以含巯基官能团有机硅烷修饰的介孔材料MCM-41和SBA-15为载体,采用浸渍-氢气还原法制备了高分散和高活性的负载型Pd催化剂.X射线衍射、N2吸附-脱附和透射电子显微镜表征结果显示,所制Pd催化剂Pd-SH-MCM-41和Pd-SH-SBA-15具有很好的长程有序结构、分布均匀的孔径、高比表面积及高度分散的Pd颗粒.苯酚加氢反应结果表明,以Pd-SH-MCM-41和Pd-SH-SBA-15为催化剂时,在80℃,1.0 MPa反应1h,苯酚转化率达99％以上,环己酮选择性为98％.它们的催化活性为商业Pd/C催化剂的5倍,Pd/MCM-41和Pd/SBA-15催化剂的3倍.这可归因于介孔材料表面修饰的巯基官能团对Pd的锚定作用,避免了Pd颗粒的团聚,使其高度分散在介孔材料上.
参考文献
| [1] | Coti K K;Belowich M E;Liong M;Ambrogio M W Lau Y A Khatib H A Zink J I Khashab N M Stoddart J F .[J].Nanoscale,2009,1:16. |
| [2] | Rosenholm J M;Sahlgren C;Linden M .[J].Nanoscale,2010,2:1870. |
| [3] | Dodgson I;Griffin K;Barberis G;Pignataro F Tauszik G .[J].Chemistry and Industry,1989,11:830. |
| [4] | Xiang Y Z;Ma L;Lu C S;Zhang Q F Li X N .[J].Green Chemistry,2008,10:939. |
| [5] | Li H;Liu J;Xie S H;Qiao M H Dai W L Lu Y F Li H X .[J].Advanced Functional Materials,2008,18:3235. |
| [6] | Li H;Liu J L;Li H X .[J].Materials Letters,2008,62:297. |
| [7] | Shore S G;Ding E;Park C;Keane M A .[J].Catalysis Communications,2002,3:77. |
| [8] | Sikhwivhilu L M;Coville N J;Naresh D;Chary K V R Vishwanathan V .[J].Applied Catalysis A:General,2007,324:52. |
| [9] | Wang, Y.;Yao, J.;Li, H.;Su, D.;Antonietti, M. .Highly selective hydrogenation of phenol and derivatives over a pd@carbon nitride catalyst in aqueous media[J].Journal of the American Chemical Society,2011(8):2362-2365. |
| [10] | Mahata N.;Vishwanathan V.;Park C.;Keane MA.;Raghavan KV. .Phenol hydrogenation over palladium supported on magnesia: Relationship between catalyst structure and performance[J].Physical chemistry chemical physics: PCCP,2001(13):2712-2719. |
| [11] | Chatterjee M;Kawanami H;Sato M;Chatterjee A Yokoyama T Suzuki T .[J].Advanced Synthesis and Catalysis,2009,351:1912. |
| [12] | Fujita S;Yamada T;Akiyama Y;Cheng H Y Zhao F Y Arai M .[J].Journal of Supercritical Fluids,2010,54:190. |
| [13] | Liu H Z;Jiang T;Han B X;Liang S G Zhou Y X .[J].Science,2009,326:1250. |
| [14] | Yang X;Du L;Liao S J;Li Y X Song H Y .[J].Catalysis Communications,2012,17:29. |
| [15] | Du L;Liao S J;Liu Q B;Yang X Song H Y Fu Z Y Ji S .[J].International Journal of Hydrogen Energy,2009,34:3810. |
| [16] | Kruk M.;Jaroniec M. .Argon adsorption at 77 K as a useful tool for the elucidation of pore connectivity in ordered materials with large cagelike mesopores[J].Chemistry of Materials,2003(15):2942-2949. |
| [17] | 王鹏;白诗扬;李博;杨启华 .[J].催化学报,2012,33:1689. |
| [18] | 宋明娟,邹成龙,牛国兴,赵东元.（NH4）2SiF6预处理改善SBA-15介孔材料的水热稳定性[J].催化学报,2012(01):140-151. |
| [19] | Li, YJ;Zhou, GW;Li, CJ;Qin, DW;Qiao, WT;Chu, B .Adsorption and catalytic activity of Porcine pancreatic lipase on rod-like SBA-15 mesoporous material[J].Colloids and Surfaces, A. Physicochemical and Engineering Aspects,2009(1/3):79-85. |
| [20] | 唐苏苏,胡燚,余定华,邹彬,江凌.功能化离子液体修饰的 SBA-15固定化 Burkholderia cepacia 脂肪酶[J].催化学报,2012(09):1565-1571. |
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%