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WO2016061584A1 - Production de carburant propre à base d'hydrocarbures et d'azote - Google Patents

Production de carburant propre à base d'hydrocarbures et d'azote Download PDF

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Publication number
WO2016061584A1
WO2016061584A1 PCT/US2015/056253 US2015056253W WO2016061584A1 WO 2016061584 A1 WO2016061584 A1 WO 2016061584A1 US 2015056253 W US2015056253 W US 2015056253W WO 2016061584 A1 WO2016061584 A1 WO 2016061584A1
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Prior art keywords
hydrocarbon
hydrogen
halogen
fuel
methane
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Kamal JAFFREY
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Solutions Labs Inc
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Solutions Labs Inc
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J31/00—Catalysts comprising hydrides, coordination complexes or organic compounds
    • B01J31/02—Catalysts comprising hydrides, coordination complexes or organic compounds containing organic compounds or metal hydrides
    • B01J31/12—Catalysts comprising hydrides, coordination complexes or organic compounds containing organic compounds or metal hydrides containing organo-metallic compounds or metal hydrides
    • 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
    • C01B3/04—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of inorganic compounds, e.g. ammonia
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G2/00—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon
    • C10G2/30—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen
    • C10G2/32—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen with the use of catalysts
    • C10G2/33—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen with the use of catalysts characterised by the catalyst used
    • 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 OR C10K; LIQUIFIED PETROLEUM GAS; USE OF ADDITIVES TO FUELS OR FIRES; FIRE-LIGHTERS
    • C10L1/00—Liquid carbonaceous fuels
    • C10L1/04—Liquid carbonaceous fuels essentially based on blends of hydrocarbons
    • 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
    • Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis

Definitions

  • Fossil fuels including coal, oil and natural gas
  • CCS Carbon Capture and Storage
  • Clean hydrocarbon or nitrogen-based fuels can be produced, for example, by decarbonizing source hydrocarbons using a halogen to produce elemental carbon and hydrogen halide species.
  • methane can be used as a source of hydrocarbons.
  • coal can be used as a source of hydrocarbon.
  • the hydrogen halide species can be separated by adding energy to produce hydrogen and halogen.
  • fuel comprising hydrocarbons having substantially homogenous composition and a vector can be synthesized from the hydrogen and carbon.
  • One such fuel comprising hydrocarbons can include octane.
  • Clean hydrocarbon fuels can include compositions of hydrocarbons that are substantially homogenous. This can include, for example, compositions of hydrocarbons that are between 70 and 99 percent homogenous. Other percentages are possible. Dirty hydrocarbon fuels can include compositions of hydrocarbons being less than 30 percent homogenous. Other percentages are possible.
  • a method of producing a hydrocarbon fuel which may comprise steps of: decarbonizing a source hydrocarbon by introducing halogen to produce elemental carbon and hydrogen halide; and producing the hydrocarbon fuel by reacting the elemental carbon with hydrogen (H 2 ).
  • the decarbonization may be performed in non-oxygen condition and the hydrocarbon fuel may be produced in the present of a catalyst.
  • the source hydrocarbon may comprise 1 to 6 carbons.
  • the halogen may be selected from the group consisting of Cl 2 , Br 2 , 1 2 , ClBr, and mixtures thereof.
  • the hydrocarbon fuel may comprise 8 to 30 carbons.
  • the decarbonizing may be performed in a combustion chamber.
  • the combustion chamber has a volume of about 1 m 3 to about 10 m 3 .
  • an internal temperature in the combustion chamber may range from about 298 K to about 2550 K, and a pressure ranges from about 1 atm to about 20 atm.
  • the catalyst may be an organometallic catalyst comprising at least one metal element selected from the group consisting of Al, Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Y, Zr, Nb, Mo, Tc, Ru, Rh, Pd, Ag, Cd, Hf, Ta, W, Re, Os, Ir, Pt, and Au.
  • metal element selected from the group consisting of Al, Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Y, Zr, Nb, Mo, Tc, Ru, Rh, Pd, Ag, Cd, Hf, Ta, W, Re, Os, Ir, Pt, and Au.
  • the hydrocarbon fuel is synthesized at a temperature ranging from about 300-350 °C.
  • the method may further comprise: decomposing the hydrogen halide by adding energy to produce the hydrogen (H 2 ) and reproduced halogen; and collecting the hydrogen (H 2 ) for synthesizing the hydrocarbon fuel.
  • the energy may be added by radiating UV light and a wavelength of the UV light may from about 100 nm to about 320 nm. Further, the UV light may be radiated at least for about 10 min, and at an intensity of about 50 mJ/cm 2 .
  • the hydrocarbon source may be methane
  • the halogen may be Br 2
  • a ratio between a partial pressure of the methane and a partial pressure Br 2 may be of about 1: 2-10.
  • the hydrocarbon fuel may be octane.
  • the method of claim may further comprise: liquefying the
  • hydrocarbon fuel that is manufactured by a method as described herein.
  • the hydrocarbon fuel obtained from the method of the present invention may comprise octane.
  • the elemental carbon may be isolated and/or purified from the hydrogen halide.
  • source hydrocarbon is meant a carbon based material comprising hydrogen, and particularly refers to a starting material for producing desired product, i.e. hydrocarbon fuels.
  • exemplary hydrocarbon fuel may be hydrocarbons comprising 1 to 12 carbons, or particularly 1 -4 carbons.
  • hydrocarbon fuel is meant a carbon based material comprising hydrogen, and particularly refers to a product or resultant from processes of the present invention.
  • exemplary hydrocarbon fuel may be hydrocarbons comprising 8 to 30 carbons, or particularly 8 -18 carbons, or otherwise, the hydrocarbon fuel may contain octane as major component.
  • decarbonization is meant a reaction that dissociates or deprives carbon from hydrogen of the source hydrocarbon, particularly by reacting oxidizer with the hydrocarbons in non-oxygen condition.
  • the oxidizer may include halogen which can make a bond (covalent bond) with hydrogen after dissociation of the carbon from the hydrogen.
  • hydrogen generation is meant a reaction that dissociates a bond between hydrogen and halide that may be formed during decarbonization.
  • the dissociated hydrogen may subsequently form hydrogen molecule (H 2 ).
  • stitching vector is meant a chemical reagent or catalyst which serves to reduce bond dissociation energy between carbons, and/or accelerates synthesis of the hydrocarbon fuel.
  • the stitching vector, i.e. catalyst, in the present invention may include organometallic catalyst, organic agent, or mixtures thereof.
  • liquefication vector is meant a chemical reagent or catalyst which serves to liquefy the hydrogen fuel in standard state (at a temperature of 298 °K, at a pressure of atmospheric pressure (1 atm)).
  • FIG. 1 is a process flow diagram illustrating a process of producing a clean hydrocarbon or nitrogen-based fuel according to the current subject matter.
  • FIG. 2 is a system block diagram illustrating the decarbonization process of a hydrocarbon mixture (C x H y ) to generate halogen halide species (HX) and carbon (C).
  • FIG. 3 is a system block illustrating the separation process of the halogen halide species 200 to hydrogen and halogen upon exposure to ultraviolet light or thermal energy.
  • FIG. 4 is a system block diagram illustrating the synthesis of hydrocarbon or nitrogen-based species from carbon or nitrogen with hydrogen optionally in the presence of one or more vector(s).
  • FIG. 5 is a system block diagram illustrating the liquefication process of hydrocarbon or nitrogen-based species optionally in the presence of energy or one or more vector(s) to generate the final hydrocarbon or nitrogen-based fuel.
  • FIG. 6 is a graph illustrating the energy released during
  • FIG. 7 is a table illustrating chemical properties of halogens, carbon, hydrogen, nitrogen and oxygen.
  • FIG. 8 is a table illustrating the ratios of hydrogen and carbon for the preparation of hydrocarbons.
  • FIG. 9 is a cross-sectional diagram of another example implementation of a combustion apparatus including a combustion chamber and cyclone that performs decarbonization.
  • FIG. 10 is a graph illustrating the heating values in Kj/mole of various fuels based on their number of hydrogen atoms during the decarbonization process with halogens.
  • FIG. 11 is a graph illustrating the adiabatic Temperature in °K as a function of the number of hydrogen atoms contained in the fuel used during decarbonization with chlorine and bromine.
  • FIG. 12 is a graph illustrating the adiabatic Temperature in °K as a function of the number of hydrogen atoms contained in the fuel used during decarbonization with fluorine.
  • FIG 13 is a process flow diagram illustrating an example method of producing clean hydrocarbons.
  • FIG. 14 is a diagram of a compact UV reactor.
  • FIG. 15 is a diagram of energy according to a wavelength in the UV light.
  • FIG. 16 is a diagram of energy according to a frequency in the UV light.
  • Clean hydrocarbon or nitrogen-based fuels can be produced, for example, by decarbonizing source hydrocarbons using halogen to produce elemental carbon and hydrogen halide species.
  • methane and/or natural gas can be used as a source of hydrocarbons.
  • the source hydrogen may include 1-18 carbons, 1-10 carbons or particularly 1-4 carbons.
  • coal can be used as a solid source of hydrocarbons.
  • the hydrogen halide species can be separated by adding energy to produce hydrogen and halogen. Additionally, fuel comprising hydrocarbons having substantially homogenous composition and a vector can be synthesized from the hydrogen and carbon. Fuels generated comprising hydrocarbons can include octane and/or methane.
  • FIG. 1 is a process flow diagram illustrating a process 100 of producing a clean hydrocarbon or nitrogen-based fuel according to the current subject matter.
  • hydrogen and carbon from hydrocarbons can be separated by combustion of the hydrocarbons in a halogen environment.
  • the halogen environment does not contain any oxygen or nitrogen gas.
  • This can be performed, for example, by introducing the hydrocarbons and halogen into a combustion chamber.
  • the non-oxygen combustion can produce at least carbon and hydrogen halide species.
  • the halide species may exist in gas, liquid or in solid states, and preferably halogen gas or halogen vapor may be introduced in the combustion chamber.
  • the produced carbon may be elemental carbon and/or active carbon.
  • methane and/ or natural gas can be used as a hydrocarbon.
  • coal can be used as a hydrocarbon.
  • hydrogen can be extracted from the hydrogen halide species produced at 110.
  • the hydrogen halide species produced in a combustion chamber can be directed to a reaction chamber.
  • Energy can be applied to break the hydrogen halide species bond to form hydrogen and halogen.
  • the energy can be applied by, for example, exposing the hydrogen halide species to ultraviolet light or thermal heating of the hydrogen halide species.
  • carbon and/or nitrogen in combination with hydrogen can react to afford a hydrocarbon and/or nitrogen-based fuel.
  • the carbon introduced at 130 can be the carbon produced at 110 during decarbonization and the hydrogen introduced at 130 can be the hydrogen produced at 120 during separation.
  • carbon and/or hydrogen can be acquired through other means.
  • a stitching vector can also be included to modify characteristics for example, low freezing points; controlled boiling points, viscosity, stable vapor pressure, controlled formation of pollutant species and the like, of the generated hydrocarbon and/or nitrogen-based species to produce a hydrocarbon or nitrogen-based fuel. Control of the addition of the reagents and subsequent product removal can aid in the production of a homogenous hydrocarbon or nitrogen-based fuel. For example, clean octane and/or methane can be produced as the hydrocarbon fuel.
  • the fuel produced by synthesis at 130 can be liquefied. Any bi- products produced by the fuel production process can also be removed at 140.
  • Addition of one or more liquefication vectors to the generated hydrocarbon or nitrogen-based species can produce a fuel, which can be a liquid and easy to handle and transport. Furthermore, all the vector(s) can compete in the subsequent combustion process with carbon dioxide (C0 2 ) and mono nitrogen oxide species (NO x ) formation.
  • the vector(s) can be water based or nitrogen based.
  • Example vector(s) can include any solvent or combinations thereof.
  • FIG. 2 is a system block diagram illustrating a system 200 for decarbonizing hydrocarbons.
  • the system can include a combustion chamber 210 and can be used, for example, during the fuel production process to decarbonize at 110 in FIG. 1.
  • Combustion of the starting hydrocarbon mixture can be carried out in a halogen environment at standard temperature and pressure, or in order to facilitate the decarbonizing, the temperature and the pressure in the chamber may be elevated.
  • the internal temperature for decarbonization may be of about 298 K to 2550 K, and the internal pressure may be of about 1 atm to about 20 atm.
  • the source of the starting hydrocarbon mixture 220 can be crude oil, processed crude oil (e.g., at an oil refinery), or any other organic material as a carbon source such as coal, natural gas, plants, etc.
  • the source of hydrocarbons can include methane.
  • Methane is the simplest alkane with the chemical formula CH 4 (one atom of carbon and four atoms of hydrogen).
  • CH 4 one atom of carbon and four atoms of hydrogen.
  • the relative abundance of methane makes it an abundant starting material for decarbonization although capture and storing it may pose challenges due to its gaseous state found in nature.
  • methane is found both below and under the sea floor as methane hydrate deposits and it often finds its way to the surface and in the earth's atmosphere where it is known as atmospheric methane.
  • Methane is also the major component found in natural gas, a naturally occurring gas mixture (about 95%) comprising addition to small quantities of nitrogen, oxygen, carbon dioxide and sulfur compounds. Natural gas can therefore also be used as a starting hydrocarbon source.
  • natural gas is used as a primary household energy source for cooking, heating and the like as well as industrial uses such as generation of electricity and polymer synthesis.
  • the source of hydrocarbons can include coal.
  • Coal is a solid fossil fuel and formed when dead plant matter is converted into peat, which in turn is converted to lignite, then sub-bituminous coal, after that butuminous coal, and lastly anthracite.
  • Coal is a mixture of compounds composed of between 50-100% carbon, by mass, with the rest being hydrogen, nitrogen, oxygen, and trace amounts of sulfur.
  • Coal is one of the largest sources of energy for the generation of electricity worldwide, as well as one of the largest worldwide anthropogenic sources of carbon dioxide.
  • Coal is also being used for the production of coke and as a source of various compounds used in synthesizing dyes, solvents, and drugs. The search for alternative energy sources has periodically revived interest in the conversion of coal into liquid fuels.
  • the source of hydrocarbons is from a distillation column at an oil refinery.
  • the source of starting hydrocarbon mixture from the distillation column may be selected from any fraction of the distillates within the column, although distillates with minor impurities are preferred as the starting hydrocarbon mixture.
  • clean (e.g., few impurities and/or homogenous) starting hydrocarbon mixture leads to more of an efficient decarbonization reaction, which is described in equation (1).
  • X 2 in equation 1 can be a halogen gas and can be selected from chlorine, bromine, iodine and fluorine, or a combination of any of the foregoing.
  • methane (CH 4 ) and/or natural gas is the clean starting hydrocarbon C x H y in equation 1.
  • the hydrocarbon mixture C x H y in equation 1 is coal.
  • This reaction can take place in a combustion chamber 210 with the initial conditions at standard temperature and pressure (e.g., 298 °K (24.58 °C) and atmospheric pressure (1 atm)). In other implementations, the reaction can take place in a pressurized and/or pre-heated reaction chamber.
  • the temperature range of the decarbonization reaction is between about 298 °K and the adiabatic flame temperature (Tp) of the combustion process (e.g., T 2 98 ⁇ T ⁇ Tp).
  • the pressure range of the decarbonization process is between about 1 atm and the pressure present when the adiabatic flame temperature is reached (e.g., 1 atm ⁇ P ⁇ PTF). However, without wishing to be bound to the theory, the pressure may range preferably from about 1 atm to about 20 atm.
  • the vapor pressure of the halogen gas 230 at 298 °K can determine the amount of halogen gas available for the starting hydrocarbon mixture 220 to react. Iodine and chlorine have a low vapor pressure range of only 10 2 -10 3 Nm "2 whereas bromine is slightly higher (10 4 -10 5 Nm "2 ) compared to fluorine (>10 6 Nm "2 ) at 298 °K.
  • the selection of the halogen gas depends on the reactivity of its vapor pressure during the decarbonization process. Furthermore, the source of the halogen can be a factor in selecting an appropriate halogen.
  • Bromine and chlorine gas can easily be generated from brine solutions such as sodium bromide and sodium chloride, which are relatively inexpensive, environmentally friendly, and easily accessible starting materials.
  • a halogen with a high vapor pressure is used relative to other halogens having a low vapor pressure at a given temperature.
  • the partial pressure of methane and the partial pressure (vapor pressure) bromine gas may be maintained at a ratio at least of about 1:2, however, in order f facilitate the decarbonization, the ratio may be controlled, for example, to be of about 1: about 2-10.
  • the halogen-hydrocarbon combustion reaction is exothermic and it is generally a function of the hydrocarbon chain length.
  • the calculations shown in FIG. 6 illustrate the amount of energy released ( ⁇ ) upon reaction of various halogens and hydrocarbons of various lengths to form hydrogen halide species 260.
  • the formation of hydrogen bromide, hydrogen chloride, and hydrogen fluoride are exothermic, and the amount of energy released is dependent on the hydrocarbon chain length.
  • the formation of hydrogen iodide is endothermic, and becomes increasingly endothermic as the hydrocarbon chain length increases.
  • a halogen that forms an exothermic reaction with the hydrocarbon chain can be used, since exothermic reactions release energy and generally do not require input of additional energy, which can be more economic and efficient.
  • methane can be used as the hydrocarbon in the halogen-hydrocarbon combustion reaction. As depicted in FIG. 6, the formation of hydrogen bromide, hydrogen chloride, and hydrogen fluoride is exothermic, while the formation of hydrogen iodide is endothermic when methane is used (e.g., the length of the carbon chain is 1). Table 1 lists the energy 250 released of methane in different halogen environments. In some implementations, natural gas is used as the hydrocarbon in the halogen-hydrocarbon combustion reaction. [0061] Table 1. Energy released during halogen-hydrocarbon combustion reaction.
  • Table 1 shows that the use of chlorine releases the most amount of energy 250.
  • coal is used as the hydrocarbon in the halogen- hydrocarbon combustion reaction to produce energy 250.
  • the energy 250 released during the exothermic reaction can be captured and used in subsequent steps of this process, or can be used as an additional energy source for the refinery.
  • ⁇ ⁇ (Bond Energy) reactants - ⁇ (Bond Energy) products
  • ⁇ 3 ⁇ 4 is the standard heat of formation
  • a, b, and m are the number of moles of the compound
  • c is the heat capacity of the compound
  • ⁇ represents the difference in temperature generated during the reaction.
  • the energy 250 released also called the heat of combustion, is equal to the change in enthalpy ( ⁇ ) of the reaction system (3).
  • ni (X) is a known amount of fuel in moles
  • c P(ave.) is the average amount of heat capacity of all products in the combustion chamber
  • Table 3 shows the heat capacity values of methane and all the halogens, which can be used in the halogen-combustion reaction with methane.
  • LHV defines the lower heating value, which is determined by subtracting the heat of vaporization of the water vapor from the higher heating value of a given fuel. If there are multiple hydrocarbon species in the reaction chamber, equation (8) can be expressed as follows:
  • LHV ave is the average lower heating value of the fuel (e.g., No. 2 fuel oil), and m is the number of moles of reactants (hydrocarbons and halogens).
  • the higher heating value is the amount of energy released during the combustion of a specified amount of given fuel. Therefore the adiabatic temperature is a function of the amount of halogen gas used in the combustion chamber as the LHV and heat capacity values are known and tabulated.
  • the LHV for methane is 802.32 kJ/mol (Table 3).
  • the adiabatic temperature T f for a decarbonization process using methane and a select halogen in any given amount can be determined, with the heat capacity values of halogen and methane provided in Table 2 together with the LHV tabulated in Table 3.
  • Analogous values can be obtained for natural gas, which consists of 95% methane.
  • Analogous calculations can also be carried for coal, which has a LHV of 24.429 MJ/Kg.
  • Table 4 shows a list of lower heating (LHV) values of various fuels, wherein kJ/mol stands for
  • Gasoline liquid 110 2.0 4,675.00 42.50 18,280
  • LPG is marketed as propane or butanes or a mixture of propane and butanes.
  • the higher heating value (HHV) is a function of the number of hydrogen atoms present in the fuel used in the decarbonization process (FIG.10). As the number of hydrogen atoms in the fuel increase the heating value becomes more exothermic. The rate of increase in the heating value of a given fuel is also dependent on the halogen used during the decarbonization process. Chlorine, bromine, and fluorine are exothermic, whereas iodine exhibits an endothermic heating value.
  • methane is used as the fuel in the decarbonization process and the HHV values of methane with any given halogen are shown in Figure 10.
  • the adiabatic flame temperature is the temperature that results from a complete combustion process if theoretically no energy is lost to the outside environment.
  • the adiabatic flame temperature is a function of the type of fuel being used (e.g., each fuel has a defined LHV value) and the amount and type of halogen gas being used at 298 °K (T;). Calculations using eq. (8) have shown adiabatic temperatures in a range of 2000 to 3800 °F.
  • the adiabatic flame temperature is also a function of the number of hydrogen atoms present in the fuel used during the decarbonization process as well as the halogen used during the decarbonization process.
  • the adiabatic temperature is within the range of about 2000 to 2550 °K, whereas when fluorine is used the adiabatic temperature increases significantly as the number of hydrogen atoms increase in a given fuel (FIG. 12). Therefore, halogens such as chlorine or bromine would be preferred during the decarbonization process because of the stability of the adiabatic temperature as halogen atoms increase within a given fuel, which facilitates the control of the temperature released during this process.
  • the adiabatic temperature during the decarbonization process of methane and/or natural gas is about 2000 or 2550 °K in a chlorine or bromine environment respectively.
  • the combustion of the starting hydrocarbon mixture 220 can be initiated using an electrical spark or pilot light in the presence of a halogenated gas 230 to initiate decarbonization and the release of heat 250.
  • the electrical spark or pilot light can provide the energy needed to overcome the activation energy of the reaction.
  • the activation energy of methane and/or natural gas would be the energy required to break C-H bonds in the methane molecule, which is about 413 Kj/mole.
  • hydrocarbons such as methane, natural gas or coal can be broken down into hydrogen halide 260 and carbon 240, e.g. amorphous.
  • carbon 240 can accumulate at the bottom of the combustion chamber, where it can be collected using a cyclone.
  • the collected carbon 240 can be used as a reagent in the synthesis of synthetic hydrocarbon fuel or various other industrial applications. Carbon can also be sold as a commodity.
  • the heat of combustion 250 generated can be used in subsequent steps of the process of FIG. 1 , which may require energy, or it can be used for other applications such as electrical power generation, and the like.
  • FIG. 9 is a cross-sectional diagram of another example implementation of a combustion apparatus 900 including a combustion chamber 910 and cyclone 920 that performs decarbonization.
  • Starting hydrocarbon 220 e.g., methane, natural gas, coal, and the like
  • halogen 230 can feed into the combustion apparatus 900 through a feed port 930 located towards the top of the combustion apparatus and/or arranged such that the starting hydrocarbon 220 (e.g., methane, natural gas, coal, and the like), and halogen 230 can feed into the combustion chamber 910.
  • the starting hydrocarbon 220 e.g., methane, natural gas, coal, and the like
  • halogen 230 can, as described in more detail above, combust to form carbon 240 and halogen halide 260.
  • the carbon 240 having a higher molecular weight than halogen halide 260, can separate from the halogen halide 260 by falling into cyclone 920 and subsequently exit the combustion apparatus 900 at a bottom exit port 960.
  • the halogen halide 260 can be forced (e.g., under pressure) out of the combustion chamber 910 through a top exit port 950.
  • the separation of the formed hydrogen halide gas 260 from the remaining hydrocarbon mixture 220, halogen gas 230, and carbon 240 can be based on the molecular weight and physical state of these individual components at 298 °K.
  • Carbon 240 can be a solid (and/or can be amorphous) and can be collected at the bottom of the reaction chamber 310 using a cyclone, whereas hydrogen halide gas 260 and halogen gas 230 are both gaseous and therefore mixed.
  • the two gases can be separated based on their electromagnetic properties shown in the table of FIG. 7. As these two gases pass through a magnetic field separation of the gases occurs and the halogen gas 230 can be recycled and used in another decarbonization process in combustion chamber 210.
  • the hydrogen halide gas 260 can be removed from decarbonization system 200 (e.g., a combustion chamber 210) and passed through a magnetic field to separate from the halogen gas 230.
  • decarbonization system 200 e.g., a combustion chamber 210
  • the strength of the magnetic field can be based on the
  • FIG. 3 is a system block diagram illustrating a hydrogen generation system 300 for performing hydrogen generation, for example, at 120 in FIG. l.
  • the hydrogen generation system 300 includes a reaction chamber 310.
  • the reaction chamber 310 can be combined with the combustion chamber 210.
  • the hydrogen halide gas 260 can be exposed to ultraviolet light, which carries energy of 397.32 kJ/mole. This energy can be derived from eq. 10:
  • h is defined as Max-Planck's Constant (6.626xl0 ⁇ 34 J/s)
  • v is the frequency of the ultra violet light source (e.g., l.OOxlO 15 Hz)
  • Av is Avogadro's number (6.02 x 10 23 )
  • ⁇ is the energy, which can be used to split the halogen halide bond.
  • the bond enthalpy which is the energy required to break a bond therefore cannot exceed 397 kJ/mole for a hydrogen halide bond.
  • Table 5 lists bond enthalpies of various halogen halide bonds.
  • Table 6 lists energy of UV light at various lengths, which is also presented in FIGS. 15-16. Type of
  • the two hydrogen halide bonds that can be split using ultraviolet light is an H-I bond or an H-Br bond because their bond enthalpies are less than 397.32 kJ/mole.
  • the remaining halogen halide bonds such as H-Cl and H-F may require more energy to be split than can be supplied by the ultraviolet light source.
  • the choice of the halogen used in reaction chamber 310 can be based on the energy 250 released when forming the halogen halide bond of 260, as was shown in FIG. 6 and the energy required to split the halogen halide bond as is required in system 300. In addition, one may consider whether the halogen is abundant, inexpensive, and/or environmentally friendly.
  • a thermal process can be used to break the hydrogen halide bond of 260 by using the energy 250 generated in system 200 during the decarbonization step.
  • the chemical reaction for splitting the halogen halide bond can be shown in the reaction equation below:
  • the UV light when the H-Br is split or dissociated, as shown in Table 6 and FIGS. 15-16, the UV light may have a suitable wavelength ranging from about 100 to about 320 nm, from about 200 to about 320 nm, or particular from about 290 to about 320 nm. Further, without wishing to be bound to the theory, the UV light may be radiated at least for about 10 min, and at an intensity of about 50 mJ/cm 2 .
  • the hydrogen gas 340 can be used as a fuel source by itself in various stationary, transportation, and heating applications.
  • hydrogen can be used as a fuel in power engines in vehicles, boats, aircraft, spacecraft, run various electrical devices, fuel cell and battery applications or can be used in the synthesis of carbon-based or nitrogen-based synthetic fuels.
  • the halogen 330 can be returned to the decarbonization chamber 210 and used during decarbonization of system 100.
  • the halogen 330 formed in eq. (11) is a liquid at room temperature.
  • the phase difference between hydrogen (gas) 340 and halogen (liquid) 330 can be advantageous as it will be easier to separate the two species.
  • bromine is a liquid at standard temperature and pressure.
  • the UV light may be radiated at least for about 10 min, and at an intensity of about 50 mJ/cm 2
  • hydrogen 340 and halogen 330 can be separated based on the magnetic properties of each element. As these two gases pass through a magnetic field separation occurs and the halogen gas 330 can be recycled and used in another decarbonization process in combustion chamber 210, whereas hydrogen gas 340 can be used in the next step of the process.
  • the strength of the magnetic field is based on the electromagnetic properties of gases being separated.
  • FIG. 4 is a system block diagram illustrating a system 400 for performing fuel synthesis also called “stitching” such as at 130 in FIG. 1.
  • the fuel synthesis system 400 can include hydrogen 340 and carbon 240 to generate one select species of hydrocarbon 440 (C x H y ), e.g., octane (C 8 H 18 ) or methane (CH 4 )(eq. 12)
  • Y and X define the amounts of hydrogen and carbon respectively.
  • a list of hydrocarbons and their corresponding carbon and hydrogen content and C/H ratios is shown.
  • the gram quantities of starting materials 340 and 240 are based on the amount of hydrocarbon 440, (e.g., octane and/or methane, and the like), desired and its corresponding C/H ratio. Preferably, higher C/H ration is preferred, such that hydrocarbon 440 may be saturated and straight hydrocarbons.
  • Table 4 shows a list of hydrocarbon fuels and their corresponding heat of formation ( ⁇ 3 ⁇ 4) and heat of combustion ( ⁇ 3 ⁇ 4), which indicate that most hydrocarbon fuels are generated in an exothermic fashion.
  • the heat of formation ( ⁇ 3 ⁇ 4) and heat of combustion ( ⁇ 3 ⁇ 4) for octane is also exothermic with values of -252.1kJ/mol and - 5.53 MJ/mol respectively.
  • Octane is a hydrocarbon and an alkane with the chemical formula CsHis and is a component of gasoline (petrol). As a low molecular weight hydrocarbon octane is volatile and flammable.
  • Methane compared to other hydrocarbon fuels when combusted produces less carbon dioxide for each unit of heat released.
  • methane's heat of combustion is lower than any other hydrocarbon but the ratio of the heat of combustion (891 kJ/mol) to the molecular mass (16.0 g/mol, of which 12.0 g/mol is carbon) shows that methane, being the simplest hydrocarbon, produces more heat per mass unit (55.7 kJ/g) than other complex hydrocarbons.
  • heat 430 may be applied to the stitching reaction chamber 410. Once the reaction has been initiated no further energy input may be required to propagate hydrocarbon fuel formation.
  • the initial energy input for the stitching process to synthesize octane and/or methane is at least about the C-H bond energy of 413 Kj/mol.
  • the range in temperature in the stitching reaction chamber is about 10-40 bars and the temperature can range from about 300-350 °C.
  • the starting materials hydrogen gas 340 and solid carbon 240 can be introduced into the stitching reaction chamber in a controlled continuous fashion at a predetermined or predefined rate, where product formation occurs and can be immediately removed from the site of reaction.
  • the hydrocarbon 440 e.g., octane and the like
  • starting materials hydrogen 340 and carbon 240 are added into the stitching reaction chamber at a predetermined rate, where product formation occurs as a droplet of about between lxlO "9 m to about lxl 0 "8 m in diameter, which is continuously removed from the stitching reaction chamber 410 via gravity.
  • the size of the droplet is about lxlO "9 m to about 500x 10 ⁇ 9 m in diameter.
  • the size of the droplet can range from 500xl0 "9 m to about lxlO "8 m in diameter.
  • the stitching reaction chamber 410 can include one or more micro-environments for producing hydrocarbon 440 as droplets.
  • synthesizing hydrocarbons can be performed by providing hydrogen, a vector, and carbon into a micro-environment, for example, having a volume of microscale dimensions.
  • the hydrogen and carbon can be provided in a predetermined ratio selected based on a target hydrocarbon composition.
  • Pressure and temperature of the micro-environment can be controlled to predetermined levels.
  • the predetermined levels can be based on the target hydrocarbon composition.
  • production of a nitrogen- based fuel may also be carried out using elemental hydrogen 340 and nitrogen 240.
  • hydrogen and nitrogen can produce nitrogen-based fuel hydrazine (N 2 H 4 ) (eq.13).
  • Both starting materials are gaseous and the formation of the nitrogen-based fuel species 440 can be controlled by the rate of addition of each gas into the stitching reaction chamber 410.
  • An analogous set-up of the stitching reaction chamber 410 can be used to generate nitrogen-based species 440 as in hydrocarbon 440 production.
  • the generated carbon-based or nitrogen-based fuel 440 can contain single, double and triple atom bonds within the hydrocarbon or nitrogen-based fuel.
  • a stitching vector 420 may be applied during the process of hydrocarbon or nitrogen-based fuel production.
  • This stitching vector 420 can be used to catalyze the formation of the desired fuel 440, e.g., octane, at 298 °K and atmospheric pressure (1 atm.).
  • the stitching vector may increase hydrogen concentration, for example, by forming saturated hydrocarbons, to thereby increase the energy value of the hydrocarbon fuel by increasing.
  • the stitching vector may be an organometallic catalyst comprising at least one metal element selected from the group consisting of Al, Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Y, Zr, Nb, Mo, Tc, Ru, Rh, Pd, Ag, Cd, Hf, Ta, W, Re, Os, Ir, Pt, and Au.
  • the stitching vector 420 can be water based or nitrogen based solvents. In case of the nitrogen-based fuels 440, the stitching vector 420 can be part of the nitrogen-based fuel 440. After the hydrocarbon or nitrogen-based fuel 440 has been produced it will further be modified in a liquefication process.
  • FIG. 5 is a system block diagram illustrating a fuel liquefying system 500 for liquefying fuel such as at 140 in FIG.l.
  • the fuel liquefying system 500 can include the hydrocarbon or nitrogen-based fuel 440 generated and at least one liquefication vector 530 in the liquefier 510.
  • the hydrocarbon, e.g., octane or methane, or nitrogen-based fuel 440 is approximately three times more efficient compared to conventional fuels.
  • the hydrocarbon, e.g., octane or methane, or nitrogen-based fuel 440 generated can be mixed with one or more liquefication vector(s) 530 to a final hydrocarbon or nitrogen-based fuel content of about 30%.
  • the liquefication vector 530 can be mixed with the highly efficient hydrocarbon or nitrogen-based fuel 440 generated but also to liquefy 440 so it is in liquid form at 298 °K at atmospheric pressure (1 atm).
  • the liquefication vector 530 can be non-toxic to the environment and can prevent carbon dioxide and NO x formation during fuel combustion.
  • the liquefication vector 530 may be water based or nitrogen based solvents.
  • the liquefication vector 530 can be part of the nitrogen-based fuel 540.
  • the liquefication vector 530 can be varying depending on the use of fuel 540 in subsequent combustion systems.
  • FIG. 13 illustrates a process flow diagram showing a process 1300 to produce hydrogen 230 and carbon 240 and exemplifies a variation of the process shown in FIG. 1.
  • chloromethane (CH 3 CI) is generated by halogenation of a starting hydrocarbon source such as methane and/or natural gas. This can be performed, for example, by introducing the hydrocarbon, e.g., methane and/or natural gas, and a mixed halogen, e.g. bromochloride (BrCl), into a halogenation chamber.
  • the halogenation can produce at least chloromethane and hydrogen bromide according to eq. (14).
  • Chlorination of methane is preferred over bromination of methane because the heat of formation ( ⁇ /298, kJ/mol) of chloromethane (339 kJ/mol) is higher than bromomethane (284 kJ/mol) making chloromethane the more stable product formed in this process.
  • the bond enthalpy which is the energy required to break a bond cannot exceed 397 kJ/mole, which is the amount of energy carried by ultraviolet light.
  • the energy required to break a C-Cl bond of a bond enthalpy of 330 kJ/mole as shown in eq. 15, 17, 19 and 21 to finally obtain elemental carbon can be provided by an ultraviolet light source.
  • the hydrobromic acid produced in 1320 is converted to hydrogen and bromine upon exposure, for example, of an ultraviolet light source.
  • an ultraviolet light source is 397.32 kJ/mole, which is enough energy to break the H-Br bond of a bond enthalpy of 366 kJ/mol (Table 5)(eq. 22)
  • the UV light may have a suitable wavelength ranging from about 100 to about 320 nm, from about 200 to about 320 nm, or particular from about 290 to about 320 nm.
  • the chlorine produced from 1320 and the bromine produced from 1330 are combined to produce the mixed halogen species, bromochloride, which is subsequently used in 1310.
  • the exposure of these two halogen species occur in the presence of an ultraviolet light source, which provides enough energy to split Br-Br bonds (193.9 Kj/mol) and Cl-Cl bonds (242.6 Kj/mol) and allow formation of Br-Cl bonds (218 Kj/mol) to form the mixed halogen species.
  • the hydrogen produced from 1330 and the carbon produced from 1320 can be combined to generate hydrocarbon species as previously described in Fig. 4 using a stitching reaction chamber analogous to 410 to carry out fuel synthesis as shown in 130 of FIG. 1.
  • Alternate process 1300 allows for the recycling of halogen sources such as bromine and chlorine, which can be expensive when used on large scale.
  • Process 1300 also does not require the separation of gases based on their electromagnetic properties such as the process described in FIG. 1. This separation technique can be challenging and expensive, particularly in the separation of hydrogen and chlorine gas.
  • the process illustrated in FIG. 13 requires several chemical transformations using an ultraviolet light source.
  • a compact UV reactor can be employed, which is able to use only one ultraviolet light source to execute multiple chemical transformations simultaneously and/or in parallel.
  • FIG. 14, for example illustrates such a schematic of a compact UV reactor for use in the processes of 1320, 1330, and/or 1340.
  • a reaction chamber 900 having a volume of 1 m 3 may be provided for decarbonization (110, FIG. 1)
  • Methane 220 may be supplied via inlet and halogen gas 230 may be supplied via inlet as shown in FIG. 9.
  • the halogen gas may be a vaporized bromine gas (Br 2 ).
  • a partial pressure of methane and a partial pressure bromine gas may be maintained at a ratio at least of about 1:2, however, in order f facilitate the decarbonization, the ratio may be controlled, for example, to be of about 1: about 2-10.
  • the reaction chamber may be heated to provide thermal energy, until an internal temperature thereof reaches to a temperature at least of about 400K, of about 500 K, 600 K, 700 K, 800 K, 900 K, 1000K, HOOK, 1200K, 1300K, 1400K, 1500K, 1600K, 1700 K, 1800 K, 1900K, 2000K, 2100K, 2200K, or 2300 K.
  • the reaction chamber may have an internal pressure of about 1 to 20 atm during the decarbonization.
  • the decarbonization may be performed for about 10 minutes to about 20 hours, to completely dissociating carbons and hydrogens and obtain elemental carbon.
  • the obtained elemental carbon 240 may be formed in microparticles and in active carbon.
  • hydrogen halide (HBr) 260 in FIG. 9 may be collected.
  • the hydrogen halide HBr may be decomposed upon radiation of UV light having a wavelength of about 290-330 nm at least for about 10 minutes.
  • the temperature may be maintained in a range of about 300 K to about 1000 K, while the pressure may be maintained in a range of about 0.1 atm to about 10 atm, preferably, reduced to about 0.1 atm.
  • hydrogen gas 340 may be further collected to be used for synthesis of hydrocarbon fuels.
  • the elemental carbon microparticles 240 may be placed in a reactor having a volume of 1 m 3 , and hydrogen gas may be supplied until the internal pressure of the chamber reaches, for example to about 10-40 bars or 7 to 20 bars, and the temperature can range from about 300-350 °C.
  • the synthesis reaction may be conducted in the present of a catalyst, for example, organometallic catalyst comprising at least one transition metal.
  • the synthesis reaction may be performed at a temperature ranging from about 300- 350 °C, however, the temperature may be increased higher upon the reaction rate based on the catalyst.
  • the synthesis of the hydrocarbon fuel may be performed at least for about 1 hour, 2 hours, 3 hours, 4 hours, 5 hours, 6 hours, 7 hours, 8 hours, 9 hours, or 10 hours.
  • the obtained hydrocarbon fuel including substantially homogeneous octane may be confirmed by using suitable mass analysis methods, for example, with GC/mass analysis by checking peak traces, but the detection methods may not be limited thereto.

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Abstract

L'invention concerne la production de carburants propres à base d'hydrocarbures ou d'azote, par exemple, par décarbonisation d'hydrocarbures sources à l'aide d'halogène pour produire du carbone élémentaire et des espèces halogénure d'hydrogène. Les espèces halogénure d'hydrogène peuvent être séparées par addition d'énergie pour produire de l'hydrogène et un halogène. En outre, un carburant comprenant des hydrocarbures de composition sensiblement homogène et un vecteur peut être synthétisé à partir de l'hydrogène et du carbone. L'invention concerne également un appareil, des systèmes, des techniques et des compositions de matériaux associés.
PCT/US2015/056253 2014-10-17 2015-10-19 Production de carburant propre à base d'hydrocarbures et d'azote Ceased WO2016061584A1 (fr)

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Citations (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0112117A2 (fr) * 1982-12-14 1984-06-27 King-Wilkinson Project Services, Inc. Procédé de conversion de matériaux carbonés
CA1222629A (fr) * 1983-05-17 1987-06-09 James J. Russ Procede de conversion de matieres carbonees en hydrogene, hydrocarbures gazeux, monoxyde de carbone et anhydride carbonique
US5389230A (en) * 1993-06-11 1995-02-14 Exxon Research & Engineering Co. Catalytic hydroconversion process
US20060078481A1 (en) * 2004-10-12 2006-04-13 Infineon Technologies Richmond Lp System and method for corrosive vapor reduction by ultraviolet light
US20060100469A1 (en) * 2004-04-16 2006-05-11 Waycuilis John J Process for converting gaseous alkanes to olefins and liquid hydrocarbons
US20110120918A1 (en) * 2009-11-24 2011-05-26 Chevron U.S.A. Inc. Hydrogenation of solid carbonaceous materials using mixed catalysts
US20110230683A1 (en) * 2008-09-26 2011-09-22 Michael Benje Process and apparatus for producing ethylenically unsaturated halogenated hydrocarbons
WO2013156620A1 (fr) * 2012-04-20 2013-10-24 Kemira Oyj Traitement de l'eau

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Publication number Priority date Publication date Assignee Title
EP0112117A2 (fr) * 1982-12-14 1984-06-27 King-Wilkinson Project Services, Inc. Procédé de conversion de matériaux carbonés
CA1222629A (fr) * 1983-05-17 1987-06-09 James J. Russ Procede de conversion de matieres carbonees en hydrogene, hydrocarbures gazeux, monoxyde de carbone et anhydride carbonique
US5389230A (en) * 1993-06-11 1995-02-14 Exxon Research & Engineering Co. Catalytic hydroconversion process
US20060100469A1 (en) * 2004-04-16 2006-05-11 Waycuilis John J Process for converting gaseous alkanes to olefins and liquid hydrocarbons
US20060078481A1 (en) * 2004-10-12 2006-04-13 Infineon Technologies Richmond Lp System and method for corrosive vapor reduction by ultraviolet light
US20110230683A1 (en) * 2008-09-26 2011-09-22 Michael Benje Process and apparatus for producing ethylenically unsaturated halogenated hydrocarbons
US20110120918A1 (en) * 2009-11-24 2011-05-26 Chevron U.S.A. Inc. Hydrogenation of solid carbonaceous materials using mixed catalysts
WO2013156620A1 (fr) * 2012-04-20 2013-10-24 Kemira Oyj Traitement de l'eau

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BRADSHAW, RW ET AL.: "PRODUCTION OF HYDROBROMIC ACID FROM BROMINE AND METHANE FOR HYDROGEN PRODUCTION.", PROCEEDINGS OF THE 2001 DOE HYDROGEN PROGRAM REVIEW NREL/CP-570-30535, 2001 *
PERRY, RH ET AL: "PERRY'S CHEMICAL ENGINEER 'S HANDBOOK", MCGRAW HILL, 00001999, article PERRY, RH ET AL. *

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