CN101237062B - A method for improving dispersing performance of the carbon power in the fused carbonate electrolyte - Google Patents

A method for improving dispersing performance of the carbon power in the fused carbonate electrolyte Download PDF

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Publication number
CN101237062B
CN101237062B CN2008100639486A CN200810063948A CN101237062B CN 101237062 B CN101237062 B CN 101237062B CN 2008100639486 A CN2008100639486 A CN 2008100639486A CN 200810063948 A CN200810063948 A CN 200810063948A CN 101237062 B CN101237062 B CN 101237062B
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powdered carbon
carbon
carbonate
preparation
mcdcfc
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CN101237062A (en
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王贵领
曹殿学
吕艳卓
王静
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HARBIN TIANBAO GRAPHITE TECHNOLOGY DEVELOPMENT CO., LTD.
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Harbin Engineering 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
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells

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Abstract

The present invention provides a method for improving the dispersion performance of carbon powder in molten carbonate electrolyte. K2CO3 and Li2CO3 are dissolved in water with a proportion of 32 to 68; carbon powder is added in so as to ensure that the K2CO3 and the Li2CO3 solution completely submerges carbon powder; the solution is stirred to be pasty, evaporated and crystallized so as to obtain the mixture of carbon powder and molten carbonate. The method has the advantages that: as the crystallization method is adopted to mix carbon and carbonate of MCDCFC, the crystallization method ensures that the carbonate can enter micropores of the carbon to be in sufficient contact with the carbon; after the carbonate is molten, the surface tension of the carbon is decreased, which is beneficial for attracting anions in the solution and reduce the hydrophobicity of the carbon. Therefore, the method can remarkably improve the performance of the MCDCFC with the carbon powder as fuel.

Description

A kind of method that improves powdered carbon dispersive property in fused carbonate electrolyte
(1) technical field
What the present invention relates to is a kind of manufacture method of battery, specifically a kind of method that improves the performance of battery.
(2) background technology
Fuel cell be a kind of directly that the chemical energy in the fuel is efficient by electrochemical reaction, change the green energy conversion equipment of electric energy into to environmental friendliness, can solve energy-conservation and environmental protection two big world difficult problems simultaneously.The direct carbon fuel cell of fused carbonate type (MCDCFC) is to be fuel with the solid powdered carbon, fused carbonate is an electrolyte, at high temperature the direct electro-oxidation reaction by charcoal transforms into electric energy with the chemical energy in the charcoal, its theoretical energy conversion efficiency can reach 100%, discharge amount of exhaust gas has only 1/10th of traditional coal fired power generation, and the solid carbon fuel source is abundant, cheap, so MCDCFC has bigger energy-saving and environmental protection and economic advantages than the molten carbonate fuel cell and the traditional coal fired power generation that with natural gas etc. are fuel.The reaction principle of the fused carbonate type fuel cell that directly acts as a fuel with solid carbon is schematically as follows:
Anode: C+2CO 3 2-→ 3CO 2+ 4e -
Negative electrode: O 2+ 2CO 2+ 4e -→ 2CO 3 2-
Overall reaction: C+O 2→ 2CO 2
The present mode such as employing machinery of mixing of powdered carbon and carbonate among the MCDCFC, the dispersive property of this mixed method charcoal in fused salt is poor, causes powdered carbon to contact poorly with electrolytical, and not only the electrochemical oxidation activity of charcoal is low, and the utilance of charcoal is also low.This is because the charcoal right and wrong are hydrophilic, and is low for the solvent affinity of polarity, CO 3 2-Be difficult to contact effectively with carbon surface, charcoal and carbonate layering are unfavorable for the reaction of (1) formula, cause the electro-chemical activity of charcoal less.This technical scheme is existing open report in following document: Cherepy N J, Krueger R, Fiet K J, et al.Direct conversion of carbon fuels in a molten carbonate fuelcell.Journal of the electrochemical society, 2005,152 (1): A80-A87, and CaoDian-Xue, Sun Yong, Wang Gui-Ling.Direct carbon fuel cell:Fundamentals andrecent developments.Journal of Power Sources, 2007,167:250-257.
(3) summary of the invention
The object of the present invention is to provide that a kind of can to overcome the mechanical mixing charcoal dispersed and contact performance is poor in fused carbonate, shortcomings such as charcoal and carbonate layering, the method for raising powdered carbon dispersive property in fused carbonate electrolyte of the problem that solution MCDCFC carbon anode discharging current is little.
The object of the present invention is achieved like this: water dissolving K 2CO 3And Li 2CO 3, its ratio is (28～36): (72～64), add powdered carbon, make K 2CO 3And Li 2CO 3The complete submergence powdered carbon of solution stirs into pasty state, at 70～95 ℃ of evaporative crystallizations, obtains the mixture of powdered carbon and fused carbonate.
The present invention can also comprise:
A kind of in powdered carbon that described powdered carbon is the powdered carbon of powdered carbon, the oil preparation of powdered carbon, the flue dust preparation of powdered carbon, the corn stalk preparation of powdered carbon, the coal preparation of pine preparation, made by organic substance pyrolysis such as polyethylene powder or the graphite powder.
The present invention proposes a kind of method of disperseing contact performance with anode charcoal in the crystallisation raising direct carbon fuel cell of fused carbonate (MCDCFC) in fused carbonate.It is dispersed and contact performance is poor in fused carbonate that this method has overcome the mechanical mixing charcoal, and shortcomings such as charcoal and carbonate layering have solved the little problem of MCDCFC carbon anode discharging current.It is characterized in that at first powdered carbon being dispersed in the carbonate aqueous solution, evaporation and concentration makes carbonate at carbon granule micropore and surface crystallization then, thereby increases charcoal and carbonate contact area, has improved the reactivity of charcoal.Essence of the present invention is by preliminary treatment, makes carbonate at carbon granule micropore and surface crystallization, increases charcoal and carbonate contact area, and the discharge performance of carbon anode has been improved in the easier duct that enters charcoal behind the carbonate fusion.
The invention has the advantages that the charcoal and the carbonate that adopt crystallisation mixing MCDCFC, crystallisation can make carbonate enter into the micropore of charcoal, fully contacts with charcoal, behind the carbonate fusion, reduce the surface tension of charcoal, helped attracting the anion in the solution, reduced the hydrophobicity of charcoal.Thereby to significantly improve with the powdered carbon be the performance of the MCDCFC of fuel.
(4) embodiment
For example the present invention is done in more detail below and describes:
Embodiment 1
Water dissolving K 2CO 3And Li 2CO 3, its ratio is 32: 68, adds the powdered carbon of pine preparation, makes K 2CO 3And Li 2CO 3The complete submergence powdered carbon of solution stirs into pasty state, and evaporative crystallization obtains the mixture of powdered carbon and fused carbonate.With NiO is negative electrode (being obtained through in-situ oxidation and lithiumation by foam Ni), 0.5atm O 2/ CO 2Be oxidant at=1: 2, γ-LiAlO 2Film is an electrolyte carrier barrier film, preparation MCDCFC, and at 700 ℃, under the 0.78V voltage, current density reaches 104mA/cm 2, corresponding power density reaches 81mW/cm 2
Embodiment 2
Water dissolving K 2CO 3And Li 2CO 3, its ratio is 32: 68, adds the powdered carbon of coal preparation, makes K 2CO 3And Li 2CO 3The complete submergence powdered carbon of solution stirs into pasty state, and evaporative crystallization obtains the mixture of powdered carbon and fused carbonate.With NiO is negative electrode (being obtained through in-situ oxidation and lithiumation by foam Ni), 0.5atm O 2/ CO 2Be oxidant at=1: 2, γ-LiAlO 2Film is an electrolyte carrier barrier film, preparation MCDCFC, and at 700 ℃, under the 0.8V voltage, current density reaches 110mA/cm 2, corresponding power density reaches 88mW/cm 2
Embodiment 3
Water dissolving K 2CO 3And Li 2CO 3, its ratio is 32: 68, adds the powdered carbon of corn stalk preparation, makes K 2CO 3And Li 2CO 3The complete submergence powdered carbon of solution stirs into pasty state, and evaporative crystallization obtains the mixture of powdered carbon and fused carbonate.With NiO is negative electrode (being obtained through in-situ oxidation and lithiumation by foam Ni), 0.5atmO 2/ CO 2Be oxidant at=1: 2, γ-LiAlO 2Film is an electrolyte carrier barrier film, preparation MCDCFC, and at 700 ℃, under the 0.8V voltage, current density reaches 115mA/cm 2, corresponding power density reaches 92mW/cm 2
Embodiment 4
Water dissolving K 2CO 3And Li 2CO 3, its ratio is 32: 68, adds flue dust, makes K 2CO 3And Li 2CO 3The complete submergence powdered carbon of solution stirs into pasty state, and evaporative crystallization obtains the mixture of powdered carbon and fused carbonate.With NiO is negative electrode (being obtained through in-situ oxidation and lithiumation by foam Ni), 0.5atm O 2/ CO 2Be oxidant at=1: 2, γ-LiAlO 2Film is an electrolyte carrier barrier film, preparation MCDCFC, and at 700 ℃, under the 0.8V voltage, current density reaches 75mA/cm 2, corresponding power density reaches 60mW/cm 2
Embodiment 5
Water dissolving K 2CO 3And Li 2CO 3, its ratio is 32: 68, adds the powdered carbon of oil preparation, makes K 2CO 3And Li 2CO 3The complete submergence powdered carbon of solution stirs into pasty state, and evaporative crystallization obtains the mixture of powdered carbon and fused carbonate.With NiO is negative electrode (being obtained through in-situ oxidation and lithiumation by foam Ni), 0.5atm O 2/ CO 2Be oxidant at=1: 2, γ-LiAlO 2Film is an electrolyte carrier barrier film, preparation MCDCFC, and at 700 ℃, under the 0.8V voltage, current density reaches 120mA/cm 2, corresponding power density reaches 96mW/cm 2
Embodiment 6
Water dissolving K 2CO 3And Li 2CO 3, its ratio is 32: 68, adds the polyethylene powder, makes K 2CO 3And Li 2CO 3The complete submergence powdered carbon of solution stirs into pasty state, and evaporative crystallization obtains the mixture of powdered carbon and fused carbonate.With NiO is negative electrode (being obtained through in-situ oxidation and lithiumation by foam Ni), 0.5atm O 2/ CO 2Be oxidant at=1: 2, γ-LiAlO 2Film is an electrolyte carrier barrier film, preparation MCDCFC, and at 700 ℃, under the 0.8V voltage, current density reaches 115mA/cm 2, corresponding power density reaches 92mW/cm 2
Embodiment 7
Water dissolving K 2CO 3And Li 2CO 3, its ratio is 32: 68, adds graphite powder, makes K 2CO 3And Li 2CO 3The complete submergence powdered carbon of solution stirs into pasty state, and evaporative crystallization obtains the mixture of powdered carbon and fused carbonate.With NiO is negative electrode (being obtained through in-situ oxidation and lithiumation by foam Ni), 0.5atm O 2/ CO 2Be oxidant at=1: 2, γ-LiAlO 2Film is an electrolyte carrier barrier film, preparation MCDCFC, and at 700 ℃, under the 0.8V voltage, current density reaches 85mA/cm 2, corresponding power density reaches 68mW/cm 2

Claims (1)

1. a method that improves powdered carbon dispersive property in fused carbonate electrolyte is characterized in that: water dissolving K 2CO 3And Li 2CO 3, its ratio is (28～36): (72～64), add powdered carbon, make K 2CO 3And Li 2CO 3The complete submergence powdered carbon of solution stirs into pasty state, at 70～95 ℃ of evaporative crystallizations, obtains the mixture of powdered carbon and fused carbonate; A kind of in powdered carbon that described powdered carbon is the powdered carbon of powdered carbon, the oil preparation of powdered carbon, the flue dust preparation of powdered carbon, the corn stalk preparation of powdered carbon, the coal preparation of pine preparation, made by the pyrolysis of polyethylene powder type organic or the graphite powder.
CN2008100639486A 2008-01-30 2008-01-30 A method for improving dispersing performance of the carbon power in the fused carbonate electrolyte Expired - Fee Related CN101237062B (en)

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JP2018185971A (en) * 2017-04-26 2018-11-22 国立大学法人岐阜大学 Direct carbon fuel cell
AU2018338093A1 (en) * 2017-09-20 2020-03-26 Energ2 Technologies, Inc. Hydrated carbon material powder and use of it for preparation of an electrode for an electrical storage device
CN114361533B (en) * 2022-01-10 2024-01-30 华北科技学院(中国煤矿安全技术培训中心) Test method of carbon fuel cell system with three-electrode structure

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Publication number Priority date Publication date Assignee Title
CN1929172A (en) * 2006-08-30 2007-03-14 天津大学 Carbon fuel battery using rod type or powder formed carbon fuel
CN101071872A (en) * 2007-06-07 2007-11-14 上海交通大学 Integrated preparing method for molten carbonate fuel cell electrolyte membrane

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN1929172A (en) * 2006-08-30 2007-03-14 天津大学 Carbon fuel battery using rod type or powder formed carbon fuel
CN101071872A (en) * 2007-06-07 2007-11-14 上海交通大学 Integrated preparing method for molten carbonate fuel cell electrolyte membrane

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