Perhydroindan (bicyclo[4.3.0]nonane) was converted in a flow-type apparatus under a hydrogen pressure of 5 MPa on six different catalysts,namely on a bifunctional Pd/Na,H-Beta zeolite,on Ir/Na,H-Y and Pt/Na,H-Y zeolites with a low concentration of Brφnsted acid sites,and on three catalysts containing the three noble metals on the non-acidic support silica.On the bifunctional zeolite Pd/Na,H-Beta,skeletal isomerization of perhydroindan was the primary reaction followed by opening of one naphthenic ring,the formation of open-chain nonanes in low yields of ca.6％,and hydrocracked products C8-.The carbon number distribution of the latter was volcano-shaped with no C1,C2,C7,and C8 indicating a carbocationic hydrocracking of C9 precursors with one naphthenic ring.On Ir/Na,H-Y and Pt/Na,H-Y(“high-performance ring-opening catalysts”),ring opening and hydrocracking to C8- occurred by hydrogenolysis on the respective metal.Opening of the five-membered ring was found to be much faster than opening of the six-membered ring,in agreement with literature reports.The maximal selectivities of open-chain nonanes (OCNs) attained on Ir/Na,H-Y and Pt/Na,H-Y were very high,viz.49％ and 54％,respectively,and significantly better than those of the open-chain decanes observed previously with decalin as model hydrocarbon.The OCNs formed on Pt/Na,H-Y were much less branched than those formed on Ir/Na,H-Y which was interpreted in terms of the different hydrogenolysis mechanisms on both metals.Valuable ancillary mechanistic information was obtained from the selectivities of perhydroindan hydroconversion on the three noble metals on silica.In contrast to Pd/silica,Ir/silica and Pt/silica gave appreciable selectivities of OCNs as well,yet the maximum values of these selectivities were lower than those obtained on the two high-performance zeolite catalysts.
参考文献
| [1] | Santana R C;Do P T;Santikunapom M;Alvarez W E Taylor J D Sughrue E L Resasco D E .[J].Fuel,2006,85:643. |
| [2] | Weitkamp J;Ertl G;Knrzinger H;Schüth F,Weitkamp J.Handbook of Heterogeneous Catalysis[M].Weinheim:Wiley-VCH,2008:3133. |
| [3] | Kubicka D.;Kumar N.;Maki-Arvela P.;Tiitta M.;Niemi V.;Salmi T. Murzin DY. .Ring opening of decalin over zeolites I. Activity and selectivity of proton-form zeolites[J].Journal of Catalysis,2004(1):65-79. |
| [4] | Santikunaporn M;Herrera JE;Jongpatiwut S;Resasco DE;Alvarez WE;Sughrue EL .Ring opening of decalin and tetralin on HY and Pt/HY zeolite catalysts[J].Journal of Catalysis,2004(1):100-113. |
| [5] | Arribas M A;Martínez A;Sastre G .[J].Studies in Surface Science and Catalysis,2002,142:1015. |
| [6] | Arribas M A;Concepcirn P;Martínez A .[J].Applied Catalysis A:General,2004,267:111. |
| [7] | Arribas M A;Corma A;Díaz-Caba(n)as M J;Martínez A .[J].Applied Catalysis A:General,2004,273:277. |
| [8] | Kubicka D;Kumar N;Maki-Arvela P;Tiitta M;Niemi V;Karhu H;Sami T;Murzin DY .Ring opening of decalin over zeolites - II. Activity and selectivity of platinum-modified zeolites[J].Journal of Catalysis,2004(2):313-327. |
| [9] | Kumar N;Lazuen A;Kubi(c)ka D;Heikkil(a) T Lehto V-P Karhu H Salmi T Murzin D Y .[J].Studies in Surface Science and Catalysis,2006,162:401. |
| [10] | Ma H;Yang X;Wen G;Tian G Wang L Xu Y Wang B Tian Z Lin L .[J].Catalysis Letters,2007,116:149. |
| [11] | Mouli K C;Sundaramurthy V;Dalai A K;Ring Z .[J].Applied Catalysis A:General,2001,321:17. |
| [12] | Murzin D Y;Kubi(c)ka D;Simakova Ⅱ L;Kumar N Lazuen A M(a)ki-Arvela P Tiitta M Salmi T .[J].Pet Chem (Neftekhimiya),2009,49:90. |
| [13] | Kumar N;Kubi(c)ka D;Garay A L;M(a)ki-Arvela P Heikkil(a) T Salmi T Murzin D Y .[J].Topics in Catalysis,2009,52:380. |
| [14] | Vuori H;Silvennoinen R J;Lindblad M;(O)sterholm H Krause AO I .[J].Catalysis Letters,2009,131:7. |
| [15] | Mouli K C;Sundaramurthy V;Dalai A K .[J].Journal of Molecular Catalysis A:Chemical,2009,304:77. |
| [16] | McVicker G B;Daage M;Touvelle M S;Hudson C W Klein D P Baird Jr W R Cook B R Chen J G Hantzer S Vaughan D E W Ellis E S Feeley O C .[J].Journal of Catalysis,2002,210:137. |
| [17] | Rabl S;Haas A;Santi D;Flego C Ferrari M Calemma V Weitkamp J .[J].Applied Catalysis A:General,2011,400:131. |
| [18] | Weitkamp J;Rabl S;Haas A;Santi D,Ferrari M,Calemma V.[A].Hamburg:DGMK,2010:77. |
| [19] | Weitkamp J;Rabl S;Haas A;Santi D Ferrari M Calemma V .[J].Oil Gas Eur Mag,2011,37:94. |
| [20] | Rabl S;Santi D;Haas A;Ferrari M Calemma V Bellussi G Weitkamp J .[J].Microporous and Mesoporous Materials,2011,146:190. |
| [21] | Ipatieff V N;Pines H;Meisinger E E .[J].Journal of the American Chemical Society,1949,71:2685. |
| [22] | Pentschev V;Davidova N .[J].Brennstoff-Chemie,1968,49:33. |
| [23] | Daage M;McVicker G B;Touvelle M S;Hudson C W Klein D P Cook B R Chen J G Hantzer S Vaughan D E W Ellis E S .[J].Studies in Surface Science and Catalysis,2001,135:159. |
| [24] | Davidova N;Pen(c)ev V;Beránek L .[J].Collection of Czechoslovak Chemical Communications,1968,33:1229. |
| [25] | Nylén U;Delgado J F;J(a)r(a)s S;Boutonnet M .[J].Applied Catalysis A:General,2004,262:189. |
| [26] | Rao P R H P;Leon y Leon C A;Ueyama K;Matsukata M .[J].Microporous and Mesoporous Materials,1998,21:305. |
| [27] | Miyamoto Y;Katada N;Niwa M .[J].Microporous and Mesoporous Materials,2000,40:271. |
| [28] | Miller J T;Schreier M;Kropf A J;Regalbuto J R .[J].Journal of Catalysis,2004,225:203. |
| [29] | Anderson J A;Fémandez-García M;Martínez-Arias A.Supported Metals in Catalysis[A].London:Imperial College Press,2005:139. |
| [30] | McVicker G B;Baker R T;Garten R L;Kugler E L .[J].Journal of Catalysis,1980,65:207. |
| [31] | Marins de Oliveira A;Costilla I;Gigola C;Baibich I M Teixeira da Silva V T Castella Pergher S B .[J].Catalysis Letters,2010,136:185. |
| [32] | Frye C F;Weitkamp A W .[J].Journal of Chemical and Engineering Data,1969,14:372. |
| [33] | Allinger N L;Coke J L .[J].Journal of the American Chemical Society,1960,82:2553. |
| [34] | Weitkamp A W .[J].Advances in Catalysis,1968,18:1. |
| [35] | Lai W C;Song C .[J].Catalysis Today,1996,31:171. |
| [36] | Foger K;Anderson J R .[J].Journal of Catalysis,1979,59:325. |
| [37] | Carter J L;Cusumano J A;Sinfelt J H .[J].Journal of Catalysis,1971,20:223. |
| [38] | Maire G;Plouidy G;Prudhomme J C;Gault F G .[J].Journal of Catalysis,1965,4:556. |
| [39] | Anderson J R;Avery N R .[J].Journal of Catalysis,1966,5:446. |
| [40] | Weitkamp J;Farag H.[A].Szeged,Hungary,1978:327. |
| [41] | Turova-Polyak M B;Sosnina I S;Belikova N A;Plate A F .[J].Zh OrgKhim,1966,2:2162. |
| [42] | Kozina M P;Mirzaeva A K;Sosnina I E;Elagina N V Skuratov S M .[J].Doklady Akademii Nauk SSSR,1964,155:1123. |
| [43] | Egan C J;Langlois G E;White R J .[J].Journal of the American Chemical Society,1962,84:1204. |
| [44] | Emst S;Weitkamp J.[A].Siófok,Hungary,1985:457. |
| [45] | Weitkamp J .[J].ACS Symposium Series,1975,20:1. |
| [46] | Martens J A;Jacobs P A;Weitkamp J .[J].Applied Catalysis,1986,20:239. |
| [47] | Nylén U;Arechederra J M;Pawelec B;Delgado J F Pascual M P Fierro J L G .[J].Energy and Fuels,2008,22:2138. |
| [48] | Engler E M;Andose J D;von R Schleyer P .[J].Journal of the American Chemical Society,1973,95:8005. |
| [49] | Gault F G .[J].Advances in Catalysis,1981,30:1. |
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