以共沉淀法所制的工业铁硅球体催化剂(indus-FS)为原料,用改进的有机胺蒸气相传输转化法,得到了负载高分散铁的交织氧化硅纳米线球体催化剂(NW-FS),并用于费托合成反应.在所制纳米线催化剂中,原料催化剂中氧化硅在氧化铁诱导下成功地转变成纳米线交织微球载体,而氧化铁组分则高度分散在氧化硅纳米线上.用扫描电镜、透射电镜、X射线衍射、低温氮吸附、X射线光电子能谱和程序升温还原等方法对所得纳米线催化剂进行了表征.在费托合成中,纳米线铁硅催化剂由于其特殊的堆积结构所导致的低的扩散阻力和高的铁活性组分分散度,提高了低碳烯烃尤其是乙烯的选择性.纳米线铁硅催化剂上低碳产物(C2-C4)的烯烷比为3.3,高于母体工业催化剂的1.9.
A catalyst consisting of SiO2 nanowires and highly dispersed Fe2O3 (denoted NW-FS) was synthe-sized in situ by iron-assisted amine-vapor-transport treatment. NW-FS was prepared by the direct transformation of an industrial spherical Fe2O3/SiO2 catalyst (denoted indus-FS). NW-FS was char-acterized by scanning electron microscopy, X-ray diffraction, transmission electron microscopy, N2-sorption measurements, X-ray photoelectron spectroscopy, and temperature-programmed re-duction. NW-FS exhibited a high selectivity for light olefins, especially for ethene in the Fischer-Tropsch synthesis. This was because of the highly dispersed Fe2O3 and low diffusion resistance of its open structure. The C2-C4 olefin/paraffin ratio was 3.3, which was higher than that of indus-FS at 1.9.
参考文献
| [1] | Astruc D;Lu F;Aranzaes J R .[J].ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2005,44:7852. |
| [2] | Mitsudome T;Mikami Y;Funai H;Mizugaki T Jitsukawa K Kaneda K .[J].ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2008,47:138. |
| [3] | Torres Galvis H M;Bitter J H;Khare C B;Ruitenbeek M Dugulan A I de Jong K P .[J].SCIENCE,2012,335:835. |
| [4] | Sun Z K;Sun B;Qiao M H;Wei J Yue Q Wang C Deng Y H Kaliaguine S Zhao D Y .[J].Journal of the American Chemical Society,2012,134:17653. |
| [5] | Goel, S.;Wu, Z.;Zones, S.I.;Iglesia, E. .Synthesis and catalytic properties of metal clusters encapsulated within small-pore (SOD, GIS, ANA) zeolites[J].Journal of the American Chemical Society,2012(42):17688-17695. |
| [6] | Bezemer G L;Bitter J H;Kuipers H P C E;Oosterbeek H Holewijn J E Xu X D Kapteijn F van Dillen A J de Jong K P .[J].Journal of the American Chemical Society,2006,128:3956. |
| [7] | den Breejen J P;Radstake P B;Bezemer G L;Bitter J H Fr?seth V Holmen A de Jong K P .[J].Journal of the American Chemical Society,2009,131:7197. |
| [8] | Rane S;Borg;Rytter E;Holmen A .[J].Applied Catalysis A:General,2012,437-438:10. |
| [9] | Prieto, G.;Martínez, A.;Concepción, P.;Moreno-Tost, R. .Cobalt particle size effects in Fischer-Tropsch synthesis: structural and in situ spectroscopic characterisation on reverse micelle-synthesised Co/ITQ-2 model catalysts[J].Journal of Catalysis,2009(1):129-144. |
| [10] | Park J Y;Lee Y J;Khanna P K;Jun K W Bae J W Kim Y H .[J].Journal of Molecular Catalysis A:Chemical,2010,323:84. |
| [11] | Kang J C;Cheng K;Zhang L;Zhang Q H Ding J S Hua W Q Lou Y C Zhai Q G Wang Y .[J].ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2011,50:5200. |
| [12] | Mei CS;Wen PY;Liu ZC;Liu HX;Wang YD;Yang WM;Xie ZK;Hua WM;Gao Z .Selective production of propylene from methanol: Mesoporosity development in high silica HZSM-5[J].Journal of Catalysis,2008(1):243-249. |
| [13] | Zhang CX;Chen P;Liu J;Zhang YH;Shen W;Xu HL;Tang Y .Ag microparticles embedded in Si nanowire arrays: a novel catalyst for gas-phase oxidation of high alcohol to aldehyde[J].Chemical communications,2008(28):3290-3292. |
| [14] | Chen D;Moljord K;Fuglerud T;Holmen A .[J].Microporous and Mesoporous Materials,1999,29:191. |
| [15] | Chen J Q;Bozzano A;Glover B;Fuglerud T Kvisle S .[J].Catalysis Today,2005,106:103. |
| [16] | Wang P F;Lv A L;Hu J;Xu J A Lu G Z .[J].Industrial and Engineering Chemistry Research,2011,50:9989. |
| [17] | Dupain X;Krul RA;Schaverien CJ;Makkee M;Moulijn JA .Production of clean transportation fuels and lower olefins from Fischer-Tropsch Synthesis waxes under fluid catalytic cracking conditions - The potential of highly paraffinic feedstocks for FCC[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2006(3/4):277-295. |
| [18] | Rao T V M;Dupain X;Makkee M .[J].Microporous and Mesoporous Materials,2012,164:148. |
| [19] | Janardanarao M .[J].Industrial and Engineering Chemistry Research,1990,29:1735. |
| [20] | Dictor R A;Bell A T .[J].Journal of Catalysis,1986,97:121. |
| [21] | 高芳芳,王洪,青明,杨勇,李永旺.铁基费托合成催化剂相变调控及反应性能[J].催化学报,2013(07):1312-1325. |
| [22] | Kuipers EW.;Oosterbeek H.;Vinkenburg IH. .CHAIN LENGTH DEPENDENCE OF ALPHA-OLEFIN READSORPTION IN FISCHER-TROPSCH SYNTHESIS[J].Journal of Catalysis,1995(1):137-146. |
| [23] | Shi B C;Davis B H .[J].Topics in Catalysis,2003,26:157. |
| [24] | Turner ML.;Marsih N.;Mann BE.;Quyoum R.;Long HC.;Maitlis PM. .Investigations by C-13 NMR spectroscopy of ethene-initiated catalytic CO hydrogenation [Review][J].Journal of the American Chemical Society,2002(35):10456-10472. |
| [25] | Kuipers EW.;Wilson JH.;Vinkenburg IH.;Oosterbeek H.;Scheper C. .NON-ASF PRODUCT DISTRIBUTIONS DUE TO SECONDARY REACTIONS DURING FISCHER-TROPSCH SYNTHESIS[J].Journal of Catalysis,1996(1):288-300. |
| [26] | Satterfield C N;Huff G A Jr;Summerhayes R .[J].Journal of Catalysis,1983,80:486. |
| [27] | Chen P;Xie S H;Ren N;Zhang Y H Dong A G Chen Y Tang Y .[J].Journal of the American Chemical Society,2006,128:1470. |
| [28] | Gurgul J;?atka K;Hnat I;Rynkowski J Dzwigaj S .[J].Microporous and Mesoporous Materials,2013,168:1. |
| [29] | Sirotin S V;Moskovskaya I F;Romanovsky B V .[J].Catal Sci Technol,2011,1:971. |
| [30] | Zielinski J;Zglinicka I;Znak L;Kaszkur Z .[J].Applied Catalysis A:General,2010,381:191. |
| [31] | Iglesia E;Reyes S C;Madon R J;Soled S L .[J].ADVANCES IN CATALYSIS,1993,39:221. |
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