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WO2009061072A1 - Fuel process apparatus of multiple desulfurizers and fuel cell system with the same - Google Patents

Fuel process apparatus of multiple desulfurizers and fuel cell system with the same Download PDF

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Publication number
WO2009061072A1
WO2009061072A1 PCT/KR2008/005430 KR2008005430W WO2009061072A1 WO 2009061072 A1 WO2009061072 A1 WO 2009061072A1 KR 2008005430 W KR2008005430 W KR 2008005430W WO 2009061072 A1 WO2009061072 A1 WO 2009061072A1
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WO
WIPO (PCT)
Prior art keywords
fuel
desulfurizer
process apparatus
pipe
reformer
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/KR2008/005430
Other languages
French (fr)
Inventor
Myoung-Hoon Choi
Ho-Suk Kim
Byung-Sun Hong
Mee-Nam Shinn
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
FuelCellPower Co Ltd
Original Assignee
FuelCellPower Co Ltd
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by FuelCellPower Co Ltd filed Critical FuelCellPower Co Ltd
Priority to CN200880115059.8A priority Critical patent/CN101849314B/en
Publication of WO2009061072A1 publication Critical patent/WO2009061072A1/en
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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Classifications

    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
    • H01M8/0606—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants
    • H01M8/0612—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants from carbon-containing material
    • H01M8/0618—Reforming processes, e.g. autothermal, partial oxidation or steam reforming
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/02—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by adsorption, e.g. preparative gas chromatography
    • B01D53/04—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by adsorption, e.g. preparative gas chromatography with stationary adsorbents
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/46—Removing components of defined structure
    • B01D53/48—Sulfur compounds
    • B01D53/485—Sulfur compounds containing only one sulfur compound other than sulfur oxides or hydrogen sulfide
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
    • C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
    • C01B3/38—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • C01B2203/0283—Processes for making hydrogen or synthesis gas containing a CO-shift step, i.e. a water gas shift step
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
    • C01B2203/0435—Catalytic purification
    • C01B2203/044—Selective oxidation of carbon monoxide
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
    • C01B2203/0435—Catalytic purification
    • C01B2203/0445—Selective methanation
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
    • C01B2203/0465—Composition of the impurity
    • C01B2203/047—Composition of the impurity the impurity being carbon monoxide
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/06—Integration with other chemical processes
    • C01B2203/066—Integration with other chemical processes with fuel cells
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
    • C01B2203/1258—Pre-treatment of the feed
    • C01B2203/1264—Catalytic pre-treatment of the feed
    • C01B2203/127—Catalytic desulfurisation
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
    • H01M8/0662—Treatment of gaseous reactants or gaseous residues, e.g. cleaning
    • H01M8/0675—Removal of sulfur
    • 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

Definitions

  • the present invention relates to a fuel cell system that generates electrical energy by an electro-chemical reaction of hydrogen and oxygen, and more particularly, to an innovative fuel process apparatus that reforms fuel in a fuel cell system and efficiently removes sulfuric components in the fuel, and to a fuel cell system with the same.
  • a fuel cell system generates electrical energy through electro-chemical reactions using a fuel, which contains hydrogen, and air, which contains oxygen.
  • the fuel cell system generally includes the following elements. That is, the fuel cell system includes as main elements a fuel cell stack in which hydrogen and oxygen are involved in electro-chemical reactions, a fuel process apparatus that reforms the fuel into a reformed gas that contains hydrogen, and provides the reformed gas for the fuel cell stack, and an air-provider that provides air that contains oxygen to the fuel cell stack.
  • a fuel cell stack in which hydrogen and oxygen are involved in electro-chemical reactions
  • a fuel process apparatus that reforms the fuel into a reformed gas that contains hydrogen, and provides the reformed gas for the fuel cell stack
  • an air-provider that provides air that contains oxygen to the fuel cell stack.
  • the fuel process apparatus includes several reactors that are capable of removing elements that damage the fuel cell's capacity, during a process in which the fuel is transformed into a reformed gas that contains hydrogen.
  • Hydrocarbon such as LNG or LPG
  • odorants that are made up of sulfuric compounds are added to the hydrocarbon. Therefore, a conventional fuel process apparatus must include a desulfurizer among other reactors in order to remove sulfuric components or compounds in the fuel.
  • the fuel process apparatus fails to lower the amount of sulfuric components or compounds in the fuel below a certain level, the sulfuric components or compounds flow into a reformer. Then, the sulfuric components or compounds in the fuel are adsorbed into or poison a reforming catalyst in the reformer, causing the capacity of the reforming catalyst to deteriorate. As described above, deterioration of the capacity of a reforming catalyst is related to the capacity of generating a reformed gas that contains hydrogen, causing the problem of lowering the efficiency of electricity generation in the fuel cell stack. Moreover, the concentration of sulfuric components or compounds may rapidly change according to surroundings.
  • the present invention has been made in an effort to provide an innovative fuel process apparatus that is capable of lowering the amount of sulfuric components or compounds to below a certain level even though the concentration of the sulfuric components or sulfuric compounds in the fuel changes rapidly, and a fuel cell system including the same.
  • the present invention has been made in an effort to provide a fuel process apparatus and a fuel cell system, wherein the capacity of a reforming catalyst in a reformer deteriorates less than a conventional one and a replacement period of the reformer may become relatively longer even though the catalyst is used for a long time.
  • a fuel process apparatus for a fuel cell system includes a first desulfurizer through which fuel for a fuel cell system passes and that includes an adsorbent that adsorbs sulfuric components in the fuel, and a second desulfurizer through which the fuel passes and that includes a desulfurizing catalyst involved in an exothermic reaction with the sulfuric components in the fuel, wherein the second desulfurizer is connected to the first desulfurizer.
  • the fuel process apparatus for the fuel cell system further includes a reformer through which the fuel passes and that reforms the fuel into a reforming gas that contains hydrogen, wherein the reformer is connected to the second desulfurizer.
  • the fuel process apparatus may further include a case body that contains the second desulfurizer and the reformer, wherein the first desulfurizer is disposed outside the case body.
  • a first pipe may be connected to the first desulfurizer such that the fuel flows into the first desulfurizer from outside, the first desulfurizer and the second desulfurizer may be connected via a second pipe, and the first pipe and the second pipe may be connected via a third pipe such that the fuel bypasses the first desulfurizer.
  • a diverter valve that converts the inflow path of the fuel may be disposed at the point where the first pipe and the third pipe are connected.
  • the second desulfurizer and the reformer may be connected via a fourth pipe, and the second pipe and the fourth pipe may be connected via a fifth pipe such that the fuel bypasses the second desulfurizer.
  • a first solenoid valve may be disposed at the second pipe, the first solenoid valve selectively controlling the flow of the fuel, and a second solenoid valve may be disposed at the fifth pipe, wherein the second solenoid valve selectively controls the flow of the fuel, and wherein the operation of the second solenoid valve is related to that of the first solenoid valve.
  • At least one of activated carbon, synthesized zeolite, and iron oxide may be used as the adsorbent in the first desulfurizer.
  • the second desulfurizer may transform the sulfuric components into hydrogen sulfide (H 2 S) and cause an exothermic reaction involving the desulfurizing catalyst.
  • Zinc oxide may be used as the desulfurizing catalyst.
  • a fuel cell system includes a fuel cell stack generating electrical energy through an electro-chemical reaction of hydrogen and oxygen, a fuel process apparatus reforming fuel into a reformed gas that contains hydrogen and providing the reformed gas to the fuel cell stack, and an air provider providing air to the fuel cell stack.
  • the fuel process apparatus may include a first desulfurizer through which the fuel passes and that includes an adsorbent that adsorbs sulfuric components in the fuel, a second desulfurizer through which the fuel passes and that includes a desulfurizing catalyst involved in an exothermic reaction with the sulfuric components in the fuel, wherein the second desulfurizer is connected to the first desulfurizer, and a reformer through which the fuel passes and that reforms the fuel into a reforming gas that contains hydrogen, wherein the reformer is connected to the second desulfurizer.
  • ADVANTAGEOUS EFFECTS ADVANTAGEOUS EFFECTS
  • a fuel process apparatus includes a multiple desulfurizing structure such that the capacity of a reforming catalyst in a reformer deteriorates less than a conventional one even though the concentration of the sulfuric components or compounds in the fuel changes rapidly. Consequently, the capacity of the reformer endures longer than a conventional one, and the stability and durability of the fuel process apparatus according to an exemplary embodiment of the present invention is improved.
  • the capacity of a reforming catalyst deteriorates less rapidly than a conventional one and a replacement period of the reformer becomes relatively longer.
  • the exemplary embodiment of the present invention costs less to maintain and is also more convenient to maintain.
  • FIG. 1 is a schematic view of elements of a fuel cell system.
  • FIG. 2 is a schematic view of elements of a fuel process apparatus according to a first exemplary embodiment of the present invention.
  • FIG. 3 is a schematic view of elements of a fuel process apparatus according to a second exemplary embodiment of the present invention.
  • FIG. 4 is a schematic view of elements of a fuel process apparatus according to a third exemplary embodiment of the present invention.
  • first desulfurizer 120, 220, 320 second desulfurizer
  • FIG. 1 is a schematic view of elements of a fuel cell system.
  • a fuel cell system includes a fuel cell stack 10 that generates electrical energy through an electro-chemical reaction of hydrogen and oxygen, a fuel process apparatus 100 that reforms fuel into a reformed gas that contains hydrogen, and an air provider 30 that provides oxygen to the fuel cell stack 10. Further, the fuel cell system includes an electrical power transformer 40 that transforms DC power into AC power, a cooler 50 that cools the fuel cell stack 10 to below a certain temperature, other devices (BOP, balance of plants), and a controller.
  • BOP balance of plants
  • the fuel cell system uses a hydrocarbon such as liquefied natural gas (LNG) or liquefied petroleum gas (LPG) as a fuel.
  • a hydrocarbon such as liquefied natural gas (LNG) or liquefied petroleum gas (LPG) as a fuel.
  • LNG liquefied natural gas
  • LPG liquefied petroleum gas
  • An odorant is added to the hydrocarbon fuel such that leaked gas can be easily detected if the gas is leaked.
  • the odorant is mainly made up of sulfuric compounds.
  • the fuel process apparatus 100 includes a desulfurizer in order to lower the amount of the sulfuric components or compounds to below a predetermined level in advance of a reformer, as well as the reformer that reforms the fuel into a reformed gas that contains hydrogen.
  • the fuel process apparatus 100 includes the following elements.
  • FIG. 2 is a schematic view of elements of a fuel process apparatus according to a first exemplary embodiment of the present invention.
  • the fuel process apparatus 100 includes a first desulfurizer 110 through which the fuel passes in the first place.
  • the first desulfurizer 110 includes an adsorbent that adsorbs sulfuric components in the fuel, and reduces the amount of the sulfuric components or compounds in the fuel as a first step.
  • At least one of activated carbon, synthesized zeolite (for example, molecular sieves), and iron oxide may be used as the adsorbent in the first desulfurizer 110. That is, the first desulfurizer 110 may reduce the amount of the sulfuric components or compounds in the fuel by causing the sulfuric components or compounds to be adsorbed into the surface of the adsorbent.
  • the first desulfurizer 110 is called a low-temperature-type desulfurizer since it involves low heat generation when the sulfuric components or compounds are adsorbed into the surface of the adsorbent.
  • the second desulfurizer 120 is connected to the first desulfurizer 110.
  • the second desulfurizer 120 is designed such that the fuel passes through it, and includes a desulfurizing catalyst that causes an exothermic reaction with the sulfuric components or compounds in the fuel.
  • the second desulfurizer 120 transforms the sulfuric components or compounds into hydrogen sulfide (H 2 S) through hydrodesulfurisation (HDS), and then removes the sulfuric components or compounds by combining the hydrogen sulfide with zinc oxide (ZnO), which is a desulfurizing catalyst.
  • the second desulfurizer 120 is more capable of removing the sulfuric components or compounds that the first desulfurizer 110.
  • the second desulfurizer 120 is called a high- temperature-type desulfurizer since it involves higher heat generation than the first desulfurizer 110.
  • the second desulfurizer 120 is disposed inside a case body 101 of the fuel process apparatus 100, and the first desulfurizer 110 is disposed outside the case body 101. That is, the first desulfurizer 110 is less capable of removing the sulfuric components or compounds than the second desulfurizer 120 such that the adsorbent in the first desulfurizer 110 is regularly replaced. Consequently, the second desulfurizer 120 is disposed inside the case body 101 together with other reactors of the fuel process apparatus 100 during the manufacturing process. On the other hand, the first desulfurizer 110 is disposed at a pipe through which the fuel flows in, other than inside the case body 101.
  • the sulfuric components or compounds in the fuel are reduced by the first desulfurizer 110 in the first instance, and then are removed to below a predetermined level by the second desulfurizer 120.
  • the first desulfurizer 10 may keep removing the sulfuric components or compounds in the fuel as long as the adsorbent is regularly replaced.
  • the second desulfurizer 120 has a longer replacement period than the first desulfurizer 110 in removing the sulfuric components or compounds in the fuel. Therefore, the second desulfurizer 120 is disposed inside the case body 101 , and the second desulfurizer 120 has a long replacement period, while it is rather difficult to replace the second desulfurizer 120.
  • the reformer 130 is connected to the second desulfurizer 120, and is designed such that the fuel passes through it. Then, the fuel loses the sulfuric components or compounds by passing through the first desulfurizer 110 and the second desulfurizer 120, and flows into the reformer 130 as a reacting gas without the sulfuric components or compounds.
  • the reformer 130 causes a catalyst reaction of the reacting gas and reforms the reacting gas into a reformed gas that contains plenty of hydrogen.
  • the carbon monoxide reducer 140 in the first place, reduces the concentration of carbon monoxide in the reformed gas that is provided by the reformer 130. Subsequently, the carbon monoxide remover 150 removes the concentration of carbon monoxide in the reformed gas below 10ppm.
  • the fuel process apparatus 100 further includes auxiliary devices such as a burner that provides heat for the reforming reaction, an igniter for igniting the burner, and a temperature sensor.
  • auxiliary devices such as a burner that provides heat for the reforming reaction, an igniter for igniting the burner, and a temperature sensor.
  • the fuel process apparatus 100 may reduce the sulfuric components or compounds through the first desulfurizer 110 in the first place and then remove them to below a predetermined level through the second desulfurizer 120 even though the concentration of the sulfuric components or compounds in the fuel changes rapidly as the surrounding condition changes.
  • the fuel process apparatus 100 may have a longer replacement period of the second desulfurizer 120 by replacing the adsorbent of the first desulfurizer 110.
  • FIG. 3 is a schematic view of elements of a fuel process apparatus according to a second exemplary embodiment of the present invention.
  • a fuel process apparatus 200 has feature that a fuel bypasses the first desulfurizer 210. That is, the first desulfurizer 210 is connected to a first pipe 202 through which the fuel flows in from outside.
  • the first desulfurizer 210 and a second desulfurizer 220 are connected via a second pipe 240.
  • the first pipe 202 and the second pipe 204 are connected via a third pipe 260 such that the fuel bypasses the first desulfurizer 210.
  • a diverter valve 270 that converts the inflow path of the fuel is disposed at the point where the first pipe 202 and the third pipe 260 are connected.
  • a solenoid valve 271 is disposed at the second pipe 204.
  • the fuel process apparatus 200 causes the diverter valve 270 to let the fuel flow into the third pipe 260, and keeps the first solenoid valve 271 closed. Then, the fuel provided from outside bypasses the first desulfurizer 210 and directly flows into the second desulfurizer 220.
  • the second desulfurizer 220 may cause a higher heat generation, and may heat up to a temperature above a predetermined level.
  • the fuel process apparatus 200 detects the temperature of the second desulfurizer 2210 by a temperature sensor and converts the inflow path of the fuel by operating the diverter valve 270 and the first solenoid valve 271 , respectively. Then, the fuel passes through the first desulfurizer 210 and the second desulfurizer 220 sequentially, dealing with plenty of sulfuric components or compounds.
  • the fuel process apparatus 200 according to the second exemplary embodiment may effectively respond to and deal with the condition when the concentration of the sulfuric components or compounds in the fuel rapidly changes according to the surrounding condition, using the first desulfurizer 210 and the second desulfurizer 220.
  • the fuel process apparatus 200 according to the second exemplary embodiment causes the fuel to bypass the first desulfurizer 210 and makes it possible to replace the adsorbent in the first desulfurizer 210 even during operation of the fuel process apparatus 200.
  • FIG. 4 is a schematic view of elements of a fuel process apparatus according to a third exemplary embodiment of the present invention.
  • the fuel process apparatus 300 features that the second desulfurizer 320 is bypassed. That is, the second desulfurizer 320 and the reformer 330 are connected via the fourth pipe 306.
  • the second pipe 304 and the fourth pipe 306 are connected via the fifth pipe 361 such that the fuel bypasses the second desulfurizer 320.
  • a first solenoid valve 371 that selectively controls the flow of the fuel is disposed at the second pipe 304
  • a second solenoid valve 372 that selectively controls the flow of the fuel is disposed at the fifth pipe 361.
  • the operation of the second solenoid valve 372 is related to that of the first solenoid valve 371.
  • a third solenoid valve 373 that selectively controls the flow of the fuel is disposed at the fourth pipe 306.
  • the fuel process apparatus 300 keeps the first and third solenoid valves 371 , 373 closed and the second solenoid valve 372 open. Consequently, the fuel that passes through the first desulfurizer 310 does not pass through the second desulfurizer 320 but directly flows into the reformer 330. That is, the fuel process apparatus 300 may deal with the fuel only by the first desulfurizer 310 when the amount of the fuel is small. Further, the fuel process apparatus 300 causes the fuel to bypass the second desulfurizer 220 and makes it possible to replace the second desulfurizer 220 even during operation of the fuel process apparatus 300.
  • the fuel process apparatus 300 may include one diverter valve at the point where the second and fifth pipes 304, 361 are connected, instead of the first and second solenoid valves 371 , 372.
  • the reference numerals 301 , 340, and 350 are a case body, a carbon monoxide reducer, and a carbon monoxide remover, respectively.

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Abstract

The present invention relates to a fuel process apparatus of multiple desulfurizers and a fuel cell system including the same. A fuel process apparatus for a fuel cell system according to an exemplary embodiment of the present invention includes a first desulfurizer through which fuel passes and that includes an adsorbent that adsorbs sulfuric components in the fuel, and a second desulfurizer through which the fuel passes and that includes a desulfurizing catalyst involved in an exothermic reaction with the sulfuric components in the fuel, wherein the second desulfurizer is connected to the first desulfurizer. The fuel process apparatus for a fuel cell system further includes a reformer through which the fuel passes and that reforms the fuel into a reformed gas that contains hydrogen, wherein the reformer is connected to the second desulfurizer.

Description

FUEL PROCESS APPARATUS OF MULTIPLE DESULFURIZERS AND FUEL
CELL SYSTEM WITH THE SAME
TECHNICAL FIELD The present invention relates to a fuel cell system that generates electrical energy by an electro-chemical reaction of hydrogen and oxygen, and more particularly, to an innovative fuel process apparatus that reforms fuel in a fuel cell system and efficiently removes sulfuric components in the fuel, and to a fuel cell system with the same. BACKGROUND ART
A fuel cell system generates electrical energy through electro-chemical reactions using a fuel, which contains hydrogen, and air, which contains oxygen.
The fuel cell system generally includes the following elements. That is, the fuel cell system includes as main elements a fuel cell stack in which hydrogen and oxygen are involved in electro-chemical reactions, a fuel process apparatus that reforms the fuel into a reformed gas that contains hydrogen, and provides the reformed gas for the fuel cell stack, and an air-provider that provides air that contains oxygen to the fuel cell stack.
The fuel process apparatus includes several reactors that are capable of removing elements that damage the fuel cell's capacity, during a process in which the fuel is transformed into a reformed gas that contains hydrogen.
Hydrocarbon, such as LNG or LPG, is used as the fuel, and odorants that are made up of sulfuric compounds are added to the hydrocarbon. Therefore, a conventional fuel process apparatus must include a desulfurizer among other reactors in order to remove sulfuric components or compounds in the fuel.
If the fuel process apparatus fails to lower the amount of sulfuric components or compounds in the fuel below a certain level, the sulfuric components or compounds flow into a reformer. Then, the sulfuric components or compounds in the fuel are adsorbed into or poison a reforming catalyst in the reformer, causing the capacity of the reforming catalyst to deteriorate. As described above, deterioration of the capacity of a reforming catalyst is related to the capacity of generating a reformed gas that contains hydrogen, causing the problem of lowering the efficiency of electricity generation in the fuel cell stack. Moreover, the concentration of sulfuric components or compounds may rapidly change according to surroundings.
Therefore, there is a problem that the conventional fuel process apparatus may not properly operate due to a rapid change of concentration of the sulfuric components or compounds.
DISCLOSURE
TECHNICAL PROBLEM
The present invention has been made in an effort to provide an innovative fuel process apparatus that is capable of lowering the amount of sulfuric components or compounds to below a certain level even though the concentration of the sulfuric components or sulfuric compounds in the fuel changes rapidly, and a fuel cell system including the same.
In addition, the present invention has been made in an effort to provide a fuel process apparatus and a fuel cell system, wherein the capacity of a reforming catalyst in a reformer deteriorates less than a conventional one and a replacement period of the reformer may become relatively longer even though the catalyst is used for a long time. TECHNICAL SOLUTION
A fuel process apparatus for a fuel cell system according to an exemplary embodiment of the present invention includes a first desulfurizer through which fuel for a fuel cell system passes and that includes an adsorbent that adsorbs sulfuric components in the fuel, and a second desulfurizer through which the fuel passes and that includes a desulfurizing catalyst involved in an exothermic reaction with the sulfuric components in the fuel, wherein the second desulfurizer is connected to the first desulfurizer. The fuel process apparatus for the fuel cell system further includes a reformer through which the fuel passes and that reforms the fuel into a reforming gas that contains hydrogen, wherein the reformer is connected to the second desulfurizer.
The fuel process apparatus may further include a case body that contains the second desulfurizer and the reformer, wherein the first desulfurizer is disposed outside the case body.
A first pipe may be connected to the first desulfurizer such that the fuel flows into the first desulfurizer from outside, the first desulfurizer and the second desulfurizer may be connected via a second pipe, and the first pipe and the second pipe may be connected via a third pipe such that the fuel bypasses the first desulfurizer. A diverter valve that converts the inflow path of the fuel may be disposed at the point where the first pipe and the third pipe are connected.
The second desulfurizer and the reformer may be connected via a fourth pipe, and the second pipe and the fourth pipe may be connected via a fifth pipe such that the fuel bypasses the second desulfurizer. A first solenoid valve may be disposed at the second pipe, the first solenoid valve selectively controlling the flow of the fuel, and a second solenoid valve may be disposed at the fifth pipe, wherein the second solenoid valve selectively controls the flow of the fuel, and wherein the operation of the second solenoid valve is related to that of the first solenoid valve. At least one of activated carbon, synthesized zeolite, and iron oxide may be used as the adsorbent in the first desulfurizer.
The second desulfurizer may transform the sulfuric components into hydrogen sulfide (H2S) and cause an exothermic reaction involving the desulfurizing catalyst. Zinc oxide may be used as the desulfurizing catalyst. A fuel cell system according to an exemplary embodiment of the present invention includes a fuel cell stack generating electrical energy through an electro-chemical reaction of hydrogen and oxygen, a fuel process apparatus reforming fuel into a reformed gas that contains hydrogen and providing the reformed gas to the fuel cell stack, and an air provider providing air to the fuel cell stack. The fuel process apparatus may include a first desulfurizer through which the fuel passes and that includes an adsorbent that adsorbs sulfuric components in the fuel, a second desulfurizer through which the fuel passes and that includes a desulfurizing catalyst involved in an exothermic reaction with the sulfuric components in the fuel, wherein the second desulfurizer is connected to the first desulfurizer, and a reformer through which the fuel passes and that reforms the fuel into a reforming gas that contains hydrogen, wherein the reformer is connected to the second desulfurizer. ADVANTAGEOUS EFFECTS
A fuel process apparatus according to an exemplary embodiment of the present invention includes a multiple desulfurizing structure such that the capacity of a reforming catalyst in a reformer deteriorates less than a conventional one even though the concentration of the sulfuric components or compounds in the fuel changes rapidly. Consequently, the capacity of the reformer endures longer than a conventional one, and the stability and durability of the fuel process apparatus according to an exemplary embodiment of the present invention is improved.
Further, according to an exemplary embodiment of the present invention, the capacity of a reforming catalyst deteriorates less rapidly than a conventional one and a replacement period of the reformer becomes relatively longer.
Consequently, the exemplary embodiment of the present invention costs less to maintain and is also more convenient to maintain.
DESCRIPTION OF DRAWINGS FIG. 1 is a schematic view of elements of a fuel cell system.
FIG. 2 is a schematic view of elements of a fuel process apparatus according to a first exemplary embodiment of the present invention.
FIG. 3 is a schematic view of elements of a fuel process apparatus according to a second exemplary embodiment of the present invention.
FIG. 4 is a schematic view of elements of a fuel process apparatus according to a third exemplary embodiment of the present invention.
<Description of Reference Numerals Indicating Primary Elements in the Drawings>
100, 200, 300 : fuel process apparatus 101 , 201 , 301 : case body
110, 210, 310 : first desulfurizer 120, 220, 320 : second desulfurizer
130, 230, 330 : reformer 140, 240, 340 : carbon monoxide reducer
150, 250, 350 : carbon monoxide remover BEST MODE
Hereinafter, a detailed description of exemplary embodiments of the present invention will be provided in reference to the accompanying drawings so that those skilled in the art will have no difficulty in realizing them. As those skilled in the art would realize, the described embodiments may be modified in various different ways, all without departing from the spirit or scope of the present invention.
FIG. 1 is a schematic view of elements of a fuel cell system.
As shown in FIG. 1 , a fuel cell system according to an exemplary embodiment of the present invention includes a fuel cell stack 10 that generates electrical energy through an electro-chemical reaction of hydrogen and oxygen, a fuel process apparatus 100 that reforms fuel into a reformed gas that contains hydrogen, and an air provider 30 that provides oxygen to the fuel cell stack 10. Further, the fuel cell system includes an electrical power transformer 40 that transforms DC power into AC power, a cooler 50 that cools the fuel cell stack 10 to below a certain temperature, other devices (BOP, balance of plants), and a controller.
The fuel cell system uses a hydrocarbon such as liquefied natural gas (LNG) or liquefied petroleum gas (LPG) as a fuel. An odorant is added to the hydrocarbon fuel such that leaked gas can be easily detected if the gas is leaked. The odorant is mainly made up of sulfuric compounds.
As described above, however, sulfuric components or compounds may lower the capacity of a reformer and cause the efficiency of electricity generation to deteriorate. Consequently, the fuel process apparatus 100 includes a desulfurizer in order to lower the amount of the sulfuric components or compounds to below a predetermined level in advance of a reformer, as well as the reformer that reforms the fuel into a reformed gas that contains hydrogen. The fuel process apparatus 100 includes the following elements. FIG. 2 is a schematic view of elements of a fuel process apparatus according to a first exemplary embodiment of the present invention.
As shown in FIG. 2, the fuel process apparatus 100 includes a first desulfurizer 110 through which the fuel passes in the first place. The first desulfurizer 110 includes an adsorbent that adsorbs sulfuric components in the fuel, and reduces the amount of the sulfuric components or compounds in the fuel as a first step. At least one of activated carbon, synthesized zeolite (for example, molecular sieves), and iron oxide may be used as the adsorbent in the first desulfurizer 110. That is, the first desulfurizer 110 may reduce the amount of the sulfuric components or compounds in the fuel by causing the sulfuric components or compounds to be adsorbed into the surface of the adsorbent. The first desulfurizer 110 is called a low-temperature-type desulfurizer since it involves low heat generation when the sulfuric components or compounds are adsorbed into the surface of the adsorbent.
The second desulfurizer 120 is connected to the first desulfurizer 110. The second desulfurizer 120 is designed such that the fuel passes through it, and includes a desulfurizing catalyst that causes an exothermic reaction with the sulfuric components or compounds in the fuel. The second desulfurizer 120 transforms the sulfuric components or compounds into hydrogen sulfide (H2S) through hydrodesulfurisation (HDS), and then removes the sulfuric components or compounds by combining the hydrogen sulfide with zinc oxide (ZnO), which is a desulfurizing catalyst. The second desulfurizer 120 is more capable of removing the sulfuric components or compounds that the first desulfurizer 110. Further, the second desulfurizer 120 is called a high- temperature-type desulfurizer since it involves higher heat generation than the first desulfurizer 110.
In addition, the second desulfurizer 120 is disposed inside a case body 101 of the fuel process apparatus 100, and the first desulfurizer 110 is disposed outside the case body 101. That is, the first desulfurizer 110 is less capable of removing the sulfuric components or compounds than the second desulfurizer 120 such that the adsorbent in the first desulfurizer 110 is regularly replaced. Consequently, the second desulfurizer 120 is disposed inside the case body 101 together with other reactors of the fuel process apparatus 100 during the manufacturing process. On the other hand, the first desulfurizer 110 is disposed at a pipe through which the fuel flows in, other than inside the case body 101. The sulfuric components or compounds in the fuel are reduced by the first desulfurizer 110 in the first instance, and then are removed to below a predetermined level by the second desulfurizer 120. In consideration of the manufacturing cost, the first desulfurizer 10 may keep removing the sulfuric components or compounds in the fuel as long as the adsorbent is regularly replaced. Further, the second desulfurizer 120 has a longer replacement period than the first desulfurizer 110 in removing the sulfuric components or compounds in the fuel. Therefore, the second desulfurizer 120 is disposed inside the case body 101 , and the second desulfurizer 120 has a long replacement period, while it is rather difficult to replace the second desulfurizer 120.
The reformer 130 is connected to the second desulfurizer 120, and is designed such that the fuel passes through it. Then, the fuel loses the sulfuric components or compounds by passing through the first desulfurizer 110 and the second desulfurizer 120, and flows into the reformer 130 as a reacting gas without the sulfuric components or compounds. The reformer 130 causes a catalyst reaction of the reacting gas and reforms the reacting gas into a reformed gas that contains plenty of hydrogen.
The carbon monoxide reducer 140, in the first place, reduces the concentration of carbon monoxide in the reformed gas that is provided by the reformer 130. Subsequently, the carbon monoxide remover 150 removes the concentration of carbon monoxide in the reformed gas below 10ppm.
In addition to the above, the fuel process apparatus 100 further includes auxiliary devices such as a burner that provides heat for the reforming reaction, an igniter for igniting the burner, and a temperature sensor.
With the above described structure, the fuel process apparatus 100 may reduce the sulfuric components or compounds through the first desulfurizer 110 in the first place and then remove them to below a predetermined level through the second desulfurizer 120 even though the concentration of the sulfuric components or compounds in the fuel changes rapidly as the surrounding condition changes. Particularly, the fuel process apparatus 100 may have a longer replacement period of the second desulfurizer 120 by replacing the adsorbent of the first desulfurizer 110. FIG. 3 is a schematic view of elements of a fuel process apparatus according to a second exemplary embodiment of the present invention.
As shown in FIG. 3, a fuel process apparatus 200 according to the second exemplary embodiment of the present invention has feature that a fuel bypasses the first desulfurizer 210. That is, the first desulfurizer 210 is connected to a first pipe 202 through which the fuel flows in from outside. The first desulfurizer 210 and a second desulfurizer 220 are connected via a second pipe 240. The first pipe 202 and the second pipe 204 are connected via a third pipe 260 such that the fuel bypasses the first desulfurizer 210. Further, a diverter valve 270 that converts the inflow path of the fuel is disposed at the point where the first pipe 202 and the third pipe 260 are connected. A solenoid valve 271 is disposed at the second pipe 204.
That is, in a normal operating condition, the fuel process apparatus 200 causes the diverter valve 270 to let the fuel flow into the third pipe 260, and keeps the first solenoid valve 271 closed. Then, the fuel provided from outside bypasses the first desulfurizer 210 and directly flows into the second desulfurizer 220. Here, when the fuel contains a lot of sulfuric components or compounds the second desulfurizer 220 may cause a higher heat generation, and may heat up to a temperature above a predetermined level. The fuel process apparatus 200 detects the temperature of the second desulfurizer 2210 by a temperature sensor and converts the inflow path of the fuel by operating the diverter valve 270 and the first solenoid valve 271 , respectively. Then, the fuel passes through the first desulfurizer 210 and the second desulfurizer 220 sequentially, dealing with plenty of sulfuric components or compounds.
As described above, the fuel process apparatus 200 according to the second exemplary embodiment may effectively respond to and deal with the condition when the concentration of the sulfuric components or compounds in the fuel rapidly changes according to the surrounding condition, using the first desulfurizer 210 and the second desulfurizer 220. Particularly, the fuel process apparatus 200 according to the second exemplary embodiment causes the fuel to bypass the first desulfurizer 210 and makes it possible to replace the adsorbent in the first desulfurizer 210 even during operation of the fuel process apparatus 200.
In FIG. 3, the reference numerals 201 , 230, 240, and 250 are a case body, a reformer, a carbon monoxide reducer, and a carbon monoxide remover, respectively. FIG. 4 is a schematic view of elements of a fuel process apparatus according to a third exemplary embodiment of the present invention.
As shown in FIG. 4, the fuel process apparatus 300 according to the third exemplary embodiment of the present invention features that the second desulfurizer 320 is bypassed. That is, the second desulfurizer 320 and the reformer 330 are connected via the fourth pipe 306. The second pipe 304 and the fourth pipe 306 are connected via the fifth pipe 361 such that the fuel bypasses the second desulfurizer 320. Further, a first solenoid valve 371 that selectively controls the flow of the fuel is disposed at the second pipe 304, and a second solenoid valve 372 that selectively controls the flow of the fuel is disposed at the fifth pipe 361. In addition, the operation of the second solenoid valve 372 is related to that of the first solenoid valve 371. Moreover, a third solenoid valve 373 that selectively controls the flow of the fuel is disposed at the fourth pipe 306.
With the above described structure, the fuel process apparatus 300 according to the third exemplary embodiment of the present invention keeps the first and third solenoid valves 371 , 373 closed and the second solenoid valve 372 open. Consequently, the fuel that passes through the first desulfurizer 310 does not pass through the second desulfurizer 320 but directly flows into the reformer 330. That is, the fuel process apparatus 300 may deal with the fuel only by the first desulfurizer 310 when the amount of the fuel is small. Further, the fuel process apparatus 300 causes the fuel to bypass the second desulfurizer 220 and makes it possible to replace the second desulfurizer 220 even during operation of the fuel process apparatus 300.
In addition, the fuel process apparatus 300 according to the third exemplary embodiment of the present invention may include one diverter valve at the point where the second and fifth pipes 304, 361 are connected, instead of the first and second solenoid valves 371 , 372. In FIG. 4, the reference numerals 301 , 340, and 350 are a case body, a carbon monoxide reducer, and a carbon monoxide remover, respectively.
While this invention has been described in connection with what is presently considered to be practical exemplary embodiments, it is to be understood that the invention is not limited to the disclosed embodiments, but, on the contrary, is intended to cover various modifications and equivalent arrangements included within the spirit and scope of the appended claims.

Claims

1. A fuel cell process apparatus comprising: a first desulfurizer through which fuel for a fuel cell system passes and that includes an adsorbent that adsorbs sulfuric components in the fuel; a second desulfurizer through which the fuel passes and that includes a desulfurizing catalyst involved in an exothermic reaction with the sulfuric components in the fuel, wherein the second desulfurizer is connected to the first desulfurizer; and a reformer through which the fuel passes and that reforms the fuel into a reforming gas that contains hydrogen, wherein the reformer is connected to the second desulfurizer.
2. The fuel process apparatus of claim 1 , further including a case body that contains the second desulfurizer and the reformer, wherein the first desulfurizer is disposed outside the case body.
3. The fuel process apparatus of claim 1 , wherein a first pipe is connected to the first desulfurizer such that the fuel flows into the first desulfurizer from outside, the first desulfurizer and the second desulfurizer are connected via a second pipe, and the first pipe and the second pipe are connected via a third pipe such that the fuel bypasses the first desulfurizer.
4. The fuel process apparatus of claim 3, wherein a diverter valve that converts the inflow path of the fuel is disposed at the point where the first pipe and the third pipe are connected.
5. The fuel process apparatus of claim 4, wherein the second desulfurizer and the reformer are connected via a fourth pipe, and the second pipe and the fourth pipe are connected via a fifth pipe such that the fuel bypasses the second desulfurizer.
6. The fuel process apparatus of claim 5, wherein a first solenoid valve is disposed at the second pipe, the first solenoid valve selectively controlling the flow of the fuel, and a second solenoid valve is disposed at the fifth pipe, wherein the second solenoid valve selectively controls the flow of the fuel, and wherein the operation of the second solenoid valve is related to that of the first solenoid valve.
7. The fuel process apparatus of one of claims 1-6, wherein at least one of activated carbon, synthesized zeolite, and iron oxide is used as the adsorbent in the first desulfurizer.
8. The fuel process apparatus of one of claims 1-6, wherein the second desulfurizer transforms the sulfuric components into hydrogen sulfide (H2S) and causes an exothermic reaction involving the desulfurizing catalyst.
9. The fuel process apparatus of claim 8, wherein zinc oxide is used as the desulfurizing catalyst.
10. A fuel cell system comprising: a fuel cell stack generating electrical energy through an electro-chemical reaction of hydrogen and oxygen; a fuel process apparatus reforming fuel into a reformed gas that contains hydrogen and providing the reformed gas to the fuel cell stack; and an air provider providing air to the fuel cell stack, wherein the fuel process apparatus includes a first desulfurizer through which the fuel passes and that includes an adsorbent that adsorbs sulfuric components in the fuel, a second desulfurizer through which the fuel passes and that includes a desulfurizing catalyst involved in an exothermic reaction with the sulfuric components in the fuel, wherein the second desulfurizer is connected to the first desulfurizer, and a reformer through which the fuel passes and that reforms the fuel into a reforming gas that contains hydrogen, wherein the reformer is connected to the second desulfurizer.
PCT/KR2008/005430 2007-11-06 2008-09-12 Fuel process apparatus of multiple desulfurizers and fuel cell system with the same Ceased WO2009061072A1 (en)

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