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13 consumingby-products.Thisnewprocesscalledbi-reform ing is a speci?c combination of steam (H20) and dry (CO2) 14 ous?oW reactorscanbeusedtocarryoutthebi-reforming alloWsforsubstantiallycompleteutiliZationandincorpora tionofalH2 produced intomethanol ordimethyl ether.This represents an e?icient and economical neW Way ofmethanol and/or dimethyl ether production, as Well as an ef?cient neW processforrecyclingofcarbondioxideintomethanol(and/or inasubsequentstepdimethylether),thusrenderingthecar bonfuelsreneWableandenvironmentallycarbonneutral.The process is not accompanied by any signi?cant coke forma tion, as presence of steam in the systems retards coke forma US 7,906,559B2 reforming of methane, practiced in tWo steps or combined intoasinglestep.Themethodcomprisesreactingmethaneor natural gas under a combination of conditions of steam (Wet) anddry(CO2)reforminginaspeci?cmoleratioofreactants suf?cienttoproducemixtureofcarbonmonoxide/hydrogen (CO/H2) in a molar ratio of (1:2), and subsequently further suf?cienttoconvertsuchmixtureofCO andH2exclusivelyto methanoland/ordimethylether.Advantageously,themixture ofreactantsistreatedWithoutseparationofitscomponentsto convert substantially all the reactants to methyl alcohol or dimethyletherWithoutanyby-products.Anyunreactedstart tionandanycarbondepositstilformedisinsituconvertedby ing or intermediate products can be readily recovered and recycled.Theprocessproducesinhighselectivityandyield of methanol or dimethyl ether. As discussed in preceding sections, syn-gas of varying composition can be produced by a variety of reactions. It is generallyproducedbythereactionofcoalormethanenatural gasWithsteam(steamreforming).Syn-gascanalsobepro ducedbythereactionofCO2 Withmethaneornaturalgasin a process called “CO2” or “dry” reforming, because itdoes not involve steam. The gas mixture produced from methane and CO2, hoW ever, has an H2/CO ratio of 1. Therefore, for methanol pro duction, hydrogen generated from other sources must be added to the obtain the needed ratio of 2. Thepresentinventionusingbi-reformingofCO2over comes this dif?culty and produces a H2/CO mixture With a molar ratio of 2, needed for methanol synthesis. It achieves the goal by using a speci?c combination of steam and dry reformingofmethane.Inthesubsequentmethanolsynthesis step,substantiallyalofthehydrogenisconvertedtometha nol.As describedinourco-pendingpatentapplications,this subsequent step can be performed, Without limitation, by direct catalytic conversion, or by a reaction Which involves a methylformateintermediate. reactingWithCO2 toformCO. As indicatedasigni?cantfurtherembodimentofourinven Steamreforming 2CH4+ZHZO Dryreforming CH4+CO;—>2C0+2H; tion is in the use of bi-reforming in preparing dimethyl ether (DME)usingdehydrationofproducedmethanol. 20 RecyclingtheequivalentamountofWaterproducedmakes theproductionofDME frommethaneandCO2 overall With no external Water needed or Water produced consuming 25 hydrogen.Thisisofsubstantialadvantagenotonlyeconomi callybutparticularlyinaridareasWhen clean,saltfreeWater isnotreadilyavailable.ItiscontrastedWiththepresentlyused process of the oxidative conversion of methane to DME, Where, hoWever, 1/3 of the methane is used up in producing 30 by-productWater. Steam and dry reforming are knoWn in the art as separate technologies.SteamreformingofmethanetoamixtureofCO 35 and3H2isanextensivelyusedandpracticedprocess(endot hermicby49.1kcal/mol).Dryreformingofmethaneto2CO+ 2H2 (endothermic by 59.1 kcal/mol), hoWever, is a relatively lessdevelopedprocess.Ourdiscoverednanostructuredsilica supportedmixedacidcatalystsmaketheCO2reformingstep, 40 hoWever,practicalandeconomical. As canbe appreciatedby one ofskillintheart,theenergy requiredforthebi-reformingprocesscancomefromany suitable energy source, including, but not limited to, excess energy fossil burning poWer plants produce in off peak use 200+6H2 Bi-reforming3CH4+ZHZO+CO;—> 45periods,anyalternativeenergysources,atomicenergy,etc. The bi-reforming process of methane or natural gas and car A preferredembodimentofthisinventiondescribestheuse ofaspeci?ccombinationofsteamanddryreformingWitha 50 molar ratio of CO:H2 of 1:2 using mixed metal-metal oxide catalysts.Thetemperaturerangefortheprocessisintherange of 800 to 11000 C., preferentially at 850-9500 C. The neWly discovered and developed catalysts for this process shoW goodstabilityandcatalyticactivity.Withoutbeinglimiting,55 etc.)and/orimpurities.Regardless,itisWithinthescopeof such combinations ofcatalysts include mixed metal oxides such as NiOiVZOS, metal-metal oxides such as NiiVZOS, (Ni2O3iV2O5), as Well as mixed oxides such as Ni2V2O7 and Ni3V2O8, on suitable high surface areas supports such as silica,alumina,metaloxideormetal.Oneofskillintheart60 gascontaininghigherhydrocarbonsinvariousconcentra Would immediately appreciate that a number of other related metal such as single or mixed catalysts based on V, Ti, Ga, Mg,Cu,Mo,Bi,Fe,Mn,Co,Nb,Zr,LaorSn,andmetaloxide catalysts, and their combinations, can achieve the process of thecurrentinvention.Suitablereactorsforthisprocesscan 65 similarly be immediately appreciated by a person of skill in theart.Withoutbeinglimiting,forexamplesuitablecontinu tions, can be used for the bi-reforming process according to thefolloWingadjustmentofthereactants: process in the indicated temperature range. The BI-REFORMINGTM process ofthe present invention bon dioxide to produce regular dimethyl ether is an energy storage and fuel producing process, but not one of energy production. Inanyembodiment,Withoutbeinglimiting,anymethane source may be used including natural gas, coalbed gas, a methanehydrate,orthehydrolysisofaluminiumcarbide.The methane source may contain, besides methane, varying amounts of higher hydrocarbons (ethane, propane, butane, thepresentinventiontoadjusttheamountsofthealkane,CO2 and H2 to achieve the reaction conditions of the BI-RE FORMINGTM process. In a further embodiment of the present invention, natural (Whenn:1representsmethaneitself) Any suitablesourceofnaturalgasormethanecanbeused formethanolorDME productionaccordingtothepresentPDF Image | CONVERSION OF CARBON DIOXIDE TO METHANOL
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