WO2001057162A1 - Huile combustible - Google Patents

Huile combustible Download PDF

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Publication number
WO2001057162A1
WO2001057162A1 PCT/JP2001/000605 JP0100605W WO0157162A1 WO 2001057162 A1 WO2001057162 A1 WO 2001057162A1 JP 0100605 W JP0100605 W JP 0100605W WO 0157162 A1 WO0157162 A1 WO 0157162A1
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WO
WIPO (PCT)
Prior art keywords
fuel oil
hydrogen
fuel
volume
catalyst
Prior art date
Application number
PCT/JP2001/000605
Other languages
English (en)
Japanese (ja)
Inventor
Hiroto Matsumoto
Hisashi Katsuno
Original Assignee
Idemitsu Kosan 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
Priority claimed from JP2000021350A external-priority patent/JP2001214179A/ja
Priority claimed from JP2000077948A external-priority patent/JP2001262164A/ja
Application filed by Idemitsu Kosan Co., Ltd. filed Critical Idemitsu Kosan Co., Ltd.
Priority to AU2001228855A priority Critical patent/AU2001228855A1/en
Publication of WO2001057162A1 publication Critical patent/WO2001057162A1/fr

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
    • C10L1/00—Liquid carbonaceous fuels
    • C10L1/04—Liquid carbonaceous fuels essentially based on blends of hydrocarbons

Definitions

  • the present invention relates to a fuel oil for producing hydrogen used in a fuel cell, and more particularly to a fuel oil for a fuel cell comprising a hydrocarbon such as a gasoline fraction.
  • hydrogen is used as fuel for fuel cells.
  • examples of such hydrogen include those using hydrogen gas as it is, those using hydrogen obtained by reforming or decomposing methanol or the like, or those at room temperature.
  • the present invention has been made to solve the above problems.
  • the present invention provides a fuel oil for a fuel cell which can efficiently produce hydrogen and has little deterioration of the reforming catalyst without adversely affecting the reforming catalyst and the fuel cell electrode.
  • the present inventors have conducted intensive studies in view of the above problems, and as a result, achieved the above object of the present invention by using a gasoline fraction having a specific composition and properties as the fuel oil for a fuel cell. I found out.
  • the present invention has been completed based on such knowledge. That is, the present invention provides a fuel characterized in that the true calorific value per volume is 33,000 J / cm 3 or more and the molar ratio of carbon / hydrogen is 0.52 or less. It relates to oil (Invention 1). Further, the present invention relates to a fuel oil for a fuel cell (Invention 2) characterized in that it contains a naphthene component in an amount of 20% by volume or more. The present invention relates to fuel oil for fuel cells containing naphtha as a main component. BEST MODE FOR CARRYING OUT THE INVENTION
  • the present invention provides a fuel oil characterized in that the true calorific value per volume is 33,000 J / cm 3 or more and the molar ratio of carbon and hydrogen is 0.52 or less. 1 invention).
  • the “true calorific value” is the calorific value generated when the fuel per unit weight is completely burned, and the calorific value obtained by subtracting the latent heat of vaporization of the generated water, that is, the vaporizing heat of the water vapor, from the total calorific value.
  • the “true calorific value per volume” is obtained by multiplying the true calorific value per unit weight by the density.
  • the fuel oil of the present invention has a true calorific value per volume of 33,000 J / cm 3 or more. If this value is smaller than 33,000 J / cm 3 , for example, there is a problem that the mileage per fuel in transportation of an automobile or the like becomes short. From this point, in the present invention, it is preferable that the true calorific value per volume is 34,000 JZ cm 3 or more.
  • the fuel oil of the present invention also has a structure in which the hydrocarbon constituting it has a carbon / hydrogen molar ratio of 0.52 or less. When the molar ratio of carbon / hydrogen exceeds 0.52, (1) the partial pressure of produced hydrogen decreases and hydrogen cannot be obtained efficiently, and (2) carbon precipitates on the reforming catalyst and the catalyst deteriorates. And other problems.
  • the molar ratio of carbon / hydrogen is preferably 0.50 or less.
  • A is the molar ratio of the carbon / hydrogen 0.5 2 below, and the true calorific value of unit volume equivalents have enough 3 3 0 0 0 as a J / cm 3 or more at which the fuel oil, specifically, , Normal paraffin having 7 or more carbon atoms, isoparaffin, cycloparaffin, saturated hydrocarbon having one naphthene ring, adamantane, a mixture thereof, and gasoline base material having 4 to 9 carbon atoms Distillate, distillate that can be a kerosene base material with 9 to 15 carbon atoms Or the like can be used.
  • naphtha obtained by distilling crude oil containing a large amount of naphthenes is desulfurized because heavy hydrogen can be produced efficiently and deterioration of the reforming catalyst and the like are small.
  • a gasoline fraction and a kerosene fraction obtained by distilling the cracked oil obtained by the hydrocracking of water can be preferably used.
  • the naphthene content is 2 0 volume 0/0 above, used properly preferred further 3 0% by volume or more.
  • the present invention relates to a fuel oil for a fuel cell (second invention) characterized by containing a naphthene content of 20% by volume or more, and in particular, containing a naphthene content of 20% by volume or more.
  • the present invention relates to a fuel oil for a fuel cell, comprising heavy desulfurized naphtha.
  • the desulfurization heavy naphtha A hereinafter sometimes referred to as DHN
  • C 6 ⁇ C 1 0 the norm Ruparafi down, Isoparafi down, the naphthene or. That consists of petroleum coal hydrocarbon fraction Say.
  • Such DHN is usually obtained by fractionating crude oil as heavy naphtha in an atmospheric distillation unit and desulfurizing it with a naphtha desulfurization unit, or fractionating crude oil as full-range naphtha in an atmospheric distillation unit.
  • DHN used for a fuel oil for a fuel cell of the present invention obtained Ri by the fractionating a heavy naphtha are those containing naphthene 2 0 volume 0/0 or more but naphthene content may 2 0 volume 0/0 yo Ri small, the effect of the present invention, in particular, can not be obtained the effect to suppress the co one click degradation of the reforming catalyst.
  • the naphthene content is 3 0% by volume or more, and preferably further 4 0 volume 0/0 above.
  • DHN containing such a naphthene component in an amount of 20% by volume or more can be produced by a conventionally known method, for example, by using a naphthenic crude oil as a crude oil before atmospheric distillation, or by using a benzene in DHN. Of heavy metals and hydrogenation of heavier fractions It can be obtained by a method such as decomposition treatment.
  • LPG hydrogen added C 5 ⁇ C 7 fraction Ri obtained by naphtha or the like distillation of fractions obtained by pyrolysis Later, the remaining fraction from which benzene, toluene and xylene were extracted is used. These contain 45 to 65% by volume of a naphthene component.
  • the DHN used in the present invention contains normal paraffin and isoparaffin as a paraffin component. It is more preferably 2.5 or more. When the above ratio is within this range, the effects unique to the present invention, such as little deterioration of the modified catalyst or the like, can be easily obtained.
  • Such DHN of the isoparaffin rich can be obtained by isomerization treatment of DHN or separation and removal of normal paraffin by a molecular sieve. ⁇
  • the fuel oil of the present invention comprising the first invention and the second invention has a sulfur content of preferably 1 ppm by weight or less, more preferably 0.5 ppm by weight or less, particularly preferably 0.1 ppm by weight. These are: If the sulfur content is higher than the above range, sulfur poisoning of the catalyst may occur, and problems such as deterioration of the reforming catalyst and the partial oxidation catalyst may occur. In the present invention, deep desulfurized heavy naphtha can be used as DH in order to obtain a fuel oil having a low sulfur content as described above.
  • the deep desulfurized heavy naphtha refers to the above DHN that has been treated so that its sulfur content is 0.5 ppm or less, and further, 0.1 ppm or less.
  • the above deep desulfurized heavy naphtha is, for example, in the presence of a catalyst commonly used in naphtha desulfurization equipment such as C0M0 / alumina, NiW / alumina, having a pressure of 1.0 to 2.5 MPa. Under pressure, temperature 250 to 350 May ° C, and the I Ri obtained Turkey in reacting feedstock and hydrogen at a liquid hourly space velocity (LHSV) 3 ⁇ 1 0 hr- hydrogen / feedstock 5 0 ⁇ 1 5 0 m 3 / k 1 conditions .
  • LHSV liquid hourly space velocity
  • the above-mentioned deep desulfurization heavy naphtha can be obtained by further performing adsorptive desulfurization using the following specific catalyst on DHN obtained by performing the above desulfurization treatment one or more times.
  • the catalyst that can be used for the adsorptive desulfurization include activated carbon, activated carbon fiber, silica gel, hydrophobic silica, zeolite, metal exchange zeolite, and alkali / alkaline.
  • Compound salts such as earth metal oxides, hydroxides and sulfite hydrates, or Fb, Sn, Fe, Ni, Co, Mn, Cr, Cu, Zn Metals, their oxides, their mixtures, composite oxides or these are supported on carriers such as silica, alumina, silica-alumina, titania, zirconia, zinc oxide, clay, diatomaceous earth, and clay.
  • carriers such as silica, alumina, silica-alumina, titania, zirconia, zinc oxide, clay, diatomaceous earth, and clay.
  • a rare earth metal such as Ce, La, Y or the like.
  • noble metals such as Pt, Pd, Rh, and Ru are supported on the above carrier can also be used.
  • DHN used in the present invention preferably has a carbon atom / hydrogen atom ratio of less than 0.55. The smaller this value is, the more excellent the hydrogen generation efficiency is, and the less adversely affects the reforming catalyst and the fuel cell electrode.
  • the fuel oil of the present invention preferably has a vapor pressure of 0.098 MFa or less. If the vapor pressure exceeds 0.098 MPa, the tank strength may need to be increased, or the release of hydrocarbons into the atmosphere may be unfavorable. Therefore, in the present invention, the vapor pressure is more preferably in the range of 0 to 0.098 MPa.
  • the aromatic content in the fuel oil of the present invention is preferably 10% by weight or less, more preferably 8% by weight or less, and particularly preferably 1% by weight or less. If the amount of the aromatic component exceeds the above-mentioned amount, the efficiency of hydrogen generation may be poor.
  • the fuel oil of the present invention has characteristics such as high purity of hydrogen produced by the method and a small decrease in hydrogen partial pressure. Therefore, the fuel oil is suitable for producing hydrogen for fuel cells. In particular, it is suitable as a fuel for fuel cells for transportation such as automobiles because it is liquid.
  • the fuel oil is desulfurized as necessary.
  • hydrodesulfurization is used as the desulfurization method, and the method uses a hydrodesulfurization catalyst such as C0-Mo / alumina or Ni-Mo / alumina and the adsorption of hydrogen sulfide such as Zn0.
  • the reaction is carried out under normal pressure to 5 MPa and a temperature of 2 ⁇ 0 to 400 t.
  • the desulfurized fuel oil is subjected to steam reforming and / or partial oxidation as required.
  • ADVANTAGE OF THE INVENTION According to this invention, the fuel oil which can produce hydrogen efficiently without carbon precipitation to a steam reforming catalyst etc. can be obtained.
  • the desulfurized fuel oil is subjected to steam reforming and / or partial oxidation as required.
  • ADVANTAGE OF THE INVENTION According to this invention, the fuel oil which can produce hydrogen efficiently without carbon precipitation to a steam reforming catalyst etc. can be obtained.
  • the method of steam reforming is not particularly limited, but is usually performed by the following method.
  • the steam reforming catalyst used in this hydrogen production method is not particularly limited, but the following are preferably used.
  • the supported metal examples include noble metals such as Ni, zirconium or ruthenium (Ru), rhodium (Rh), and platinum (Pt). These may be used alone or in combination of two or more. Among these, a catalyst supporting Ru is particularly desirable, and steam reforming is preferable. The effect of suppressing carbon deposition during the reaction is great. Supported amount information about the R u, 0 in carrier reference. 0 5-2 0 weight 0/0, the Raniwa, 0. 0 5-1 5% by weight preferred arbitrariness. If the supported amount is less than 0.05% by weight, the activity of the steam reforming reaction may be extremely reduced, which is not preferable. Even if it exceeds 20% by weight, a remarkable increase in the activity is hardly obtained.
  • noble metals such as Ni, zirconium or ruthenium (Ru), rhodium (Rh), and platinum (Pt). These may be used alone or in combination of two or more.
  • Ru ruthenium
  • Rh rhodium
  • a combination supporting Ru and zirconium ′ can be given.
  • Ru and zirconium may be carried simultaneously or separately.
  • those further added with cobalt and Z or magnesium are preferred.
  • the content of cobalt is preferably in the range of 0.1 to 30 and more preferably 0.1 to 30 in terms of the atomic ratio of cobalt to ruthenium, and the content of magnesium is magnesia ( M g O) converted at from 0.5 to 1 0 weight 0/0, the Raniwa 0.5 to 1 5 weight 0/0 are preferred.
  • inorganic oxides are used as the carrier of the catalyst used for steam reforming, and specific examples include alumina, silica, zirconia, magnesium, and mixtures thereof. Of these, alumina and zirconia are particularly preferred.
  • One preferred embodiment of the steam reforming catalyst is a catalyst in which Ru is supported on zirconium.
  • This Jirukoyua is may be the single Jirukonia (Z r 0 2), may be stable I spoon Jirukonia including stabilizing components such as magnesia.
  • the stabilized zirconia those containing magnesia, yttria, seria, and the like are preferable.
  • One preferred embodiment of the steam reforming catalyst is Ru and zirconium, or Ru and zirconium as well as cobalt and / or zirconium.
  • a catalyst in which magnesium and magnesium are supported on an alumina carrier is preferable.
  • alumina As alumina, ⁇ -alumina, which is particularly excellent in heat resistance and mechanical strength, is preferable.
  • the ratio S / C (molar ratio) of steam (S) to carbon (C) derived from fuel oil is 2-5, and furthermore, 2-4.
  • a reforming method is preferred. If steam reforming is performed with S / C (molar ratio) higher than 5, excess steam must be produced, resulting in large heat loss and reduced hydrogen production efficiency. On the other hand, if S / C is less than 2, the amount of generated hydrogen decreases.
  • the inlet temperature of the steam reforming catalyst layer it is preferable to carry out steam reforming while maintaining the inlet temperature of the steam reforming catalyst layer at 63 ° C. or lower.
  • the steam reforming catalyst bed inlet temperature tends to rise with the addition of oxygen, so it is necessary to control this. If the inlet temperature exceeds 630 ° C, thermal decomposition of the raw material hydrocarbons is promoted, and carbon is deposited on the catalyst or reaction tube wall via generated radicals, which may make operation difficult.
  • the catalyst layer outlet temperature is not particularly limited, but is preferably set at 65 to 800 ° C. If the outlet temperature of the catalyst layer is lower than 650 ° C, the amount of hydrogen generated is not sufficient, and in order to react at a temperature higher than 800 ° C, the reactor may need to be made of a particularly heat-resistant material. However, it is not economical.
  • the reaction pressure is preferably normal pressure to 3 MPa, and more preferably normal pressure to lMFa.
  • the flow rate of fuel oil is 0.1 to 100 h- 1 in LHSV.
  • the partial oxidation reaction is preferably carried out under a catalyst in which a noble metal such as ruthenium or the like is supported on a heat-resistant oxide, at a reaction pressure of normal pressure to 5 MFa, a reaction temperature of 400 to 100 ° C., and oxygen / It is carried out at a carbon ratio of 0.2 to 0.8 and an LHSV of 0.1 to 100 h- 1 .
  • the S / C ratio should be 0.4 to 4.
  • the present invention provides that the true calorific value per volume is 33,000 J / cm 3 or more and the molar ratio of carbon / hydrogen is 0.52 or less.
  • a fuel oil characterized by a characteristic or a fuel oil containing a naphthene content of 20% by volume or more especially a fuel oil composed of desulfurized heavy naphtha having a naphthene content of 20% by volume or more
  • Hydrogen used in the pond can be produced efficiently, and there is little deterioration of the reforming catalyst without adversely affecting the reforming catalyst and fuel cell electrodes.
  • a fuel oil for a fuel cell can be provided. .
  • Reforming catalyst 20% by weight of water was added to ⁇ -alumina powder, mixed and compression-molded in a single die to form a cylindrical molded body having a diameter of 5 mm and a length of 5 mm. After drying at 200 ° C. for 3 hours, it was calcined at 12.80 ° C. for 26 hours to obtain an alumina carrier.
  • Carbon deposition rate (%) length of carbon deposition / length of total catalyst The amount of generated hydrogen was measured by gas chromatography of hydrogen obtained from the above hydrogen production experiment.
  • Example 2 A hydrogen production experiment was conducted in the same manner as in Example 1 using DHN (composition shown in Table 2) obtained by distilling a high naphthenic crude oil with a theoretical 15-stage batch distillation apparatus. The coking test was performed on the catalyst after the reaction in the same manner as in Example 1. The results are shown in Table 2.
  • DHN composition is shown in Table 2 obtained by distilling low naphthenic crude oil with a batch type still with 15 theoretical stages, hydrogen production experiment and hydrogen production were conducted in the same manner as in Example 3. A caulking test was performed. Table 2 shows the results.
  • the present invention relates to a fuel oil for producing hydrogen used for a fuel cell, and more particularly to a fuel oil for a fuel cell which is made of a hydrocarbon such as a gasoline fraction and is suitable for transportation such as automobiles.

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  • Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Hydrogen, Water And Hydrids (AREA)
  • Fuel Cell (AREA)

Abstract

L'invention concerne une huile combustible caractérisée en ce qu'elle possède une capacité calorifique nette supérieure ou égale à 33 000 J/cm3 et une rapport molaire carbone/hydrogène inférieur ou égal à 0,52. Ladite huile combustible sert de combustible pour une pile à combustible capable de produire de l'hydrogène avec un rendement satisfaisant, et ce sans avoir d'effets négatifs sur le catalyseur de reformage ou les électrodes d'une pile à combustible, ce qui permet de réduire toute détérioration du catalyseur de reformage ou analogue. Par conséquent, ladite huile combustible convient à un véhicule de transport tel qu'une automobile.
PCT/JP2001/000605 2000-01-31 2001-01-30 Huile combustible WO2001057162A1 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
AU2001228855A AU2001228855A1 (en) 2000-01-31 2001-01-30 Fuel oil

Applications Claiming Priority (4)

Application Number Priority Date Filing Date Title
JP2000021350A JP2001214179A (ja) 2000-01-31 2000-01-31 燃料油
JP2000-21350 2000-01-31
JP2000-77948 2000-03-21
JP2000077948A JP2001262164A (ja) 2000-03-21 2000-03-21 燃料電池用燃料油

Publications (1)

Publication Number Publication Date
WO2001057162A1 true WO2001057162A1 (fr) 2001-08-09

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PCT/JP2001/000605 WO2001057162A1 (fr) 2000-01-31 2001-01-30 Huile combustible

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AU (1) AU2001228855A1 (fr)
WO (1) WO2001057162A1 (fr)

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO1985000619A1 (fr) * 1983-07-15 1985-02-14 The Broken Hill Proprietary Company Limited Production de carburants, en particulier des carburants pour des moteurs a reaction et des moteurs diesels, ainsi que leurs constituants
JPS6340702A (ja) * 1986-08-01 1988-02-22 Nippon Oil Co Ltd 燃料電池用水素の製造方法
JPH02113092A (ja) * 1988-10-20 1990-04-25 Nippon Oil Co Ltd 高性能灯油
JPH0680972A (ja) * 1992-07-17 1994-03-22 Sekiyu Sangyo Kasseika Center 中軽質油の深度脱硫方法
US5609653A (en) * 1994-07-26 1997-03-11 Elf Antar France Fuel compositions containing at least one fulvene derivative and their use

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO1985000619A1 (fr) * 1983-07-15 1985-02-14 The Broken Hill Proprietary Company Limited Production de carburants, en particulier des carburants pour des moteurs a reaction et des moteurs diesels, ainsi que leurs constituants
JPS6340702A (ja) * 1986-08-01 1988-02-22 Nippon Oil Co Ltd 燃料電池用水素の製造方法
JPH02113092A (ja) * 1988-10-20 1990-04-25 Nippon Oil Co Ltd 高性能灯油
JPH0680972A (ja) * 1992-07-17 1994-03-22 Sekiyu Sangyo Kasseika Center 中軽質油の深度脱硫方法
US5609653A (en) * 1994-07-26 1997-03-11 Elf Antar France Fuel compositions containing at least one fulvene derivative and their use

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Publication number Publication date
AU2001228855A1 (en) 2001-08-14

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