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Ideally,Sshouldbeequaltoorslightlyabove2.Avalueabove 2 indicates excess hydrogen, While a value beloW 2 indicates relativehydrogende?ciency.Reformingoffeedstockshaving ahigherH/C ratio,suchaspropane,butaneornaphthas,leads toSvaluesinthevicinityof2,idealforconversiontometha nol. When coal is used, hoWever, additional treatment is requiredtoobtainanoptimalSvalue.Synthesisgasfromcoal requires treatment to avoid formation of undesired byprod ucts. The most Widely used technology to produce syn-gas for methanol synthesis is steam reforming. In this process, natu ralgas(ofWhichmethaneisthemajorcomponent)isreacted in a highly endothermic reaction With steam over a catalyst, typically based on nickel, at high temperatures (800-l,000o C.,20-30atm)toformCO andH2.A partoftheCO formed react consequently With steam in the Water gas shift reaction (WGS) toyieldmore H2 andalsoC02. The gasobtainedis thusamixtureofH2,CO andCO2invariousconcentrations depending on the reaction conditions: temperature, pressure and HZO/CH4 ratio 20 10 AnotherWay toproducesyn-gasfrommethaneisthrough the partial oxidation reaction With insuf?cient oxygen, Which can be performed With or Without a catalyst. This reaction is exothermicandoperatedathightemperature(1,200tol,5000 C.).TheproblemWithpartialoxidationisthattheproducts, CO andH2arereadilyfurtheroxidiZedtoformundesiredCO2 andWaterinhighlyexothermicreactionsleadingtoSvalues typicallyWellbeloW2andcontributingtoCO2inducedglobal Warming. co+1/2o2 co2AH298K:—67.6kcal/mol Toproducesyn-gasWithouteitherconsumingorproducing muchheat,modernplantsareusuallycombiningexothermic partial oxidation With endothermic steam reforming in order to have an overall thermodynamically neutral reaction While obtaining a syn-gas With a composition suited for methanol synthesis (S close to 2). In this process, called autothermal reforming,heatproducedbytheexothermicpartialoxidation is consumed by the endothermic steam reforming reaction. Partialoxidationandsteamreformingcanbeconductedsepa ratelyorsimultaneouslyinthesamereactorbyreactingmeth ane With a mixture of steam and oxygen. The process as mentionedhoWever,produceslargeamounts ofCO2 necessi tatingitscostlysequesteringorventingintotheatmosphere. Anycarboncontainingfuelorderivedsynthetichydrocarbon productWhenoxidativelyusedinevitablyformscarbondiox ide and thus isnot reneWable on the human time scale. There isanessentialneedtomake carbonfuelsreneWableandthus contains Water and other impurities, such as dissolved gases (e.g.,methane,CO,andCO2),dimethylether,methylfor US 7,906,559B2 Since the overall methane steam reforming process is highlyendothermic,heatmustbesuppliedtothesystemby 25 burning a part ofthe natural gas used as the feedstock. The stoichiometric number S obtained by steam reforming of methane iscloseto3,much higherthanthedesiredvalueof2. This can generally be corrected by addition of CO2 to the steamreformer’sexitgasoruseofexcesshydrogeninsome 30 otherprocesssuchasammonia synthesis.HoWever,natural gas isstilthepreferredfeedstockformethanol production becauseitoffershighhydrogencontentand,additionally,the loWestenergyconsumption,capitalinvestmentandoperating alsoenvironmentallyneutraltominimiZetheirharmfuleffect costs.NaturalgasalsocontainsfeWerimpuritiessuchas35 sulfur, halogenated compounds, and metals Which may poi son the catalysts used in the process. Theexistingprocessesinvariablyemployextremelyactive and selective copper-based catalysts, differing only in the reactordesignandcatalystarrangement.Becauseonlypartof40 syn-gasisconvertedtomethanolafterpassingoverthecata lyst, the remaining syn-gas is recycled after separation of methanolandWater.Thereisalsoamorerecentlydeveloped liquidphaseprocessformethanolproduction,duringWhich syn-gasisbubbledintoliquid.Althoughtheexistingpro 45 cesseshavemethanolselectivitygreaterthan99% andenergy ef?ciencyabove70%,crudemethanolleavingthereactorstil (naturalorindustriallyproduced)byanovelspeci?ccombi mate,acetone,higheralcohols(ethanol,propanol,butanol),50 andlong-chainhydrocarbons.Commercially,methanolis ingprocess.Itcomprisesreactingmethaneunderaspeci?c available in three grades of purity: fuel grade, “A” grade, generally used as a solvent, and “AA” or chemical grade. Chemical grade has the highest purity With a methanol con tentexceeding99.85%andisthestandardgenerallyobserved 55 intheindustryformethanolproduction.Thesyn-gasgenera tion and puri?cation steps are critical in the existing pro cesses,andtheendresultWouldlargelydependonthenature and purity of the feedstock. To achieve the desired level of purity,methanolproducedbytheexistingprocessesisusually60 puri?edbysu?icientdistilation.Anothermajordisadvantage oftheexistingprocessforproducingmethanolthroughsyn gasistheenergyrequirementofthe?rsthighlyendothermic steam reforming step. The process is also inef?cient because itinvolvestransformationofmethaneinanoxidativereaction 65 to carbon monoxide (and some CO2), Which in turn must be reduced to methanol. combination of conditions With steam (Wet) and CO2 in a speci?c sequence and mole ratio of reactants su?icient to produce a syn-gas mixture of carbon monoxide/hydrogen (CO/H2)inaratioof1:2andsubsequentfurtherconversionof this mixture to methanol and/or dimethyl ether (DME). Advantageously, the bi-reforming mixture can be treated to convertitsubstantiallytomethylalcoholorDME Without by-products. Alternatively, unreacted feed components can bereadilyrecoveredandrecycled. The needed methane source, depending on itsavailability, can be natural gas, coal-bed methane, any other natural sources of methane, methane hydrates, as Well methane formed by the hydrolysis of aluminium carbide or any other convenient source. The methane source may also contain, besides methane, varying amounts of higher hydrocarbons (ethane, propane, butane, etc.) and/or impurities. ItisWithin onglobalWarming. The selective conversion and recycling of carbon dioxide to methanol Without generating unWanted by-products isthus amajorchallengeandamuch desiredpracticalgoal.Thereis a great need to effectively and economically produce metha nolfromcarbondioxideWithhighselectivityandyieldof conversion.SuchisnoW disclosedinthepresentinvention. SUMMARY OF THE INVENTION nation of steam and dry reforming of methane or natural gas togivetheneededH2toCO moleratioof2incorporating externalcarbondioxide.ThismethodWecallthebi-reform Ourinventionrelatestoamethodofpreparingmethanol and/or dimethyl ether from any source of carbon dioxidePDF Image | CONVERSION OF CARBON DIOXIDE TO METHANOL
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