对 CO2 气氛下 Fe-Li/AC 催化剂上的乙苯脱氢反应性能进行了详细研究. N2 吸附-脱附、CO2 程序升温脱附和 X 射线衍射表征结果表明, 助剂 Li 不仅增加了催化剂比表面积和活性组分分散性, 而且增强了催化剂碱性和 CO2 吸附能力, 从而提高了 Fe/AC 对乙苯脱氢的催化性能. 助剂 Li 能显著提高 Fe/AC 催化剂的乙苯脱氢活性和 CO2 的促进作用, 抑制催化剂的失活. 在 Fe(3.0)-Li(0.6)/AC 催化剂(Fe 和 Li 的负载量分别为 3.0 和 0.6 mmol/g)上, 550 ℃、接触时间为 3.57 (g·h)/mol 和 CO2/乙苯摩尔比为 20 的条件下, 苯乙烯收率可达 62.9%, 选择性为 96.2%. CO2 气氛下的苯乙烯收率显著高于 N2 气氛下的, 归因于 CO2 能保持催化剂表面铁物种的高价态, 并通过逆水煤气变换反应在线除去脱氢反应生成的氢.
参考文献
| [1] | Lee E H .[J].Catalysis Review,1973,8:285. |
| [2] | Mimura N;Takahara I;Saito M;Hattori T Ohkuma K Ando M .[J].Catalysis Today,1998,45:61. |
| [3] | Sakurai Y;Suzaki T;Nakagawa K;Ikenaga N Aota H Suzuki T .[J].Journal of Catalysis,2002,209:16. |
| [4] | Sakurai Y;Suzaki T;Ikenaga N;Suzuki T .[J].Applied Catalysis A:General,2000,192:281. |
| [5] | 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. |
| [6] | Badstube T;Papp H;Dziembaj R;Kustrowski P .[J].Applied Catalysis A:General,2000,204:153. |
| [7] | Sun A L;Qin Z F;Wang J G .[J].Applied Catalysis A:General,2002,234:179. |
| [8] | Kustrowski P.;Majda D.;Tomaszewska D.;Dziembaj R.;Rafalska-Lasocha A. .Preparation and characterization of new Mg-Al-Fe oxide catalyst precursors for dehydrogenation of ethylbenzene in the presence of carbon dioxide[J].Solid state ionics,2001(Special Issue SI):237-242. |
| [9] | Mimura N;Takahara I;Saito M;Sasaki Y Murata K .[J].Catalysis Letters,2002,78:125. |
| [10] | Carja G.;Nakamura R.;Aida T.;Niiyama H. .Mg-V-Al mixed oxides with mesoporous properties using layered double hydroxides as precursors: catalytic behavior for the process of ethylbenzene dehydrogenation to styrene under a carbon dioxide flow[J].Journal of Catalysis,2003(1):104-110. |
| [11] | 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. |
| [12] | 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. |
| [13] | Chang J S;Vislovskiy V P;Park M S;Hong D Y Yoo J S Park S E .[J].Green Chemistry,2003,5:587. |
| [14] | Park M S;Vislovskiy V P;Chang J S;Shul Y G Yoo J S Park S E .[J].Catalysis Today,2003,87:205. |
| [15] | Saito M;Kimura H;Mimura N;Wu J Murata K .[J].Applied Catalysis A:General,2003,239:71. |
| [16] | Sun A L;Qin Z F;Chen S W;Wang J G .[J].Journal of Molecular Catalysis A:Chemical,2004,210:189. |
| [17] | Sun A L;Qin Z F;Chen S W;Wang J G .[J].Catalysis Today,2004,93-95:273. |
| [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] | Chen S W;Qin Z F;Sun A L;Wang J G .[J].Journal of Natural Gas Chemistry,2006,15:11. |
| [20] | Qin Z F;Liu J G;Sun A L;Wang J G .[J].Industrial and Engineering Chemistry Research,2003,42:1329. |
| [21] | Li H Y;Yue Y H;Miao C X;Xie Z K Hua W M Gao Z .[J].Catalysis Communications,2007,8:1317. |
| [22] | 叶兴南,华伟明,乐英红,缪长喜,谢在库,高滋.CO2气氛下负载型Cr2O3催化剂上乙苯脱氢制苯乙烯反应[J].催化学报,2004(07):581-585. |
| [23] | 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. |
| [24] | 李文英,李晓红,宋瑞伟.钒/钛复合氧化物催化剂用于二氧化碳气氛中乙苯氧化脱氢[J].催化学报,2006(12):1117-1121. |
| [25] | 张维光,葛欣,孙磊,王喜章,沈俭一.乙苯脱氢与逆水煤气变换偶合反应的铁/活性炭催化剂研究[J].催化学报,2000(01):27-30. |
| [26] | 蔡卫权,李会泉,张懿.CO2选择性氧化乙苯制苯乙烯[J].化学进展,2004(03):406-413. |
| [27] | 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. |
上一张
下一张
上一张
下一张
计量
- 下载量()
- 访问量()
文章评分
- 您的评分：
-
10%
-
20%
-
30%
-
40%
-
50%