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(12)United States Patent Olah eta1. (54) CONVERSIONOFCARBONDIOXIDETO METHANOL USING BLREFORMING 01: METHANE 0R NATURAL GAS _ (75) Inventors: GeorgeA.Olah,BeverlyH1lls,CA (US); G. K. Surya Prakash, Hacienda Heights CA (Us) ’ (73) Assignee: UniversityofSouthernCalifornia,Los (10)PatentNo.: US 8,440,729B2 (45)Date ofPatent: *May 14,2013 (*) Notice: Angeles,CA (US) Subjecttoanydisclaimer,thetermofthis patentisextendedoradjustedunder35 U_S_C_ 154(1)) by 2 day, This patent is subject to a terminal dis- Clalmer' EP GB (21) Appl NO .13/354042 '"’ (22) Filed: Jam 19,2012 (65) Prior Publication Data US 2012/0115965A1 May 10,2012 Related US. Application Data (63) Continuation of application No. 12/941,773, ?led on NW 8’2010,Whlch1SacomlnuanonofaPPllcatlon No. 11/850,501, ?led on Sep. 5, 2007, noW Pat. No. 7, 906,559- (60) Provisional application No. 60/945,501, ?led on Jun. 21,2007. (51)I11t-C1- C07C 29/151 C07C 29/157 B01] 23/847 (52) US.C]. (200691) (200601) (200691) USPC ..518/704 (58) FieldofClassi?cationSearch ..None (56) See application ?le for complete search history. References Cited US. PATENT DOCUMENTS 3,993,457 A 11/1976 Cahn et al. ................. 48/197 R 4,093,029 A 6/1978 WeisZ etal. .............. 166/305 R US008440729B2 4,395,495 A 4,640,766 A 5,599,638 A 5,767,165 A 7,132,183 B2 7,605,293 B2 7,608,743 B2 7,705,059 B2 7,795,175 B2 2004/0034255 A1 FOREIGN PATENT DOCUMENTS W0 WO2006/113294A1 10/2006 W0 WO 2007/014487 A1 2/2007 OTHER PUBLICATIONS 7/1983 Cummings .. 518/704 2/1987 Postetal. .. 2/1997 Surampudi eta1. 6/1998 Steinbergetal. . 11/2006 Galloway ....... 10/2009 Olaheta1, , 10/2009 Olahetal. 0 159 759 A2 10/1985 1545329 A 5/1979 208/111 429/33 518/703 ..... 429/17 563/335 568/885 518/700 InternationalSearchReportandWrittenOpinionoftheInternational Searching Authority, Application No. PCT/US2008/067480, Oct. 1, 2008. InternationalSearchReport,ApplicationNo.PCT/US2008/067462, Oct. 1,2008. Non-Final Of?ce Action, U.S. Appl. No. 12/941,773, dated Feb. 18, 2011. Advisory Action Of?ce Action, U.S. Appl. No. 12/941,773, dated Nov. 4, 2011. FinalOf?ceAction,U.S.Appl.No. 12/941,773,datedJul.26,2011. 231613131Of?ceAcnon’U'S'Appl'NO'11/850’501’datedMan 19’ Final Of?ceAction, U.S.Appl.No. 11/850,501, datedAug. 27, 2010. PrimaryExaminer* RosalyndKeys (74)A110""6%Agent)0"Firm* Winston& SlraWnLLP (57) ABSTRACT The'1nvent1'onprov1'edsforameth0dfoform1'ngmethanolby combining a mixture of methane, Water and carbon dioxide underspeci?creactionconditionssu?icienttoformamixture of hydrogen and carbon monoxide Which are then reacted underconditionssu?icienttoformmethanol.Themolarratio of hydrogen to carbon monoxide is at least tWo moles of hydrogen to one mole of carbon monoxide and the overall molar ratio betWeen methane, Water and carbon dioxide is about 3:211. Methane, carbon dioxide and Water are bi-re formed over a catalyst. The catalyst includes a single metal, a metal oxide, a mixed catalyst of a metal and a metal oxide or a mixed catalyst of at least tWo metal oxides. 20Claims,1DrawingSheet 4/2010 Olahetal. 9/2010 Olahetal. . 2/2004 Shopeta1‘""""""""""568/698 502/401PDF Image | CONVERSION OF CARBON DIOXIDE TO METHANOL BIOREFORMING
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