以碳包铁纳米晶(Fe@C)为载体,采用浸渍法制备了一种磁可分离的Pd/Fe@C催化剂,并运用X射线荧光光谱、透射电镜、X射线衍射和X射线光电了能谱对催化剂进行了表征,结果表明,纳米Pd颗粒的粒径分布在4～10 nm,平均粒径约为7nm,Pd物种以Pd0为主,其Pd 3d5/2结合能为335.6 eV.将该催化剂应用于苯甲醇选择性氧化反应,考察了催化剂用量、溶剂、温度对反应的影响以及催化剂的循环使用性能.结果表明,催化剂可使苯甲醇高选择性生成苯甲醛,在催化剂用量(摩尔分数)为0.5％、乙腈为溶剂、80℃常压O2条件下,苯甲醇的氧化反应效果最佳(苯甲醇转化率为96％,苯甲醛选择性为95％).催化剂易干磁分离和回收,循环使用4次仍保持较佳的催化性能.
参考文献
| [1] | 沈彬,李游,王志飞,何农跃.磁性纳米颗粒负载钯催化剂对Heck反应的催化活性[J].催化学报,2007(06):509-513. |
| [2] | Siamaki, A.R.;Khder, A.E.R.S.;Abdelsayed, V.;El-Shall, M.S.;Gupton, B.F. .Microwave-assisted synthesis of palladium nanoparticles supported on graphene: A highly active and recyclable catalyst for carbon-carbon cross-coupling reactions[J].Journal of Catalysis,2011(1):1-11. |
| [3] | Liu H Z;Jiang T;Han B X;Liang S G Zhou Y X .[J].Science,2009,326:1250. |
| [4] | Kwon M S;Kim N;Park C M;Lee J S Kang K Y Park J .[J].Organic Letters,2005,7:1077. |
| [5] | Hackett S E J;Brydson R M;Gass M H;Harvey I,Newman A D,Wilson K,Lee A F .[J].Angewandte Chemie International Edition,2007,46:8593. |
| [6] | Motokura K;Fujita N;Mori K;Mizugaki T;Ebitani K;Kaneda K .One-pot synthesis of alpha-alkylated nitriles with carbonyl compounds through consecutive aldol reaction/hydrogenation using a hydrotalcite-supported palladium nanoparticle as a multifunctional heterogeneous catalyst[J].Tetrahedron letters: The International Journal for the Rapid Publication of Preliminary Communications in Organic Chemistry,2005(33):5507-5510. |
| [7] | Mori, K;Hara, T;Mizugaki, T;Ebitani, K;Kaneda, K .Hydroxyapatite-supported palladium nanoclusters: A highly active heterogeneous catalyst for selective oxidation of alcohols by use of molecular oxygen[J].Journal of the American Chemical Society,2004(34):10657-10666. |
| [8] | Chert Y T;Guo Z;Chen T;Yang Y H .[J].Journal of Catalysis,2010,275:11. |
| [9] | Karimi B;Abedi S;Clark J H;Budarin V .[J].Angewandte Chemie International Edition,2006,45:4776. |
| [10] | Feng B;Hou Z S;Yang H M;Wang X R Hu Y Li H Qiao Y X Zhao X G Huang Q F .[J].Langmuir,2010,26:2505. |
| [11] | Hou W B;Dehm N A;Scott R W J .[J].Journal of Catalysis,2008,253:22. |
| [12] | 杜建平,宋昌,宋金玲,赵江红,朱珍平.纳米碳材料负载铂催化剂在环己烷脱氢反应中的催化性能研究[J].燃料化学学报,2009(04):468-472. |
| [13] | 黄钟斌,严新焕,江玲超,蒋虹.高效组合型Pd/C催化剂用于Suzuki偶联反应[J].催化学报,2010(01):90-94. |
| [14] | Jiang M.;Liu Y.;Hao GM.;Lin H.;Zhang XG. .Ferromagnetic carbon-coated iron and its compounds nanocrystallite synthesized at high metal to carbon rate and high yield by a modified AC arc method[J].Materials Science & Engineering, B. Solid-State Materials for Advanced Technology,2001(1):66-69. |
| [15] | Tsang S C;Caps V;Paraskevas I;Chadwick D,Thompsett D .[J].Angewandte Chemie International Edition,2004,43:5645. |
| [16] | Teranishi T.;Miyake M. .Size control of palladium nanoparticles and their crystal structures[J].Chemistry of Materials,1998(2):594-600. |
| [17] | 程传煊.表面物理化学[M].北京:科学技术文献出版社,1995:354. |
| [18] | Lee A F;Chang Z;Ellis P;Hackett S F J Wilson K .[J].Journal of Physical Chemistry C,2007,111:18844. |
| [19] | Ferri D;Mondelli C;Krumeich F;Baiker A .[J].Journal of Physical Chemistry B,2006,110:22982. |
| [20] | Borasio M;de la Fuente O R;Rupprechter G;Freund H-J .[J].Journal of Physical Chemistry B,2005,109:17791. |
| [21] | Fu X Y;Wang Y;Wu N Z;Gui L L Tang Y Q .[J].Journal of Colloid and Interface Science,2001,243:326. |
| [22] | Keresszegi C;Ferri D;Mallat T;Baiker A .On the role of CO formation during the aerobic oxidation of alcohols on Pd/Al2O3: an, in situ attenuated total reflection infrared study[J].Journal of Catalysis,2005(1):64-75. |
| [23] | Meier D M;Urakawa A;Baiker A .[J].Journal of Physical Chemistry C,2009,113:21849. |
| [24] | Mallat T;Baiker A .[J].Chemical Reviews,2004,104:3037. |
| [25] | Mondelli C;Ferri D;Grunwaldt J-D;Krumeich F Mangold S Psaro R Baiker A .[J].Journal of Catalysis,2007,252:77. |
| [26] | Steinhoff B A;Stahl S S .[J].Journal of the American Chemical Society,2006,128:4348. |
| [27] | 刘成,谭蓉,银董红,喻宁亚,周裕旭.Pd/PMO-SBA-15催化剂催化苯甲醇选择氧化反应性能[J].催化学报,2010(11):1369-1373. |
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%