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US 7,906,559B2 15 16 invention. Other than the conventional natural gas sources, they can be produced, for instance, from “biogas,” a result of anaerobic bacteria’s breaking doWn organic material in the absenceofoxygen.Biogasisproducedinthedigestivetracks ofmost mammals, organisms such as termites, and microor ganismsduringdigestion,asWellasinWetlands,sWamps and bogs,Wherelargeamountsofrottingvegetationaccumulate. Biogasiscomposedmainlyofmethaneandcarbondioxidein varying proportions, and contains trace levels of other ele ments such as hydrogen sul?de (HZS), hydrogen, and/or car bon monoxide. In all these embodiments, carbon dioxide obtained from any available source, such as, Without being limiting, emis sionsofpoWerplantsburningfossilfuels,fermentationpro cesses, calcination of limestone, other industrial sources, or even the atmosphere is utiliZed via its chemical recycling providingreneWablecarbonfuelsintomitigatingtheenviron mentallyharmfuleffectofexcessCO2. Inapreferredembodi ment ofthe invention, the carbon dioxide source isan exhaust streamfromfossilfuelburningpoWerorindustrialplant,ora 20 sourceaccompanyingnaturalgas.A non-limitingutilityof the present invention is the chemical recycling of carbon dioxide, instead of its sequestration, produced by coal and otherfossilfuelburningpoWerplantsandindustriesproduc ing large amounts of carbon dioxide. 25 In an alternative embodiment of the invention, the carbon dioxide source is the atmosphere. If carbon dioxide content can be separated and absorbed by using various processes as describedintheco-pendingpatentapplication,(publication no.20060235091).As analternative,itisalsopossibleto 30 utiliZe and recycle the carbon dioxide content of the atmo sphere by different chemical processes, as disclosed and claimed in co-pending patent application, publication no. 20060235088. In these embodiments, the needed hydrogen may be 35 derivedfromavarietyofsources,includingthehydrolysisor cleavage of Water In a preferred embodiment, an e?icient sourceforH2 istheprocessofsteamreformingofnaturalgas, including,Withoutlimitation,incombinationWiththeWater gas shiftreaction. 40 duced. This concept isbased on the synergetic combination of dry reforming, steam reforming and partial oxidation of methane in a single step. The exothermic oxidation of meth ane With oxygen produces the heat needed for the endother mic steam and dry reforming reactions alloWing to reach a suitableSvalueofsyngasformethanolproduction.HoWever, theinvolvedoxidationofmethaneWithoxygenalsoproduces excessofcarbondioxidebecauseofitseffectonglobalWarm ing represents a serious environmental haZard. The disclosed bi-reformingprocessminimiZesthisproblem. Methanol or dimethyl ether produced according to our disclosed invention can ?nd utility in numerous applications, either on their oWn, or With subsequent conversion to other products. Without being limiting, methanol and dimethyl ether can be used as suitable synthetic fuels, replacing our diminishing fossil fuel sources improved diesel fuels, trans portation fuels. They are also useful as convenient energy storage and transportation materials, Which minimize or eliminatethedisadvantagesordangersinherentintheuseand transportationofLNG orLPG.Theyarealsoofgreatsigni? cance as starting materials for light ole?ns (ethylene, propy lene, etc.) and subsequently to synthetic hydrocarbons and their varied products. It is also possible to use them for pre paring singlecellproteinsforhuman oranimal alimentation. The invention described and claimed herein is not to be limited in scope by the speci?c embodiments herein dis closed, as these embodiments are intended as illustrative of severalaspectsoftheinvention.Anyequivalentembodiments areintendedtobeWithinthescopeofthisinvention,asthey Will become apparent to those skilled in the art from the present description. Such embodiments are also intended to fall Within the scope of the appended claims. EXAMPLE 1 A suitablemolarmixtureofCO2,methane(ornaturalgas) and steams is bi-reformed in a How reactor over VZOS/NiO catalyst support on silica at a temperature of ~800-850° C. producing a gas mixture With a molecular approximate ratio ofCO and2H2WithaconversionofmethaneandCO2in excess of 90%. The disclosed bi-reforming process can ?nd multiple utili ties.Withoutbeinglimiting,thecombinationofsteamanddry reformingcanbeusedfortherecyclingofCO2 emissions fromcoalandotherfossilfuelsburningpoWerplants.Itisalso advantageousforuseandrecyclingofCO2fromnaturalgas 45 sources,WhichtypicallycontainsubstantialCO2 concentra tions.Thisisadditionallypractical,asCO2Would,otherWise, havetoberemovedtoalloWfurtherprocessingofthenatural suitablylargenanostructuralsurface. gas. Some natural gas sources contain CO2 concentration from 5 to 20%. For example, the natural gas at the Sleipner platforminNorWaycontains,forexample,9% CO2.There, the CO2 is currently already separated and sequestered beneath the North Sea in a deep saline aquifer. Other CO2 separation and sequestration processes are already being practicedinAlgeriaandotherlocations,butsequestrationis 55 only a temporary, costly storage process With the danger of catastrophicreleaseoflargeamountsofCO2Whengeological events (such as earthquakes) occur. Methane hydrates are composed of methane trapped by Water in cage like structures called clathrates. Methane 60 hydrate could be processed using a combination With bi reforming Where Water in the from of steam is added to react With methane. The transformation to syn-gas and further to methanolorDME mightrendertheexploitationofmethane hydratemore economical. Building on the experience With autothermal reforming, theconceptof“thermoneutraltri-reforming”hasbeenintro EXAMPLE 3 Recycling of Water formed in the bi-reforming process of Example 1alloWscontinuousconversionofCO2 Withmeth ane(naturalgas)exclusivelytogivedimethyether. EXAMPLE 4 ExitstreamsofExamples 1and2Werecombinedinaratio to obtain gas mixture of a 2:1 mole ratio of H2 and CO, Which issubsequentlyconvertedtomethanolusingusuallypractical conditions over copper based catalysis. EXAMPLE 5 A mixture of methane, CO2 and H20 (3:1:2 mole ratio) Were reacted (bi-reformed) over a catalyst composed of VZOS/NiO supported on nanostructural high surface area 50 65 EXAMPLE 2 Support of catalyst in example 1 is fused silica having aPDF Image | CONVERSION OF CARBON DIOXIDE TO METHANOL
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