以介孔氧化硅泡沫MCF为载体合成了一系列负载型氧化钒催化剂(V含量为2%～10%).采用N2吸附、X射线衍射和H2程序升温还原对V/MCF催化剂的结构和织构性质进行了表征,并评价了催化剂在CO2气氛下的乙苯脱氢性能.V/MCF催化剂具有较高的乙苯脱氢活性,其中V含量为6%的催化剂具有最高的反应活性.V/MCF催化剂的乙苯脱氢活性显著高于V/MCM-41,这是由于前者具有较高的可还原性以及较好的扩散性能.CO2气氛下的乙苯转化率明显高于N2气氛下的,这归因于CO2与乙苯发生氧化脱氢,并通过逆水煤气变换反应在线除去脱氢反应生成的氢.
A series of vanadia catalysts supported on mesocellular silica foam (MCF) with a V content ranging from 2% to 10% were studied with respect to their performance in the dehydrogenation of ethylbenzene (EB) to styrene in the presence of CO2. The structural and textural characterization of these catalysts was done using N2 adsorption, X-ray diffraction, and temperature-programmed reduction. These catalysts were found to be effective for the dehydrogenation reaction and the 6% V/MCF catalyst showed the highest activity. The MCF-supported vanadia catalysts exhibited far higher activity than their conventional V/MCM-41 counterparts, which can be attributed to the higher reducibility and better diffusion of reactants and products in the former catalysts. A higher conversion was obtained during EB dehydrogenation with CO2 than with N2. This is due to the oxidative dehydrogenation of EB with the help of oxygen that originates from CO2 as well as the coupling of EB simple dehydrogenation with the reverse water-gas shift reaction.
参考文献
| [1] | Mross W D .[J].CatalRev-SciEng,1983,25:591. |
| [2] | Ohishi Y;Kawabata T;Shishido T;Takaki K Zhang Q Wang Y Takehira K .[J].Journal of Molecular Catalysis A:Chemical,2005,230:49. |
| [3] | Ye Y N;Yue Y H;Miao C X;Xie Z K Hua W M Gao Z .[J].Green Chemistry,2005,7:524. |
| [4] | 李惠云,乐英红,缪长喜,谢在库,华伟明,高滋.溶胶-凝胶法制备用于CO2气氛下乙苯胶氢反应的高活性Cr2O3-SiO2催化剂[J].催化学报,2006(01):4-6. |
| [5] | Chang J S;Hong D Y;Vislovskiy V P;Park S E .[J].Catalysis Surveys From Asia,2007,11:59. |
| [6] | Reddy B M;Han D S;Jiang N;Park S E .[J].CATALYSIS SURVEYS FROM ASIA,2008,12:56. |
| [7] | 陈树伟,秦张峰,孙爱灵,王建国.助剂Li对CO2气氛下Fe-Li/AC催化剂上乙苯脱氢反应性能的影响[J].催化学报,2009(04):359-364. |
| [8] | 陈桂丽,陈鑫,王新葵,贺民,纪敏,蔡天锡.铁系催化剂上乙苯与CO2氧化脱氢反应[J].催化学报,2009(07):619-623. |
| [9] | Qiao Y Y;Miao C X;Yue Y H;Xie Z K Yang W M Hua W M Gao Z .[J].Microporous and Mesoporous Materials,2009,119:150. |
| [10] | Li Z H;Su K M;Cheng B W;Shen D X Zhou Y .[J].Catalysis Letters,2010,135:135. |
| [11] | Mimura N;Takahara I;Saito M;Hattori T Ohkuma K Ando M .[J].Catalysis Today,1998,45:61. |
| [12] | Liu B S;Rui G;Chang R Z;Au C T .[J].Applied Catalysis A:General,2008,335:88. |
| [13] | Liu B S;Chang R Z;Jiang L;Liu W Au C T .[J].Journal of Physcial Chemistry C,2008,112:15490. |
| [14] | Schmidt-Winkel P Jr;Lukens W W;Yang P;Margolese D I Lettow J S Ying J Y Stucky G D .[J].Chemistry of Materials,2000,12:686. |
| [15] | Ungureanu A;On D T;Dumitriu E;Kaliaguine S .[J].Applied Catalysis A:General,2003,254:203. |
| [16] | Trong-On D.;Ungureanu A.;Kaliaguine S. .TS-1 coated mesocellular titano-silica foams as new catalysts for oxidation of bulky molecules[J].Physical chemistry chemical physics: PCCP,2003(16):3534-3538. |
| [17] | Solsona, B;Nieto, JML;Diaz, U .Siliceous ITQ-6: A new support for vanadia in the oxidative dehydrogenation of propane[J].Microporous and Mesoporous Materials,2006(1/3):339-347. |
| [18] | Chen SW;Qin ZF;Xu XF;Wang JG .Structure and properties of the alumina-supported vanadia catalysts for ethylbenzene dehydrogenation in the presence of carbon dioxide[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2006(2):185-192. |
| [19] | Rao K N;Reddy B M;Abhishek B;Seo Y H Jiang N Z Park S E .[J].Applied Catalysis B:Environmental,2009,91:649. |
| [20] | Sakurai Y;Suzaki T;Nakagawa K;Ikenaga N Aota H Suzuki T .[J].Journal of Catalysis,2002,209:16. |
| [21] | Chang J S;Vislovskiy V P;Park M S;Hong D Y Yoo J S Park S E .[J].Green Chemistry,2003,5:587. |
| [22] | Liu Y M;Feng W L;Li T C;He H Y Dai W L Huang W Cao Y Fan K N .[J].Journal of Catalysis,2006,239:125. |
| [23] | Sugino M;Shimada H;Turuda T;Miura H Ikenaga N Suzuki T .[J].Applied Catalysis A:General,1995,121:125. |
| [24] | Ye X N;Hua W M;Yue Y H;Dai W L Miao C X Xie Z K Gao Z .[J].New Journal of Chemistry,2004,28:373. |
| [25] | Ye X N;Ma N;Hua W M;Yue Y H Miao C X Xie Z K Gao Z .[J].Journal of Molecular Catalysis A:Chemical,2004,217:103. |
| [26] | Badstube T.;Kustrowski P.;Dziembaj R.;Papp H. .Oxidative dehydrogenation of ethylbenzene with carbon dioxide on alkali-promoted Fe active carbon catalysts[J].Catalysis Letters,1998(3/4):169-172. |
| [27] | Park JN.;Chang JS.;Park SE.;Noh J. .Ethylbenzene to styrene in the presence of carbon dioxide over zirconia[J].Catalysis Letters,2000(1/3):75-78. |
| [28] | Mimura N.;Saito M. .Dehydrogenation of ethylbenzene to styrene over Fe2O3/Al2O3 catalysts in the presence of carbon dioxide[J].Catalysis Letters,1999(1):59-62. |
| [29] | Sun A L;Qin Z F;Wang J G .[J].Applied Catalysis A:General,2002,234:179. |
- 下载量()
- 访问量()
- 您的评分：
-
10%
-
20%
-
30%
-
40%
-
50%