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US 8,440,729B2 12 CONVERSION OF CARBON DIOXIDE TO METHANOL USING BI-REFORMING OF METHANE OR NATURAL GAS CROSS-REFERENCE TO RELATED APPLICATIONS This application is a continuation of application Ser. No. 12/941,773 ?led Nov. 8, 2010, Which is a continuation of applicationSer.No. 11/850,501?ledSep.5,2007,nowUS. Pat. No. 7,906,559, Which claims the bene?t of application No. 60/945,501 ?led Jun. 21, 2007. Each document is expresslyincorporatedhereinbyreferencethereto. BACKGROUND Hydrocarbons are essential in modern life. Hydrocarbons are used as fuel and raW material in various ?elds, including thechemical,petrochemical,plastics,andrubberindustries. Fossilfuels,suchascoal,oilandnaturalgas,arecomposedof 20 hydrocarbons With varying ratios of carbon to hydrogen. DespitetheirWideapplicationandhighdemand,fossilfuels also have limitations and disadvantages, particularly due to their ?nite reserve, irreversible combustion and contribution toairpollution(andthustoglobalWarming).Regardlessof25 theseproblems themore e?icientuse ofstilexistingnatural gassourcesishighlydesirable.FurtherneW sourcesandWays for recyclable and environmentally benign carbon fuels are needed. Onealternativefrequentlymentionednon-carbonfuelis30 hydrogen, and its use in the so-called “hydrogen economy.” Hydrogen isthought to be bene?cial as a clean fuel, produc ing only Water When combusted. Free hydrogen, hoWever, is notanaturalprimaryenergysourceonearth,duetoitsincom patibilityWiththeatmosphericoxygen.Itmustbegenerated35 from hydrocarbons or Water, Which is a highly energy-con suming process. Further, as hydrogen is produced from hydrocarbons or coal, any claimed bene?t of hydrogen as a cleanfuelisoutWeighedbythefactthatitsgeneration,mainly byreformingofnaturalgas,oilorcoaltosynthesisgas40 (“syn-gas”amixtureofCO andH2),orthegenerationof electricity for the electrolysis of Water is far from clean, besides hydrogen is dif?cult and costly to handle, transport anddistribute.Asitisextremelylight,volatileandpotentially explosive,itrequireshigh-pressureequipment.Theneeded45 non-existentinfrastructurealsonecessitatesspecialmaterials to minimize diffusion and leakage, and extensive safety pre cautionstopreventexplosions. The continued importation of natural gas from far aWay andfrequentlydif?culttoaccesslocationsalsonecessitates 50 its safe storage and transportation particularly When involv ing lique?ed natural gas (LNG). This necessitates transport ingLNG atloWtemperaturesinitsliquidformexposingitto seriousenvironmentalandsafetyhaZards.Itissuggestedthat amorepracticalandsafealternativeforLNG ismethanol,or 55 dimethyl ether (DME), Which are readily produced from natural gas. Methanol is the simplest liquid oxygenated hydrocarbon,differingfrommethane(CH4)byasingleaddi tional oxygen atom. Methanol, also called methyl alcohol or Woodalcohol,isacolorless,Water-solubleliquidWithamild 60 alcoholic odor. It is easy to store and transport. It freeZes at —97.60 C., boils at 64.60 C., and has a density of0.791 at 200 C. Methanol is a convenient safe liquid easily obtained from existingcoalornaturalgassourcesviamethodsdeveloped 65 andpracticedsincethe1920’s.HoWever,thesemethodsusing conversion (reforming) of coal and subsequently natural gas to syn-gas (a mixture of H2 and CO) are highly energy con suming and produce large amount of CO2 as a by-product. Thisisnotablyaneconomicdisadvantagebutalsorepresents a serious environmental problem by increasing one of the maingreenhousegascausingglobalWarming. Methanol not only represent a convenient and safe Way to storeandtransportenergy,buttogetherWithitsderivedprod uct dimethyl ether (DME), is an excellent fuel. Dimethyl ether is easily obtained from methanol by dehydration or frommethane(naturalgas)WithCO2 viaabi-reformingpro cess. It is a particularly effective fuel for diesel engines because of itshigh cetane number and favorable combustion properties. Methanol and dimethyl ether exceedingly blend Well With gasoline or diesel oil to be used as fuels in internal combustionenginesorelectricitygenerators.One ofthemost e?icient use of methanol is in fuel cells, particularly in direct methanol fuel cells (DMFC), in Which methanol is directly oxidiZed With air to carbon dioxide and Water While produc ingelectricity. Contrarytogasoline,Whichisacomplexmixtureofmany different hydrocarbons and additives, methanol is a single simple chemical compound. Itcontains about halfthe energy density of gasoline, meaning that tWo liters of methanol pro vide the same energy as a liter of gasoline. Even though the energycontentofmethanolisloWer,ithasahigheroctane rating of 100 (average of the research octane number (RON) of107andmotoroctanenumber(MON) of92),Whichmeans that the fuel/air mixture can be compressed to a smaller vol ume before being ignited. This alloWs the engine to run at a highercompressionratioof10-11to1moree?icientlythan the 8-9 to 1 ratio of a gasoline-poWered engine. Ef?ciency is also increased by methanol’s (oxygenates’) higher “?ame speed,”Whichenablesfaster,morecompletefuelcombustion in the engines. These factors explain the high ef?ciency of methanoldespiteitsloWerenergydensitythangasoline.Fur ther, to render methanol more ignitable even under the mo st frigidconditions,methanolismixedWithgasoline,andother volatile components or With a device to vaporiZe or atomiZe methanol. For example, an effective automotive fuel com prisedbyaddingmethanoltogasolineWiththefuelhavinga minimum gasoline content of at least 15% by volume (M85 fuel) so that the engine can readily start even in loW tempera tureenvironmentsWerecommerciallyusedintheUS inthe 1980’s.M20fuel(With20volume% methanol)isalsobeing introduced.Similarly,dimethylether(DME)mixedWithdie seloilorinhouseholduse asasubstituteofnaturalgasorLPG is of commercial interest. These mixtures are not only e?i cient fuels but conserve or replace decreasing oil resources. The amount of methanol or dimethyl ether added can be determineddependinguponthespeci?cconditionandneeds. Methanol has a latent heat of vaporiZation of about 3.7 times higher than gasoline, and can absorb a signi?cantly larger amount of heat When passing from liquid to gaseous state. This helps to remove heat aWay from the engine and enablestheuseofanair-cooledradiatorinsteadofaheavier Water-cooledsystem.Thus,comparedtoagasoline-poWered car, a methanol-powered engine provides a smaller, lighter engineblock,reducedcoolingrequirements,andbetteraccel erationandmileagecapabilities.MethanolandDME arealso moreenvironmentally-friendlythangasolineordieseloil, and produce loW overall emissions of air pollutants such as certain hydrocarbons, NOX, S02 and particulates. Methanol is also one of the safest fuels available. Com paredtogasoline,itsphysicalandchemicalpropertiessig ni?cantlyreducetheriskof?re.MethanolhasloWervolatil ity,andmethanolvapormustbefourtimesmore concentrated thangasolineforignitiontooccur.EvenWhenignited,methaPDF Image | CONVERSION OF CARBON DIOXIDE TO METHANOL BIOREFORMING
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