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US 7,906,559B2 12 CONVERSION OF CARBON DIOXIDE TO METHANOL AND/OR DIMETHYL ETHER USING BI-REFORMING OF METHANE OR NATURAL GAS This application claims the bene?t of application No. 60/945,501 ?led Jun. 21, 2007. The entire content of that application is expressly incorporated herein by reference thereto. 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 hydrocarbons With varying ratios of carbon to hydrogen. DespitetheirWideapplicationandhighdemand,fossilfuels alsohavelimitationsanddisadvantages,particularlydueto 20 their ?nite reserve, irreversible combustion and contribution to air pollution (and thus to global Warming). Regardless of theseproblems themore e?icientuse ofstilexistingnatural gassourcesishighlydesirable.FurtherneW sourcesandWays forrecyclableandenvironmentallybenigncarbonfuelsare25 needed. One alternative frequently mentioned non-carbon fuel is hydrogen, and its use in the so-called “hydrogen economy.” Hydrogen isthought to be bene?cial as a clean fuel, produc ingonlyWaterWhencombusted.Freehydrogen,hoWever,is30 notanaturalprimaryenergysourceonearth,duetoitsincom patibilityWithatmosphericoxygen.Itmustbegeneratedfrom hydrocarbonsorWaterisahighlyenergy-consumingprocess. Further,ashydrogenisproducedfromhydrocarbonsorcoal, anyclaimedbene?tofhydrogenasacleanfuelisoutWeighed 35 bythefactthatitsgeneration,mainlybyreformingofnatural gas,oilorcoaltosynthesisgas (“syn-gas”amixtureofCO andH2),orthegenerationofelectricityfortheelectrolysisof Water is far from clean, besides hydrogen is dif?cult and costlytohandle,transportanddistribute.Asitisextremely40 light,volatileandpotentiallyexplosive,itrequireshigh-pres sure equipment. The needed non-existent infrastructure also necessitatesspecialmaterialstominimiZediffusionandleak age,andextensivesafetyprecautionstopreventexplosions. ThecontinuedimportationofnaturalgasfromfaraWay 45 and frequently dif?cult to access locations also necessitates its safe storage and transportation particularly When involv ingtoLNG (lique?ednaturalgas).Thisnecessitiestransport ingLNG atloWtemperaturesinitsliquidformovertheseas exposingittoseriousenvironmentalandsafetyhaZards50 including terrorism. Itis suggested that a more practical and safe alternative for LNG is methanol, or dimethyl ether (DME), Which are readily produced from natural gas (vide infra).Methanol,CH3OH,isthesimplestliquidoxygenated hydrocarbon,differingfrommethane(CH4)byasingleaddi 55 tional oxygen atom. Methanol, also called methyl alcohol or Wood alcohol,isacolorless,Water-solubleliquidWithamild 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 existing coal or natural gas sources via methods developed andpracticedsincethe1920’s.HoWever,thesemethodsusing conversion (reforming) of coal and subsequently natural gas tosyn-gas(amixtureofH2andCO)arehighlyenergycon 65 sumingandproducelargeamountofCO2 asaby-product. Thisisnotablyaneconomicdisadvantagebutalsorepresents a serious environmental problem by increasing a main green housegas(causingglobalWarming). 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 viabi-reforming.Itisa particularly effective fuel for diesel engines because of its high 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 combus tion engines or electricity generators. One of the most e?i cient 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 densityofgasoline,meaningthattWolitersofmethanolpro vide the same energy as a liter of gasoline. Even though methanol’s energy content is loWer, it has a higher octane rating of 100 (average of the research octane number (RON) of107andmotoroctanenumber(MON) of92),Whichmeans thatthefuel/airmixturecanbecompressedtoasmallervol ume before being ignited. This alloWs the engine to run at a higher compression ratio of 10-11 to 1 more e?iciently than the 8-9 to 1 ratio of a gasoline-poWered engine. Ef?ciency is alsoincreasedbymethanol’s(andoxygenate)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 volatilecomponentsorWithadevicetovaporiZeoratomiZe methanol. For example, an effective automotive fuel com prisedbyaddingmethanoltogasolineWiththefuelhavinga minimum gasoline content of at least 15% by volume (M85 fuel) so that it can readily start even in loW temperature environmentsWerecommerciallyusedintheUS inthe 1980’s.M20 fuel(With20volume% methanol)isalsobeing introduced.Similarly,dimethylether(DME)mixedWithdie seloilorinhouseholduse asasubstituteofnaturalgasorLPG is of commercial interest. These mixtures are not only e?i cientfuelsbutconserveorreplacedecreasingoilresources. 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 largeramountofheatWhenpassingfromliquidtogaseous state. This helps remove heat aWay from the engine and enables the use of an air-cooled radiator instead of a heavier Water-cooledsystem.Thus,comparedtoagasoline-poWered car,amethanol-poWeredengineprovidesasmaller,lighter engineblock,reducedcoolingrequirements,andbetteraccel erationandmileagecapabilities.MethanolandDME arealso more environment-friendly than gasoline or diesel oil, and produceloWoverallemissionsofairpollutantssuchascertain hydrocarbons,NOX,S02andparticulates. Methanol is also one of the safest fuels available. Com paredtogasoline,methanol’sphysicalandchemicalproper ties signi?cantly reduce the risk of ?re. Methanol has loWer volatility, and methanol vapor must be four times more con centrated than gasoline for ignition to occur. Even When ignited,methanolburnsaboutfourtimessloWerthangaso line,releasesheatonlyatone-eighththerateofgasoline?re, andisfarlesslikelytospreadtosurroundingignitablemate 60PDF Image | CONVERSION OF CARBON DIOXIDE TO METHANOL
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