CN102306809A - Conductor catalyst for enhancing performance of direct carbon fuel battery and method - Google Patents

Conductor catalyst for enhancing performance of direct carbon fuel battery and method Download PDF

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CN102306809A
CN102306809A CN201110194653A CN201110194653A CN102306809A CN 102306809 A CN102306809 A CN 102306809A CN 201110194653 A CN201110194653 A CN 201110194653A CN 201110194653 A CN201110194653 A CN 201110194653A CN 102306809 A CN102306809 A CN 102306809A
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conductor
catalyst
carbon
direct
cell performance
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蔡宁生
史翊翔
王洪建
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Tsinghua University
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Tsinghua 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
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells

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Abstract

The invention discloses a conductor catalyst for enhancing the performance of a direct carbon fuel battery and a method, which relate to the technical field of cleaning energy. The conductor catalyst is prepared by mixing an ion conductor, an electronic conductor and a carbon gasification catalyst and then processing by a mechanical crushing method or a solid phase synthesizing method. The conductor catalyst provided by the invention is applied for generating power for the direct carbon fuel battery; a conductor network is formed in a battery anode; the direct electrochemical reaction of carbon is enlarged; the reaction speed of carbon gasification is enhanced through the carbon gasification catalyst; and the reaction speed of carbon gasification is enhanced.

Description

A kind of conductor catalyst and method that improves direct carbon consuming cell performance
Technical field
The invention belongs to the clean energy technology field, be specifically related to a kind of conductor catalyst and method that improves the direct carbon consuming cell performance of soild oxide.
Background technology
China is maximum in the world coal production and country of consumption, and the coal consumption amount accounts for more than 70% of primary energy total amount, wherein surpasses 50% coal and is used for thermal power generation.Simultaneously, coal also occupies main status in China's electric structure.With the coal is that main energy resource structure does not have very about-face at short notice.But China's coal fired power generation efficient is low at present, and energy waste and environmental situation are serious; Simultaneously, as CO in the world 2Discharge first big country, we are faced with huge CO 2Reduce discharging pressure.Therefore exploring efficiently, the clean coal power generation technology is the inevitable direction of energy industry development.
Directly (Direct Carbon Fuel Cell DCFC) adopts solid carbon to act as a fuel to carbon consuming cell, receives domestic and international researcher's extensive attention in recent years, and is classified as one of following ten technology of meriting attention greatly.Directly carbon consuming cell has very special advantages:
1. battery efficiency is higher.Because direct carbon consuming cell overall reaction (C+O 2=CO 2) the very little (2.5J.K of Entropy Changes -1.mol -1), when 800 ℃ of left and right sides, theoretical efficiency reaches 100%, and fuel availability can reach 100%.
2. disposal of pollutants is few.Do not have direct combustion process, the discharge capacity of pollutants such as SOx, NOx can significantly reduce.
3. directly carbon consuming cell can be converted into CO with the C in the coal 2, carbon fuel discord air directly contacts mixing, helps CO 2Enrichment and reduction of discharging.
4. from world wide, the coal resources reserves are abundant, low price; It is one of energy pillar of the world today; And solid carbon fuel is expected to obtain through reserves abundant in coal, biomass etc. are carried out simple processed, and fuel source is extensive, is easy to obtain.
5.DCFC employed solid carbon fuel volume is little, calorific value is high, transportation is convenient with storage.
6. as high-temperature fuel cell, DCFC is applicable to extensive generating and middle-size and small-size distributed generation system.
If directly carbon consuming cell can realize being the commercial applications of fuel with the coal directly; Utilize mode with change traditional energy revolutionaryly; Realize the perfect adaptation of traditional fossil energy utilization and fuel cell technology; Can alleviate the nervous present situation of China's petroleum resources effectively, improve efficiency of energy utilization, alleviate CO 2Reduce discharging pressure.Therefore, directly the research of carbon consuming cell generation technology is significant to energy technology progress and national energy security.
In recent years, along with the development of material science and fuel cell technology, developed the direct carbon consuming cell of multiple electrolyte, common direct carbon consuming cell electrolyte comprises fusible hydrate, fused carbonate and solid oxide electrolyte.Comparatively speaking; The direct carbon consuming cell of solid oxide electrolyte (Solid Oxide Direct Carbon Fuel Cell, SO-DCFC) minimum to the requirement of carbon fuel purity, being hopeful most to realize directly is fuel with the coal; And galvanic anode can be used for reference existing combustion apparatus (like fluid bed etc.); Solve solid-fuelled feed problem, improve the internal heat transfer mass transfer, improve battery performance; Be easy to enlarge the battery scale, and do not have the sealing and the etching problem of liquid electrolyte in the course of reaction.But SO-DCFC does not preponderate on current density at present, and reaction speed is slower.Main cause is that (1) fuel and anode contact-making surface only limit in the two dimensional surface, and the Direct Electrochemistry reaction interface of carbon is limited; (2) the coal gasification reaction rate limit the carrying out of gas eletrochemistry reaction.Therefore the limiting factor of improving above two aspects of SO-DCFC becomes its development key of restriction.
Summary of the invention
The object of the present invention is to provide a kind of additive that improves the direct carbon consuming cell performance of soild oxide.
A kind of conductor catalyst that improves the direct carbon consuming cell performance of soild oxide, said conductor catalyst are to be prepared from through mechanical crushing method or solid-phase synthesis after ion conductor, electronic conductor and the carbon gasification catalyst mix; Wherein, ion conductor, electronic conductor and carbon gasification catalyst account for the 10-93% of conductor catalyst gross mass, 5-93%, 1-93% respectively.
Said ion conductor does
Figure BDA0000075294440000031
Ion conductor or O 2-Ion conductor.
Said
Figure BDA0000075294440000032
Ion conductor is Li 2CO 3, Na 2CO 3Or K 2CO 3O 2-Ion conductor is the zirconia or the gadolinium oxide doped cerium oxide of stabilized with yttrium oxide.
Said electronic conductor is selected from Ni, Fe, Ag, W, NiO, Ag 2Among the O one or more.
Said carbon gasification catalyst is at least a material in carbonate, bicarbonate, sulfate or the nitrate of lithium, sodium, potassium, beryllium, magnesium, calcium, strontium, scandium, titanium, vanadium, manganese, iron, nickel, molybdenum or silver.
A kind of method that improves the direct carbon consuming cell performance of soild oxide; In solid carbon, add conductor catalyst as claimed in claim 1; The solid carbon that adds the conductor catalyst acted as a fuel place in the direct carbonate fuel cell anodes cavity; Feed anode carrier gas holding anode reaction atmosphere simultaneously, negative electrode bubbling air or oxygen are as oxidant, and operating temperature range is 600～1000 ℃.
The conductor catalyst that adds accounts for the 1-50% of solid carbon quality.
Said solid carbon is selected from one or more in carbon black, graphite, coke, biomass, coal, petroleum coke or the organic waste materials.
Said anode carrier gas is N 2, Ar, He, CO 2Or H 2O.
Beneficial effect of the present invention: use conductor catalyst of the present invention and carry out direct carbon consuming cell generating; In galvanic anode, formed the Direct Electrochemistry reaction that a kind of conductor networks has increased carbon; And the reaction speed that has strengthened carbon gasification through the carbon gasification catalyst is recorded, and has improved the speed of carbon gasification course of reaction.Can under given working temperature and operating voltage, improve the power density of battery through this dual mode.
Embodiment
With specific embodiment the present invention is further specified below.
Embodiment 1
With Li 2CO 3, MgSO 4, W is respectively 30%, 50%, 20% mechanical crushing method according to mass fraction and processes the conductor catalyst, as solid carbon fuel, in fuel, adds 20% conductor catalyst with carbon black.The carbon black that adds the conductor catalyst acted as a fuel place in the direct carbonate fuel cell anodes cavity, with 50mlmin -1The CO of flow 2As the anode carrier gas, with 100mlmin -1The O of flow 2As cathode oxidant, 800 ℃ of battery operated temperature.At this moment, SO-DCFC average power density under 0.7V constant voltage discharge operating mode is 1274Wm -2
Embodiment 2
With Na 2CO 3, K 2CO 3, Fe is respectively 30%, 50%, 20% mechanical crushing method according to mass fraction and processes the conductor catalyst, as solid carbon fuel, in fuel, adds 20% conductor catalyst with coke.The coke that adds the conductor catalyst acted as a fuel place in the direct carbonate fuel cell anodes cavity, with 50mlmin -1The He of flow is as the anode carrier gas, with 100mlmin -1The O of flow 2As cathode oxidant, 600 ℃ of battery operated temperature.At this moment, SO-DCFC average power density under 0.7V constant voltage discharge operating mode is 1204Wm -2
Embodiment 3
With K 2CO 3, MgSO 4, W is respectively 30%, 50%, 20% mechanical crushing method according to mass fraction and processes the conductor catalyst, as solid carbon fuel, in fuel, adds 20% conductor catalyst with petroleum coke.The petroleum coke that adds the conductor catalyst acted as a fuel place in the direct carbonate fuel cell anodes cavity, with 50mlmin -1The N of flow 2As the anode carrier gas, with 100mlmin -1The O of flow 2As cathode oxidant, 1000 ℃ of battery operated temperature.At this moment, SO-DCFC average power density under 0.7V constant voltage discharge operating mode is 1121Wm -2
Embodiment 4
Zirconia, NiO, Ca (NO with stabilized with yttrium oxide 3) 2Be respectively 40%, 30%, 30% solid-phase synthesis according to mass fraction and process the conductor catalyst, as solid carbon fuel, in fuel, add 15% conductor catalyst with carbon black.The carbon black that adds the conductor catalyst acted as a fuel place in the direct carbonate fuel cell anodes cavity, with 50mlmin -1The CO of flow 2As the anode carrier gas, with 100mlmin -1The O of flow 2As cathode oxidant, 800 ℃ of battery operated temperature.At this moment, SO-DCFC average power density under 0.7V constant voltage discharge operating mode is 1104Wm -2
Embodiment 5
With gadolinium oxide doped cerium oxide, Ag 2O, Mg (NO 3) 2Be respectively 40%, 30%, 30% solid-phase synthesis according to mass fraction and process the conductor catalyst, as solid carbon fuel, in fuel, add 15% conductor catalyst with organic waste materials.The organic waste materials that adds the conductor catalyst acted as a fuel place in the direct carbonate fuel cell anodes cavity, with 50mlmin -1The H of flow 2O is as the anode carrier gas, with 100mlmin -1The O of flow 2As cathode oxidant, 900 ℃ of battery operated temperature.At this moment, SO-DCFC average power density under 0.7V constant voltage discharge operating mode is 1004Wm -2
Embodiment 6
Zirconia, Ag with stabilized with yttrium oxide 2O, Mn (NO 3) 2Be respectively 40%, 30%, 30% solid-phase synthesis according to mass fraction and process the conductor catalyst, as solid carbon fuel, in fuel, add 15% conductor catalyst with graphite.The graphite that adds the conductor catalyst acted as a fuel place in the direct carbonate fuel cell anodes cavity, with 50mlmin -1The H of flow 2O is as the anode carrier gas, with 100mlmin -1The O of flow 2As cathode oxidant, 1000 ℃ of battery operated temperature.At this moment, SO-DCFC average power density under 0.7V constant voltage discharge operating mode is 1201Wm -2

Claims (9)

1. a conductor catalyst that improves the direct carbon consuming cell performance of soild oxide is characterized in that, said conductor catalyst is to be prepared from through mechanical crushing method or solid-phase synthesis after ion conductor, electronic conductor and the carbon gasification catalyst mix; Wherein, ion conductor, electronic conductor and carbon gasification catalyst account for the 10-93% of conductor catalyst gross mass, 5-93%, 1-93% respectively.
2. according to the said a kind of conductor catalyst that improves the direct carbon consuming cell performance of soild oxide of claim 1, it is characterized in that said ion conductor does Ion conductor or O 2-Ion conductor.
3. according to the said a kind of conductor catalyst that improves the direct carbon consuming cell performance of soild oxide of claim 2, it is characterized in that, said
Figure FDA0000075294430000012
Ion conductor is Li 2CO 3, Na 2CO 3Or K 2CO 3O 2-Ion conductor is the zirconia or the gadolinium oxide doped cerium oxide of stabilized with yttrium oxide.
4. according to the said a kind of conductor catalyst that improves the direct carbon consuming cell performance of soild oxide of claim 1, it is characterized in that said electronic conductor is selected from Ni, Fe, Ag, W, NiO, Ag 2Among the O one or more.
5. according to the said a kind of conductor catalyst that improves the direct carbon consuming cell performance of soild oxide of claim 1; It is characterized in that said carbon gasification catalyst is at least a material in carbonate, bicarbonate, sulfate or the nitrate of lithium, sodium, potassium, beryllium, magnesium, calcium, strontium, scandium, titanium, vanadium, manganese, iron, nickel, molybdenum or silver.
6. method that improves the direct carbon consuming cell performance of soild oxide; It is characterized in that; In solid carbon, add conductor catalyst as claimed in claim 1, the solid carbon that adds the conductor catalyst is acted as a fuel to be placed in the direct carbonate fuel cell anodes cavity, feeds anode carrier gas holding anode reaction atmosphere simultaneously; Negative electrode bubbling air or oxygen are as oxidant, and operating temperature range is 600～1000 ℃.
7. according to right 6 said a kind of methods that improve the direct carbon consuming cell performance of soild oxide, it is characterized in that the conductor catalyst of interpolation accounts for the 1-50% of solid carbon quality.
8. according to right 6 said a kind of methods that improve the direct carbon consuming cell performance of soild oxide, it is characterized in that said solid carbon is selected from one or more in carbon black, graphite, coke, biomass, coal, petroleum coke or the organic waste materials.
9. according to right 6 said a kind of methods that improve the direct carbon consuming cell performance of soild oxide, it is characterized in that said anode carrier gas is N 2, Ar, He, CO 2Or H 2O.
CN201110194653A 2011-07-12 2011-07-12 Conductor catalyst for enhancing performance of direct carbon fuel battery and method Pending CN102306809A (en)

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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN104538645A (en) * 2014-12-22 2015-04-22 山西大学 Preparation method of active coal coke powder for solid oxide fuel cells
CN110707347A (en) * 2019-09-11 2020-01-17 华中科技大学 High-power-density molten carbonate direct coal/carbon fuel cell

Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN101540411A (en) * 2009-04-15 2009-09-23 中国科学院上海硅酸盐研究所 Solid electrolyte direct carbon fuel cell
CN201845075U (en) * 2010-09-20 2011-05-25 东南大学 Tester for direct carbon fuel cell and direct carbon fuel half-cell of fluidized bed electrode
CN102088100A (en) * 2010-12-16 2011-06-08 清华大学 Method for improving performance of direct carbon fuel cell of solid oxide

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN101540411A (en) * 2009-04-15 2009-09-23 中国科学院上海硅酸盐研究所 Solid electrolyte direct carbon fuel cell
CN201845075U (en) * 2010-09-20 2011-05-25 东南大学 Tester for direct carbon fuel cell and direct carbon fuel half-cell of fluidized bed electrode
CN102088100A (en) * 2010-12-16 2011-06-08 清华大学 Method for improving performance of direct carbon fuel cell of solid oxide

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN104538645A (en) * 2014-12-22 2015-04-22 山西大学 Preparation method of active coal coke powder for solid oxide fuel cells
CN104538645B (en) * 2014-12-22 2016-09-28 山西大学 Active coke raw powder's production technology for SOFC
CN110707347A (en) * 2019-09-11 2020-01-17 华中科技大学 High-power-density molten carbonate direct coal/carbon fuel cell
CN110707347B (en) * 2019-09-11 2021-10-22 华中科技大学 High-power-density molten carbonate direct coal/carbon fuel cell

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Application publication date: 20120104