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ahigherH/C ratio,suchaspropane,butaneornaphthas,leads to S values in the vicinity of 2, ideal for the conversion to methanol.When coalisused,hoWever,additionaltreatmentis 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 a temperature of about 800° C. to about l,000° C., and a pressure of about 20 atm to 30 atm) to formCO andH2.A partoftheCO formedreactsconsequently With steam in the Water gas shift reaction (WGS) to yield more H2 and also C02. The gas obtained isthus a mixture of H2,CO andCO2 invariousconcentrationsdependingonthe reaction conditions, such as temperature, pressure and H2O/ CH4 ratioaccordingtothefolloWingreactions: 20 Since the overall methane steam reforming process is highlyendothermic,heatmustbesuppliedtothesystemby 25 burning a part of the natural gas used as the feedstock. The stoichiometric number S obtained by steam reforming of methaneiscloseto3,muchhigherthanthedesiredvalueof2. This can generally be corrected by addition of CO2 to the steamreformer’sexitgasoruseofexcesshydrogeninsome 30 other process such as ammonia synthesis. HoWever, natural gas isstilthepreferredfeedstockformethanol production becauseitoffershighhydrogencontentand,additionally,the loWestenergyconsumption,capitalinvestmentandoperating 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.Becauseonlypartof 40 the syn-gas is converted to methanol after passing over the catalyst,theremainingsyn-gasisrecycledafterseparationof methanol and Water. There is also a more recently developed liquidphaseprocessformethanolproduction,duringWhich thesyn-gasisbubbledintothereactionmixture.Althoughthe45 existing processes have methanol selectivity greater than 99% and energy ef?ciency above 70%, crude methanol leav ingthereactorstilcontainsWaterandotherimpurities,such as dissolved gases (e.g., methane, CO, and CO2), dimethyl ether,methylformate,acetone,higheralcohols(ethanol,pro 50 panol, butanol), and long-chain hydrocarbons. Commer cially, methanol is available in three grades of purity: fuel grade, “A” grade, generally used as a solvent, and “AA” or chemicalgrade.ChemicalgradehasthehighestpurityWitha methanolcontentexceeding99.85%andisthestandardgen 55 erallyobservedintheindustryformethanolproduction.The syn-gas generation and puri?cation steps are critical to the existing processes, and the end result Would largely depend on the nature and purity of the feedstock. To achieve the desiredlevelofpurity,methanolproducedbytheexisting60 processesisusuallypuri?edbysuf?cientdistillation.Another major disadvantage of the existing process for producing methanol through syn-gas is the energy requirement of the ?rsthighlyendothermicsteamreformingstep.Theprocessis alsoinef?cientbecauseitinvolvestransformationofmethane 65 inanoxidativereactiontoCO (andsomeCO2),Whichinturn must be reduced to methanol. 10 AnotherWaytoproducesyn-gasfrommethaneisthrough thepartialoxidationreactionWithinsuf?cientoxygen,Which can be performed With or Without a catalyst. This reaction is exothermic and is conducted at high temperature of about 1,2000C.toabout1,5000C.TheproblemWithpartialoxida tionisthattheproducts,CO andH2arereadilyfurtheroxi diZedtoformundesiredCO2 andWaterinhighlyexothermic reactions leading to S values typically Well beloW 2 and contributing to CO2 induced global Warming. The folloWing reactions are illustrative of the process. 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(Scloseto2).Inthisprocess,calledautothermal reforming,heat-producedbytheexothermicpartialoxidation is consumed by the endothermic steam reforming reaction. Partialoxidationandsteamreformingcanbeconductedsepa ratelyorsimultaneouslyinthesamereactorbyreactingmeth ane With a mixture of steam and oxygen. The process as mentionedhoWever,produceslargeamountsofCO2 necessi tatingitscostlysequesteringorventingintotheatmosphere. Any carboncontainingfuelorderivedsynthetichydrocarbon product When oxidatively used results in the formation of carbondioxideandthusisnotreneWableonthehumantime scale.Thereisanessentialneedtomake carbonfuelsreneW ableandthusalsoenvironmentallyneutraltominimiZetheir harmful effect on global Warming. The selective conversion and recycling of carbon dioxide tomethanolWithoutgeneratingunWantedby-productsisthus amajorchallengeandamuch desiredpracticalgoal.Thereis agreatneedtoeffectivelyandeconomicallyproducemetha nolfromcarbondioxideWithhighselectivityandyieldof conversion. SUMMARY OF THE INVENTION The inventionnoW provides novel methods forconverting methane and carbon dioxide to methanol Without any release ofcarbondioxidetotheatmosphereorWithoutby-product formation or the use of hydrogen to form Water. In one embodiment, the invention provides for a method of formingmethanol,bycombiningmethane,Waterandcarbon dioxide, preferably in a mixture, in single or multiple steps underreactionconditionssuf?cienttoformamolarmixture ofhydrogenandcarbonmonoxideinaspeci?cratioofatleast tWo moles of hydrogen to one mole of carbon monoxide, and reactingthemixtureofhydrogenandcarbonmonoxideunder conditionssuf?cienttoexclusivelyformmethanol.Themolar ratioofhydrogentocarbonmonoxideispreferablybetWeen 2:1 and 2.1:1. The molar ratio betWeen the methane, Water and carbon dioxide is about 3:2:1. In another embodiment, the invention provides for a methodofformingmethanolbyreactingmethaneandWater understeamreformingreactionconditionssuf?cienttoform hydrogen and carbon monoxide, reacting methane and car bon dioxide under dry reforming reaction conditions su?i cient to form hydrogen and carbon monoxide, forming a mixture ofthe combined hydrogen and carbon monoxide in a molarratioofatleast2molesofhydrogentoonemoleof carbon monoxide, and reacting the carbon monoxide and hydrogen under reaction conditions suf?cient to exclusively US 8,440,729B2PDF Image | CONVERSION OF CARBON DIOXIDE TO METHANOL BIOREFORMING
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