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17 Example 3 Carbon dioxide is electrochemically reduced to carbon monoxide and subsequently is reacted further as in Example 7. Example4 ThemethylformateobtainedbytheprocessesofExamples 1-3 is catalytically reduced With molecular hydrogen in the gas phase over copper chromite or noble metal catalysts at atmosphericpressureinthetemperaturerangeof100-2300C. Selectivitytomethanolis>90% andmethylformateconver sionisabout85to90%.A similarreductiveconversioncan alsobeachievedelectrochemically. Example 5 Methyl formate is catalytically reduced With formic acid over Pt/C, Rh/C, Ru/C, copper chromite and the like catalyts in the gas phase at atmospheric pressure in the temperature range of 100-2000 C. Selectivity to methanol is over 70-90% andmethylformateconversionis50% inasinglepass. Example 6 25 18 converting the carbon dioxide thus obtained under con ditions su?icient to produce methanol as the material or fuel. 2. The method of claim 1, Wherein the methanol is pro duced by reducing the carbon dioxide under conditions suf ?cient to produce a reaction mixture containing formic acid With concomittant formation of formaldehyde and small amounts of methanol and methane, folloWed, Without sepa ration of the reaction mixture, by a treatment step conducted under conditions su?icient to convert the formaldehyde to formic acid and methanol. 3. The method of claim 2, Wherein the methanol is pro ducedbygeneratingcarbonmonoxidefromthecarbondiox idethroughahightemperaturereactionWithcarbon,reacting thecarbonmonoxideWiththepreviouslyproducedmethanol underconditionssuf?cienttoformmethylformate,folloWed bycatalyticallyhydrogenatingthemethylformateundercon ditions suf?cient to form additional methanol. 4. The method of claim 1, Wherein the methanol is pro duced by reducing the carbon dioxide under conditions suf ?cient to produce a reaction mixture containing formic acid With concomittant formation of formaldehyde and small amounts of methanol and methane, augmenting the reaction mixturebyreacting,Withoutseparationofthereactionmix ture, the formaldehyde into methanol With some ofthe formic acid used as a hydrogen source, and reacting some of the formic acid With methanol to form methyl formate, folloWed by catalyticallyhydrogenatingthemethylformateundercon ditionssuf?cienttoformmethanol. 5.The method ofclaim 1,Which furthercomprises trans portingthethusproducedmethanolfueltoafacilityWherethe fuelistobecombustedtogenerateenergy. 6. The method of claim 5, Which further comprises com bustingthemethanolfuelinapoWerplanttoformanexhaust stream that contains carbon dioxide, and recovering the car bon dioxide of the exhaust stream for use as the chemically recyclable source of carbon dioxide for preparing additional fuel. 7.Themethodofclaim1Whereinthemethanolisproduced by hydrogenatively converting the carbon dioxide to form a reaction mixture that contains methanol, formic acid and formaldehyde, folloWed, Without separation of the reaction mixture, by a treatment step conducted under conditions suf ?cienttoconverttheformaldehydeandformicacidtometha nol. 8. The method of claim 7, Which comprises reacting the formaldehyde With the co-formed formic acid as a hydrogen source, Without separation of the reaction mixture, into methanol,includingreactingoftheformicacidWithmetha nol to form methyl formate, folloWed by hydrogenating the methylformateunderconditionssu?icienttoformdoublethe starting amount of methanol. 9.Themethodofclaim8,Whereinthehydrogenneededfor thehydrogenationofmethylformateisobtainedatleastin part from cleavage of the formic acid from the reaction mix ture. 10. The method of claim 1, Wherein the hydrogen needed for the hydrogenative conversion of carbon dioxide is obtainedbythereformingofmethaneornaturalgasorby electrolysisofWaterusinganavailableenergysource. 11. The method of claim 1, Which further comprises com busting the fuel to form an exhaust stream that contains car bon dioxide and in a manner that alloWs collection of the exhauststream,andrecoveringthecarbondioxideofthe exhaust stream for use as the chemically recyclable source of carbon dioxide for preparing additional fuel. MethaneisreformedWithcarbondioxideand(dryreform ing) steam (Wet reforming) inproportions to give a 1:2 mix tureofcarbonmonoxideandhydrogenunderconditionsof30 ourco-pending“bi-reforming”Patentapplications.Thismix ture is subsequently used to produce methanol according to the equation CO+2H2—>CH3OH. The carbon monoxide formed can also reacted as in examples 1-3 With methanol to givemethylformate,WhichaccordingtoExamples4and535 can be hydrogenatively converted doubling the amount of methanol under moderate temperatures and pressures. These examples illustrate the general utility of the present process of carbon dioxide to methanol conversion but skilled practitionerscanutiliZethedisclosureandteachingsprovided 40 herein to generate a suitable variation thereof. The process alloWsproductionofderivedfuels,productsthereofandother applicationsreducingorreplacingrelianceonfossilfuels.At the same time italso safeguards the environment by signi? cantlyreducingcarbondioxideemissionsandthepresenceof45 harmful lighter carbon dioxide content in the atmosphere. The present invention provides a convenient Way to recycle carbon dioxide to either prevent its emission into the atmo sphereortoremovepartofitfromtheatmospheretogenerate areneWablefuelsuchasmethanolordimethylether. Example7 CO2 is electrochemically reduced in aqueous solutions overgoldandrelatedcatalystsatthecathodetoCO andalso 55 H2 (by concomitant electrolysis). The CO and H2 mixture (syngas)iscatalyticallyconvertedtomethanol(seeco-pend ingbireformingaplication). Whatisclaimedis: 1.An environmentallybene?cialmethodofpreparinga reneWable fuel, Which method comprises: obtaining carbon dioxide from a natural or chemical source thatWouldotherWisebepresentinordischargedintothe atmosphere;and producing an energy storage and transportation material or a fuel suf?cient to generate energy by hydrogenatively 60 65 US 8,212,088B2 50PDF Image | CHEMICAL RECYCLING OF CO2 TO METHANOEDIMETHYL ETHER
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