide fuel heap biomass gas, it is characterized in that in circulating fluidized bed or fixed bed reactors, putting into fuse salt earlier and be heated to 700～900 ℃ forming the fusion salt pond, then proper amount of oxidant and catalyst are disperseed to put into fuse salt or load on to be placed in the fuse salt on the honeycomb support; By air supply plant biogas is sent in the molten bath, made impurity S in the biogas and heavy metal etc. be melted salt and absorb, methane wherein then generates CO and H with Lattice Oxygen generation partial oxidation reaction 2Forming gas; This forming gas is transported to anode chamber and the carrier of oxygen effect that intermediate temperature solid oxide fuel cell is piled, makes it be turned to CO by electrochemistry oxygen 2And H 2O, the Lattice Oxygen that consumes when in the molten bath, blasting simultaneously compressed air with the recovery methane portion oxidation; By gas delivery and gathering-device, anode is not participated in the CO and the H of reaction 2Recycling, most of reaction product of anode CO 2After the renewable sorbing material of process carries out the absorption-desorption purification, as industrial chemicals.
7, the round-robin method of solid oxide fuel heap biomass gas according to claim 6, it is characterized in that fuse salt is a carbonate, oxidant and catalyst can be the variable valency metal oxide or the Ca-Ti ore type catalysis materials of high valence state, and renewable sorbing material is Li 4SiO 4
8, the round-robin method of solid oxide fuel heap biomass gas according to claim 7 is characterized in that the carbonate in the fusion salt pond can be one or both mixture.
9, according to the round-robin method of claim 6 or 7 described solid oxide fuel heap biomass gas, it is characterized in that electrolyte, anode, the cathode material of intermediate temperature solid oxide fuel cell is respectively LaGaO 3Sill, LaCrO 3Sill, LaFeO 3Sill.
10, the round-robin method of solid oxide fuel heap biomass gas according to claim 6, it is characterized in that can be with segment anode product CO 2And H 2O is transported in the fuse salt device and CH 4Reforming reaction takes place, and obtains CO and H 2, send into the anode of solid oxide fuel cell chamber again and react.
CNB200610011051XA 2006-07-17 2006-07-17 A kind of solid-oxide fuel cell stack biogas systemic circulatory system and method Expired - Fee Related CN100553020C (en)

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CN112827467A (en) * 2021-01-07 2021-05-25 广东工业大学 Cage-shaped adsorbent and preparation method and application thereof
CN113178605A (en) * 2021-03-17 2021-07-27 东南大学 Fluidized bed anode solid oxide fuel cell
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CN115744823A (en) * 2023-01-09 2023-03-07 清华大学 Method for preparing synthesis gas by coupling pyrolysis of hydrocarbon fuel and steam reforming and synthesis gas preparation system

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CN105838449A (en) * 2016-05-23 2016-08-10 太原理工大学 System and method for catalytic purification treatment on coal chemical industry crude synthesis gas
CN107525427A (en) * 2016-06-15 2017-12-29 南方研究所 High temperature heat chemistry energy storage system
US11478743B2 (en) 2018-09-21 2022-10-25 Southern Research Institute High temperature thermochemical energy storage system
CN111082097A (en) * 2019-11-19 2020-04-28 曾庆福 Fuel cell system
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CN112827467A (en) * 2021-01-07 2021-05-25 广东工业大学 Cage-shaped adsorbent and preparation method and application thereof
CN113178605A (en) * 2021-03-17 2021-07-27 东南大学 Fluidized bed anode solid oxide fuel cell
CN115744823A (en) * 2023-01-09 2023-03-07 清华大学 Method for preparing synthesis gas by coupling pyrolysis of hydrocarbon fuel and steam reforming and synthesis gas preparation system

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