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13 catalystsmay beusedasasinglemetal,oracombinationofa metal and metal oxide, or a combination of metal oxides, supported on a suitable support such as a high surface area nanostructured oxide support such as fumed silica or fumed alumina. By Way ofexample, NiO, metal-metal oxides such as NiiVZOS, (M2O3iV2O5), and NiO:V2O5, as Well as mixedoxidessuchasNi2V2O7 andNi3V2O8 canbeused.One ofskillintheartWouldimmediatelyappreciatethatanumber of other related metal and metal oxide catalysts, and their combinations, can also be used. Suitable reactors for the conversion reactions can also be used. For example, a con tinuous?oW reactorundertheappropriatereactionconditions canbeusedforthereactionstoproceedtocompletioneither at ambient pressure or high pressure. Carbon dioxide is not sequestered or released into the atmosphereandmethaneiscompletelyconvertedtomethanol Withoutproducinganyby-product.Thisprovidesforsigni? cant economical and environmental advantages. By contrast Withtheprocessesdescribedherein,thetri-reformingprocess ofmethaneinWhichasynergeticcombinationofdryreform 20 ing, steam reforming and partial oxidation of methane is carried out in a single step, but produces by-products (CO2 and H20) in the oxidation step. By contrast With the tri reformingprocess,theprocessoftheinventionprovidesfor, control,highselectivityandyieldoftheconversionofcarbon25 dioxide to methanol Without any by-products and Without encountering the di?iculties and having the disadvantages associated With concurrent partial oxidation resulting in undesirable excess carbon dioxide and Water. Thebi-reformingprocessesoftheinventioncanbeusedfor 30 the preparation of dimethyl ether Without Water formation as a by-product, as is the case in the presently used dehydration ofmethanol. This provides an additional advantage as com paredtothedryreformingprocessofproducingmethaneasit givesonlya1:1molarmixtureofCOandH2andisnot35 suitableWithoutmodi?cationstotheproductionofdimethyl ether as illustrated by the folloWing reaction. Fortheproductionofdimethylether,Waterobtainedfrom 40 thedehydrationofmethanolcanberecycledandreactedWith carbon dioxide and methane With no by-product (H2O or CO2) formation in the overall process. Water removal is achieved over a suitable dry silica catalyst or a polymeric per?uoroalkanesulfonicacidcatalystatatemperatureoffrom 45 about 100° C. to 2000 C. An example of such catalyst is Na?on-H. 14 production of methanol Application to natural gas is illus tratedbythefolloWingreaction: Theprocessesoftheinventionhavesigni?cantadvantages over the use of syn-gas as itWould apply to the production of methanol.Syn-gasofvaryingcompositionscanbeproduced by a variety of reactions. It is generally produced by the reaction of coal, methane, or natural gas With steam (steam reforming). As mentioned in Step B, syn-gas can also be producedbythereactionofCO2 Withmethaneornaturalgas inaprocesscalled“CO2” or“dry”reforming,becauseitdoes not involve steam. The gas mixture produced from methane and CO2, has an H2/CO ratiocloseto 1.Therefore, formetha nolproduction,hydrogengeneratedfromothersourcesmust be added to obtain the molar ratio of about 2:1. There is no upper limit for this ratio as long as there is an excess of hydrogen. Therefore, the present invention overcomes this dif?cultyandproducesaH2/COmixtureWithamolarratioof at least 2 to 1, Which is a requirement for the formation of methanol,Whichisachievedbyusingaspeci?ccombination ofsteamanddryreformingofmethaneandsubstantiallyalof thehydrogenconvertedtomethanol.As describedinU.S.Pat. No.7,705,059,thissubsequentstepcanbeperformed,With outlimitation,bydirectcatalyticconversion,orbyareaction, Which involves methyl formate as an intermediate. The processes of the present invention alloW for the sub stantially complete utiliZation of carbon monoxide to form methanolordimethylether.Thisrepresentsane?icientand economical neW Way ofmethanol ordimethyl etherproduc tion, as Well as an ef?cient neW process for recycling of carbon dioxide into methanol or dimethyl ether, thus render ing the carbon fuels reneWable and environmentally carbon neutral.Theprocessisnotaccompaniedbyanysigni?cant coke formation, as presence of steam in the bi-reforming process retards coke formation and any carbon deposit stil formedisinsituconvertedbyreactingWithCO2 toformCO. The processes of the invention to produce dimethyl ether alsoalloWforrecyclingoftheWaterproducedfromthesub sequent dehydration of formed methanol and do not require the use of external Water. As canbe appreciatedby one ofskillintheart,theenergy required for the bi-reforming processes can come from any suitableenergysource,including,butnotlimitedto,excess energyfossilburningpoWerplantsproducedinoffpeakuse periods, any alternative energy sources, atomic energy, etc. The bi-reforming process of methane or natural gas and car bon dioxide to form dimethyl ether is an energy storage and fuelproducingprocess,butnotoneofenergyproduction. Natural gas as used in this application Would include all conventional natural gas sources, and any suitable source of natural gas or methane can be used. Natural gas is a naturally occurring hydrocarbon gas mixture that primarily includes methane,Withupto20percentofotherhydrocarbonssuchas ethane as Well as small amounts of impurities such as carbon dioxide. Natural gas can be found in deep underground natu ral rock formations or associated With other hydrocarbon reservoirs, in coal beds, and as methane clathrates. Most naturalgasWascreatedovertimebytWomechanisms:bio genicandthermogenic.Biogenicgasorbiogasiscreatedby methanogenic organisms in marshes, bogs, land?lls, and shalloW sediments. Deeper in the earth, at greater tempera tures and pressures, thermogenic gas is created from buried organicmaterial. Biogas is generally a result of anaerobic bacteria’s break ingdoWnorganicmaterialintheabsenceofoxygen.Biogasis The stepsoftheprocessoftheinventionfortheproduction of dimethyl ether are illustrated by the folloWing reactions: In an embodiment of the invention, the Water formed dur ingthedehydrationofmethanolisreactedWithCH4 andCO2 ofabout2:3:1overallmolarratiotoformdimethylether.With Waterrecycling,dimethyletherisformedusingmethaneand 60 CO2 inanoverallratioofabout3:1. The dry-reforming process of the invention can also be directly applied to natural gas (mixture of hydrocarbons) itselfto form methanol or dimethyl ether in a separate step or inasinglestepWithproperselectionofmixingtoobtainthe 65 needed H2 and CO molar mixture of at least 2 moles of hydrogen to one mole of carbon monoxide required for the US 8,440,729B2 50 55PDF Image | CONVERSION OF CARBON DIOXIDE TO METHANOL BIOREFORMING
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